Characterization of ice nucleating particles during continuous springtime measurements in Prudhoe Bay: an Arctic oilfield location

NASA Astrophysics Data System (ADS)

Creamean, J.; Spada, N. J.; Kirpes, R.; Pratt, K.

2017-12-01

Aerosols that serve as ice nucleating particles (INPs) have the potential to modulate cloud microphysical properties. INPs can thus subsequently impact cloud radiative forcing in addition to modification of precipitation formation processes. In regions such as the Arctic, aerosol-cloud interactions are severely understudied yet have significant implications for surface radiation reaching the sea ice and snow surfaces. Further, uncertainties in model representations of heterogeneous ice nucleation are a significant hindrance to simulating Arctic mixed-phase cloud processes. Characterizing a combination of aerosol chemical, physical, and ice nucleating properties is pertinent to evaluating of the role of aerosols in altering Arctic cloud microphysics. We present preliminary results from an aerosol sampling campaign called INPOP (Ice Nucleating Particles at Oliktok Point), which took place at a U.S. Department of Energy's Atmospheric Radiation Measurement (DOE ARM) facility on the North Slope of Alaska. Three time- and size-resolved aerosol samplers were deployed from 1 Mar to 31 May 2017 and were co-located with routine measurements of aerosol number, size, chemical, and radiative property measurements conducted by DOE ARM at their Aerosol Observing System (AOS). Offline analysis of samples collected at a daily time resolution included composition and morphology via single-particle analysis and drop freezing measurements for INP concentrations, while analysis of 12-hourly samples included mass, optical, and elemental composition. We deliberate the possible influences on the aerosol and INP population from the Prudhoe Bay oilfield resource extraction and daily operations in addition to what may be local background or long-range transported aerosol. To our knowledge our results represent some of the first INP characterization measurements in an Arctic oilfield location and can be used as a benchmark for future INP characterization studies in Arctic locations impacted by local resource extraction pollution. Ultimately, these results can be used to evaluate the impacts of oil exploration activities on Arctic cloud aerosol composition and possible linkages to Arctic cloud ice formation.

Laboratory, Computational and Theoretical Investigations of Ice Nucleation and its Implications for Mixed Phase Clouds

NASA Astrophysics Data System (ADS)

Yang, Fan

Ice particles in atmospheric clouds play an important role in determining cloud lifetime, precipitation and radiation. It is therefore important to understand the whole life cycle of ice particles in the atmosphere, e.g., where they come from (nucleation), how they evolve (growth), and where they go (precipitation). Ice nucleation is the crucial step for ice formation, and in this study, we will mainly focus on ice nucleation in the lab and its effect on mixed-phase stratiform clouds. In the first half of this study, we investigate the relevance of moving contact lines (i.e., the region where three or more phases meet) on the phenomenon of contact nucleation. High speed video is used to investigate heterogeneous ice nucleation in supercooled droplets resting on cold substrates under two different dynamic conditions: droplet electrowetting and droplet vibration. The results show that contact-line motion is not a sufficient condition to trigger ice nucleation, while locally curved contact lines that can result from contact-line motion are strongly related to ice nucleation. We propose that pressure perturbations due to locally curved contact lines can strongly enhance the ice nucleation rate, which gives another interpretation for the mechanism for contact nucleation. Corresponding theoretical results provide a quantitative connection between pressure perturbations and temperature, providing a useful tool for ice nucleation calculations in atmospheric models. In this second half of the study, we build a minimalist model for long lifetime mixed-phase stratiform clouds based on stochastic ice nucleation. Our result shows that there is a non-linear relationship between ice water contact and ice number concentration in the mixed-phase cloud, as long as the volume ice nucleation rate is constant. This statistical property may help identify the source of ice nuclei in mixed-phase clouds. In addition, results from Lagrangian ice particle tracking in time dependent fields show that long lifetime ice particles exist in mixed-phase stratiform clouds. We find that small ice particle can be trapped in eddy-like structures. Whether ice particles grow or sublimate depends on the thermodynamic field in the trapping region. This dynamic-thermodynamic coupling effect on the lifetime of ice particles might explain the fast phase-partition change observed in the mixed phase cloud.

The enhancement and suppression of immersion mode heterogeneous ice-nucleation by solutes.

PubMed

Whale, Thomas F; Holden, Mark A; Wilson, Theodore W; O'Sullivan, Daniel; Murray, Benjamin J

2018-05-07

Heterogeneous nucleation of ice from aqueous solutions is an important yet poorly understood process in multiple fields, not least the atmospheric sciences where it impacts the formation and properties of clouds. In the atmosphere ice-nucleating particles are usually, if not always, mixed with soluble material. However, the impact of this soluble material on ice nucleation is poorly understood. In the atmospheric community the current paradigm for freezing under mixed phase cloud conditions is that dilute solutions will not influence heterogeneous freezing. By testing combinations of nucleators and solute molecules we have demonstrated that 0.015 M solutions (predicted melting point depression <0.1 °C) of several ammonium salts can cause suspended particles of feldspars and quartz to nucleate ice up to around 3 °C warmer than they do in pure water. In contrast, dilute solutions of certain alkali metal halides can dramatically depress freezing points for the same nucleators. At 0.015 M, solutes can enhance or deactivate the ice-nucleating ability of a microcline feldspar across a range of more than 10 °C, which corresponds to a change in active site density of more than a factor of 10 5 . This concentration was chosen for a survey across multiple solutes-nucleant combinations since it had a minimal colligative impact on freezing and is relevant for activating cloud droplets. Other nucleators, for instance a silica gel, are unaffected by these 'solute effects', to within experimental uncertainty. This split in response to the presence of solutes indicates that different mechanisms of ice nucleation occur on the different nucleators or that surface modification of relevance to ice nucleation proceeds in different ways for different nucleators. These solute effects on immersion mode ice nucleation may be of importance in the atmosphere as sea salt and ammonium sulphate are common cloud condensation nuclei (CCN) for cloud droplets and are internally mixed with ice-nucleating particles in mixed-phase clouds. In addition, we propose a pathway dependence where activation of CCN at low temperatures might lead to enhanced ice formation relative to pathways where CCN activation occurs at higher temperatures prior to cooling to nucleation temperature.

The enhancement and suppression of immersion mode heterogeneous ice-nucleation by solutes

PubMed Central

Holden, Mark A.; Wilson, Theodore W.; O'Sullivan, Daniel; Murray, Benjamin J.

2018-01-01

Heterogeneous nucleation of ice from aqueous solutions is an important yet poorly understood process in multiple fields, not least the atmospheric sciences where it impacts the formation and properties of clouds. In the atmosphere ice-nucleating particles are usually, if not always, mixed with soluble material. However, the impact of this soluble material on ice nucleation is poorly understood. In the atmospheric community the current paradigm for freezing under mixed phase cloud conditions is that dilute solutions will not influence heterogeneous freezing. By testing combinations of nucleators and solute molecules we have demonstrated that 0.015 M solutions (predicted melting point depression <0.1 °C) of several ammonium salts can cause suspended particles of feldspars and quartz to nucleate ice up to around 3 °C warmer than they do in pure water. In contrast, dilute solutions of certain alkali metal halides can dramatically depress freezing points for the same nucleators. At 0.015 M, solutes can enhance or deactivate the ice-nucleating ability of a microcline feldspar across a range of more than 10 °C, which corresponds to a change in active site density of more than a factor of 105. This concentration was chosen for a survey across multiple solutes–nucleant combinations since it had a minimal colligative impact on freezing and is relevant for activating cloud droplets. Other nucleators, for instance a silica gel, are unaffected by these ‘solute effects’, to within experimental uncertainty. This split in response to the presence of solutes indicates that different mechanisms of ice nucleation occur on the different nucleators or that surface modification of relevance to ice nucleation proceeds in different ways for different nucleators. These solute effects on immersion mode ice nucleation may be of importance in the atmosphere as sea salt and ammonium sulphate are common cloud condensation nuclei (CCN) for cloud droplets and are internally mixed with ice-nucleating particles in mixed-phase clouds. In addition, we propose a pathway dependence where activation of CCN at low temperatures might lead to enhanced ice formation relative to pathways where CCN activation occurs at higher temperatures prior to cooling to nucleation temperature. PMID:29780544

A detailed study of ice nucleation by feldspar minerals

NASA Astrophysics Data System (ADS)

Whale, T. F.; Murray, B. J.; Wilson, T. W.; Carpenter, M. A.; Harrison, A.; Holden, M. A.; Vergara Temprado, J.; Morris, J.; O'Sullivan, D.

2015-12-01

Immersion mode heterogeneous ice nucleation plays a crucial role in controlling the composition of mixed phase clouds, which contain both supercooled liquid water and ice particles. The amount of ice in mixed phase clouds can affect cloud particle size, lifetime and extent and so affects radiative properties and precipitation. Feldspar minerals are probably the most important minerals for ice nucleation in mixed phase clouds because they nucleate ice more efficiently than other components of atmospheric mineral dust (Atkinson et al. 2013). The feldspar class of minerals is complex, containing numerous chemical compositions, several crystal polymorphs and wide variations in microscopic structure. Here we present the results of a study into ice nucleation by a wide range of different feldspars. We found that, in general, alkali feldspars nucleate ice more efficiently than plagioclase feldspars. However, we also found that particular alkali feldspars nucleate ice relatively inefficiently, suggesting that chemical composition is not the only important factor that dictates the ice nucleation efficiency of feldspar minerals. Ice nucleation by feldspar is described well by the singular model and is probably site specific in nature. The alkali feldspars that do not nucleate ice efficiently possess relatively homogenous structure on the micrometre scale suggesting that the important sites for nucleation are related to surface topography. Ice nucleation active site densities for the majority of tested alkali feldspars are similar to those found by Atkinson et al (2013), meaning that the validity of global aerosol modelling conducted in that study is not affected. Additionally, we have found that ice nucleation by feldspars is strongly influenced, both positively and negatively, by the solute content of droplets. Most other nucleants we have tested are unaffected by solutes. This provides insight into the mechanism of ice nucleation by feldspars and could be of importance when modelling ice nucleation in mixed phase clouds. Atkinson, J. D., Murray, B. J., Woodhouse, M. T., Carslaw, K. S., Whale, T. F., Baustian, K. J., Dobbie, S., O'Sullivan, D., and Malkin, T. L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds, Nature, 10.1038/nature12278, (2013).

The effect of mineral dust and soot aerosols on ice microphysics near the foothills of the Himalayas: A numerical investigation

NASA Astrophysics Data System (ADS)

Hazra, Anupam; Padmakumari, B.; Maheskumar, R. S.; Chen, Jen-Ping

2016-05-01

This study investigates the influence of different ice nuclei (IN) species and their number concentrations on cloud ice production. The numerical simulation with different species of ice nuclei is investigated using an explicit bulk-water microphysical scheme in a Mesoscale Meteorological Model version 5 (MM5). The species dependent ice nucleation parameterization that is based on the classical nucleation theory has been implemented into the model. The IN species considered include dust and soot with two different concentrations (Low and High). The simulated cloud microphysical properties like droplet number concentration and droplet effective radii as well as macro-properties (equivalent potential temperature and relative humidity) are comparable with aircraft observations. When higher dust IN concentrations are considered, the simulation results showed good agreement with the cloud ice and cloud water mixing ratio from aircraft measurements during Cloud Aerosol Interactions and Precipitation Enhancement Experiment (CAIPEEX) and Modern Era Retrospective Analysis for Research and Applications (MERRA) reanalysis. Relative importance of IN species is shown as compared to the homogeneous freezing nucleation process. The tendency of cloud ice production rates is also analyzed and found that dust IN is more efficient in producing cloud ice when compared to soot IN. The dust IN with high concentration can produce more surface precipitation than soot IN at the same concentration. This study highlights the need to improve the ice nucleation parameterization in numerical models.

Microphysical Consequences of the Spatial Distribution of Ice Nucleation in Mixed-Phase Stratiform Clouds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Fan; Ovchinnikov, Mikhail; Shaw, Raymond A.

Mixed-phase stratiform clouds can persist even with steady ice precipitation fluxes, and the origin and microphysical properties of the ice crystals are of interest. Vapor deposition growth and sedimentation of ice particles along with a uniform volume source of ice nucleation, leads to a power law relation between ice water content wi and ice number concentration ni with exponent 2.5. The result is independent of assumptions about the vertical velocity structure of the cloud and is therefore more general than the related expression of Yang et al. [2013]. The sensitivity of the wi-ni relationship to the spatial distribution of icemore » nucleation is confirmed by Lagrangian tracking and ice growth with cloud-volume, cloud-top, and cloud-base sources of ice particles through a time-dependent cloud field. Based on observed wi and ni from ISDAC, a lower bound of 0.006 m^3/s is obtained for the ice crystal formation rate.« less

Minimalist model of ice microphysics in mixed-phase stratiform clouds

NASA Astrophysics Data System (ADS)

Yang, Fan; Ovchinnikov, Mikhail; Shaw, Raymond A.

2013-07-01

The question of whether persistent ice crystal precipitation from supercooled layer clouds can be explained by time-dependent, stochastic ice nucleation is explored using an approximate, analytical model and a large-eddy simulation (LES) cloud model. The updraft velocity in the cloud defines an accumulation zone, where small ice particles cannot fall out until they are large enough, which will increase the residence time of ice particles in the cloud. Ice particles reach a quasi-steady state between growth by vapor deposition and fall speed at cloud base. The analytical model predicts that ice water content (wi) has a 2.5 power-law relationship with ice number concentration (ni). wi and ni from a LES cloud model with stochastic ice nucleation confirm the 2.5 power-law relationship, and initial indications of the scaling law are observed in data from the Indirect and Semi-Direct Aerosol Campaign. The prefactor of the power law is proportional to the ice nucleation rate and therefore provides a quantitative link to observations of ice microphysical properties.

Minimalist Model of Ice Microphysics in Mixed-phase Stratiform Clouds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, F.; Ovchinnikov, Mikhail; Shaw, Raymond A.

The question of whether persistent ice crystal precipitation from super cooled layer clouds can be explained by time-dependent, stochastic ice nucleation is explored using an approximate, analytical model, and a large-eddy simulation (LES) cloud model. The updraft velocity in the cloud defines an accumulation zone, where small ice particles cannot fall out until they are large enough, which will increase the residence time of ice particles in the cloud. Ice particles reach a quasi-steady state between growth by vapor deposition and fall speed at cloud base. The analytical model predicts that ice water content (wi) has a 2.5 power lawmore » relationship with ice number concentration ni. wi and ni from a LES cloud model with stochastic ice nucleation also confirm the 2.5 power law relationship. The prefactor of the power law is proportional to the ice nucleation rate, and therefore provides a quantitative link to observations of ice microphysical properties.« less

Importance of Chemical Composition of Ice Nuclei on the Formation of Arctic Ice Clouds

NASA Astrophysics Data System (ADS)

Keita, Setigui Aboubacar; Girard, Eric

2016-09-01

Ice clouds play an important role in the Arctic weather and climate system but interactions between aerosols, clouds and radiation remain poorly understood. Consequently, it is essential to fully understand their properties and especially their formation process. Extensive measurements from ground-based sites and satellite remote sensing reveal the existence of two Types of Ice Clouds (TICs) in the Arctic during the polar night and early spring. TICs-1 are composed by non-precipitating small (radar-unseen) ice crystals of less than 30 μm in diameter. The second type, TICs-2, are detected by radar and are characterized by a low concentration of large precipitating ice crystals ice crystals (>30 μm). To explain these differences, we hypothesized that TIC-2 formation is linked to the acidification of aerosols, which inhibits the ice nucleating properties of ice nuclei (IN). As a result, the IN concentration is reduced in these regions, resulting to a lower concentration of larger ice crystals. Water vapor available for deposition being the same, these crystals reach a larger size. Current weather and climate models cannot simulate these different types of ice clouds. This problem is partly due to the parameterizations implemented for ice nucleation. Over the past 10 years, several parameterizations of homogeneous and heterogeneous ice nucleation on IN of different chemical compositions have been developed. These parameterizations are based on two approaches: stochastic (that is nucleation is a probabilistic process, which is time dependent) and singular (that is nucleation occurs at fixed conditions of temperature and humidity and time-independent). The best approach remains unclear. This research aims to better understand the formation process of Arctic TICs using recently developed ice nucleation parameterizations. For this purpose, we have implemented these ice nucleation parameterizations into the Limited Area version of the Global Multiscale Environmental Model (GEM-LAM) and use them to simulate ice clouds observed during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) in Alaska. Simulation results of the TICs-2 observed on April 15th and 25th (acidic cases) and TICs-1 observed on April 5th (non-acidic cases) are presented. Our results show that the stochastic approach based on the classical nucleation theory with the appropriate contact angle is better. Parameterizations of ice nucleation based on the singular approach tend to overestimate the ice crystal concentration in TICs-1 and TICs-2. The classical nucleation theory using the appropriate contact angle is the best approach to use to simulate the ice clouds investigated in this research.

Sensitivity Studies of Dust Ice Nuclei Effect on Cirrus Clouds with the Community Atmosphere Model CAM5

NASA Technical Reports Server (NTRS)

Liu, Xiaohong; Zhang, Kai; Jensen, Eric J.; Gettelman, Andrew; Barahona, Donifan; Nenes, Athanasios; Lawson, Paul

2012-01-01

In this study the effect of dust aerosol on upper tropospheric cirrus clouds through heterogeneous ice nucleation is investigated in the Community Atmospheric Model version 5 (CAM5) with two ice nucleation parameterizations. Both parameterizations consider homogeneous and heterogeneous nucleation and the competition between the two mechanisms in cirrus clouds, but differ significantly in the number concentration of heterogeneous ice nuclei (IN) from dust. Heterogeneous nucleation on dust aerosol reduces the occurrence frequency of homogeneous nucleation and thus the ice crystal number concentration in the Northern Hemisphere (NH) cirrus clouds compared to simulations with pure homogeneous nucleation. Global and annual mean shortwave and longwave cloud forcing are reduced by up to 2.0+/-0.1Wm (sup-2) (1 uncertainty) and 2.4+/-0.1Wm (sup-2), respectively due to the presence of dust IN, with the net cloud forcing change of -0.40+/-0.20W m(sup-2). Comparison of model simulations with in situ aircraft data obtained in NH mid-latitudes suggests that homogeneous ice nucleation may play an important role in the ice nucleation at these regions with temperatures of 205-230 K. However, simulations overestimate observed ice crystal number concentrations in the tropical tropopause regions with temperatures of 190- 205 K, and overestimate the frequency of occurrence of high ice crystal number concentration (greater than 200 L(sup-1) and underestimate the frequency of low ice crystal number concentration (less than 30 L(sup-1) at NH mid-latitudes. These results highlight the importance of quantifying the number concentrations and properties of heterogeneous IN (including dust aerosol) in the upper troposphere from the global perspective.

Contributions of Heterogeneous Ice Nucleation, Large-Scale Circulation, and Shallow Cumulus Detrainment to Cloud Phase Transition in Mixed-Phase Clouds with NCAR CAM5

NASA Astrophysics Data System (ADS)

Liu, X.; Wang, Y.; Zhang, D.; Wang, Z.

2016-12-01

Mixed-phase clouds consisting of both liquid and ice water occur frequently at high-latitudes and in mid-latitude storm track regions. This type of clouds has been shown to play a critical role in the surface energy balance, surface air temperature, and sea ice melting in the Arctic. Cloud phase partitioning between liquid and ice water determines the cloud optical depth of mixed-phase clouds because of distinct optical properties of liquid and ice hydrometeors. The representation and simulation of cloud phase partitioning in state-of-the-art global climate models (GCMs) are associated with large biases. In this study, the cloud phase partition in mixed-phase clouds simulated from the NCAR Community Atmosphere Model version 5 (CAM5) is evaluated against satellite observations. Observation-based supercooled liquid fraction (SLF) is calculated from CloudSat, MODIS and CPR radar detected liquid and ice water paths for clouds with cloud-top temperatures between -40 and 0°C. Sensitivity tests with CAM5 are conducted for different heterogeneous ice nucleation parameterizations with respect to aerosol influence (Wang et al., 2014), different phase transition temperatures for detrained cloud water from shallow convection (Kay et al., 2016), and different CAM5 model configurations (free-run versus nudged winds and temperature, Zhang et al., 2015). A classical nucleation theory-based ice nucleation parameterization in mixed-phase clouds increases the SLF especially at temperatures colder than -20°C, and significantly improves the model agreement with observations in the Arctic. The change of transition temperature for detrained cloud water increases the SLF at higher temperatures and improves the SLF mostly over the Southern Ocean. Even with the improved SLF from the ice nucleation and shallow cumulus detrainment, the low SLF biases in some regions can only be improved through the improved circulation with the nudging technique. Our study highlights the challenges of representations of large-scale moisture transport, cloud microphysics, ice nucleation, and cumulus detrainment in order to improve the mixed-phase transition in GCMs.

On the Ice Nucleation Spectrum

NASA Technical Reports Server (NTRS)

Barahona, D.

2012-01-01

This work presents a novel formulation of the ice nucleation spectrum, i.e. the function relating the ice crystal concentration to cloud formation conditions and aerosol properties. The new formulation is physically-based and explicitly accounts for the dependency of the ice crystal concentration on temperature, supersaturation, cooling rate, and particle size, surface area and composition. This is achieved by introducing the concepts of ice nucleation coefficient (the number of ice germs present in a particle) and nucleation probability dispersion function (the distribution of ice nucleation coefficients within the aerosol population). The new formulation is used to generate ice nucleation parameterizations for the homogeneous freezing of cloud droplets and the heterogeneous deposition ice nucleation on dust and soot ice nuclei. For homogeneous freezing, it was found that by increasing the dispersion in the droplet volume distribution the fraction of supercooled droplets in the population increases. For heterogeneous ice nucleation the new formulation consistently describes singular and stochastic behavior within a single framework. Using a fundamentally stochastic approach, both cooling rate independence and constancy of the ice nucleation fraction over time, features typically associated with singular behavior, were reproduced. Analysis of the temporal dependency of the ice nucleation spectrum suggested that experimental methods that measure the ice nucleation fraction over few seconds would tend to underestimate the ice nuclei concentration. It is shown that inferring the aerosol heterogeneous ice nucleation properties from measurements of the onset supersaturation and temperature may carry significant error as the variability in ice nucleation properties within the aerosol population is not accounted for. This work provides a simple and rigorous ice nucleation framework where theoretical predictions, laboratory measurements and field campaign data can be reconciled, and that is suitable for application in atmospheric modeling studies.

Minimalist model of ice microphysics in mixed-phase stratiform clouds

NASA Astrophysics Data System (ADS)

Yang, F.; Ovchinnikov, M.; Shaw, R. A.

2013-12-01

The question of whether persistent ice crystal precipitation from supercooled layer clouds can be explained by time-dependent, stochastic ice nucleation is explored using an approximate, analytical model and a large-eddy simulation (LES) cloud model. The updraft velocity in the cloud defines an accumulation zone, where small ice particles cannot fall out until they are large enough, which will increase the residence time of ice particles in the cloud. Ice particles reach a quasi-steady state between growth by vapor deposition and fall speed at cloud base. The analytical model predicts that ice water content (wi) has a 2.5 power-law relationship with ice number concentration (ni). wi and ni from a LES cloud model with stochastic ice nucleation confirm the 2.5 power-law relationship, and initial indications of the scaling law are observed in data from the Indirect and Semi-Direct Aerosol Campaign. The prefactor of the power law is proportional to the ice nucleation rate and therefore provides a quantitative link to observations of ice microphysical properties. Ice water content (wi) and ice number concentration (ni) relationship from LES. a and c: Accumulation zone region; b and d: Selective accumulation zone region. Black lines in c and d are best fitted 2.5 slope lines. Colors in Figures a and b represent updraft velocity, while colors in c and d represent altitude. The cloud base and top are at about 600 m and 800 m, respectively. Ice water content (wi) and ice number concentration (ni) relationship for two ice nucleation rates. Blue points are from LES with low ice nucleation rate and red points with high ice nucleation rate. Solid and dashed lines are best fitted 2.5 slope lines.

Evaluating aerosol influence on cloud models using in-situ measurements during the INUPIAQ campaign

NASA Astrophysics Data System (ADS)

Farrington, R.; Connolly, P.; Choularton, T.; Bower, K.; Lloyd, G.; Flynn, M.; Crosier, J.; Field, P.

2014-12-01

At temperatures between -35°C and 0°C, the presence of insoluble aerosols acting as ice nuclei (IN) initiate the nucleation of ice under atmospheric conditions. Previous field and laboratory campaigns have suggested that mineral dust present in the atmosphere act as IN at temperatures around -20°C (e.g. Sassen et al. 2003), however the cause of ice nucleation at temperatures of around -5°C is less certain. Coupled with the limited representation of aerosol and cloud processes in large-scale weather and climate models, the need for improved in-situ measurements of aerosol properties and cloud micro-physical processes to drive the improvement of aerosol-clouds processes in models is evident. As part of the Ice NUcleation Process Investigation and Quantification (INUPIAQ) project, two field campaigns were conducted in early 2013 and early 2014. Both campaigns included measurements of cloud micro-physical properties at the summit of Jungfraujoch in Switzerland (3580m asl). Using data from the 2013 campaign and modelling simulations from the Weather Research and Forecasting model (WRF), an upwind site, located at Schilthorn (2970m asl), was determined for measuring aerosol properties out of cloud during the 2014 campaign. Further measurements of the cloud and aerosols properties were taken remotely using a doppler LiDAR located at Kleine Scheidegg (2061m asl). The aim of this project is to determine whether detailed aerosol information is important to determining cloud and precipitation properties downwind. To this end WRF was run using the aerosol number concentrations and size distributions measured at the Schilthorn site to compare modelled ice number concentrations with measurements taken at Jungfraujoch using state of the science cloud ice probes, including the Three-View Cloud Particle Imager (3V-CPI) and the Cloud Aerosol Spectrometer with Depolarization (CAS-DPOL), with the results of the comparison presented and discussed at this meeting. ReferencesSassen, K., et al, 2003: Saharan dust storms and indirect aerosol effects on clouds: Crystal-face results. Geophys. Res. Lett., 30(12), 1633-1636.

A Hierarchical Modeling Study of the Interactions Among Turbulence, Cloud Microphysics, and Radiative Transfer in the Evolution of Cirrus Clouds

NASA Technical Reports Server (NTRS)

Curry, Judith; Khvorostyanov, V. I.

2005-01-01

This project used a hierarchy of cloud resolving models to address the following science issues of relevance to CRYSTAL-FACE: What ice crystal nucleation mechanisms are active in the different types of cirrus clouds in the Florida area and how do these different nucleation processes influence the evolution of the cloud system and the upper tropospheric humidity? How does the feedback between supersaturation and nucleation impact the evolution of the cloud? What is the relative importance of the large-scale vertical motion and the turbulent motions in the evolution of the crystal size spectra? How does the size spectra impact the life-cycle of the cloud, stratospheric dehydration, and cloud radiative forcing? What is the nature of the turbulence and waves in the upper troposphere generated by precipitating deep convective cloud systems? How do cirrus microphysical and optical properties vary with the small-scale dynamics? How do turbulence and waves in the upper troposphere influence the cross-tropopause mixing and stratospheric and upper tropospheric humidity? The models used in this study were: 2-D hydrostatic model with explicit microphysics that can account for 30 size bins for both the droplet and crystal size spectra. Notably, a new ice crystal nucleation scheme has been incorporated into the model. Parcel model with explicit microphysics, for developing and evaluating microphysical parameterizations. Single column model for testing bulk microphysics parameterizations

Ice nucleation by particles immersed in supercooled cloud droplets.

PubMed

Murray, B J; O'Sullivan, D; Atkinson, J D; Webb, M E

2012-10-07

The formation of ice particles in the Earth's atmosphere strongly affects the properties of clouds and their impact on climate. Despite the importance of ice formation in determining the properties of clouds, the Intergovernmental Panel on Climate Change (IPCC, 2007) was unable to assess the impact of atmospheric ice formation in their most recent report because our basic knowledge is insufficient. Part of the problem is the paucity of quantitative information on the ability of various atmospheric aerosol species to initiate ice formation. Here we review and assess the existing quantitative knowledge of ice nucleation by particles immersed within supercooled water droplets. We introduce aerosol species which have been identified in the past as potentially important ice nuclei and address their ice-nucleating ability when immersed in a supercooled droplet. We focus on mineral dusts, biological species (pollen, bacteria, fungal spores and plankton), carbonaceous combustion products and volcanic ash. In order to make a quantitative comparison we first introduce several ways of describing ice nucleation and then summarise the existing information according to the time-independent (singular) approximation. Using this approximation in combination with typical atmospheric loadings, we estimate the importance of ice nucleation by different aerosol types. According to these estimates we find that ice nucleation below about -15 °C is dominated by soot and mineral dusts. Above this temperature the only materials known to nucleate ice are biological, with quantitative data for other materials absent from the literature. We conclude with a summary of the challenges our community faces.

Cirrus Parcel Model Comparison Project. Phase 1: The Critical Components to Simulate Cirrus Initiation Explicitly.

NASA Astrophysics Data System (ADS)

Lin, Ruei-Fong; O'C. Starr, David; Demott, Paul J.; Cotton, Richard; Sassen, Kenneth; Jensen, Eric; Kärcher, Bernd; Liu, Xiaohong

2002-08-01

The Cirrus Parcel Model Comparison Project, a project of the GCSS [Global Energy and Water Cycle Experiment (GEWEX) Cloud System Studies] Working Group on Cirrus Cloud Systems, involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. In Phase 1 of the project reported here, simulated cirrus cloud microphysical properties from seven models are compared for `warm' (40°C) and `cold' (60°C) cirrus, each subject to updrafts of 0.04, 0.2, and 1 m s1. The models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins or the evolution of each individual particle is traced. Simulations are made including both homogeneous and heterogeneous ice nucleation mechanisms (all-mode simulations). A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. Heterogeneous nucleation is disabled for a second parallel set of simulations in order to isolate the treatment of the homogeneous freezing (of haze droplets) nucleation process. Analysis of these latter simulations is the primary focus of this paper.Qualitative agreement is found for the homogeneous-nucleation-only simulations; for example, the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, significant quantitative differences are found. Detailed analysis reveals that the homogeneous nucleation rate, haze particle solution concentration, and water vapor uptake rate by ice crystal growth (particularly as controlled by the deposition coefficient) are critical components that lead to differences in the predicted microphysics.Systematic differences exist between results based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each method is constrained by critical freezing data from laboratory studies, but each includes assumptions that can only be justified by further laboratory research. Consequently, it is not yet clear if the two approaches can be made consistent. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (0.2-1 m s1) at 60°C. The equilibrium assumption is commonly invoked in cirrus parcel models. The resulting difference in particle-size-dependent solution concentration of haze particles may significantly affect the ice particle formation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of particle number concentration and ice crystal diffusional growth rate, which is particularly sensitive to the deposition coefficient when ice particles are small, modulates the peak particle formation rate achieved in an air parcel and the duration of the active nucleation time period. The consequent differences in cloud microphysical properties, and thus cloud optical properties, between state-of-the-art models of ice crystal initiation are significant.Intermodel differences in the case of all-mode simulations are correspondingly greater than in the case of homogeneous nucleation acting alone. Definitive laboratory and atmospheric benchmark data are needed to improve the treatment of heterogeneous nucleation processes.

Investigating the differences of cirrus cloud properties in nucleation, growth and sublimation regions based on airborne water vapor lidar measurements

NASA Astrophysics Data System (ADS)

Urbanek, Benedikt; Groß, Silke; Wirth, Martin

2017-04-01

Cirrus clouds impose high uncertainties on weather and climate prediction, as knowledge on important processes is still incomplete. For instance it remains unclear how cloud optical, microphysical, and radiative properties change as the cirrus evolves. To gain better understanding of cirrus clouds, their optical and microphysical properties and their changes with cirrus cloud evolution the ML-CIRRUS campaign was conducted in March and April 2014. Measurements with a combined in-situ and remote sensing payload were performed with the German research aircraft HALO based in Oberpfaffenhofen. 16 research flights with altogether 88 flight hours were performed over the North-Atlantic, western and central Europe to probe different cirrus cloud regimes and cirrus clouds at different stages of evolution. One of the key remotes sensing instruments during ML-CIRRUS was the airborne differential absorption and high spectral lidar system WALES. It measures the 2-dimensional distribution of water vapor inside and outside of cirrus clouds as well as the optical properties of the clouds. Bases on these airborne lidar measurements a novel classification scheme to derive the stage of cirrus cloud evolution was developed. It identifies regions of ice nucleation, particle growth by deposition of water vapor, and ice sublimation. This method is used to investigate differences in the distribution and value of optical properties as well as in the distribution of water vapor and relative humidity depending on the stage of evolution of the cloud. We will present the lidar based classification scheme and its application on a wave driven cirrus cloud case, and we will show first results of the dependence of optical cloud properties and relative humidity distributions on the determined stage of evolution.

Satellite Data Analysis of Impact of Anthropogenic Air Pollution on Ice Clouds

NASA Astrophysics Data System (ADS)

Gu, Y.; Liou, K. N.; Zhao, B.; Jiang, J. H.; Su, H.

2017-12-01

Despite numerous studies about the impact of aerosols on ice clouds, the role of anthropogenic aerosols in ice processes, especially over pollution regions, remains unclear and controversial, and has not been considered in a regional model. The objective of this study is to improve our understanding of the ice process associated with anthropogenic aerosols, and provide a comprehensive assessment of the contribution of anthropogenic aerosols to ice nucleation, ice cloud properties, and the consequent regional radiative forcing. As the first attempt, we evaluate the effects of different aerosol types (mineral dust, air pollution, polluted dust, and smoke) on ice cloud micro- and macro-physical properties using satellite data. We identify cases with collocated CloudSat, CALIPSO, and Aqua observations of vertically resolved aerosol and cloud properties, and process these observations into the same spatial resolution. The CALIPSO's aerosol classification algorithm determines aerosol layers as one of six defined aerosol types by taking into account the lidar depolarization ratio, integrated attenuated backscattering, surface type, and layer elevation. We categorize the cases identified above according to aerosol types, collect relevant aerosol and ice cloud variables, and determine the correlation between column/layer AOD and ice cloud properties for each aerosol type. Specifically, we investigate the correlation between aerosol loading (indicated by the column AOD and layer AOD) and ice cloud microphysical properties (ice water content, ice crystal number concentration, and ice crystal effective radius) and macro-physical properties (ice water path, ice cloud fraction, cloud top temperature, and cloud thickness). By comparing the responses of ice cloud properties to aerosol loadings for different aerosol types, we infer the role of different aerosol types in ice nucleation and the evolution of ice clouds. Our preliminary study shows that changes in the ice crystal effective radius with respect to AOD over Eastern Asia for the aerosol types of polluted continental and mineral dust look similar, implying that both air pollution and mineral dust could affect the microphysical properties of ice clouds.

Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings

NASA Astrophysics Data System (ADS)

Schill, G. P.; Tolbert, M. A.

2013-05-01

Atmospheric ice nucleation on aerosol particles relevant to cirrus clouds remains one of the least understood processes in the atmosphere. Upper tropospheric aerosols as well as sub-visible cirrus residues are known to be enhanced in both sulfates and organics. The hygroscopic phase transitions of organic-sulfate particles can have an impact on both the cirrus cloud formation mechanism and resulting cloud microphysical properties. In addition to deliquescence and efflorescence, organic-sulfate particles are known to undergo another phase transition known as liquid-liquid phase separation. The ice nucleation properties of particles that have undergone liquid-liquid phase separation are unknown. Here, Raman microscopy coupled with an environmental cell was used to study the low temperature deliquescence, efflorescence, and liquid-liquid phase separation behavior of 2 : 1 mixtures of organic polyols (1,2,6-hexanetriol and 1 : 1 1,2,6-hexanetriol + 2,2,6,6-tetrakis(hydroxymethyl)cyclohexanol) and ammonium sulfate from 240-265 K. Further, the ice nucleation efficiency of these organic-sulfate systems after liquid-liquid phase separation and efflorescence was investigated from 210-235 K. Raman mapping and volume-geometry analysis indicate that these particles contain solid ammonium sulfate cores fully engulfed in organic shells. For the ice nucleation experiments, we find that if the organic coatings are liquid, water vapor diffuses through the shell and ice nucleates on the ammonium sulfate core. In this case, the coatings minimally affect the ice nucleation efficiency of ammonium sulfate. In contrast, if the coatings become semi-solid or glassy, ice instead nucleates on the organic shell. Consistent with recent findings that glasses can be efficient ice nuclei, the phase-separated particles are nearly as efficient at ice nucleation as pure crystalline ammonium sulfate.

Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings

NASA Astrophysics Data System (ADS)

Schill, G. P.; Tolbert, M. A.

2012-12-01

Atmospheric ice nucleation on aerosol particles relevant to cirrus clouds remains one of the least understood processes in the atmosphere. Upper tropospheric aerosols as well as sub-visible cirrus residues are known to be enhanced in both sulfates and organics. The hygroscopic phase transitions of organic-sulfate particles can have an impact on both the cirrus cloud formation mechanism and resulting cloud microphysical properties. In addition to deliquescence and efflorescence, organic-sulfate particles are known to undergo another phase transition known as liquid-liquid phase separation. The ice nucleation properties of particles that have undergone liquid-liquid phase separation are unknown. Here, Raman microscopy coupled with an environmental cell was used to study the low temperature deliquescence, efflorescence, and liquid-liquid phase separation behavior of 2:1 mixtures of organic polyols (1,2,6-hexanetriol, and 1:1 1,2,6-hexanetriol +2,2,6,6-tetrakis(hydroxymethyl)cycohexanol) and ammonium sulfate from 240-265 K. Further, the ice nucleation efficiency of these organic-sulfate systems after liquid-liquid phase separation and efflorescence was investigated from 210-235 K. Raman mapping and volume-geometry analysis indicates that these particles contain solid ammonium sulfate cores fully engulfed in organic shells. For the ice nucleation experiments, we find that if the organic coatings are liquid, water vapor diffuses through the shell and ice nucleates on the ammonium sulfate core. In this case, the coatings minimally affect the ice nucleation efficiency of ammonium sulfate. In contrast, if the coatings become semi-solid or glassy, ice instead nucleates on the organic shell. Consistent with recent findings that glasses can be efficient ice nuclei, the phase separated particles are nearly as efficient at ice nucleation as pure crystalline ammonium sulfate.

Ice Nucleation in the Tropical Tropopause Layer: Implications for Cirrus Occurrence, Cirrus Microphysical Properties, and Dehydration of Air Entering the Stratosphere

NASA Technical Reports Server (NTRS)

Jensen, Eric; Kaercher, Bernd; Ueyama, Rei; Pfister, Leonhard

2017-01-01

Recent laboratory experiments have advanced our understanding of the physical properties and ice nucleating abilities of aerosol particles atlow temperatures. In particular, aerosols containing organics will transition to a glassy state at low temperatures, and these glassy aerosols are moderately effective as ice nuclei. These results have implications for ice nucleation in the cold Tropical Tropopause Layer (TTL; 13-19 km). We have developed a detailed cloud microphysical model that includes heterogeneous nucleation on a variety of aerosol types and homogeneous freezing of aqueous aerosols. This model has been incorporated into one-dimensional simulations of cirrus and water vapor driven by meteorological analysis temperature and wind fields. The model includes scavenging of ice nuclei by sedimenting ice crystals. The model is evaluated by comparing the simulated cloud properties and water vapor concentrations with aircraft and satellite measurements. In this presentation, I will discuss the relative importance of homogeneous and heterogeneous ice nucleation, the impact of ice nuclei scavenging as air slowly ascends through the TTL, and the implications for the final dehydration of air parcels crossing the tropical cold-point tropopause and entering the tropical stratosphere.

Cellulose and Their Characteristic Ice Nucleation Activity- Freezing on a Chip

NASA Astrophysics Data System (ADS)

Häusler, Thomas; Felgitsch, Laura; Grothe, Hinrich

2016-04-01

The influence of clouds on the Earth's climate system is well known (IPCC, 2013). Cloud microphysics determines for example cloud lifetime and precipitation properties. Clouds are cooling the climate system by reflecting incoming solar radiation and warm its surface by trapping outgoing infrared radiation (Baker and Peter, 2008). In all these processes, aerosol particles play a crucial role by acting as cloud condensation nuclei (CCN) for liquid droplets and as an ice nucleation particle (INP) for the formation of ice particles. Freezing processes at higher temperatures than -38°C occur heterogeneously (Pruppacher and Klett 1997). Therefore aerosol particles act like a catalyst, which reduces the energy barrier for nucleation. The nucleation mechanisms, especially the theory of functional sites are not entirely understood. It remains unclear which class of compound nucleates ice. Here we present a unique technique to perform drop- freezing experiments in a more efficient way. A self-made freezing- chip will be presented. Measurements done to proof the efficiency of our setup as well as advantages compared with other setups will be discussed. Furthermore we present a proxy for biological INPs, microcrystalline cellulose. Cellulose is the main component of herbal cell walls (about 50 wt%). It is a polysaccharide consisting of a linear chain of several hundred to many thousands of β(1→4) linked D-glucose units. Cellulose can contribute to the diverse spectrum of ice nucleation particles. We present results of the nucleation activity measurements of MCCs as well as the influence of concentration, preparation or chemical modification.

The Leipzig Ice Nucleation chamber Comparison (LINC): An overview of ice nucleation measurements observed with four on-line ice nucleation devices

NASA Astrophysics Data System (ADS)

Kohn, Monika; Wex, Heike; Grawe, Sarah; Hartmann, Susan; Hellner, Lisa; Herenz, Paul; Welti, André; Stratmann, Frank; Lohmann, Ulrike; Kanji, Zamin A.

2016-04-01

Mixed-phase clouds (MPCs) are found to be the most relevant cloud type leading to precipitation in mid-latitudes. The formation of ice crystals in MPCs is not completely understood. To estimate the effect of aerosol particles on the radiative properties of clouds and to describe ice nucleation in models, the specific properties of aerosol particles acting as ice nucleating particles (INPs) still need to be identified. A number of devices are able to measure INPs in the lab and in the field. However, methods can be very different and need to be tested under controlled conditions with respect to aerosol generation and properties in order to standardize measurement and data analysis approaches for subsequent ambient measurements. Here, we present an overview of the LINC campaign hosted at TROPOS in September 2015. We compare four ice nucleation devices: PINC (Portable Ice Nucleation Chamber, Chou et al., 2011) and SPIN (SPectrometer for Ice Nuclei) are operated in deposition nucleation and condensation freezing mode. LACIS (Leipzig Aerosol Cloud Interaction Simulator, Hartmann et al., 2011) and PIMCA (Portable Immersion Mode Cooling chamber) measure in the immersion freezing mode. PIMCA is used as a vertical extension to PINC and allows activation and droplet growth prior to exposure to the investigated ice nucleation temperature. Size-resolved measurements of multiple aerosol types were performed including pure mineral dust (K-feldspar, kaolinite) and biological particles (Birch pollen washing waters) as well as some of them after treatment with sulfuric or nitric acid prior to experiments. LACIS and PIMCA-PINC operated in the immersion freezing mode showed very good agreement in the measured frozen fraction (FF). For the comparison between PINC and SPIN, which were scanning relative humidity from below to above water vapor saturation, an agreement was found for the obtained INP concentration. However, some differences were observed, which may result from ice detection and data treatment. A difference was observed between FF from LACIS and PIMCA-PINC compared to the ice activated fractions (AF) from PINC and SPIN. This requires further investigations. Acknowledgements Part of this work was funded by the DFG Research Unit FOR 1525 INUIT, grant WE 4722/1-2. References Chou et al. (2011), Atmos. Chem. Phys., 11, 4725-4738. Hartmann et al. (2011), Atmos. Chem. Phys., 11, 1753-1767.

Ice nucleation by plant structural materials and its potential contribution to glaciation in clouds

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Hoose, C.; Järvinen, E.; Kiselev, A. A.; Moehler, O.; Schnaiter, M.; Ullrich, R.; Cziczo, D. J.; Felgitsch, L.; Gourihar, K.; Grothe, H.; Reicher, N.; Rudich, Y.; Tobo, Y.; Zawadowicz, M. A.

2015-12-01

Glaciation of supercooled clouds through immersion freezing is an important atmospheric process affecting the formation of precipitation and the Earth's energy budget. Currently, the climatic impact of ice-nucleating particles (INPs) is being reassessed due to increasing evidence of their diversity and abundance in the atmosphere as well as their ability to influence cloud properties. Recently, it has been found that microcrystalline cellulose (MCC; extracted from natural wood pulp) can act as an efficient INP and may add crucial importance to quantify the role of primary biological INP (BINP) in the troposphere. However, it is still unclear if the laboratory results of MCC can be representatively scaled up to the total cellulose content in the atmosphere to assess the overall role of BINPs in clouds and the climate system. Here, we use the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber in Karlsruhe, Germany to demonstrate that several important plant constituents as well as natural plant debris can act as BINPs in simulated super-cooled clouds of the lower and middle troposphere. More specifically, we measured the surface-scaled ice nucleation activity of a total 16 plant structural materials (i.e., celluloses, lignins, lipids and carbohydrates), which were dispersed and immersed in cloud droplets in the chamber, and compared to that of dried leaf powder as a model proxy for atmospheric BINPs. Using these surface-based activities, we developed parameters describing the ice nucleation ability of these particles. Subsequently, we applied them to observed airborne plant debris concentrations and compared to the background INP simulated in a global aerosol model. Our results suggest that cellulose is the most active BINPs amongst the 16 materials and the concentration of ice nucleating cellulose and plant debris to become significant (>0.1 L-1) below about -20 ˚C. Overall, our findings support the view that MCC may be a good proxy for inferring ice nucleating properties of natural plant debris. More atmospheric observations of airborne cellulose-containing particles are necessary to allow better estimates of their effects on clouds and the global climate. Acknowledgement: We acknowledge support by German Research Society (DFG) and Ice Nuclei research UnIT (FOR 1525 INUIT).

Immersion freezing by natural dust based on a soccer ball model with the Community Atmospheric Model version 5: climate effects

NASA Astrophysics Data System (ADS)

Wang, Yong; Liu, Xiaohong

2014-12-01

We introduce a simplified version of the soccer ball model (SBM) developed by Niedermeier et al (2014 Geophys. Res. Lett. 41 736-741) into the Community Atmospheric Model version 5 (CAM5). It is the first time that SBM is used in an atmospheric model to parameterize the heterogeneous ice nucleation. The SBM, which was simplified for its suitable application in atmospheric models, uses the classical nucleation theory to describe the immersion/condensation freezing by dust in the mixed-phase cloud regime. Uncertain parameters (mean contact angle, standard deviation of contact angle probability distribution, and number of surface sites) in the SBM are constrained by fitting them to recent natural dust (Saharan dust) datasets. With the SBM in CAM5, we investigate the sensitivity of modeled cloud properties to the SBM parameters, and find significant seasonal and regional differences in the sensitivity among the three SBM parameters. Changes of mean contact angle and the number of surface sites lead to changes of cloud properties in Arctic in spring, which could be attributed to the transport of dust ice nuclei to this region. In winter, significant changes of cloud properties induced by these two parameters mainly occur in northern hemispheric mid-latitudes (e.g., East Asia). In comparison, no obvious changes of cloud properties caused by changes of standard deviation can be found in all the seasons. These results are valuable for understanding the heterogeneous ice nucleation behavior, and useful for guiding the future model developments.

Nucleation in Synoptically Forced Cirrostratus

NASA Technical Reports Server (NTRS)

Lin, R.-F.; Starr, D. OC.; Reichardt, J.; DeMott, P. J.

2004-01-01

Formation and evolution of cirrostratus in response to weak, uniform and constant synoptic forcing is simulated using a one-dimensional numerical model with explicit microphysics, in which the particle size distribution in each grid box is fully resolved. A series of tests of the model response to nucleation modes (homogeneous-freezing-only/heterogeneous nucleation) and heterogeneous nucleation parameters are performed. In the case studied here, nucleation is first activated in the prescribed moist layer. A continuous cloud-top nucleation zone with a depth depending on the vertical humidity gradient and one of the nucleation parameters is developed afterward. For the heterogeneous nucleation cases, intermittent nucleation zones in the mid-upper portion of the cloud form where the relative humidity is on the rise, because existent ice crystals do not uptake excess water vapor efficiently, and ice nuclei (IN) are available. Vertical resolution as fine as 1 m is required for realistic simulation of the homogeneous-freezing-only scenario, while the model resolution requirement is more relaxed in the cases where heterogeneous nucleation dominates. Bulk microphysical and optical properties are evaluated and compared. Ice particle number flux divergence, which is due to the vertical gradient of the gravity-induced particle sedimentation, is constantly and rapidly changing the local ice number concentration, even in the nucleation zone. When the depth of the nucleation zone is shallow, particle number concentration decreases rapidly as ice particles grow and sediment away from the nucleation zone. When the depth of the nucleation zone is large, a region of high ice number concentration can be sustained. The depth of nucleation zone is an important parameter to be considered in parametric treatments of ice cloud generation.

Cirrus clouds as seen by the CALIPSO satellite and ECHAM-HAM global climate model

NASA Astrophysics Data System (ADS)

Gasparini, Blaz; Meyer, Angela; Neubauer, David; Münch, Steffen; Lohmann, Ulrike

2017-04-01

Ice clouds impact the planetary energy balance and upper tropospheric water vapour transport and are therefore relevant for climate. In this study ice clouds at temperatures below -40°C simulated by the ECHAM-HAM global climate model are compared to CALIPSO/CALIOP satellite data. The model reproduces well the mean occurrence of ice clouds, while the ice water path, ice crystal radius, cloud optical depth and extinction are overestimated in terms of annual means and temperature dependent frequency histograms. Two distinct types of cirrus clouds are found: in-situ formed cirrus dominating at temperatures below -60°C and liquid-origin cirrus, dominating at temperatures warmer than -55°C. The latter form in anvils of deep convective clouds or by glaciation of mixed-phase clouds. They are associated with ice water contents of up to 0.1 g m-3 and extinctions of up to 0.1 km-1, while the in-situ formed cirrus are optically thinner and contain at least an order of magnitude less ice. The ice cloud properties do not differ significantly between the southern and the northern hemisphere. In-situ formed ice clouds are further divided into homogeneously and heterogeneously nucleated ones. The simulated liquid-origin ice crystals mainly form in convective outflow in large number concentrations, similar to in-situ homogeneously nucleated ice crystals. On the contrary, heterogeneously nucleated ice crystals are associated with smaller number concentrations. However, ice crystal aggregation and depositional growth smooth the differences between several formation mechanisms making the attribution to a specific ice nucleation mechanism challenging.

Aerosol Indirect Effects on Cirrus Clouds in Global Aerosol-Climate Models

NASA Astrophysics Data System (ADS)

Liu, X.; Zhang, K.; Wang, Y.; Neubauer, D.; Lohmann, U.; Ferrachat, S.; Zhou, C.; Penner, J.; Barahona, D.; Shi, X.

2015-12-01

Cirrus clouds play an important role in regulating the Earth's radiative budget and water vapor distribution in the upper troposphere. Aerosols can act as solution droplets or ice nuclei that promote ice nucleation in cirrus clouds. Anthropogenic emissions from fossil fuel and biomass burning activities have substantially perturbed and enhanced concentrations of aerosol particles in the atmosphere. Global aerosol-climate models (GCMs) have now been used to quantify the radiative forcing and effects of aerosols on cirrus clouds (IPCC AR5). However, the estimate uncertainty is very large due to the different representation of ice cloud formation and evolution processes in GCMs. In addition, large discrepancies have been found between model simulations in terms of the spatial distribution of ice-nucleating aerosols, relative humidity, and temperature fluctuations, which contribute to different estimates of the aerosol indirect effect through cirrus clouds. In this presentation, four GCMs with the start-of-the art representations of cloud microphysics and aerosol-cloud interactions are used to estimate the aerosol indirect effects on cirrus clouds and to identify the causes of the discrepancies. The estimated global and annual mean anthropogenic aerosol indirect effect through cirrus clouds ranges from 0.1 W m-2 to 0.3 W m-2 in terms of the top-of-the-atmosphere (TOA) net radiation flux, and 0.5-0.6 W m-2 for the TOA longwave flux. Despite the good agreement on global mean, large discrepancies are found at the regional scale. The physics behind the aerosol indirect effect is dramatically different. Our analysis suggests that burden of ice-nucleating aerosols in the upper troposphere, ice nucleation frequency, and relative role of ice formation processes (i.e., homogeneous versus heterogeneous nucleation) play key roles in determining the characteristics of the simulated aerosol indirect effects. In addition to the indirect effect estimate, we also use field campaign measurements and satellite retrievals to evaluate the simulated micro- and macro- physical properties of ice clouds in the four GCMs.

The Role of Clouds in the Long-Term Habitability of Planets

NASA Technical Reports Server (NTRS)

Toon, Owen B.; Tolbert, Margaret

2000-01-01

We proposed to conduct theoretical and laboratory investigations of the role that clouds play in the long-term climate history of the Earth and other habitable planets. We made significant progress in the first area we proposed to consider- the properties of carbon dioxide clouds in atmospheres that are rich in carbon dioxide. We submitted a modeling paper on the microphysical properties of the clouds to Icarus showing that such clouds are unlikely to play an important role in the early greenhouses on Earth or Mars. The model was based on lab studies of the nucleation and growth of carbon dioxide. We have also submitted a manuscript describing these lab studies to Icarus. These lab studies are critical not only to the ancient Mars atmosphere, but also to the current one. We also submitted a paper to Nature describing modeling of current Martian CO2 clouds. We will also model the properties of water clouds in the early history of Earth. Early in Earth's history the atmosphere contained no free oxygen. Without oxygen, sulfate aerosols that are currently the dominant cloud nuclei, cannot form. Without such nuclei the cloud structure would have been far different than it is now. We initiated studies of the aerosols on Titan as part of this work. We reported these studies in a short paper on nucleation and in several conferences.

The effect of ice nuclei on a deep convective cloud in South China

NASA Astrophysics Data System (ADS)

Deng, Xin; Xue, Huiwen; Meng, Zhiyong

2018-07-01

This study uses the Weather Research and Forecasting Model to simulate a deep convective cloud under a relatively polluted condition in South China. Ice nuclei (IN) aerosols near the surface are effectively transported upwards to above the 0 °C level by the strong updrafts in the convective cloud. Four cases with initial surface IN aerosol concentrations of 1, 10, 100, and 1000 L-1 are simulated. All simulations can well reproduce the major characteristics of the deep convective cloud in terms of the evolution, spatial distribution, and its track. IN aerosols have little effect on these macrophysical characteristics but can significantly affect ice formation. When IN concentration is increased, all heterogeneous nucleation modes are significantly enhanced, whereas the homogeneous freezing of cloud droplets is unchanged or weakened depending on the IN concentration and the development stages of the deep convective cloud. The homogeneous freezing of haze particles is generally not affected by increased IN but is slightly weakened in the extremely high IN case. As IN concentration is increased by 10 and 100 times, the enhanced heterogeneous nucleation is still not strong enough to compete with homogeneous freezing. Ice formation is hence still dominated by the homogenous freezing of cloud droplets and haze particles in the layer of 9-14 km, where most of the ice crystals are produced. The microphysical properties are generally unaffected in all the stages of cloud evolution. As IN concentration is increased by 1000 times and heterogeneous nucleation is further enhanced, the homogeneous freezing of cloud droplets and haze particles dominates only in the mature and dissipating stages, leading to unaffected ice number mixing ratio in the anvil region (approximately above 9 km) for these two stages. However, in the developing stage, when the supply of cloud droplets is limited, the homogeneous freezing of cloud droplets is weakened or even suppressed due to the very strong competition for liquid water with heterogeneous nucleation, leading to significantly lower ice number mixing ratio in the anvil regions. In addition, the microphysical properties in the convective core regions below the cloud anvil (approximately below 9 km) are also affected in the case of 1000 L-1. The enhanced heterogeneous nucleation produces more ice crystals below 9 km, leading to a stronger conversion from ice crystals to snow particles, and hence higher number and mass mixing ratios of snow. The IN effect on the spatial distributions and temporal evolutions of the surface precipitation and updraft velocity is generally insignificant.

Anvil Glaciation in a Deep Cumulus Updraught over Florida Simulated with the Explicit Microphysics Model. I: Impact of Various Nucleation Processes

NASA Technical Reports Server (NTRS)

Phillips, Vaughan T. J.; Andronache, Constantin; Sherwood, Steven C.; Bansemer, Aaron; Conant, William C.; Demott, Paul J.; Flagan, Richard C.; Heymsfield, Andy; Jonsson, Haflidi; Poellot, Micheal;

Ice Nucleation of Bare and Sulfuric Acid-coated Mineral Dust Particles and Implication for Cloud Properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kulkarni, Gourihar R.; Sanders, Cassandra N.; Zhang, Kai

2014-08-27

Ice nucleation properties of different dust species coated with soluble material are not well understood. We determined the ice nucleation ability of bare and sulfuric acid coated mineral dust particles as a function of temperature (-25 to -35 deg C) and relative humidity with respect to water (RHw). Five different mineral dust species: Arizona test dust (ATD), illite, montmorillonite, quartz and kaolinite were dry dispersed and size-selected at 150 nm and exposed to sulfuric acid vapors in the coating apparatus. The condensed sulfuric acid soluble mass fraction per particle was estimated from the cloud condensation nuclei activated fraction measurements. Themore » fraction of dust particles nucleating ice at various temperatures and RHw was determined using a compact ice chamber. In water-subsaturated conditions, compared to bare dust particles, we found that only coated ATD particles showed suppression of ice nucleation ability while other four dust species did not showed the effect of coating on the fraction of particles nucleating ice. The results suggest that interactions between the dust surface and sulfuric acid vapor are important, such that interactions may or may not modify the surface via chemical reactions with sulfuric acid. At water-supersaturated conditions we did not observed the effect of coating, i.e. the bare and coated dust particles had similar ice nucleation behavior.« less

Application of an online-coupled regional climate model, WRF-CAM5, over East Asia for examination of ice nucleation schemes. Part II. Sensitivity to heterogeneous ice nucleation parameterizations and dust emissions

DOE PAGES

Zhang, Yang; Chen, Ying; Fan, Jiwen; ...

2015-09-14

Aerosol particles can affect cloud microphysical properties by serving as ice nuclei (IN). Large uncertainties exist in the ice nucleation parameterizations (INPs) used in current climate models. In this Part II paper, to examine the sensitivity of the model predictions to different heterogeneous INPs, WRF-CAM5 simulation using the INP of Niemand et al. (N12) [1] is conducted over East Asia for two full years, 2006 and 2011, and compared with simulation using the INP of Meyers et al. (M92) [2], which is the original INP used in CAM5. M92 calculates the nucleated ice particle concentration as a function of icemore » supersaturation, while N12 represents the nucleated ice particle concentration as a function of temperature and the number concentrations and surface areas of dust particles. Compared to M92, the WRF-CAM5 simulation with N12 produces significantly higher nucleated ice crystal number concentrations (ICNCs) in the northern domain where dust sources are located, leading to significantly higher cloud ice number and mass concentrations and ice water path, but the opposite is true in the southern domain where temperatures and moistures play a more important role in ice formation. Overall, the simulation with N12 gives lower downward shortwave radiation but higher downward longwave radiation, cloud liquid water path, cloud droplet number concentrations, and cloud optical depth. The increase in cloud optical depth and the decrease in downward solar flux result in a stronger shortwave and longwave cloud forcing, and decreases temperature at 2-m and precipitation. Changes in temperature and radiation lower surface concentrations of OH, O₃, SO₄²⁻, and PM 2.5, but increase surface concentrations of CO, NO₂, and SO₂ over most of the domain. By acting as cloud condensation nuclei (CCN) and IN, dust particles have different impacts on cloud water and ice number concentrations, radiation, and temperature at 2-m and precipitation depending on whether the dominant role of dust is CCN or IN. These results indicate the importance of the heterogeneous ice nucleation treatments and dust emissions in accurately simulating regional climate and air quality.« less

Application of an online-coupled regional climate model, WRF-CAM5, over East Asia for examination of ice nucleation schemes. Part II. Sensitivity to heterogeneous ice nucleation parameterizations and dust emissions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Yang; Chen, Ying; Fan, Jiwen

Aerosol particles can affect cloud microphysical properties by serving as ice nuclei (IN). Large uncertainties exist in the ice nucleation parameterizations (INPs) used in current climate models. In this Part II paper, to examine the sensitivity of the model predictions to different heterogeneous INPs, WRF-CAM5 simulation using the INP of Niemand et al. (N12) [1] is conducted over East Asia for two full years, 2006 and 2011, and compared with simulation using the INP of Meyers et al. (M92) [2], which is the original INP used in CAM5. M92 calculates the nucleated ice particle concentration as a function of icemore » supersaturation, while N12 represents the nucleated ice particle concentration as a function of temperature and the number concentrations and surface areas of dust particles. Compared to M92, the WRF-CAM5 simulation with N12 produces significantly higher nucleated ice crystal number concentrations (ICNCs) in the northern domain where dust sources are located, leading to significantly higher cloud ice number and mass concentrations and ice water path, but the opposite is true in the southern domain where temperatures and moistures play a more important role in ice formation. Overall, the simulation with N12 gives lower downward shortwave radiation but higher downward longwave radiation, cloud liquid water path, cloud droplet number concentrations, and cloud optical depth. The increase in cloud optical depth and the decrease in downward solar flux result in a stronger shortwave and longwave cloud forcing, and decreases temperature at 2-m and precipitation. Changes in temperature and radiation lower surface concentrations of OH, O₃, SO₄²⁻, and PM 2.5, but increase surface concentrations of CO, NO₂, and SO₂ over most of the domain. By acting as cloud condensation nuclei (CCN) and IN, dust particles have different impacts on cloud water and ice number concentrations, radiation, and temperature at 2-m and precipitation depending on whether the dominant role of dust is CCN or IN. These results indicate the importance of the heterogeneous ice nucleation treatments and dust emissions in accurately simulating regional climate and air quality.« less

Application of an Online-Coupled Regional Climate Model, WRF-CAM5, over East Asia for Examination of Ice Nucleation Schemes: Part II. Sensitivity to Heterogeneous Ice Nucleation Parameterizations and Dust Emissions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Yang; Chen, Ying; Fan, Jiwen

Aerosol particles can affect cloud microphysical properties by serving as ice nuclei (IN). Large uncertainties exist in the ice nucleation parameterizations (INPs) used in current climate models. In this Part II paper, to examine the sensitivity of the model predictions to different heterogeneous INPs, WRF-CAM5 simulation using the INP of Niemand et al. (N12) [1] is conducted over East Asia for two full years, 2006 and 2011, and compared with simulation using the INP of Meyers et al. (M92) [2], which is the original INP used in CAM5. M92 calculates the nucleated ice particle concentration as a function of icemore » supersaturation, while N12 represents the nucleated ice particle concentration as a function of temperature and the number concentrations and surface areas of dust particles. Compared to M92, the WRF-CAM5 simulation with N12 produces significantly higher nucleated ice crystal number concentrations (ICNCs) in the northern domain where dust sources are located, leading to significantly higher cloud ice number and mass concentrations and ice water path, but the opposite is true in the southern domain where temperatures and moistures play a more important role in ice formation. Overall, the simulation with N12 gives lower downward shortwave radiation but higher downward longwave radiation, cloud liquid water path, cloud droplet number concentrations, and cloud optical depth. The increase in cloud optical depth and the decrease in downward solar flux result in a stronger shortwave and longwave cloud forcing, and decreases temperature at 2-m and precipitation. Changes in temperature and radiation lower surface concentrations of OH, O 3, SO 4 2-, and PM2.5, but increase surface concentrations of CO, NO 2, and SO 2 over most of the domain. By acting as cloud condensation nuclei (CCN) and IN, dust particles have different impacts on cloud water and ice number concentrations, radiation, and temperature at 2-m and precipitation depending on whether the dominant role of dust is CCN or IN. These results indicate the importance of the heterogeneous ice nucleation treatments and dust emissions in accurately simulating regional climate and air quality.« less

Explicit Cloud Nucleation from Arbitrary Mixtures of Aerosol Types and Sizes Using an Ultra-Efficient In-Line Aerosol Bin Model in High-Resolution Simulations of Hurricanes

NASA Astrophysics Data System (ADS)

Walko, R. L.; Ashby, T.; Cotton, W. R.

2017-12-01

The fundamental role of atmospheric aerosols in the process of cloud droplet nucleation is well known, and there is ample evidence that the concentration, size, and chemistry of aerosols can strongly influence microphysical, thermodynamic, and ultimately dynamic properties and evolution of clouds and convective systems. With the increasing availability of observation- and model-based environmental representations of different types of anthropogenic and natural aerosols, there is increasing need for models to be able to represent which aerosols nucleate and which do not in supersaturated conditions. However, this is a very complex process that involves competition for water vapor between multiple aerosol species (chemistries) and different aerosol sizes within each species. Attempts have been made to parameterize the nucleation properties of mixtures of different aerosol species, but it is very difficult or impossible to represent all possible mixtures that may occur in practice. As part of a modeling study of the impact of anthropogenic and natural aerosols on hurricanes, we developed an ultra-efficient aerosol bin model to represent nucleation in a high-resolution atmospheric model that explicitly represents cloud- and subcloud-scale vertical motion. The bin model is activated at any time and location in a simulation where supersaturation occurs and is potentially capable of activating new cloud droplets. The bins are populated from the aerosol species that are present at the given time and location and by multiple sizes from each aerosol species according to a characteristic size distribution, and the chemistry of each species is represented by its absorption or adsorption characteristics. The bin model is integrated in time increments that are smaller than that of the atmospheric model in order to temporally resolve the peak supersaturation, which determines the total nucleated number. Even though on the order of 100 bins are typically utilized, this leads only to a 10 or 20% increase in overall computational cost due to the efficiency of the bin model. This method is highly versatile in that it automatically accommodates any possible number and mixture of different aerosol species. Applications of this model to simulations of Typhoon Nuri will be presented.

Direct comparisons of ice cloud macro- and microphysical properties simulated by the Community Atmosphere Model version 5 with HIPPO aircraft observations

NASA Astrophysics Data System (ADS)

Wu, Chenglai; Liu, Xiaohong; Diao, Minghui; Zhang, Kai; Gettelman, Andrew; Lu, Zheng; Penner, Joyce E.; Lin, Zhaohui

2017-04-01

In this study we evaluate cloud properties simulated by the Community Atmosphere Model version 5 (CAM5) using in situ measurements from the HIAPER Pole-to-Pole Observations (HIPPO) campaign for the period of 2009 to 2011. The modeled wind and temperature are nudged towards reanalysis. Model results collocated with HIPPO flight tracks are directly compared with the observations, and model sensitivities to the representations of ice nucleation and growth are also examined. Generally, CAM5 is able to capture specific cloud systems in terms of vertical configuration and horizontal extension. In total, the model reproduces 79.8 % of observed cloud occurrences inside model grid boxes and even higher (94.3 %) for ice clouds (T ≤ -40 °C). The missing cloud occurrences in the model are primarily ascribed to the fact that the model cannot account for the high spatial variability of observed relative humidity (RH). Furthermore, model RH biases are mostly attributed to the discrepancies in water vapor, rather than temperature. At the micro-scale of ice clouds, the model captures the observed increase of ice crystal mean sizes with temperature, albeit with smaller sizes than the observations. The model underestimates the observed ice number concentration (Ni) and ice water content (IWC) for ice crystals larger than 75 µm in diameter. Modeled IWC and Ni are more sensitive to the threshold diameter for autoconversion of cloud ice to snow (Dcs), while simulated ice crystal mean size is more sensitive to ice nucleation parameterizations than to Dcs. Our results highlight the need for further improvements to the sub-grid RH variability and ice nucleation and growth in the model.

Morphology and mixing state of atmospheric particles: Links to optical properties and cloud processing

NASA Astrophysics Data System (ADS)

China, Swarup

Atmospheric particles are ubiquitous in Earth's atmosphere and impact the environment and the climate while affecting human health and Earth's radiation balance, and degrading visibility. Atmospheric particles directly affect our planet's radiation budget by scattering and absorbing solar radiation, and indirectly by interacting with clouds. Single particle morphology (shape, size and internal structure) and mixing state (coating by organic and inorganic material) can significantly influence the particle optical properties as well as various microphysical processes, involving cloud-particle interactions and including heterogeneous ice nucleation and water uptake. Conversely, aerosol cloud processing can affect the morphology and mixing of the particles. For example, fresh soot has typically an open fractal-like structure, but aging and cloud processing can restructure soot into more compacted shapes, with different optical and ice nucleation properties. During my graduate research, I used an array of electron microscopy and image analysis tools to study morphology and mixing state of a large number of individual particles collected during several field and laboratory studies. To this end, I investigated various types of particles such as tar balls (spherical carbonaceous particles emitted during biomass burning) and dust particles, but with a special emphasis on soot particles. In addition, I used the Stony Brook ice nucleation cell facility to investigate heterogeneous ice nucleation and water uptake by long-range transported particles collected at the Pico Mountain Observatory, in the Archipelago of the Azores. Finally, I used ice nucleation data from the SAAS (Soot Aerosol Aging Study) chamber study at the Pacific Northwest National Laboratory to understand the effects that ice nucleation and supercooled water processing has on the morphology of residual soot particles. Some highlights of our findings and implications are discussed next. We found that the morphology of fresh soot emitted by vehicles depends on the driving conditions (i.e.; the vehicle specific power). Soot emitted by biomass burning is often heavily coated by other materials while processing of soot in urban environment exhibits complex mixing. We also found that long-range transported soot over the ocean after atmospheric processing is very compacted. In addition, our results suggest that freezing process can facilitate restructuring of soot and results into collapsed soot. Furthermore, numerical simulations showed strong influence on optical properties when fresh open fractal-like soot evolved to collapsed soot. Further investigation of long-range transported aged particles exhibits that they are efficient in water uptake and can induce ice nucleation in colder temperature. Our results have implications for assessing the impact of the morphology and mixing state of soot particles on human health, environment and climate. Our findings can provide guidance to numerical models such as particle-resolved mixing state models to account for, and better understand, vehicular emissions and soot evolution since its emission to atmospheric processing in urban environment and finally in remote regions after long-range transport. Morphology and mixing state information can be used to model observational-constrained optical properties. The details of morphology and mixing state of soot particles are crucial to assess the accuracy of climate models in describing the contribution of soot radiative forcing and their direct and indirect climate effects. Finally, our observations of ice nucleation ability by aged particles show that nucleated particles are internally mixed and coated with several materials.

Leipzig Ice Nucleation chamber Comparison (LINC): intercomparison of four online ice nucleation counters

NASA Astrophysics Data System (ADS)

Burkert-Kohn, Monika; Wex, Heike; Welti, André; Hartmann, Susan; Grawe, Sarah; Hellner, Lisa; Herenz, Paul; Atkinson, James D.; Stratmann, Frank; Kanji, Zamin A.

2017-09-01

Ice crystal formation in atmospheric clouds has a strong effect on precipitation, cloud lifetime, cloud radiative properties, and thus the global energy budget. Primary ice formation above 235 K is initiated by nucleation on seed aerosol particles called ice-nucleating particles (INPs). Instruments that measure the ice-nucleating potential of aerosol particles in the atmosphere need to be able to accurately quantify ambient INP concentrations. In the last decade several instruments have been developed to investigate the ice-nucleating properties of aerosol particles and to measure ambient INP concentrations. Therefore, there is a need for intercomparisons to ensure instrument differences are not interpreted as scientific findings.In this study, we intercompare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid-treated mineral dusts (microcline, which is a K-feldspar, and kaolinite), as well as birch pollen washing waters. Experiments exploring heterogeneous ice nucleation above and below water saturation are performed to cover the whole range of atmospherically relevant thermodynamic conditions that can be investigated with the intercompared chambers. The Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the Portable Immersion Mode Cooling chAmber coupled to the Portable Ice Nucleation Chamber (PIMCA-PINC) performed measurements in the immersion freezing mode. Additionally, two continuous-flow diffusion chambers (CFDCs) PINC and the Spectrometer for Ice Nuclei (SPIN) are used to perform measurements below and just above water saturation, nominally presenting deposition nucleation and condensation freezing.The results of LACIS and PIMCA-PINC agree well over the whole range of measured frozen fractions (FFs) and temperature. In general PINC and SPIN compare well and the observed differences are explained by the ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for the ice nucleation in the four instruments, the FF (from LACIS and PIMCA-PINC) and the activated fraction, AF (from PINC and SPIN), are compared. Measured FFs are on the order of a factor of 3 higher than AFs, but are not consistent for all aerosol types and temperatures investigated. It is shown that measurements from CFDCs cannot be assumed to produce the same results as those instruments exclusively measuring immersion freezing. Instead, the need to apply a scaling factor to CFDCs operating above water saturation has to be considered to allow comparison with immersion freezing devices. Our results provide further awareness of factors such as the importance of dispersion methods and the quality of particle size selection for intercomparing online INP counters.

Heterogeneous Ice Nucleation by Soufriere Hills Volcanic Ash Immersed in Water Droplets.

PubMed

Mangan, T P; Atkinson, J D; Neuberg, J W; O'Sullivan, D; Wilson, T W; Whale, T F; Neve, L; Umo, N S; Malkin, T L; Murray, B J

2017-01-01

Fine particles of ash emitted during volcanic eruptions may sporadically influence cloud properties on a regional or global scale as well as influencing the dynamics of volcanic clouds and the subsequent dispersion of volcanic aerosol and gases. It has been shown that volcanic ash can trigger ice nucleation, but ash from relatively few volcanoes has been studied for its ice nucleating ability. In this study we quantify the efficiency with which ash from the Soufriere Hills volcano on Montserrat nucleates ice when immersed in supercooled water droplets. Using an ash sample from the 11th February 2010 eruption, we report ice nucleating efficiencies from 246 to 265 K. This wide range of temperatures was achieved using two separate droplet freezing instruments, one employing nanolitre droplets, the other using microlitre droplets. Soufriere Hills volcanic ash was significantly more efficient than all other ash samples that have been previously examined. At present the reasons for these differences are not understood, but may be related to mineralogy, amorphous content and surface chemistry.

Heterogeneous Ice Nucleation by Soufriere Hills Volcanic Ash Immersed in Water Droplets

PubMed Central

Atkinson, J. D.; Neuberg, J. W.; O’Sullivan, D.; Wilson, T. W.; Whale, T. F.; Neve, L.; Umo, N. S.; Malkin, T. L.; Murray, B. J.

2017-01-01

Fine particles of ash emitted during volcanic eruptions may sporadically influence cloud properties on a regional or global scale as well as influencing the dynamics of volcanic clouds and the subsequent dispersion of volcanic aerosol and gases. It has been shown that volcanic ash can trigger ice nucleation, but ash from relatively few volcanoes has been studied for its ice nucleating ability. In this study we quantify the efficiency with which ash from the Soufriere Hills volcano on Montserrat nucleates ice when immersed in supercooled water droplets. Using an ash sample from the 11th February 2010 eruption, we report ice nucleating efficiencies from 246 to 265 K. This wide range of temperatures was achieved using two separate droplet freezing instruments, one employing nanolitre droplets, the other using microlitre droplets. Soufriere Hills volcanic ash was significantly more efficient than all other ash samples that have been previously examined. At present the reasons for these differences are not understood, but may be related to mineralogy, amorphous content and surface chemistry. PMID:28056077

The adsorption of fungal ice-nucleating proteins on mineral dusts: a terrestrial reservoir of atmospheric ice-nucleating particles

NASA Astrophysics Data System (ADS)

O'Sullivan, Daniel; Murray, Benjamin J.; Ross, James F.; Webb, Michael E.

2016-06-01

The occurrence of ice-nucleating particles (INPs) in our atmosphere has a profound impact on the properties and lifetime of supercooled clouds. To date, the identities, sources and abundances of particles capable of nucleating ice at relatively low supercoolings (T > -15 °C) remain enigmatic. While biomolecules such as proteins and carbohydrates have been implicated as important high-temperature INPs, the lack of knowledge on the environmental fates of these species makes it difficult to assess their potential atmospheric impacts. Here we show that such nanoscale ice-nucleating proteins from a common soil-borne fungus (Fusarium avenaceum) preferentially bind to and confer their ice-nucleating properties to kaolinite. The ice-nucleating activity of the proteinaceous INPs is unaffected by adsorption to the clay, and once bound the proteins do not readily desorb, retaining much of the activity even after multiple washings with pure water. The atmospheric implications of the finding that biological residues can confer their ice-nucleating ability to dust particles are discussed.

Ice nucleation activity of diesel soot particles at Cirrus relevant conditions: Effects of hydration, secondary organics coating, hydration, soot morphology, and coagulation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kulkarni, Gourihar R.; China, Swarup; Liu, Shang

The role of atmospheric relevant soot particles that are processed in the atmosphere toward ice nucleation at cirrus cloud condition is poorly understood. In this study, the ice nucleating properties of diesel soot particles subjected to various physical and chemical aging treatments were investigated at temperatures ranging from -40 to -50 °C. We show that bare soot particles nucleate ice in deposition mode, but coating with secondary organics suppresses the heterogeneous ice nucleation potential of soot particles requiring homogeneous freezing threshold conditions. However, the ice nucleation efficiency of soot particles coated with an aqueous organic layer was similar to baremore » soot particles. Hydration of bare soot particles slightly enhanced the ice nucleation efficiency, and the IN abilities of compact soot particles (roundness = ~ 0.6) were similar to bare lacey soot particles (roundness = ~ 0.4). These results indicate that ice nucleation properties are sensitive to the various aging treatments.« less

Comparing modelled and measured ice crystal concentrations in orographic clouds during the INUPIAQ campaign

NASA Astrophysics Data System (ADS)

Farrington, Robert; Connolly, Paul J.; Lloyd, Gary; Bower, Keith N.; Flynn, Michael J.; Gallagher, Martin W.; Field, Paul R.; Dearden, Chris; Choularton, Thomas W.; Hoyle, Chris

2016-04-01

At temperatures between -35°C and 0°C, the presence of insoluble aerosols acting as ice nuclei (IN) is the only way in which ice can nucleate under atmospheric conditions. Previous field and laboratory campaigns have suggested that mineral dust present in the atmosphere act as IN at temperatures warmer than -35°C (e.g. Sassen et al. 2003); however, the cause of ice nucleation at temperatures greater than -10°C is less certain. In-situ measurements of aerosol properties and cloud micro-physical processes are required to drive the improvement of aerosol-cloud processes in numerical models. As part of the Ice NUcleation Process Investigation and Quantification (INUPIAQ) project, two field campaigns were conducted in the winters of 2013 and 2014 (Lloyd et al. 2014). Both campaigns included measurements of cloud micro-physical properties at the summit of Jungfraujoch in Switzerland (3580m asl), using cloud probes, including the Two-Dimensional Stereo Hydrometeor Spectrometer (2D-S), the Cloud Particle Imager 3V (CPI-3V) and the Cloud Aerosol Spectrometer with Depolarization (CAS-DPOL). The first two of these probes measured significantly higher ice number concentrations than those observed in clouds at similar altitudes from aircraft. In this contribution, we assess the source of the high ice number concentrations observed by comparing in-situ measurements at Jungfraujoch with WRF simulations applied to the region around Jungfraujoch. During the 2014 field campaign the model simulations regularly simulated ice particle concentrations that were 3 orders of magnitude per litre less than the observed ice number concentration, even taking into account the aerosol properties measured upwind. WRF was used to investigate a number of potential sources of the high ice crystal concentrations, including: an increased ice nucleating particle (INP) concentration, secondary ice multiplication and the advection of surface ice or snow crystals into the clouds. It was found that the influence of these processes on the ice particle concentrations could not explain the observations. We also assessed whether the inclusion of a surface flux of hoar crystals into the WRF model could account for the increased ice concentrations in the orographic clouds found at Jungfraujoch. By including a simple parameterisation based on the surface wind speed, the inclusion of the surface crystal flux provided good agreement with the measurements at Jungfraujoch. A summary of these results will be presented at the meeting. References Lloyd, G., et al., 2015. The origins of ice crystals measured in mixed-phase clouds at the high-alpine site Jungfraujoch. Atmos. Chem. Phys., 15, 12953-12969. Sassen, K., et al., 2003. Saharan dust storms and indirect aerosol effects on clouds: Crystal-face results. Geophys. Res. Lett., 30, 1633-1636.

Harmonization of Initial Estimates of Shale Gas Life Cycle Greenhouse Gas Emissions for Electric Power Generation

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Hoose, C.; Järvinen, E.; Kiselev, A. A.; Moehler, O.; Schnaiter, M.; Ullrich, R.; Cziczo, D. J.; Felgitsch, L.; Gourihar, K.; Grothe, H.; Reicher, N.; Rudich, Y.; Tobo, Y.; Zawadowicz, M. A.

2014-12-01

Glaciation of supercooled clouds through immersion freezing is an important atmospheric process affecting the formation of precipitation and the Earth's energy budget. Currently, the climatic impact of ice-nucleating particles (INPs) is being reassessed due to increasing evidence of their diversity and abundance in the atmosphere as well as their ability to influence cloud properties. Recently, it has been found that microcrystalline cellulose (MCC; extracted from natural wood pulp) can act as an efficient INP and may add crucial importance to quantify the role of primary biological INP (BINP) in the troposphere. However, it is still unclear if the laboratory results of MCC can be representatively scaled up to the total cellulose content in the atmosphere to assess the overall role of BINPs in clouds and the climate system. Here, we use the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber in Karlsruhe, Germany to demonstrate that several important plant constituents as well as natural plant debris can act as BINPs in simulated super-cooled clouds of the lower and middle troposphere. More specifically, we measured the surface-scaled ice nucleation activity of a total 16 plant structural materials (i.e., celluloses, lignins, lipids and carbohydrates), which were dispersed and immersed in cloud droplets in the chamber, and compared to that of dried leaf powder as a model proxy for atmospheric BINPs. Using these surface-based activities, we developed parameters describing the ice nucleation ability of these particles. Subsequently, we applied them to observed airborne plant debris concentrations and compared to the background INP simulated in a global aerosol model. Our results suggest that cellulose is the most active BINPs amongst the 16 materials and the concentration of ice nucleating cellulose and plant debris to become significant (>0.1 L-1) below about -20 ˚C. Overall, our findings support the view that MCC may be a good proxy for inferring ice nucleating properties of natural plant debris. More atmospheric observations of airborne cellulose-containing particles are necessary to allow better estimates of their effects on clouds and the global climate. Acknowledgement: We acknowledge support by German Research Society (DFG) and Ice Nuclei research UnIT (FOR 1525 INUIT).

Cirrus Susceptibility to Changes in Ice Nuclei: Physical Processes, Model Uncertainties, and Measurement Needs

NASA Technical Reports Server (NTRS)

Jensen, Eric

2017-01-01

In this talk, I will begin by discussing the physical processes that govern the competition between heterogeneous and homogeneous ice nucleation in upper tropospheric cirrus clouds. Next, I will review the current knowledge of low-temperature ice nucleation from laboratory experiments and field measurements. I will then discuss the uncertainties and deficiencies in representations of cirrus processes in global models used to estimate the climate impacts of changes in cirrus clouds. Lastly, I will review the critical field measurements needed to advance our understanding of cirrus and their susceptibility to changes in aerosol properties.

The chemical composition of cirrus forming aerosol: Lessons from the MACPEX field study

NASA Astrophysics Data System (ADS)

Cziczo, D. J.; Froyd, K. D.; Murphy, D. M.

2012-12-01

Cirrus clouds are an important factor in the Earth's climate system. These clouds exert a large radiative forcing due to their extensive global coverage and high altitude despite minimal physical and optical thickness. During the Mid-latitude Aerosol and Cloud Properties EXperiment (MACPEX) we measured chemical and physical properties of the aerosols on which cirrus ice crystals formed in situ and in real time using a laser ablation single particle mass spectrometry technique deployed aboard the NASA WB-57 research aircraft. Ice residual particles were also collected for off-line laboratory investigation including electron microscopy. Flights spanned from the Gulf of Mexico to the mid-latitudes over the United States. In most cases heterogeneous freezing was the inferred mechanism of cloud formation and aerosol composition had a significant impact on the nucleation of the ice phase. Mineral dust and some metallic particles were highly enhanced in the ice phase when compared to their abundance outside of cloud. Particles such as soot and biological material, previously suggested as ice nuclei, were not found either due to an inability to nucleate ice or low abundance. Atmospheric implications of these measurements and more advanced future analyses will be discussed.

Ice nuclei emissions from biomass burning

Treesearch

Markus D. Petters; Matthew T. Parsons; Anthony J. Prenni; Paul J. DeMott; Sonia M. Kreidenweis; Christian M. Carrico; Amy P. Sullivan; Gavin R. McMeeking; Ezra Levin; Cyle E. Wold; Jeffrey L. Collett; Hans Moosmuller

2009-01-01

Biomass burning is a significant source of carbonaceous aerosol in many regions of the world. When present, biomass burning particles may affect the microphysical properties of clouds through their ability to function as cloud condensation nuclei or ice nuclei. We report on measurements of the ice nucleation ability of biomass burning particles performed on laboratory-...

Sedimentation Efficiency of Condensation Clouds in Substellar Atmospheres

NASA Astrophysics Data System (ADS)

Gao, Peter; Marley, Mark S.; Ackerman, Andrew S.

2018-03-01

Condensation clouds in substellar atmospheres have been widely inferred from spectra and photometric variability. Up until now, their horizontally averaged vertical distribution and mean particle size have been largely characterized using models, one of which is the eddy diffusion–sedimentation model from Ackerman and Marley that relies on a sedimentation efficiency parameter, f sed, to determine the vertical extent of clouds in the atmosphere. However, the physical processes controlling the vertical structure of clouds in substellar atmospheres are not well understood. In this work, we derive trends in f sed across a large range of eddy diffusivities (K zz ), gravities, material properties, and cloud formation pathways by fitting cloud distributions calculated by a more detailed cloud microphysics model. We find that f sed is dependent on K zz , but not gravity, when K zz is held constant. f sed is most sensitive to the nucleation rate of cloud particles, as determined by material properties like surface energy and molecular weight. High surface energy materials form fewer, larger cloud particles, leading to large f sed (>1), and vice versa for materials with low surface energy. For cloud formation via heterogeneous nucleation, f sed is sensitive to the condensation nuclei flux and radius, connecting cloud formation in substellar atmospheres to the objects’ formation environments and other atmospheric aerosols. These insights could lead to improved cloud models that help us better understand substellar atmospheres. For example, we demonstrate that f sed could increase with increasing cloud base depth in an atmosphere, shedding light on the nature of the brown dwarf L/T transition.

Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Kazil, J.; Stier, P.; Zhang, K.; Quaas, J.; Kinne, S.; O'Donnell, D.; Rast, S.; Esch, M.; Ferrachat, S.; Lohmann, U.; Feichter, J.

2010-05-01

Nucleation from the gas phase is an important source of aerosol particles in the Earth's atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosol-climate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth's radiative budget. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are -1.15 W/m2 for charged H2SO4/H2O nucleation, -0.235 W/m2 for cluster activation, and -0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is -2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with -2.18 W/m2 to total absorbed solar short-wave radiation, compared to -0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth's radiative budget over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local measurements: over southern Finland, where cluster activation proceeds efficiently, we find that charged nucleation of sulfuric acid and water contributes on average less than 10% to ultrafine aerosol concentrations, in good agreement with observations.

Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Kazil, J.; Stier, P.; Zhang, K.; Quaas, J.; Kinne, S.; O'Donnell, D.; Rast, S.; Esch, M.; Ferrachat, S.; Lohmann, U.; Feichter, J.

2010-11-01

Nucleation from the gas phase is an important source of aerosol particles in the Earth's atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosol-climate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth's radiative forcing. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are -1.15 W/m2 for charged H2SO4/H2O nucleation, -0.235 W/m2 for cluster activation, and -0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is -2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with -2.18 W/m2 to total absorbed solar short-wave radiation, compared to -0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth's radiative forcing over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local measurements: over southern Finland, where cluster activation proceeds efficiently, we find that charged nucleation of sulfuric acid and water contributes on average less than 10% to ultrafine aerosol concentrations, in good agreement with observations.

Partitioning the primary ice formation modes in large eddy simulations of mixed-phase clouds

NASA Astrophysics Data System (ADS)

Hande, Luke B.; Hoose, Corinna

2017-11-01

State-of-the-art aerosol-dependent parameterisations describing each heterogeneous ice nucleation mode (contact, immersion, and deposition ice nucleation), as well as homogeneous nucleation, were incorporated into a large eddy simulation model. Several cases representing commonly occurring cloud types were simulated in an effort to understand which ice nucleation modes contribute the most to total concentrations of ice crystals. The cases include a completely idealised warm bubble, semi-idealised deep convection, an orographic cloud, and a stratiform case. Despite clear differences in thermodynamic conditions between the cases, the results are remarkably consistent between the different cloud types. In all the investigated cloud types and under normal aerosol conditions, immersion freezing dominates and contact freezing also contributes significantly. At colder temperatures, deposition nucleation plays only a small role, and homogeneous freezing is important. To some extent, the temporal evolution of the cloud determines the dominant freezing mechanism and hence the subsequent microphysical processes. Precipitation is not correlated with any one ice nucleation mode, instead occurring simultaneously when several nucleation modes are active. Furthermore, large variations in the aerosol concentration do affect the dominant ice nucleation mode; however, they have only a minor influence on the precipitation amount.

Cirrus Susceptibility to Changes in Ice Nuclei: Physical Processes, Model Uncertainties, and Measurement Needs

NASA Technical Reports Server (NTRS)

Jensen, Eric

2018-01-01

One of the proposed concepts for mitigating the warming effect of increasing greenhouse gases is seeding cirrus cloud with ice nuclei (IN) in order to reduce the lifetime and coverage of cold cirrus that have a net warming impact on the earth's surface. Global model simulations of the net impact of changing upper tropospheric IN have given widely disparate results, partly as a result of poor understanding of ice nucleation processes in the current atmosphere, and partly as a result of poor representation of these processes in global models. Here, we present detailed process-model simulations of tropical tropopause layer (TTL) transport and cirrus formation with ice nuclei properties based on recent laboratory nucleation experiments and field measurements of aerosol composition. The model is used to assess the sensitivity of TTL cirrus occurrence frequency and microphysical properties to the abundance and efficacy of ice nuclei. The simulated cloud properties compared with recent high-altitude aircraft measurements of TTL cirrus and ice supersaturation. We find that abundant effective IN (either from glassy organic aerosols or crystalline ammonium sulfate with concentrations greater than about 100/L) prevent the occurrences of large ice concentration and large ice supersaturations, both of which are clearly indicated by the in situ observations. We find that concentrations of effective ice nuclei larger than about 50/L can drive significant changes in cirrus microphysical properties and occurrence frequency. However, the cloud occurrence frequency can either increase or decrease, depending on the efficacy and abundance of IN added to the TTL. We suggest that our lack of information about ice nuclei properties in the current atmosphere, as well as uncertainties in ice nucleation processes and their representations in global models, preclude meaningful estimates of climate impacts associated with addition of ice nuclei in the upper troposphere. We will briefly discuss the key field measurements needed to constrain ice nucleation processes.

Ambient in-situ immersion freezing measurements - findings from the ZAMBIS 2014 field campaign for three ice nucleation techniques

NASA Astrophysics Data System (ADS)

Kohn, Monika; Atkinson, James D.; Lohmann, Ulrike; Kanji, Zamin A.

2015-04-01

To estimate the influence of clouds on the Earth's radiation budget, it is crucial to understand cloud formation processes in the atmosphere. A key process, which significantly affects cloud microphysical properties and the initiation of precipitation thus contributing to the hydrological cycle, is the prevailing type of ice nucleation mechanism. In mixed-phase clouds immersion freezing is the dominant ice crystal forming mechanism, whereby ice nucleating particles (INP) first act as cloud condensation nuclei (CCN) and are activated to cloud droplets followed by freezing upon supercooling. There are a number of experimental methods and techniques to investigate the ice nucleating ability in the immersion mode, however most techniques are offline for field sampling or only suitable for laboratory measurements. In-situ atmospheric studies are needed to understand the ice formation processes of 'real world' particles. Laboratory experiments simulate conditions of atmospheric processes like ageing or coating but are still idealized. Our method is able to measure ambient in-situ immersion freezing on single immersed aerosol particles. The instrumental setup consists of the recently developed portable immersion mode cooling chamber (PIMCA) as a vertical extension to the portable ice nucleation chamber (PINC, [1]), where the frozen fraction of activated aerosol particles are detected by the ice optical depolarization detector (IODE, [2]). Two additional immersion freezing techniques based on a droplet freezing array [3,4] are used to sample ambient aerosol particles either in a suspension (fraction larger ~0.6 μm) or on PM10-filters to compare different ice nucleation techniques. Here, we present ambient in-situ measurements at an urban forest site in Zurich, Switzerland held during the Zurich ambient immersion freezing study (ZAMBIS) in spring 2014. We investigated the ice nucleating ability of natural atmospheric aerosol with the PIMCA/PINC immersion freezing setup as well as a droplet freezing method on aerosol particles either collected in a suspension or on PM10-filters to obtain atmospheric IN concentrations based on the measured ambient aerosol. Investigation of physical properties (number and size distribution) and chemical composition as well as the meteorological conditions provide supplementary information that help to understand the nature of particles and air masses that contribute to immersion freezing. Acknowledgements We thank Hannes Wydler and Hansjörg Frei from ETH Zurich for their technical support. Furthermore, the authors want thank Franz Conen from the University of Basel for sharing equipment and training in the drop freezing experiment. References [1] Chou et al. (2011), Atmos. Chem. Phys., 11, 4725-4738. [2] Nicolet et al. (2010), Atmos. Chem. Phys., 10, 313-325. [3] Conen et al. (2012), Atmos. Meas. Tech., 5, 321-327. [4] Stopelli et al. (2014), Atmos. Meas. Tech., 7, 129-134.

Probing Individual Ice Nucleation Events with Environmental Scanning Electron Microscopy

NASA Astrophysics Data System (ADS)

Wang, Bingbing; China, Swarup; Knopf, Daniel; Gilles, Mary; Laskin, Alexander

2016-04-01

Heterogeneous ice nucleation is one of the processes of critical relevance to a range of topics in the fundamental and the applied science and technologies. Heterogeneous ice nucleation initiated by particles proceeds where microscopic properties of particle surfaces essentially control nucleation mechanisms. Ice nucleation in the atmosphere on particles governs the formation of ice and mixed phase clouds, which in turn influence the Earth's radiative budget and climate. Heterogeneous ice nucleation is still insufficiently understood and poses significant challenges in predictive understanding of climate change. We present a novel microscopy platform allowing observation of individual ice nucleation events at temperature range of 193-273 K and relative humidity relevant for ice formation in the atmospheric clouds. The approach utilizes a home built novel ice nucleation cell interfaced with Environmental Scanning Electron Microscope (IN-ESEM system). The IN-ESEM system is applied for direct observation of individual ice formation events, determining ice nucleation mechanisms, freezing temperatures, and relative humidity onsets. Reported microanalysis of the ice nucleating particles (INP) include elemental composition detected by the energy dispersed analysis of X-rays (EDX), and advanced speciation of the organic content in particles using scanning transmission x-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). The performance of the IN-ESEM system is validated through a set of experiments with kaolinite particles with known ice nucleation propensity. We demonstrate an application of the IN-ESEM system to identify and characterize individual INP within a complex mixture of ambient particles.

Heterogeneous ice nucleation of α-pinene SOA particles before and after ice cloud processing

NASA Astrophysics Data System (ADS)

Wagner, Robert; Höhler, Kristina; Huang, Wei; Kiselev, Alexei; Möhler, Ottmar; Mohr, Claudia; Pajunoja, Aki; Saathoff, Harald; Schiebel, Thea; Shen, Xiaoli; Virtanen, Annele

2017-05-01

The ice nucleation ability of α-pinene secondary organic aerosol (SOA) particles was investigated at temperatures between 253 and 205 K in the Aerosol Interaction and Dynamics in the Atmosphere cloud simulation chamber. Pristine SOA particles were nucleated and grown from pure gas precursors and then subjected to repeated expansion cooling cycles to compare their intrinsic ice nucleation ability during the first nucleation event with that observed after ice cloud processing. The unprocessed α-pinene SOA particles were found to be inefficient ice-nucleating particles at cirrus temperatures, with nucleation onsets (for an activated fraction of 0.1%) as high as for the homogeneous freezing of aqueous solution droplets. Ice cloud processing at temperatures below 235 K only marginally improved the particles' ice nucleation ability and did not significantly alter their morphology. In contrast, the particles' morphology and ice nucleation ability was substantially modified upon ice cloud processing in a simulated convective cloud system, where the α-pinene SOA particles were first activated to supercooled cloud droplets and then froze homogeneously at about 235 K. As evidenced by electron microscopy, the α-pinene SOA particles adopted a highly porous morphology during such a freeze-drying cycle. When probing the freeze-dried particles in succeeding expansion cooling runs in the mixed-phase cloud regime up to 253 K, the increase in relative humidity led to a collapse of the porous structure. Heterogeneous ice formation was observed after the droplet activation of the collapsed, freeze-dried SOA particles, presumably caused by ice remnants in the highly viscous material or the larger surface area of the particles.

Ice nucleation properties of atmospheric aerosol particles collected during a field campaign in Cyprus

NASA Astrophysics Data System (ADS)

Yordanova, Petya; Maier, Stefanie; Lang-Yona, Naama; Tamm, Alexandra; Meusel, Hannah; Pöschl, Ulrich; Weber, Bettina; Fröhlich-Nowoisky, Janine

2017-04-01

Atmospheric aerosol particles, including desert and soil dust as well as marine aerosols, are well known to act as ice nuclei (IN) and thus have been investigated in numerous ice nucleation studies. Based on their cloud condensation nuclei potential and their impacts on radiative properties of clouds (via scattering and absorption of solar radiation), aerosol particles may significantly affect the cloud and precipitation development. Atmospheric aerosols of the Eastern Mediterranean have been described to be dominated by desert dust, but only little is known on their composition and ice nucleating properties. In this study we investigated the ice nucleating ability of total suspended particles (TSP), collected at the remote site Agia Marina Xyliatou on Cyprus during a field campaign in April 2016. Airborne TSP samples containing air masses of various types such as African (Saharan) and Arabian dust and European and Middle Eastern pollution were collected on glass fiber filters at 24 h intervals. Sampling was performed ˜5 m above ground level and ˜521 m above sea level. During the sampling period, two major dust storms (PM 10max 118 μg/m3 and 66 μg/m3) and a rain event (rainfall amount: 3.4 mm) were documented. Chemical and physical characterizations of the particles were analyzed experimentally through filtration, thermal, chemical and enzyme treatments. Immersion freezing experiments were performed at relatively high subzero temperatures (-1 to -15˚ C) using the mono ice nucleation array. Preliminary results indicate that highest IN particle numbers (INPs) occurred during the second dust storm event with lower particle concentrations. Treatments at 60˚ C lead to a gradual IN deactivation, indicating the presence of biological INPs, which were observed to be larger than 300 kDa. Additional results originating from this study will be shown. Acknowledgement: This work was funded by the DFG Ice Nuclei Research Unit (INUIT).

Temperature Dependence in Homogeneous and Heterogeneous Nucleation

DOE Office of Scientific and Technical Information (OSTI.GOV)

McGraw R. L.; Winkler, P. M.; Wagner, P. E.

2017-08-01

Heterogeneous nucleation on stable (sub-2 nm) nuclei aids the formation of atmospheric cloud condensation nuclei (CCN) by circumventing or reducing vapor pressure barriers that would otherwise limit condensation and new particle growth. Aerosol and cloud formation depend largely on the interaction between a condensing liquid and the nucleating site. A new paper published this year reports the first direct experimental determination of contact angles as well as contact line curvature and other geometric properties of a spherical cap nucleus at nanometer scale using measurements from the Vienna Size Analyzing Nucleus Counter (SANC) (Winkler et al., 2016). For water nucleating heterogeneouslymore » on silver oxide nanoparticles we find contact angles around 15 degrees compared to around 90 degrees for the macroscopically measured equilibrium angle for water on bulk silver. The small microscopic contact angles can be attributed via the generalized Young equation to a negative line tension that becomes increasingly dominant with increasing curvature of the contact line. These results enable a consistent theoretical description of heterogeneous nucleation and provide firm insight to the wetting of nanosized objects.« less

Soot Aerosol Particles as Cloud Condensation Nuclei: from Ice Nucleation Activity to Ice Crystal Morphology

NASA Astrophysics Data System (ADS)

Pirim, Claire; Ikhenazene, Raouf; Ortega, Isamel Kenneth; Carpentier, Yvain; Focsa, Cristian; Chazallon, Bertrand; Ouf, François-Xavier

2016-04-01

Emissions of solid-state particles (soot) from engine exhausts due to incomplete fuel combustion is considered to influence ice and liquid water cloud droplet activation [1]. The activity of these aerosols would originate from their ability to be important centers of ice-particle nucleation, as they would promote ice formation above water homogeneous freezing point. Soot particles are reported to be generally worse ice nuclei than mineral dust because they activate nucleation at higher ice-supersaturations for deposition nucleation and at lower temperatures for immersion freezing than ratios usually expected for homogeneous nucleation [2]. In fact, there are still numerous opened questions as to whether and how soot's physico-chemical properties (structure, morphology and chemical composition) can influence their nucleation ability. Therefore, systematic investigations of soot aerosol nucleation activity via one specific nucleation mode, here deposition nucleation, combined with thorough structural and compositional analyzes are needed in order to establish any association between the particles' activity and their physico-chemical properties. In addition, since the morphology of the ice crystals can influence their radiative properties [3], we investigated their morphology as they grow over both soot and pristine substrates at different temperatures and humidity ratios. In the present work, Combustion Aerosol STandart soot samples were produced from propane using various experimental conditions. Their nucleation activity was studied in deposition mode (from water vapor), and monitored using a temperature-controlled reactor in which the sample's relative humidity is precisely measured with a cryo-hygrometer. Formation of water/ice onto the particles is followed both optically and spectroscopically, using a microscope coupled to a Raman spectrometer. Vibrational signatures of hydroxyls (O-H) emerge when the particle becomes hydrated and are used to characterize ice crystals. [1] Koop, T. Atmospheric water, Water: Fundamentals as the Basis for Understanding the Environment and Promoting Technology, 187, 45-75 (2015). [2] Hoose & Möhler. Atmospheric Chemistry and Physics. 12, 9817-9854. (2012) [3] Schumann et al. Journal of Applied Meteorology and Climatology. 51, 1391-1406 (2012)

Global Simulations of Ice nucleation and Ice Supersaturation with an Improved Cloud Scheme in the Community Atmosphere Model

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gettelman, A.; Liu, Xiaohong; Ghan, Steven J.

2010-09-28

A process-based treatment of ice supersaturation and ice-nucleation is implemented in the National Center for Atmospheric Research (NCAR) Community Atmosphere Model (CAM). The new scheme is designed to allow (1) supersaturation with respect to ice, (2) ice nucleation by aerosol particles and (3) ice cloud cover consistent with ice microphysics. The scheme is implemented with a 4-class 2 moment microphysics code and is used to evaluate ice cloud nucleation mechanisms and supersaturation in CAM. The new model is able to reproduce field observations of ice mass and mixed phase cloud occurrence better than previous versions of the model. Simulations indicatemore » heterogeneous freezing and contact nucleation on dust are both potentially important over remote areas of the Arctic. Cloud forcing and hence climate is sensitive to different formulations of the ice microphysics. Arctic radiative fluxes are sensitive to the parameterization of ice clouds. These results indicate that ice clouds are potentially an important part of understanding cloud forcing and potential cloud feedbacks, particularly in the Arctic.« less

Heterogeneous Formation of Polar Stratospheric Clouds- Part 1: Nucleation of Nitric Acid Trihydrate (NAT)

NASA Technical Reports Server (NTRS)

Hoyle, C. R.; Engel, I.; Luo, B. P.; Pitts, M. C.; Poole, L. R.; Grooss, J.-U.; Peter, T.

2013-01-01

Satellite-based observations during the Arctic winter of 2009/2010 provide firm evidence that, in contrast to the current understanding, the nucleation of nitric acid trihydrate (NAT) in the polar stratosphere does not only occur on preexisting ice particles. In order to explain the NAT clouds observed over the Arctic in mid-December 2009, a heterogeneous nucleation mechanism is required, occurring via immersion freezing on the surface of solid particles, likely of meteoritic origin. For the first time, a detailed microphysical modelling of this NAT formation pathway has been carried out. Heterogeneous NAT formation was calculated along more than sixty thousand trajectories, ending at Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) observation points. Comparing the optical properties of the modelled NAT with these observations enabled a thorough validation of a newly developed NAT nucleation parameterisation, which has been built into the Zurich Optical and Microphysical box Model (ZOMM). The parameterisation is based on active site theory, is simple to implement in models and provides substantial advantages over previous approaches which involved a constant rate of NAT nucleation in a given volume of air. It is shown that the new method is capable of reproducing observed polar stratospheric clouds (PSCs) very well, despite the varied conditions experienced by air parcels travelling along the different trajectories. In a companion paper, ZOMM is applied to a later period of the winter, when ice PSCs are also present, and it is shown that the observed PSCs are also represented extremely well under these conditions.

First Principles Simulations of Ice Nucleation at Metal Surfaces

NASA Astrophysics Data System (ADS)

Michaelides, Angelos

2005-03-01

Ice nucleation at solid surfaces is of relevance to countless scientific and technological processes. In particular the nucleation of ice nano-crystals on metal surfaces is often a key first step in cloud formation and corrosion [1]. Yet unfortunately this remains one of the most poorly understood natural phenomena; severely lacking in atomic level understanding. Here, we discuss detailed density functional theory studies aimed at putting our understanding of ice nucleation at metals on a much firmer footing. Specifically the properties of H2O hexamers - the smallest `building blocks' of ice - adsorbed on a number of close-packed transition metal surfaces have been examined. We find that the competing influences of substrate reactivity and hexamer-substrate epitaxial mismatch conspire to yield a rich variety of (novel) hexameric ice structures, some of which have been observed by recent scanning tunnelling microscopy experiments [2]. [1] H.R. Pruppacher and J.D. Klett, Microphysics of Clouds and Precipitation, (Kluwer, Dordrecht, 2003). [2] K. Morgenstern, et al., (To be published).

New particle formation leads to cloud dimming

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sullivan, Ryan C.; Crippa, Paola; Matsui, Hitoshi

New particle formation (NPF), nucleation of condensable vapors to the solid or liquid phase, is a significant source of atmospheric aerosol particle number concentrations. With sufficient growth, these nucleated particles may be a significant source of cloud condensation nuclei (CCN), thus altering cloud albedo, structure, and lifetimes, and insolation reaching the Earth's surface. Herein we present one of the first numerical experiments to quantify the impact of NPF on cloud radiative properties that is conducted at a convection permitting resolution and that explicitly simulates cloud droplet number concentrations. Consistent with observations, these simulations suggest that in spring over the Midwesternmore » U.S.A., NPF occurs frequently and on regional scales. However, the simulations suggest that NPF is not associated with enhancement of regional cloud albedos as would be expected from an increase of CCN. These simulations indicate that NPF reduces ambient sulfuric acid concentrations sufficiently to inhibit growth of preexisting particles to CCN sizes. This reduction in CCN-sized particles reduces cloud albedo, resulting in a domain average positive top of atmosphere cloud radiative forcing of 10 W m-2 and up to ~ 50 W m-2 in individual grid cells relative to a simulation in which NPF is excluded.« less

New approaches to quantifying aerosol influence on the cloud radiative effect

DOE PAGES

Feingold, Graham; McComiskey, Allison; Yamaguchi, Takanobu; ...

2016-02-01

The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol–cloud interactions at ever-increasing levels of detail, but these models lack the resolution tomore » represent clouds and aerosol–cloud interactions adequately. There is a dearth of observational constraints on aerosol–cloud interactions. In this paper, we develop a conceptual approach to systematically constrain the aerosol–cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. Finally, we heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol–cloud radiation system.« less

New approaches to quantifying aerosol influence on the cloud radiative effect

PubMed Central

Feingold, Graham; McComiskey, Allison; Yamaguchi, Takanobu; Johnson, Jill S.; Carslaw, Kenneth S.; Schmidt, K. Sebastian

2016-01-01

The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol−cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol−cloud interactions adequately. There is a dearth of observational constraints on aerosol−cloud interactions. We develop a conceptual approach to systematically constrain the aerosol−cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol−cloud radiation system. PMID:26831092

New approaches to quantifying aerosol influence on the cloud radiative effect.

PubMed

Feingold, Graham; McComiskey, Allison; Yamaguchi, Takanobu; Johnson, Jill S; Carslaw, Kenneth S; Schmidt, K Sebastian

2016-05-24

The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol-cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol-cloud interactions adequately. There is a dearth of observational constraints on aerosol-cloud interactions. We develop a conceptual approach to systematically constrain the aerosol-cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol-cloud radiation system.

Optical nucleation of bubble clouds in a high pressure spherical resonator.

PubMed

Anderson, Phillip; Sampathkumar, A; Murray, Todd W; Gaitan, D Felipe; Glynn Holt, R

2011-11-01

An experimental setup for nucleating clouds of bubbles in a high-pressure spherical resonator is described. Using nanosecond laser pulses and multiple phase gratings, bubble clouds are optically nucleated in an acoustic field. Dynamics of the clouds are captured using a high-speed CCD camera. The images reveal cloud nucleation, growth, and collapse and the resulting emission of radially expanding shockwaves. These shockwaves are reflected at the interior surface of the resonator and then reconverge to the center of the resonator. As the shocks reconverge upon the center of the resonator, they renucleate and grow the bubble cloud. This process is repeated over many acoustic cycles and with each successive shock reconvergence, the bubble cloud becomes more organized and centralized so that subsequent collapses give rise to stronger, better defined shockwaves. After many acoustic cycles individual bubbles cannot be distinguished and the cloud is then referred to as a cluster. Sustainability of the process is ultimately limited by the detuning of the acoustic field inside the resonator. The nucleation parameter space is studied in terms of laser firing phase, laser energy, and acoustic power used.

Modelling heterogeneous ice nucleation on mineral dust and soot with parameterizations based on laboratory experiments

NASA Astrophysics Data System (ADS)

Hoose, C.; Hande, L. B.; Mohler, O.; Niemand, M.; Paukert, M.; Reichardt, I.; Ullrich, R.

2016-12-01

Between 0 and -37°C, ice formation in clouds is triggered by aerosol particles acting as heterogeneous ice nuclei. At lower temperatures, heterogeneous ice nucleation on aerosols can occur at lower supersaturations than homogeneous freezing of solutes. In laboratory experiments, the ability of different aerosol species (e.g. desert dusts, soot, biological particles) has been studied in detail and quantified via various theoretical or empirical parameterization approaches. For experiments in the AIDA cloud chamber, we have quantified the ice nucleation efficiency via a temperature- and supersaturation dependent ice nucleation active site density. Here we present a new empirical parameterization scheme for immersion and deposition ice nucleation on desert dust and soot based on these experimental data. The application of this parameterization to the simulation of cirrus clouds, deep convective clouds and orographic clouds will be shown, including the extension of the scheme to the treatment of freezing of rain drops. The results are compared to other heterogeneous ice nucleation schemes. Furthermore, an aerosol-dependent parameterization of contact ice nucleation is presented.

Final Technical Report for Award SC0008613

DOE Office of Scientific and Technical Information (OSTI.GOV)

Knopf, Daniel A.

Discovering how aerosol particles, present in the atmosphere in sizes of a few nanometers to hundred micrometers, initiate ice crystal formation represents a great challenge. Atmospheric ice nucleation is important because ice crystals alter the radiative properties of clouds and thus climate, and impact precipitation and thus the hydrological cycle. The difficulty in predicting atmospheric ice formation is attributable at least in part, to the diversity of ice nucleation pathways, the physical and chemical complexity of the ice nucleating particles (INPs), and the relatively small numbers of INPs (compared with all other aerosol particles), sometimes less than one in 100000.more » These factors in turn makes constraining ice nucleation parameterizations for modeling applications challenging. The majority of airborne particles are known to be organic in nature or contain organic biogenic material. The presence of organic material adds to the complexity of the particles and therefore the predictability of ice nucleation events since the organic species can display different phase states, e.g. liquid or solid, in response to temperature and humidity. The award DE-SC0008613 to PI Prof. Daniel Knopf at Stony Brook University, “Relating the Chemical and Physical Properties of Aerosols to the Water Uptake and Ice Nucleation Potential of Particles Collected During the Carbonaceous Aerosols and Radiative Effects Study (CARES)”, allowed examination of laboratory generated aerosol particles and field-collected particles for their propensity to nucleate ice under typical tropospheric conditions and relate ice nucleation to the physicochemical properties of the particles including their morphology and chemical composition. This in turn allowed for development of ice nucleation parameterizations for implementation in cloud models. The award resulted in 10 peer-reviewed publications and more than 20 seminar and conference presentations. We demonstrated that the rate of immersion freezing, when a particle immersed in an aqueous droplet acts as an ice nucleus (IN), can be predicted by knowledge of the IN particle type present and the droplet’s water activity which is equal to ambient relative humidity. Our water activity based immersion freezing model is successful in predicting freezing data including INPs such as mineral dusts, marine biological material, organic species, and surfactant molecules. Its mathematical simplicity makes it an ideal candidate for implementation in cloud and climate models. Furthermore, we could show that this model can reproduce many past laboratory measurements which were generated using a variety of instruments to study immersion freezing. Lastly, we have demonstrated that this model can also be applied to field collected particles. Currently, this novel physical parameterization of immersion freezing is being implemented in a cloud model. We examined the physicochemical properties and the ice nucleation potential of particles collected during CARES applying a novel experimental method that allows identification of the individual INPs within a large population of particles sampled from an ambient environment. Taking advantage of a variety of micro-spectroscopic techniques, we characterized the composition and morphology of IN and non-IN particles present in the airborne population. We developed a new parameterization for quantifying the mixing state of the entire aerosol populations by introducing a mixing state index. We found that the identified INPs belong to the most common particle-type classes observed in the CARES field samples and as such are not special or rare particles. In other words, the INPs can be shown not to be unique in contrast to the common paradigm of being rare and exceptional. Either there are differences between particles acting as IN and particles not acting as IN which are beyond our current detection limit or nucleation occurs randomly on the surface of any one of these compositionally equivalent particles. These results suggest that total particle surface area of the different particle types present in the aerosol population is also a crucial factor when predicting ice nucleation in an air mass. We also observed that ambient organic aerosol particles can initiate ice nucleation and corroborated these findings using laboratory generated organic particles. These experiments demonstrated that information of the organic phase state is important for predicting the ice nucleation pathway and the ability of an organic particle to participate in atmospheric ice crystal formation. This award resulted in substantial new insights in the processes governing immersion freezing, the role of organic aerosol particles in ice cloud formation, and the importance of the ambient aerosol population for prediction of ice nucleation in an air parcel. These findings have significant implications for modeling and field measurement strategies of atmospheric ice nucleation.« less

Cloud chamber experiments on the origin of ice crystal complexity in cirrus clouds

NASA Astrophysics Data System (ADS)

Schnaiter, Martin; Järvinen, Emma; Vochezer, Paul; Abdelmonem, Ahmed; Wagner, Robert; Jourdan, Olivier; Mioche, Guillaume; Shcherbakov, Valery N.; Schmitt, Carl G.; Tricoli, Ugo; Ulanowski, Zbigniew; Heymsfield, Andrew J.

2016-04-01

This study reports on the origin of small-scale ice crystal complexity and its influence on the angular light scattering properties of cirrus clouds. Cloud simulation experiments were conducted at the AIDA (Aerosol Interactions and Dynamics in the Atmosphere) cloud chamber of the Karlsruhe Institute of Technology (KIT). A new experimental procedure was applied to grow and sublimate ice particles at defined super- and subsaturated ice conditions and for temperatures in the -40 to -60 °C range. The experiments were performed for ice clouds generated via homogeneous and heterogeneous initial nucleation. Small-scale ice crystal complexity was deduced from measurements of spatially resolved single particle light scattering patterns by the latest version of the Small Ice Detector (SID-3). It was found that a high crystal complexity dominates the microphysics of the simulated clouds and the degree of this complexity is dependent on the available water vapor during the crystal growth. Indications were found that the small-scale crystal complexity is influenced by unfrozen H2SO4 / H2O residuals in the case of homogeneous initial ice nucleation. Angular light scattering functions of the simulated ice clouds were measured by the two currently available airborne polar nephelometers: the polar nephelometer (PN) probe of Laboratoire de Métérologie et Physique (LaMP) and the Particle Habit Imaging and Polar Scattering (PHIPS-HALO) probe of KIT. The measured scattering functions are featureless and flat in the side and backward scattering directions. It was found that these functions have a rather low sensitivity to the small-scale crystal complexity for ice clouds that were grown under typical atmospheric conditions. These results have implications for the microphysical properties of cirrus clouds and for the radiative transfer through these clouds.

Can we define an asymptotic value for the ice active surface site density for heterogeneous ice nucleation?

NASA Astrophysics Data System (ADS)

Niedermeier, Dennis; Augustin-Bauditz, Stefanie; Hartmann, Susan; Wex, Heike; Ignatius, Karoliina; Stratmann, Frank

2015-04-01

The formation of ice in atmospheric clouds has a substantial influence on the radiative properties of clouds as well as on the formation of precipitation. Therefore much effort has been made to understand and quantify the major ice formation processes in clouds. Immersion freezing has been suggested to be a dominant primary ice formation process in low and mid-level clouds (mixed-phase cloud conditions). It also has been shown that mineral dust particles are the most abundant ice nucleating particles in the atmosphere and thus may play an important role for atmospheric ice nucleation (Murray et al., 2012). Additionally, biological particles like bacteria and pollen are suggested to be potentially involved in atmospheric ice formation, at least on a regional scale (Murray et al., 2012). In recent studies for biological particles (SNOMAX and birch pollen), it has been demonstrated that freezing is induced by ice nucleating macromolecules and that an asymptotic value for the mass density of these ice nucleating macromolecules can be determined (Hartmann et al., 2013; Augustin et al., 2013, Wex et al., 2014). The question arises whether such an asymptotic value can also be determined for the ice active surface site density ns, a parameter which is commonly used to describe the ice nucleation activity of e.g., mineral dust. Such an asymptotic value for ns could be an important input parameter for atmospheric modeling applications. In the presented study, we therefore investigated the immersion freezing behavior of droplets containing size-segregated, monodisperse feldspar particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). For all particle sizes considered in the experiments, we observed a leveling off of the frozen droplet fraction reaching a plateau within the heterogeneous freezing temperature regime (T > -38°C) which was proportional to the particle surface area. Based on these findings, we could determine an asymptotic value for the ice active surface site density, which we named ns*, for the investigated feldspar sample. The comparison of these results with those of other studies elucidates the general feasibility of determining such an asymptotic value and also show that the value of ns* strongly depends on the method of the particle surface area determination. Acknowledgement This work is partly funded by the Federal Ministry of Education and Research (BMBF - project CLOUD 12) and by the German Research Foundation (DFG project WE 4722/1-1, part of the research unit INUIT, FOR 1525). D. Niedermeier acknowledges financial support from the Alexander von Humboldt-foundation. References Augustin et al.: Immersion freezing of birch pollen washing water, Atmos. Chem. Phys., 13, 10989-11003, doi:10.5194/acp-13-10989-2013, 2013. Hartmann et al.: Immersion freezing of ice nucleation active protein complexes, Atmos. Chem. Phys., 13, 5751-5766, doi:10.5194/acp-13-5751-2013, 2013. Murray et al.: Ice nucleation by particles immersed in supercooled cloud droplets, Chem. Soc. Rev., 41, 6519-6554, 2012. Wex et al.: Intercomparing different devices for the investigation of ice nucleating particles using Snomax® as test substance, Atmos. Chem. Phys. Discuss., 14, 22321-22384, doi:10.5194/acpd-14-22321-2014, 2014.

Heterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of α-pinene

NASA Astrophysics Data System (ADS)

Ignatius, Karoliina; Kristensen, Thomas B.; Järvinen, Emma; Nichman, Leonid; Fuchs, Claudia; Gordon, Hamish; Herenz, Paul; Hoyle, Christopher R.; Duplissy, Jonathan; Garimella, Sarvesh; Dias, Antonio; Frege, Carla; Höppel, Niko; Tröstl, Jasmin; Wagner, Robert; Yan, Chao; Amorim, Antonio; Baltensperger, Urs; Curtius, Joachim; Donahue, Neil M.; Gallagher, Martin W.; Kirkby, Jasper; Kulmala, Markku; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Tomé, Antonio; Virtanen, Annele; Worsnop, Douglas; Stratmann, Frank

2016-05-01

There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate heterogeneous ice nucleation and thus influence cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles. The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from -38 to -10 °C at 5-15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between -39.0 and -37.2 °C ranged from 6 to 20 % and did not depend on the particle surface area. Global modelling of monoterpene SOA particles suggests that viscous biogenic SOA particles are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nucleating particle budget.

The impact on UT/LS cirrus clouds in the CAM/CARMA model using a new interactive aerosol parameterization.

NASA Astrophysics Data System (ADS)

Maloney, C.; Toon, B.; Bardeen, C.

2017-12-01

Recent studies indicate that heterogeneous nucleation may play a large role in cirrus cloud formation in the UT/LS, a region previously thought to be primarily dominated by homogeneous nucleation. As a result, it is beneficial to ensure that general circulation models properly represent heterogeneous nucleation in ice cloud simulations. Our work strives towards addressing this issue in the NSF/DOE Community Earth System Model's atmospheric model, CAM. More specifically we are addressing the role of heterogeneous nucleation in the coupled sectional microphysics cloud model, CARMA. Currently, our CAM/CARMA cirrus model only performs homogenous ice nucleation while ignoring heterogeneous nucleation. In our work, we couple the CAM/CARMA cirrus model with the Modal Aerosol Model (MAM). By combining the aerosol model with CAM/CARMA we can both account for heterogeneous nucleation, as well as directly link the sulfates used for homogeneous nucleation to computed fields instead of the current static field being utilized. Here we present our initial results and compare our findings to observations from the long running CALIPSO and MODIS satellite missions.

The role of marine organic ice nuclei in a global climate model

NASA Astrophysics Data System (ADS)

Hummel, Matthias; Egill Kristjansson, Jon

2016-04-01

Ice particle concentrations are a key parameter for cold clouds, exerting a strong influence on cloud lifetime, precipitation release, and the cloud radiative effect. The availability of ice-nucleating particles (INPs) and the temperature range in which they become activated determine the rate of ice formation in clouds (Hoose und Möhler, 2012). Particles from marine sources may contribute to ice formation in clouds, as they are abundant in the atmosphere and some of them have been found to be ice-nucleating active, but the extent of their influence on clouds is not known (Wilson et al., 2015). Wilson et al. (2015) collected marine INPs from the sea surface microlayer and analyzed their ice nucleation efficiency with a cold stage. Even in cirrus clouds, marine INPs may play a role, as their ice nucleation surface site density as a function of RHice at -40° C has been shown to be larger than for mineral dusts (ATD, kaolinite, and feldspar). In this study, we test the influence of marine organic aerosols on clouds via immersion freezing with the earth system model NorESM2 (Version 2 of the Norwegian Earth System Model; Bentsen et al., 2013). The model is based on the Community Earth System Model (CESM1.2) and its atmospheric part (CAM5 Oslo) is based on the Community Atmosphere Model (CAM5.3). The parameterization of ice nucleation of marine INPs is expressed as an exponential function of temperature multiplied by the total organic content. Marine organic aerosols are part of the sea spray aerosol and are ejected during bubble bursting. INPs are associated with exudates or other macromolecules mainly from diatoms. Hence, their concentration is related to the sea salt aerosols in the model simulation. Our first results indicate that the high marine INP concentrations at around 850 hPa occur at high latitudes. These regions have low mineral dust concentrations, which might increase the influence of marine INP on clouds. However, they do not coincide with regions of high winds and therefore large sea spray aerosol concentrations, contrary to model simulations in Wilson et al. (2015) with the global aerosol process model (GLOMAP), but are shifted further polewards. Therefore, marine INP concentrations strongly depend on temperature and do not necessarily coincide with large sea spray concentrations. At mid-latitudes, marine INP concentrations rank below dust INP by at least one order of magnitude. Further, this presentation will describe the influence of marine INP on cloud properties and give an estimate of the cloud radiative effect of marine INP. Bentsen, M., I. Bethke, et al. (2013): The Norwegian Earth System Model, NorESM1-M - Part 1: Description and basic evaluation of the physical climate, Geosci. Model Dev. 6(3): 687-720. Hoose, C. und O. Möhler (2012): Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments, Atmos. Chem. Phys. 12(20): 9817-9854. Wilson, T. W., L. A. Ladino, et al. (2015): A marine biogenic source of atmospheric ice-nucleating particles, Nature 525(7568): 234-238.

Internally mixed sulfate and organic particles as potential ice nuclei in the tropical tropopause region

PubMed Central

Tolbert, Margaret A.

2010-01-01

Cirrus clouds are ubiquitous in the tropical tropopause region and play a major role in the Earth’s climate. Any changes to cirrus abundance due to natural or anthropogenic influences must be considered to evaluate future climate change. The detailed impact of cirrus clouds on climate depends on ice particle number, size, morphology, and composition. These properties depend in turn on the nucleation mechanism of the ice particles. Although it is often assumed that ice nucleates via a homogeneous mechanism, recent work points to the possibility that heterogeneous ice nucleation is important in the tropical tropopause region. However, there are very few studies of depositional ice nucleation on the complex types of particles likely to be found in this region of the atmosphere. Here, we use a unique method to probe depositional ice nucleation on internally mixed ammonium sulfate/palmitic acid particles, namely optical microscopy coupled with Raman microscopy. The deliquescence and efflorescence phase transitions of the mixed particles were first studied to gain insight into whether the particles are likely to be liquid or solid in the tropical tropopause region. The ice nucleating ability of the particles was then measured under typical upper tropospheric conditions. It was found that coating the particles with insoluble palmitic acid had little effect on the deliquescence, efflorescence, or ice nucleating ability of ammonium sulfate. Additional experiments involving Raman mapping provide new insights into how the composition and morphology of mixed particles impact their ability to nucleate ice. PMID:20388912

Midlatitude Cirrus Clouds Derived from Hurricane Nora: A Case Study with Implications for Ice Crystal Nucleation and Shape.

NASA Astrophysics Data System (ADS)

Sassen, Kenneth; Arnott, W. Patrick; O'C. Starr, David; Mace, Gerald G.; Wang, Zhien; Poellot, Michael R.

2003-04-01

Hurricane Nora traveled up the Baja Peninsula coast in the unusually warm El Niño waters of September 1997 until rapidly decaying as it approached southern California on 24 September. The anvil cirrus blowoff from the final surge of tropical convection became embedded in subtropical flow that advected the cirrus across the western United States, where it was studied from the Facility for Atmospheric Remote Sensing (FARS) in Salt Lake City, Utah, on 25 September. A day later, the cirrus shield remnants were redirected southward by midlatitude circulations into the southern Great Plains, providing a case study opportunity for the research aircraft and ground-based remote sensors assembled at the Clouds and Radiation Testbed (CART) site in northern Oklahoma. Using these comprehensive resources and new remote sensing cloud retrieval algorithms, the microphysical and radiative cloud properties of this unusual cirrus event are uniquely characterized.Importantly, at both the FARS and CART sites the cirrus generated spectacular halos and arcs, which acted as a tracer for the hurricane cirrus, despite the limited lifetimes of individual ice crystals. Lidar depolarization data indicate widespread regions of uniform ice plate orientations, and in situ particle replicator data show a preponderance of pristine, solid hexagonal plates and columns. It is suggested that these unusual aspects are the result of the mode of cirrus particle nucleation, presumably involving the lofting of sea salt nuclei in strong thunderstorm updrafts into the upper troposphere. This created a reservoir of haze particles that continued to produce halide-salt-contaminated ice crystals during the extended period of cirrus cloud maintenance. The inference that marine microbiota are embedded in the replicas of some ice crystals collected over the CART site points to the longevity of marine effects. Various nucleation scenarios proposed for cirrus clouds based on this and other studies, and the implications for understanding cirrus radiative properties on a global scale, are discussed.

Midlatitude Cirrus Clouds Derived from Hurricane Nora: A Case Study with Implications for Ice Crystal Nucleation and Shape

NASA Technical Reports Server (NTRS)

Sassen, Kenneth; Arnott, W. Patrick; OCStarr, David; Mace, Gerald G.; Wang, Zhien; Poellot, Michael R.

2002-01-01

Hurricane Nora traveled up the Bala Peninsula coast in the unusually warm El Nino waters of September 1997, until rapidly decaying as it approached Southern California on 24 September. The anvil cirrus blowoff from the final surge of tropical convection became embedded in subtropical flow that advected the cirrus across the western US, where it was studied from the Facility for Atmospheric Remote Sensing (FARS) in Salt Lake City, Utah. A day later, the cirrus shield remnants were redirected southward by midlatitude circulations into the Southern Great Plains, providing a case study opportunity for the research aircraft and ground-based remote sensors assembled at the Clouds and Radiation Testbed (CART) site in northern Oklahoma. Using these comprehensive resources and new remote sensing cloud retrieval algorithms, the microphysical and radiative cloud properties of this unusual cirrus event are uniquely characterized. Importantly, at both the FARS and CART sites the cirrus generated spectacular optical displays, which acted as a tracer for the hurricane cirrus, despite the limited lifetimes of individual ice crystals. Lidar polarization data indicate widespread regions of uniform ice plate orientations, and in situ particle masticator data show a preponderance of pristine, solid hexagonal plates and columns. It is suggested that these unusual aspects are the result of the mode of cirrus particle nucleation, presumably involving the lofting of sea-salt nuclei in thunderstorm updrafts into the upper troposphere. This created a reservoir of haze particles that continued to produce halide-saltcontaminated ice crystals during the extended period of cirrus cloud maintenance. The reference that marine microliters are embedded in the replicas of ice crystals collected over the CART site points to the longevity of marine effects. Various nucleation scenarios proposed for cirrus clouds based on this and other studies, and the implications for understanding cirrus radiative properties or a global scale, are discussed.

Thermodynamic Derivation of the Activation Energy for Ice Nucleation

NASA Technical Reports Server (NTRS)

Barahona, D.

2015-01-01

Cirrus clouds play a key role in the radiative and hydrological balance of the upper troposphere. Their correct representation in atmospheric models requires an understanding of the microscopic processes leading to ice nucleation. A key parameter in the theoretical description of ice nucleation is the activation energy, which controls the flux of water molecules from the bulk of the liquid to the solid during the early stages of ice formation. In most studies it is estimated by direct association with the bulk properties of water, typically viscosity and self-diffusivity. As the environment in the ice-liquid interface may differ from that of the bulk, this approach may introduce bias in calculated nucleation rates. In this work a theoretical model is proposed to describe the transfer of water molecules across the ice-liquid interface. Within this framework the activation energy naturally emerges from the combination of the energy required to break hydrogen bonds in the liquid, i.e., the bulk diffusion process, and the work dissipated from the molecular rearrangement of water molecules within the ice-liquid interface. The new expression is introduced into a generalized form of classical nucleation theory. Even though no nucleation rate measurements are used to fit any of the parameters of the theory the predicted nucleation rate is in good agreement with experimental results, even at temperature as low as 190 K, where it tends to be underestimated by most models. It is shown that the activation energy has a strong dependency on temperature and a weak dependency on water activity. Such dependencies are masked by thermodynamic effects at temperatures typical of homogeneous freezing of cloud droplets; however, they may affect the formation of ice in haze aerosol particles. The new model provides an independent estimation of the activation energy and the homogeneous ice nucleation rate, and it may help to improve the interpretation of experimental results and the development of parameterizations for cloud formation.

The competition between mineral dust and soot ice nuclei in mixed-phase clouds (Invited)

NASA Astrophysics Data System (ADS)

Murray, B. J.; Atkinson, J.; Umo, N.; Browse, J.; Woodhouse, M. T.; Whale, T.; Baustian, K. J.; Carslaw, K. S.; Dobbie, S.; O'Sullivan, D.; Malkin, T. L.

2013-12-01

The amount of ice present in mixed-phase clouds, which contain both supercooled liquid water droplets and ice particles, affects cloud extent, lifetime, particle size and radiative properties. The freezing of cloud droplets can be catalysed by the presence of aerosol particles known as ice nuclei. In this talk our recent laboratory and global aerosol modelling work on mineral dust and soot ice nuclei will be presented. We have performed immersion mode experiments to quantify ice nucleation by the individual minerals which make up desert mineral dusts and have shown that the feldspar component, rather than the clay component, is most important for ice nucleation (Atkinson et al. 2013). Experiments with well-characterised soot generated with eugenol, an intermediate in biomass burning, and n-decane show soot has a significant ice nucleation activity in mixed-phase cloud conditions. Our results for soot are in good agreement with previous results for acetylene soot (DeMott, 1990), but extend the efficiency to much higher temperatures. We then use a global aerosol model (GLOMAP) to map the distribution of soot and feldspar particles on a global basis. We show that below about -15oC that dust and soot together can explain most observed ice nuclei in the Earth's atmosphere, while at warmer temperatures other ice nuclei types are needed. We show that in some regions soot is the most important ice nuclei (below -15oC), while in others feldspar dust dominates. Our results suggest that there is a strong anthropogenic contribution to the ice nuclei population, since a large proportion of soot aerosol in the atmosphere results from human activities. Atkinson, J. D., Murray, B. J., Woodhouse, M. T., Carslaw, K. S., Whale, T. F., Baustian, K. J., Dobbie, S., O'Sullivan, D., and Malkin, T. L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds, Nature, 10.1038/nature12278, (2013). Demott, P. J. 1990. An Exploratory-Study of Ice Nucleation by Soot Aerosols. Journal of Applied Meteorology, 29, 1072-1079.

Modeling Studying the Role of Bacteria on ice Nucleation Processes

NASA Astrophysics Data System (ADS)

Sun, J.

2006-12-01

Certain air-borne bacteria have been recognized as active ice nuclei at the temperatures warm than - 10°C. Ice nucleating bacteria commonly found in plants and ocean surface. These ice nucleating bacteria are readily disseminated into the atmosphere and have been observed in clouds and hailstones, and their importance in cloud formation process and precipitation, as well as causing diseases in plants and animal kingdom, have been considered for over two decades, but their significance in atmospheric processes are yet to be understood. A 1.5-D non-hydrostatic cumulus cloud model with bin-resolved microphysics is developed and is to used to examine the relative importance of sulphate aerosol concentrations on the evolution of cumulus cloud droplet spectra and ice multiplication process, as well as ice initiation process by ice nucleating bacteria in the growing stage of cumulus clouds and the key role of this process on the ice multiplication in the subsequent dissipating stage of cumulus clouds. In this paper, we will present some sensitivity test results of the evolution of cumulus cloud spectra, ice concentrations at various concentrations of sulfate aerosols, and at different ideal sounding profiles. We will discuss the implication of our results in understanding of ice nucleation processes.

Heterogeneous chemistry of atmospheric mineral dust particles and their resulting cloud-nucleation properties

NASA Astrophysics Data System (ADS)

Sullivan, Ryan Christopher

Mineral dust particles are a major component of tropospheric aerosol mass and affect regional and global atmospheric chemistry and climate. Dust particles experience heterogeneous reactions with atmospheric gases that alter the gas and particle-phase chemistry. These in turn influence the warm and cold cloud nucleation ability and optical properties of the dust particles. This dissertation investigates the atmospheric chemistry of mineral dust particles and their role in warm cloud nucleation through a combination of synergistic field measurements, laboratory experiments, and theoretical modeling. In-situ measurements made with a single-particle mass spectrometer during the ACE-Asia field campaign in 2001 provide the motivation for this work. The observed mixing state of the individual ambient particles with secondary organic and inorganic components is described in Chapter 2. A large Asian dust storm occurred during the campaign and produced dramatic changes in the aerosol's composition and mixing state. The effect of particle size and mineralogy on the atmospheric processing of individual dust particles is explored in Chapters 3 & 4. Sulfate was found to accumulate preferentially in submicron iron and aluminosilicate-rich dust particles, while nitrate and chloride were enriched in supermicron calcite-rich dust. The mineral dust (and sea salt particles) were also enriched in oxalic acid, the dominant component of water soluble organic carbon. Chapter 5 explores the roles of gas-phase photochemistry and partitioning of the diacids to the alkaline particles in producing this unique behavior. The effect of the dust's mixing state with secondary organic and inorganic components on the dust particles' solubility, hygroscopicity, and thus warm cloud nucleation properties is explored experimentally and theoretically in Chapter 6. Cloud condensation nucleation (CCN) activation curves revealed that while calcium nitrate and calcium chloride particles were very hygroscopic and CCN-active, due to the high solubility of these compounds, calcium sulfate and calcium oxalate were not. Particles composed of these two sparingly soluble compounds had apparent hygroscopicities similar to pure calcium carbonate. This implies that the commonly made assumption that all dust particles become more hygroscopic after atmospheric processing must be revisited. Calcium sulfate and oxalate represent two forms of aged mineral dust particles that remain non-hygroscopic and thus have poor CCN nucleation ability. The particle generation method (dry versus wet) was found to significantly affect the chemistry and hygroscopicity of the aerosolized particles. Finally, in Chapter 7 the timescale for the atmospheric conversion of insoluble calcite particles to soluble, CCN-active calcium nitrate particles was derived from aerosol flow tube experiments. The reaction rate is rapid was used to estimate the conversion of calcite particles to very hygroscopic particles can occur in just a few hours of exposure to tropospheric levels of nitric acid. This process will therefore be controlled by the availability of nitric acid and its precursors, as opposed to the available atmospheric reaction time.

Spatial and temporal distributions of ice nucleating particles during the Atmospheric Radiation Measurement (ARM) Cloud Aerosol Precipitation Experiment (ACAPEX)

NASA Astrophysics Data System (ADS)

Levin, E. J.; DeMott, P. J.; Suski, K. J.; Boose, Y.; Hill, T. C. J.; McCluskey, C. S.; Schill, G. P.; Duncan, D.; Al-Mashat, H.; Prather, K. A.; Sedlacek, A. J., III; Tomlinson, J. M.; Mei, F.; Hubbe, J. M.; Pekour, M. S.; Leung, L. R.; Kreidenweis, S. M.

2016-12-01

California is currently under drought conditions and changes in precipitation due to future climate change scenarios are uncertain. Thus, understanding the controlling factors for precipitation in this region, and having the capability to accurately model these scenarios, is important. A crucial area in understanding precipitation is in the interplay between atmospheric moisture and aerosols. Specifically, ice nucleation in clouds is an important process controlling precipitation formation. A major component of CA's yearly precipitation comes from wintertime atmospheric river (AR) events which were the focus of the 2015 Atmospheric Radiation Measurement (ARM) Cloud Aerosol Precipitation Experiment (ACAPEX) and CalWater 2 campaigns. These two campaigns provided sampling platforms on four aircraft, including the ARM Aerial Facility G-1, as well as the NOAA Ron Brown research vessel and at a ground station at Bodega Bay, CA. Measurements of ice nucleating particles (INPs) were made with the Colorado State University (CSU) Continuous Flow Diffusion Chamber (CFDC) aboard the G-1 and at Bodega Bay, and using aerosol filter collections on these platforms as well as the Ron Brown for post-processing via immersion freezing in the CSU Ice Spectrometer. Aerosol composition was measured aboard the G-1 with the Aerosol Time-of-Flight Mass Spectrometer (ATOFMS). Both the CFDC and ATOFMS sampled off of an isokinetic inlet when flying in clear air and a counter-flow virtual impactor in clouds to capture ice crystal and cloud droplet residuals. In this presentation we present ice nucleating particle concentrations before, during and after an AR event from air, ground and ocean-based measurements. We also examine INP concentration variability in orographic clouds and in clear air at altitude along the Sierra Nevada range, in the marine boundary layer and through the Central Valley, and relate these INP measurements to other aerosol physical and chemical properties.

Effects of surface-active organic matter on carbon dioxide nucleation in atmospheric wet aerosols: a molecular dynamics study.

PubMed

Daskalakis, Vangelis; Charalambous, Fevronia; Panagiotou, Fostira; Nearchou, Irene

2014-11-21

Organic matter (OM) uptake in cloud droplets produces water-soluble secondary organic aerosols (SOA) via aqueous chemistry. These play a significant role in aerosol properties. We report the effects of OM uptake in wet aerosols, in terms of the dissolved-to-gas carbon dioxide nucleation using molecular dynamics (MD) simulations. Carbon dioxide has been implicated in the natural rainwater as well as seawater acidity. Variability of the cloud and raindrop pH is assumed in space and time, as regional emissions, local human activities and geophysical characteristics differ. Rain scavenging of inorganic SOx, NOx and NH3 plays a major role in rain acidity in terms of acid-base activity, however carbon dioxide solubility also remains a key parameter. Based on the MD simulations we propose that the presence of surface-active OM promotes the dissolved-to-gas carbon dioxide nucleation in wet aerosols, even at low temperatures, strongly decreasing carbon dioxide solubility. A discussion is made on the role of OM in controlling the pH of a cloud or raindrop, as a consequence, without involving OM ionization equilibrium. The results are compared with experimental and computational studies in the literature.

Heterogeneous ice nucleation and phase transition of viscous α-pinene secondary organic aerosol

NASA Astrophysics Data System (ADS)

Ignatius, Karoliina; Kristensen, Thomas B.; Järvinen, Emma; Nichman, Leonid; Fuchs, Claudia; Gordon, Hamish; Herenz, Paul; Hoyle, Christopher R.; Duplissy, Jonathan; Baltensperger, Urs; Curtius, Joachim; Donahue, Neil M.; Gallagher, Martin W.; Kirkby, Jasper; Kulmala, Markku; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Virtanen, Annele; Stratmann, Frank

2016-04-01

There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate deposition ice nucleation and thus influence cirrus cloud properties. Global model simulations of monoterpene SOA particles suggest that viscous biogenic SOA are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nucleating particle (INP) budget. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles at the CLOUD (Cosmics Leaving OUtdoor Droplets) experiment at CERN (Ignatius et al., 2015, Järvinen et al., 2015). In the CLOUD chamber, the SOA particles were produced from the ozone initiated oxidation of α-pinene at temperatures in the range from -38 to -10° C at 5-15 % relative humidity with respect to water (RHw) to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. As the RHw was increased to between 35 % at -10° C and 80 % at -38° C, a transition to spherical shape was observed with a new in-situ optical method. This transition confirms previous modelling of the viscosity transition conditions. The ice nucleation ability of SOA particles was investigated with a new continuous flow diffusion chamber SPIN (Spectrometer for Ice Nuclei) for different SOA particle sizes. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA in the deposition mode for ice saturation ratios between 1.3 and 1.4, significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between -36.5 and -38.3° C ranged from 6 to 20 % and did not depend on the particle surface area. References Ignatius, K. et al., Heterogeneous ice nucleation of secondary organic aerosol produced from ozonolysis of α-pinene, Atmos. Chem. Phys. Discuss., 15, 35719-35752, doi:10.5194/acpd-15-35719-2015, 2015. Järvinen, E. et al., Observation of viscosity transition in α-pinene secondary organic aerosol, Atmos. Chem. Phys. Discuss., 15, 28575-28617, doi:10.5194/acpd-15-28575-2015, 2015.

Impacts of New Particle Formation on Midwestern Climate and Air Quality as Determined by the NPF-explicit WRF-Chem

NASA Astrophysics Data System (ADS)

Dong, C.; Stanier, C. O.; Bullard, R.; Singh, A.

2016-12-01

A one month simulation has been performed using the New particle formation (NPF)-explicit WRF-Chem (Matsui et al, Journal of Geophysical Research, 116(D19208), 2011). The simulation was run for a domain of the continental United States, with analysis focused on the Midwestern and eastern portions of the U.S. Analysis focused on quantification and explanation of planetary boundary layer (PBL) NPF in the model on variables beyond condensation nuclei (CN), cloud condensation nuclei (CCN), and cloud droplet size distributions. The model was evaluated against meteorology, chemical species and aerosol physical property observations. Comparison shows the model performance was comparable to that of other studies. Nucleation enhanced the concentration of condensation nuclei (CN). Cloud condensation nuclei (CCN) concentrations were enhanced and suppressed at high and low supersaturations, respectively. For air pollutants, the most pronounced influence of PBL nucleation was PM2.5 reduction, which was mainly caused by SO4 decreases (62.7%). For shortwave radiation, changes due to indirect effects of NPF were larger than direct effects. Shortwave radiation and cloud droplet concentration typically changed in the same way. Similar change patterns were found for T2 and PBL height. PBL nucleation led to a net increase of precipitation during the simulation period. Sensitivity tests showed that the combination of PBL NPF together with aqueous chemistry was the predominant cause of SO4 reduction.

The Hygroscopicity Parameter of Marine Organics in Sea Spray Aerosols

NASA Astrophysics Data System (ADS)

Boyer, M.; Chang, R. Y. W.

2015-12-01

The effects of aerosols on climate are poorly understood, specifically with respect to their influence on cloud properties. Since oceans cover >70% of Earth's surface, sea spray aerosols (SSA), which act efficiently as cloud condensation nuclei (CCN), may have important implications on Earth's radiation budget. Surface active organic species readily accumulate in the sea surface microlayer (SML), located at the ocean-atmosphere interface, and transfer onto nascent SSA. While it is understood that SSA are commonly enriched with organics, the resulting effect of the organic content on CCN activation remains unresolved. The hygroscopicity parameter, kappa (k), allows for the cloud nucleating properties of individual components to be predicted in particles of mixed composition; however, most studies typically infer k from ambient measurements without assessing the contribution of the individual components to the overall k. In this study, a method for quantifying the cloud nucleating properties of the organic species in surface seawater using k-Kohler theory is proposed. Ambient SML and bulk water samples will be collected and atomized to generate particles such that the overall k can be inferred from CCN measurements. The inorganic and organic components will be quantified, and the organic component will be separated so that the hygroscopicity of only the organic constituents can be determined. By comparing the inferred k values for the samples before and after removal of the inorganic component, the hygroscopicity of the organic constituents alone can be calculated, providing insight on the effect of organic species on CCN activation in SSA.

The adsorption of fungal ice-nucleating proteins on mineral dusts: a terrestrial reservoir of atmospheric ice-nucleating particles

NASA Astrophysics Data System (ADS)

O'Sullivan, Daniel; Murray, Benjamin J.; Ross, James; Webb, Michael E.

2016-04-01

The occurrence of ice-nucleating particles (INPs) in our atmosphere has a profound impact on the properties and lifetime of supercooled clouds. However, the identities, sources and abundances of airborne particles capable of efficiently nucleating ice at relatively low supercoolings (T > -15 °C) remain enigmatic. Recently, several studies have suggested that unidentified biogenic residues in soil dusts are likely to be an important source of these efficient atmospheric INPs. While it has been shown that cell-free proteins produced by common soil-borne fungi are exceptional INPs, whether these fungi are a source of ice-nucleating biogenic residues in soils has yet to be shown. In particular, it is unclear whether upon adsorption to soil mineral particles, the activity of fungal ice-nucleating proteins is retained or is reduced, as observed for other soil enzymes. Here we show that proteins from a common soil fungus (Fusarium avenaceum) do in fact preferentially bind to and impart their ice-nucleating properties to the common clay mineral kaolinite. The ice-nucleating activity of the proteinaceous INPs is found to be unaffected by adsorption to the clay, and once bound the proteins do not readily desorb, retaining much of their activity even after multiple washings with pure water. The atmospheric implications of the finding that nanoscale fungal INPs can effectively determine the nucleating abilities of lofted soil dusts are discussed.

Further evidence for particle nucleation in clear air adjacent to marine cumulus clouds

NASA Astrophysics Data System (ADS)

Perry, Kevin D.; Hobbs, Peter V.

1994-11-01

Observational evidence is presented for the nucleation of condensation nuclei (CN) in the clear air adjacent to an isolated, marine, cumulus cloud. Two separate regions of particle nucleation are identified: one located above the cloud top, and the second located downwind of the cloud near the level of the anvil outflow. The regions of high CN concentrations were located in extremely clean marine air, with unactivated aerosol surface area (excluding the nucleation mode) less than 2 sq micrometers/cu cm, air temperature -31 C, and higher relative humidities than the undisturbed environment. Vertical profile measurements downwind of the cloud showed that CN concentrations at the level of the anvil outflow (4.9 km) were 8 times greater than at any other level between the surface and 5.3 km. A conceptual model is formulated in which aerosol particles, sulfur dioxide (SO2), sulfuric acid vapor (H2SO4), dimethyl sulfide (DMS), and ozone (O3) from the boundary layer are entrained into the cumulus cloud. Total aerosol number concentrations and unactivated aerosol surface area decrease with height in the cloud due to Brownian diffusion and diffusiophoresis of cloud interstitial aerosol to hydrometeors, coalescence scavenging by cloud droplets, collisional scavenging by ice particles, and subsequent removal by precipitation. The air that is detrained from the cloud raises the relative humidity and vents the clean air, SO2, H2SO4, DMS, and O3 to the near-cloud environment. Hydroxyl radicals then oxidize the SO2 and DMS to H2SO4. Under the conditions of high relative humidity, low total aerosol surface area, low temperatures, and high SO2 concentrations near cloud top, significant concentrations of new particles can be produced by homogeneous-bimolecular nucleation of sulfuric acid solution droplets from H2SO4 and H2O vapor molecules. The concentration of CN as a function of time is calculated for the case described in this paper using a bimodal integral nucleation model. The model results show that significant numbers of CN could have been produced within a few hours by the homogeneous-bimolecular nucleation of sulfuric acid solution droplets under the observed conditions provided the concentration of SO2 near cloud top was enhanced by vertical transport.

Ice Nucleation of Fungal Spores from the Classes Agaricomycetes, Ustilaginomycetes, and Eurotiomycetes, and the effect on the Atmospheric Transport of these Spores

DOE Office of Scientific and Technical Information (OSTI.GOV)

Haga, D. I.; Burrows, Susannah M.; Iannone, R.

2014-08-26

Ice nucleation on fungal spores may affect the frequency and properties of ice and mixed-phase clouds. We studied the ice nucleation properties of 12 different species of fungal spores chosen from three classes: Agaricomycetes, Ustilagomycetes, and Eurotiomycetes. Agaricomycetes include many types of mushroom species and are cosmopolitan all over the globe. Ustilagomycetes are agricultural pathogens and have caused widespread damage to crops. Eurotiomycetes are found on all types of decaying material and include important human allergens. We focused on these classes since they are thought to be abundant in the atmosphere and because there is very little information on themore » ice nucleation ability of these classes of spores in the literature. All of the fungal spores investigated were found to cause freezing of water droplets at temperatures warmer than homogeneous freezing. The cumulative number of ice nuclei per spore was 0.001 at temperatures between -19 °C and -29 °C, 0.01 between -25.5 °C and -31 °C, and 0.1 between -26 °C and -36 °C. On average, the order of ice nucleating ability for these spores is Ustilagomycetes > Agaricomycetes ≅ Eurotiomycetes. We show that at temperatures below -20 °C, all of the fungal spores studied here are less efficient ice nuclei compared to Asian mineral dust on a per surface area basis. We used our new freezing results together with data in the literature to compare the freezing temperatures of spores from the phyla Basidiomycota and Ascomycota, which together make up 98 % of known fungal species found on Earth. The data show that within both phyla (Ascomycota and Basidiomycota) there is a wide range of freezing properties, and also that the variation within a phylum is greater than the variation between the average freezing properties of the phyla. Using a global chemistry-climate transport model, we investigated whether ice nucleation on the studied spores, followed by precipitation, can influence the atmospheric transport and global distributions of these spores in the atmosphere. Simulations show that inclusion of ice nucleation scavenging of fungal spores in mixed-phase clouds can decrease the surface annual mean mixing ratios of fungal spores over the oceans and polar regions and decrease annual mean mixing ratios in the upper troposphere.« less

Chlorine-containing salts as water ice nucleating particles on Mars

NASA Astrophysics Data System (ADS)

Santiago-Materese, D. L.; Iraci, L. T.; Clapham, M. E.; Chuang, P. Y.

2018-03-01

Water ice cloud formation on Mars largely is expected to occur on the most efficient ice nucleating particle available. Salts have been observed on the Martian surface and have been known to facilitate water cloud formation on Earth. We examined heterogeneous ice nucleation onto sodium chloride and sodium perchlorate substrates under Martian atmospheric conditions, in the range of 150 to 180 K and 10-7 to 10-5 Torr water partial pressure. Sub-155 K data for the critical saturation ratio (Scrit) suggests an exponential model best describes the temperature-dependence of nucleation onset of water ice for all substrates tested. While sodium chloride does not facilitate water ice nucleation more easily than bare silicon, sodium perchlorate does support depositional nucleation at lower saturation levels than other substrates shown and is comparable to smectite-rich clay in its ability to support cloud initiation. Perchlorates could nucleate water ice at partial pressures up to 40% lower than other substrates examined to date under Martian atmospheric conditions. These findings suggest air masses on Mars containing uplifted salts such as perchlorates could form water ice clouds at lower saturation ratios than in air masses absent similar particles.

Cirrus Parcel Model Comparison Project. Phase 1; The Critical Components to Simulate Cirrus Initiation Explicitly

NASA Technical Reports Server (NTRS)

Lin, Ruei-Fong; Starr, David OC; DeMott, Paul J.; Cotton, Richard; Sassen, Kenneth; Jensen, Eric; Einaudi, Franco (Technical Monitor)

2001-01-01

The Cirrus Parcel Model Comparison Project, a project of the GCSS (GEWEX Cloud System Studies) Working Group on Cirrus Cloud Systems, involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. In Phase I of the project reported here, simulated cirrus cloud microphysical properties are compared for situations of "warm" (40 C) and "cold" (-60 C) cirrus, both subject to updrafts of 4, 20 and 100 centimeters per second. Five models participated. The various models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins or treated separately. Simulations are made including both the homogeneous and heterogeneous ice nucleation mechanisms. A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. To isolate the treatment of the homogeneous freezing (of haze droplets) nucleation process, the heterogeneous nucleation mechanism is disabled for a second parallel set of simulations. Qualitative agreement is found for the homogeneous-nucleation- only simulations, e.g., the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, significant quantitative differences are found. Detailed analysis reveals that the homogeneous nucleation rate, haze particle solution concentration, and water vapor uptake rate by ice crystal growth (particularly as controlled by the deposition coefficient) are critical components that lead to differences in predicted microphysics. Systematic bias exists between results based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each approach is constrained by critical freezing data from laboratory studies, but each includes assumptions that can only be justified by further laboratory research. Consequently, it is not yet clear if the two approaches can be made consistent. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (20-100 centimeters per second) at -60 C when the commonly invoked equilibrium assumption is lifted. The resulting difference in particle-size- dependent solution concentration of haze particles may significantly affect the ice particle formation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of particle number concentration and ice crystal diffusional growth rate, which is particularly sensitive to the deposition coefficient when ice particles are small, modulates the peak particle formation rate achieved in an air parcel and the duration of the active nucleation time period. The effects of heterogeneous nucleation are most pronounced in weak updraft situations. Vapor competition by the heterogeneously nucleated ice crystals may limit the achieved ice supersaturation and thus suppresses the contribution of homogeneous nucleation. Correspondingly, ice crystal number density is markedly reduced. Definitive laboratory and atmospheric benchmark data are needed for the heterogeneous nucleation process. Inter-model differences are correspondingly greater than in the case of the homogeneous nucleation process acting alone.

Ice nucleation by cellulose and its potential impact on clouds and climate

NASA Astrophysics Data System (ADS)

Hiranuma, Naruki; Möhler, Ottmar; Yamashita, Katsuya; Tajiri, Takuya; Saito, Atsushi; Kiselev, Alexei; Hoose, Corinna; Murakami, Masataka

2014-05-01

Biological aerosol particles have recently been accentuated by their efficient ice nucleating activity as well as potential impact on clouds and global climate. Despite their potential importance, little is known about the abundance of biological particles in the atmosphere and their role compared to non-biological material and, consequently, their potential role in the cloud-hydrology and climate system is also poorly constrained. However, field observations show that the concentration of airborne cellulose, which is one of the most important derivatives of glucose and atmospherically relevant biopolymers, is consistently prevalent (>10 ng per cubic meter) throughout the whole year even at remote- and elevated locations. Here we use a novel cloud simulation chamber in Tsukuba, Japan to demonstrate that airborne cellulose of biological origin can act as efficient ice nucleating particles in super-cooled clouds of the lower and middle troposphere. In specific, we measured the surface-based ice nucleation activity of microcrystalline cellulose particles immersed in cloud droplets, which may add crucial importance to further quantify the role of biological particles as ice nuclei in the troposphere. Our results suggest that the concentration of ice nucleating cellulose to become significant (>0.1 per liter) below about -17 °C and nearly comparable to other known ice nucleating clay mineral particles (e.g., illite rich clay mineral - INUIT comparisons are also presented). An important and unique characteristic of microcrystalline cellulose compared to other particles of biological origin is its high molecular packing density, enhancing resistance to hydrolysis degradation. More in-depth microphysical understandings as well as quantitative observations of ice nucleating cellulose particles in the atmosphere are necessary to allow better estimates of their effects on clouds and the global climate. Acknowledgement: We acknowledge support by German Research Society (DfG) and Ice Nucleation research UnIT (FOR 1525 INUIT).

Ice Nucleation Activity of Graphene and Graphene Oxides

PubMed Central

2018-01-01

Aerosols can act as cloud condensation nuclei and/or ice-nucleating particles (INPs), influencing cloud properties. In particular, INPs show a variety of different and complex mechanisms when interacting with water during the freezing process. To gain a fundamental understanding of the heterogeneous freezing mechanisms, studies with proxies for atmospheric INPs must be performed. Graphene and its derivatives offer suitable model systems for soot particles, which are ubiquitous aerosols in the atmosphere. In this work, we present an investigation of the ice nucleation activity (INA) of different types of graphene and graphene oxides. Immersion droplet freezing experiments as well as additional analytical analyses, such as X-ray photoelectron spectroscopy, Raman spectroscopy, and transmission electron microscopy, were performed. We show within a group of samples that a highly ordered graphene lattice (Raman G band intensity >50%) can support ice nucleation more effectively than a lowly ordered graphene lattice (Raman G band intensity <20%). Ammonia-functionalized graphene revealed the highest INA of all samples. Atmospheric ammonia is known to play a primary role in the formation of secondary particulate matter, forming ammonium-containing aerosols. The influence of functionalization on interactions between the particle interface and water molecules, as well as on hydrophobicity and agglomeration processes, is discussed. PMID:29707097

Abundance of fluorescent biological aerosol particles at temperatures conducive to the formation of mixed-phase and cirrus clouds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Twohy, Cynthia H.; McMeeking, Gavin R.; DeMott, Paul J.

Some types of biological particles are known to nucleate ice at warmer temperatures than mineral dust, with the potential to influence cloud microphysical properties and climate. However, the prevalence of these particle types above the atmospheric boundary layer is not well known. Many types of biological particles fluoresce when exposed to ultraviolet light, and the Wideband Integrated Bioaerosol Sensor takes advantage of this characteristic to perform real-time measurements of fluorescent biological aerosol particles (FBAPs). This instrument was flown on the National Center for Atmospheric Research Gulfstream V aircraft to measure concentrations of fluorescent biological particles from different potential sources andmore » at various altitudes over the US western plains in early autumn. Clear-air number concentrations of FBAPs between 0.8 and 12 µm diameter usually decreased with height and generally were about 10–100 L -1 in the continental boundary layer but always much lower at temperatures colder than 255 K in the free troposphere. At intermediate temperatures where biological ice-nucleating particles may influence mixed-phase cloud formation (255 K ≤ T ≤ 270 K), concentrations of fluorescent particles were the most variable and were occasionally near boundary-layer concentrations. Predicted vertical distributions of ice-nucleating particle concentrations based on FBAP measurements in this temperature regime sometimes reached typical concentrations of primary ice in clouds but were often much lower. If convection was assumed to lift boundary-layer FBAPs without losses to the free troposphere, better agreement between predicted ice-nucleating particle concentrations and typical ice crystal concentrations was achieved. Ice-nucleating particle concentrations were also measured during one flight and showed a decrease with height, and concentrations were consistent with a relationship to FBAPs established previously at the forested surface site below. The vertical distributions of FBAPs measured on five flights were also compared with those for bacteria, fungal spores, and pollen predicted from the EMAC global chemistry–climate model for the same geographic region.« less

Abundance of fluorescent biological aerosol particles at temperatures conducive to the formation of mixed-phase and cirrus clouds

NASA Astrophysics Data System (ADS)

Twohy, Cynthia H.; McMeeking, Gavin R.; DeMott, Paul J.; McCluskey, Christina S.; Hill, Thomas C. J.; Burrows, Susannah M.; Kulkarni, Gourihar R.; Tanarhte, Meryem; Kafle, Durga N.; Toohey, Darin W.

2016-07-01

Some types of biological particles are known to nucleate ice at warmer temperatures than mineral dust, with the potential to influence cloud microphysical properties and climate. However, the prevalence of these particle types above the atmospheric boundary layer is not well known. Many types of biological particles fluoresce when exposed to ultraviolet light, and the Wideband Integrated Bioaerosol Sensor takes advantage of this characteristic to perform real-time measurements of fluorescent biological aerosol particles (FBAPs). This instrument was flown on the National Center for Atmospheric Research Gulfstream V aircraft to measure concentrations of fluorescent biological particles from different potential sources and at various altitudes over the US western plains in early autumn. Clear-air number concentrations of FBAPs between 0.8 and 12 µm diameter usually decreased with height and generally were about 10-100 L-1 in the continental boundary layer but always much lower at temperatures colder than 255 K in the free troposphere. At intermediate temperatures where biological ice-nucleating particles may influence mixed-phase cloud formation (255 K ≤ T ≤ 270 K), concentrations of fluorescent particles were the most variable and were occasionally near boundary-layer concentrations. Predicted vertical distributions of ice-nucleating particle concentrations based on FBAP measurements in this temperature regime sometimes reached typical concentrations of primary ice in clouds but were often much lower. If convection was assumed to lift boundary-layer FBAPs without losses to the free troposphere, better agreement between predicted ice-nucleating particle concentrations and typical ice crystal concentrations was achieved. Ice-nucleating particle concentrations were also measured during one flight and showed a decrease with height, and concentrations were consistent with a relationship to FBAPs established previously at the forested surface site below. The vertical distributions of FBAPs measured on five flights were also compared with those for bacteria, fungal spores, and pollen predicted from the EMAC global chemistry-climate model for the same geographic region.

Effects of pre-existing ice crystals on cirrus clouds and comparison between different ice nucleation parameterizations with the Community Atmosphere Model (CAM5)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shi, Xiangjun; Liu, Xiaohong; Zhang, Kai

In order to improve the treatment of ice nucleation in a more realistic manner in the Community Atmosphere Model version 5.3 (CAM5.3), the effects of pre-existing ice crystals on ice nucleation in cirrus clouds are considered. In addition, by considering the in-cloud variability in ice saturation ratio, homogeneous nucleation takes place spatially only in a portion of the cirrus cloud rather than in the whole area of the cirrus cloud. Compared to observations, the ice number concentrations and the probability distributions of ice number concentration are both improved with the updated treatment. The pre-existing ice crystals significantly reduce ice numbermore » concentrations in cirrus clouds, especially at mid- to high latitudes in the upper troposphere (by a factor of ~10). Furthermore, the contribution of heterogeneous ice nucleation to cirrus ice crystal number increases considerably. Besides the default ice nucleation parameterization of Liu and Penner (2005, hereafter LP) in CAM5.3, two other ice nucleation parameterizations of Barahona and Nenes (2009, hereafter BN) and Kärcher et al. (2006, hereafter KL) are implemented in CAM5.3 for the comparison. In-cloud ice crystal number concentration, percentage contribution from heterogeneous ice nucleation to total ice crystal number, and pre-existing ice effects simulated by the three ice nucleation parameterizations have similar patterns in the simulations with present-day aerosol emissions. However, the change (present-day minus pre-industrial times) in global annual mean column ice number concentration from the KL parameterization (3.24 × 10 6 m -2) is less than that from the LP (8.46 × 10 6 m -2) and BN (5.62 × 10 6 m -2) parameterizations. As a result, the experiment using the KL parameterization predicts a much smaller anthropogenic aerosol long-wave indirect forcing (0.24 W m -2) than that using the LP (0.46 W m −2) and BN (0.39 W m -2) parameterizations.« less

Effects of pre-existing ice crystals on cirrus clouds and comparison between different ice nucleation parameterizations with the Community Atmosphere Model (CAM5)

DOE PAGES

Shi, Xiangjun; Liu, Xiaohong; Zhang, Kai

2015-02-11

In order to improve the treatment of ice nucleation in a more realistic manner in the Community Atmosphere Model version 5.3 (CAM5.3), the effects of pre-existing ice crystals on ice nucleation in cirrus clouds are considered. In addition, by considering the in-cloud variability in ice saturation ratio, homogeneous nucleation takes place spatially only in a portion of the cirrus cloud rather than in the whole area of the cirrus cloud. Compared to observations, the ice number concentrations and the probability distributions of ice number concentration are both improved with the updated treatment. The pre-existing ice crystals significantly reduce ice numbermore » concentrations in cirrus clouds, especially at mid- to high latitudes in the upper troposphere (by a factor of ~10). Furthermore, the contribution of heterogeneous ice nucleation to cirrus ice crystal number increases considerably. Besides the default ice nucleation parameterization of Liu and Penner (2005, hereafter LP) in CAM5.3, two other ice nucleation parameterizations of Barahona and Nenes (2009, hereafter BN) and Kärcher et al. (2006, hereafter KL) are implemented in CAM5.3 for the comparison. In-cloud ice crystal number concentration, percentage contribution from heterogeneous ice nucleation to total ice crystal number, and pre-existing ice effects simulated by the three ice nucleation parameterizations have similar patterns in the simulations with present-day aerosol emissions. However, the change (present-day minus pre-industrial times) in global annual mean column ice number concentration from the KL parameterization (3.24 × 10 6 m -2) is less than that from the LP (8.46 × 10 6 m -2) and BN (5.62 × 10 6 m -2) parameterizations. As a result, the experiment using the KL parameterization predicts a much smaller anthropogenic aerosol long-wave indirect forcing (0.24 W m -2) than that using the LP (0.46 W m −2) and BN (0.39 W m -2) parameterizations.« less

Heterogeneous nucleation of ice on carbon surfaces.

PubMed

Lupi, Laura; Hudait, Arpa; Molinero, Valeria

2014-02-26

Atmospheric aerosols can promote the heterogeneous nucleation of ice, impacting the radiative properties of clouds and Earth's climate. The experimental investigation of heterogeneous freezing of water droplets by carbonaceous particles reveals widespread ice freezing temperatures. It is not known which structural and chemical characteristics of soot account for the variability in ice nucleation efficiency. Here we use molecular dynamics simulations to investigate the nucleation of ice from liquid water in contact with graphitic surfaces. We find that atomically flat carbon surfaces promote heterogeneous nucleation of ice, while molecularly rough surfaces with the same hydrophobicity do not. Graphitic surfaces and other surfaces that promote ice nucleation induce layering in the interfacial water, suggesting that the order imposed by the surface on liquid water may play an important role in the heterogeneous nucleation mechanism. We investigate a large set of graphitic surfaces of various dimensions and radii of curvature and find that variations in nanostructures alone could account for the spread in the freezing temperatures of ice on soot in experiments. We conclude that a characterization of the nanostructure of soot is needed to predict its ice nucleation efficiency.

Investigating Freezing Point Depression and Cirrus Cloud Nucleation Mechanisms Using a Differential Scanning Calorimeter

ERIC Educational Resources Information Center

Bodzewski, Kentaro Y.; Caylor, Ryan L.; Comstock, Ashley M.; Hadley, Austin T.; Imholt, Felisha M.; Kirwan, Kory D.; Oyama, Kira S.; Wise, Matthew E.

2016-01-01

A differential scanning calorimeter was used to study homogeneous nucleation of ice from micron-sized aqueous ammonium sulfate aerosol particles. It is important to understand the conditions at which these particles nucleate ice because of their connection to cirrus cloud formation. Additionally, the concept of freezing point depression, a topic…

Microbial ice nucleators scavenged from the atmosphere during simulated rain events

NASA Astrophysics Data System (ADS)

Hanlon, Regina; Powers, Craig; Failor, Kevin; Monteil, Caroline L.; Vinatzer, Boris A.; Schmale, David G.

2017-08-01

Rain and snow collected at ground level have been found to contain biological ice nucleators. These ice nucleators have been proposed to have originated in clouds, where they may have participated in the formation of precipitation via ice phase nucleation. We conducted a series of field experiments to test the hypothesis that at least some of the microbial ice nucleators (prokaryotes and eukaryotes) present in rain may not originate in clouds but instead be scavenged from the lower atmosphere by rainfall. Thirty-three simulated rain events were conducted over four months off the side of the Smart Road Bridge in Blacksburg, VA, USA. In each event, sterile water was dispensed over the side of the bridge and recovered in sterile containers in an open fallow agricultural field below (a distance of ∼55 m). Microbes scavenged from the simulated rain events were cultured and their ice nucleation activity was examined. Putative microbial ice nucleators were cultured from 94% (31/33) of the simulated rain events, and represented 1.5% (121/8331) of the total colonies assayed. Putative ice nucleators were subjected to additional droplet freezing assays, and those confirmed through these repeated assays represented 0.4% (34/8331) of the total. Mean CFUs scavenged by simulated rain ranged from 2 to 267 CFUs/mL. Scavenged ice nucleators belong to a number of taxa including the bacterial genera Pseudomonas, Pantoea, and Xanthomonas, and the fungal genera Fusarium, Humicola, and Mortierella. An ice-nucleating strain of the fungal genus Penicillium was also recovered from a volumetric air sampler at the study site. This work expands our knowledge of the scavenging properties of rainfall, and suggests that at least some ice nucleators in natural precipitation events may have been scrubbed from the atmosphere during rainfall, and thus are not likely to be involved in precipitation.

SUCCESS Evidence for Cirrus Cloud Ice Nucleation Mechanisms

NASA Technical Reports Server (NTRS)

Jensen, Eric; Gore, Warren J. Y. (Technical Monitor)

1997-01-01

During the SUCCESS mission, several measurements were made which should improve our understanding of ice nucleation processes in cirrus clouds. Temperature and water vapor concentration were made with a variety of instruments on the NASA DC-8. These observations should provide accurate upper tropospheric humidities. In particular, we will evaluate what humidities are required for ice nucleation. Preliminary results suggest that substantial supersaturations frequently exist in the upper troposphere. The leading-edge region of wave-clouds (where ice nucleation occurs) was sampled extensively at temperatures near -40 and -60C. These observations should give precise information about conditions required for ice nucleation. In addition, we will relate the observed aerosol composition and size distributions to the ice formation observed to evaluate the role of soot or mineral particles on ice nucleation. As an alternative technique for determining what particles act as ice nuclei, numerous samples of aerosols inside ice crystals were taken. In some cases, large numbers of aerosols were detected in each crystal, indicating that efficient scavenging occurred. Analysis of aerosols in ice crystals when only one particle per crystal was detected should help with the ice nucleation issue. Direct measurements of the ice nucleating activity of ambient aerosols drawn into airborne cloud chambers were also made. Finally, measurements of aerosols and ice crystals in contrails should indicate whether aircraft exhaust soot particles are effective ice nuclei.

Climate Impacts of Ice Nucleation

NASA Technical Reports Server (NTRS)

Gettelman, Andrew; Liu, Xiaohong; Barahona, Donifan; Lohmann, Ulrike; Chen, Celia

2012-01-01

Several different ice nucleation parameterizations in two different General Circulation Models (GCMs) are used to understand the effects of ice nucleation on the mean climate state, and the Aerosol Indirect Effects (AIE) of cirrus clouds on climate. Simulations have a range of ice microphysical states that are consistent with the spread of observations, but many simulations have higher present-day ice crystal number concentrations than in-situ observations. These different states result from different parameterizations of ice cloud nucleation processes, and feature different balances of homogeneous and heterogeneous nucleation. Black carbon aerosols have a small (0.06 Wm(exp-2) and not statistically significant AIE when included as ice nuclei, for nucleation efficiencies within the range of laboratory measurements. Indirect effects of anthropogenic aerosols on cirrus clouds occur as a consequence of increasing anthropogenic sulfur emissions with different mechanisms important in different models. In one model this is due to increases in homogeneous nucleation fraction, and in the other due to increases in heterogeneous nucleation with coated dust. The magnitude of the effect is the same however. The resulting ice AIE does not seem strongly dependent on the balance between homogeneous and heterogeneous ice nucleation. Regional effects can reach several Wm2. Indirect effects are slightly larger for those states with less homogeneous nucleation and lower ice number concentration in the base state. The total ice AIE is estimated at 0.27 +/- 0.10 Wm(exp-2) (1 sigma uncertainty). This represents a 20% offset of the simulated total shortwave AIE for ice and liquid clouds of 1.6 Wm(sup-2).

Biological aerosol effects on clouds and precipitation

NASA Astrophysics Data System (ADS)

Hallar, A. Gannet; Huffman, J. Alex; Fridlind, Ann

2012-12-01

Bioaerosol Effects on Clouds Workshop;Steamboat Springs, Colorado, 5-6August 2012 Bioaerosols such as bacteria have been proposed as significant contributors to cloud ice nucleation, but too little is known about the properties and impacts of bioaerosol and other ice nuclei to make reliable conclusions about their wide-scale impact on clouds and precipitation. During late summer an international group of 40 participants met at a Steamboat Springs ski resort to share perspectives on bioaerosol sources, activity, and influence on clouds. Participants who were invited collectively spanned a broad range of expertise, including atmospheric chemistry, microbiology, micrometeorology, and cloud physics, as well as a broad range of research approaches, including laboratory measurement, field measurement, and modeling. Tours of Storm Peak Laboratory (http://www.stormpeak.dri.edu) were offered before and after the workshop.

Estimating the Influence of Biological Ice Nuclei on Clouds with Regional Scale Simulations

NASA Astrophysics Data System (ADS)

Hummel, Matthias; Hoose, Corinna; Schaupp, Caroline; Möhler, Ottmar

2014-05-01

Cloud properties are largely influenced by the atmospheric formation of ice particles. Some primary biological aerosol particles (PBAP), e.g. certain bacteria, fungal spores or pollen, have been identified as effective ice nuclei (IN). The work presented here quantifies the IN concentrations originating from PBAP in order to estimate their influences on clouds with the regional scale atmospheric model COSMO-ART in a six day case study for Western Europe. The atmospheric particle distribution is calculated for three different PBAP (bacteria, fungal spores and birch pollen). The parameterizations for heterogeneous ice nucleation of PBAP are derived from AIDA cloud chamber experiments with Pseudomonas syringae bacteria and birch pollen (Schaupp, 2013) and from published data on Cladosporium spores (Iannone et al., 2011). A constant fraction of ice-active bacteria and fungal spores relative to the total bacteria and spore concentration had to be assumed. At cloud altitude, average simulated PBAP number concentrations are ~17 L-1 for bacteria and fungal spores and ~0.03 L-1 for birch pollen, including large temporal and spatial variations of more than one order of magnitude. Thus, the average, 'diagnostic' in-cloud PBAP IN concentrations, which only depend on the PBAP concentrations and temperature, without applying dynamics and cloud microphysics, lie at the lower end of the range of typically observed atmospheric IN concentrations . Average PBAP IN concentrations are between 10-6 L-1 and 10-4 L-1. Locally but not very frequently, PBAP IN concentrations can be as high as 0.2 L-1 at -10° C. Two simulations are compared to estimate the cloud impact of PBAP IN, both including mineral dust as an additional background IN with a constant concentration of 100 L-1. One of the simulations includes additional PBAP IN which can alter the cloud properties compared to the reference simulation without PBAP IN. The difference in ice particle and cloud droplet concentration between both simulations is a result of the heterogeneous ice nucleation of PBAP. In the chosen case setup, two effects can be identified which are occurring at different altitudes. Additional PBAP IN directly enhance the ice crystal concentration at lower parts of a mixed-phase cloud. This increase comes with a decrease in liquid droplet concentration in this part of a cloud. Therefore, a second effect takes place, where less ice crystals are formed by dust-driven heterogeneous as well as homogeneous ice nucleation in upper parts of a cloud, probably due to a lack of liquid water reaching these altitudes. Overall, diagnostic PBAP IN concentrations are very low compared to typical IN concentration, but reach maxima at temperatures where typical IN are not very ice-active. PBAP IN can therefore influence clouds to some extent. Iannone, R., Chernoff, D. I., Pringle, A., Martin, S. T., and Bertram, A. K.: The ice nucleation ability of one of the most abundant types of fungal spores found in the atmosphere, Atmos. Chem. Phys., 11, 1191-1201, 10.5194/acp-11-1191-2011, 2011. Schaupp, C.: Untersuchungen zur Rolle von Bakterien und Pollen als Wolkenkondensations- und Eiskeime in troposphärischen Wolken, Ph.D. thesis, Institute of Environmental Physics, Heidelberg University, Heidelberg, Germany, 2013.

Impact of bacterial ice nucleating particles on weather predicted by a numerical weather prediction model

NASA Astrophysics Data System (ADS)

Sahyoun, Maher; Korsholm, Ulrik S.; Sørensen, Jens H.; Šantl-Temkiv, Tina; Finster, Kai; Gosewinkel, Ulrich; Nielsen, Niels W.

2017-12-01

Bacterial ice-nucleating particles (INP) have the ability to facilitate ice nucleation from super-cooled cloud droplets at temperatures just below the melting point. Bacterial INP have been detected in cloud water, precipitation, and dry air, hence they may have an impact on weather and climate. In modeling studies, the potential impact of bacteria on ice nucleation and precipitation formation on global scale is still uncertain due to their small concentration compared to other types of INP, i.e. dust. Those earlier studies did not account for the yet undetected high concentration of nanoscale fragments of bacterial INP, which may be found free or attached to soil dust in the atmosphere. In this study, we investigate the sensitivity of modeled cloud ice, precipitation and global solar radiation in different weather scenarios to changes in the fraction of cloud droplets containing bacterial INP, regardless of their size. For this purpose, a module that calculates the probability of ice nucleation as a function of ice nucleation rate and bacterial INP fraction was developed and implemented in a numerical weather prediction model. The threshold value for the fraction of cloud droplets containing bacterial INP needed to produce a 1% increase in cloud ice was determined at 10-5 to 10-4. We also found that increasing this fraction causes a perturbation in the forecast, leading to significant differences in cloud ice and smaller differences in convective and total precipitation and in net solar radiation reaching the surface. These effects were most pronounced in local convective events. Our results show that bacterial INP can be considered as a trigger factor for precipitation, but not an enhancement factor.

Responses of Mixed-Phase Cloud Condensates and Cloud Radiative Effects to Ice Nucleating Particle Concentrations in NCAR CAM5 and DOE ACME Climate Models

NASA Astrophysics Data System (ADS)

Liu, X.; Shi, Y.; Wu, M.; Zhang, K.

2017-12-01

Mixed-phase clouds frequently observed in the Arctic and mid-latitude storm tracks have the substantial impacts on the surface energy budget, precipitation and climate. In this study, we first implement the two empirical parameterizations (Niemand et al. 2012 and DeMott et al. 2015) of heterogeneous ice nucleation for mixed-phase clouds in the NCAR Community Atmosphere Model Version 5 (CAM5) and DOE Accelerated Climate Model for Energy Version 1 (ACME1). Model simulated ice nucleating particle (INP) concentrations based on Niemand et al. and DeMott et al. are compared with those from the default ice nucleation parameterization based on the classical nucleation theory (CNT) in CAM5 and ACME, and with in situ observations. Significantly higher INP concentrations (by up to a factor of 5) are simulated from Niemand et al. than DeMott et al. and CNT especially over the dust source regions in both CAM5 and ACME. Interestingly the ACME model simulates higher INP concentrations than CAM5, especially in the Polar regions. This is also the case when we nudge the two models' winds and temperature towards the same reanalysis, indicating more efficient transport of aerosols (dust) to the Polar regions in ACME. Next, we examine the responses of model simulated cloud liquid water and ice water contents to different INP concentrations from three ice nucleation parameterizations (Niemand et al., DeMott et al., and CNT) in CAM5 and ACME. Changes in liquid water path (LWP) reach as much as 20% in the Arctic regions in ACME between the three parameterizations while the LWP changes are smaller and limited in the Northern Hemispheric mid-latitudes in CAM5. Finally, the impacts on cloud radiative forcing and dust indirect effects on mixed-phase clouds are quantified with the three ice nucleation parameterizations in CAM5 and ACME.

Role of Gravity Waves in Determining Cirrus Cloud Properties

NASA Technical Reports Server (NTRS)

OCStarr, David; Singleton, Tamara; Lin, Ruei-Fong

2008-01-01

Cirrus clouds are important in the Earth's radiation budget. They typically exhibit variable physical properties within a given cloud system and from system to system. Ambient vertical motion is a key factor in determining the cloud properties in most cases. The obvious exception is convectively generated cirrus (anvils), but even in this case, the subsequent cloud evolution is strongly influenced by the ambient vertical motion field. It is well know that gravity waves are ubiquitous in the atmosphere and occur over a wide range of scales and amplitudes. Moreover, researchers have found that inclusion of statistical account of gravity wave effects can markedly improve the realism of simulations of persisting large-scale cirrus cloud features. Here, we use a 1 -dimensional (z) cirrus cloud model, to systematically examine the effects of gravity waves on cirrus cloud properties. The model includes a detailed representation of cloud microphysical processes (bin microphysics and aerosols) and is run at relatively fine vertical resolution so as to adequately resolve nucleation events, and over an extended time span so as to incorporate the passage of multiple gravity waves. The prescribed gravity waves "propagate" at 15 m s (sup -1), with wavelengths from 5 to 100 km, amplitudes range up to 1 m s (sup -1)'. Despite the fact that the net gravity wave vertical motion forcing is zero, it will be shown that the bulk cloud properties, e.g., vertically-integrated ice water path, can differ quite significantly from simulations without gravity waves and that the effects do depend on the wave characteristics. We conclude that account of gravity wave effects is important if large-scale models are to generate realistic cirrus cloud property climatology (statistics).

Snow-borne nanosized particles: Abundance, distribution, composition, and significance in ice nucleation processes

NASA Astrophysics Data System (ADS)

Rangel-Alvarado, Rodrigo Benjamin; Nazarenko, Yevgen; Ariya, Parisa A.

2015-11-01

Physicochemical processes of nucleation constitute a major uncertainty in understanding aerosol-cloud interactions. To improve the knowledge of the ice nucleation process, we characterized physical, chemical, and biological properties of fresh snow using a suite of state-of-the-art techniques based on mass spectrometry, electron microscopy, chromatography, and optical particle sizing. Samples were collected at two North American Arctic sites, as part of international campaigns (2006 and 2009), and in the city of Montreal, Canada, over the last decade. Particle size distribution analyses, in the range of 3 nm to 10 µm, showed that nanosized particles are the most numerous (38-71%) in fresh snow, with a significant portion (11 to 19%) less than 100 nm in size. Particles with diameters less than 200 nm consistently exhibited relatively high ice-nucleating properties (on average ranged from -19.6 ± 2.4 to -8.1 ± 2.6°C). Chemical analysis of the nanosized fraction suggests that they contain bioorganic materials, such as amino acids, as well as inorganic compounds with similar characteristics to mineral dust. The implication of nanoparticle ubiquity and abundance in diverse snow ecosystems are discussed in the context of their importance in understanding atmospheric nucleation processes.

Comparing the ice nucleation efficiencies of ice nucleating substrates to natural mineral dusts

NASA Astrophysics Data System (ADS)

Steinke, Isabelle; Funk, Roger; Höhler, Kristina; Haarig, Moritz; Hoffmann, Nadine; Hoose, Corinna; Kiselev, Alexei; Möhler, Ottmar; Leisner, Thomas

2014-05-01

Mineral dust particles in the atmosphere may act as efficient ice nuclei over a wide range of temperature and relative humidity conditions. The ice nucleation capability of dust particles mostly depends on the particle surface area and the associated physico-chemical surface properties. It has been observed that the surface-related ice nucleation efficiency of different dust particles and mineral species can vary by several orders of magnitude. However, the relation between aerosol surface properties and observed ice nucleation efficiency is still not completely understood due to the large variability of chemical compositions and morphological features. In order to gain a better understanding of small scale freezing processes, we investigated the freezing of several hundreds of small droplets (V=0.4 nl) deposited on materials with reasonably well defined surfaces such as crystalline silicon wafers, graphite and freshly cleaved mica sheets under atmospherically relevant conditions. These substrates are intended to serve as simple model structures compared to the surface of natural aerosol particles. To learn more about the impact of particle morphology on ice nucleation processes, we also investigated micro-structured silicon wafers with prescribed trenches. The ice nucleation efficiencies deduced from these experiments are expressed as ice nucleation active surface site density values. With this approach, the freezing properties of the above-described substrates could be compared to those of natural mineral dusts such as agricultural soil dusts, volcanic ash and fossil diatoms, which have been investigated in AIDA cloud chamber experiments. All tested ice nucleating substrates were consistently less efficient at nucleating ice than the natural mineral dusts. Crystalline silicon only had a negligible influence on the freezing of small droplets, leading to freezing near the homogeneous freezing temperature threshold. Applying surface structures to silicon led to a shift towards heterogeneous freezing. However, the measured ice nucleation active surface site densities were still smaller than those of mineral dusts.

The relevance of nanoscale biological fragments for ice nucleation in clouds

NASA Astrophysics Data System (ADS)

O‧Sullivan, D.; Murray, B. J.; Ross, J. F.; Whale, T. F.; Price, H. C.; Atkinson, J. D.; Umo, N. S.; Webb, M. E.

2015-01-01

Most studies of the role of biological entities as atmospheric ice-nucleating particles have focused on relatively rare supermicron particles such as bacterial cells, fungal spores and pollen grains. However, it is not clear that there are sufficient numbers of these particles in the atmosphere to strongly influence clouds. Here we show that the ice-nucleating activity of a fungus from the ubiquitous genus Fusarium is related to the presence of nanometre-scale particles which are far more numerous, and therefore potentially far more important for cloud glaciation than whole intact spores or hyphae. In addition, we quantify the ice-nucleating activity of nano-ice nucleating particles (nano-INPs) washed off pollen and also show that nano-INPs are present in a soil sample. Based on these results, we suggest that there is a reservoir of biological nano-INPs present in the environment which may, for example, become aerosolised in association with fertile soil dust particles.

Nucleation of nitric acid hydrates in polar stratospheric clouds by meteoric material

NASA Astrophysics Data System (ADS)

James, Alexander D.; Brooke, James S. A.; Mangan, Thomas P.; Whale, Thomas F.; Plane, John M. C.; Murray, Benjamin J.

2018-04-01

Heterogeneous nucleation of crystalline nitric acid hydrates in polar stratospheric clouds (PSCs) enhances ozone depletion. However, the identity and mode of action of the particles responsible for nucleation remains unknown. It has been suggested that meteoric material may trigger nucleation of nitric acid trihydrate (NAT, or other nitric acid phases), but this has never been quantitatively demonstrated in the laboratory. Meteoric material is present in two forms in the stratosphere: smoke that results from the ablation and re-condensation of vapours, and fragments that result from the break-up of meteoroids entering the atmosphere. Here we show that analogues of both materials have a capacity to nucleate nitric acid hydrates. In combination with estimates from a global model of the amount of meteoric smoke and fragments in the polar stratosphere we show that meteoric material probably accounts for NAT observations in early season polar stratospheric clouds in the absence of water ice.

The relevance of nanoscale biological fragments for ice nucleation in clouds.

PubMed

O'Sullivan, D; Murray, B J; Ross, J F; Whale, T F; Price, H C; Atkinson, J D; Umo, N S; Webb, M E

2015-01-28

Most studies of the role of biological entities as atmospheric ice-nucleating particles have focused on relatively rare supermicron particles such as bacterial cells, fungal spores and pollen grains. However, it is not clear that there are sufficient numbers of these particles in the atmosphere to strongly influence clouds. Here we show that the ice-nucleating activity of a fungus from the ubiquitous genus Fusarium is related to the presence of nanometre-scale particles which are far more numerous, and therefore potentially far more important for cloud glaciation than whole intact spores or hyphae. In addition, we quantify the ice-nucleating activity of nano-ice nucleating particles (nano-INPs) washed off pollen and also show that nano-INPs are present in a soil sample. Based on these results, we suggest that there is a reservoir of biological nano-INPs present in the environment which may, for example, become aerosolised in association with fertile soil dust particles.

Global atmospheric particle formation from CERN CLOUD measurements

NASA Astrophysics Data System (ADS)

Dunne, Eimear M.; Gordon, Hamish; Carslaw, Kenneth S.

2017-04-01

New particle formation (or nucleation) is acknowledged as a significant source of climate-relevant aerosol throughout the atmosphere. However, performing atmospherically relevant nucleation experiments in a laboratory setting is extremely challenging. As a result, until now, the parameterisations used to represent new particle formation in global aerosol models were largely based on in-situ observations or theoretical nucleation models, and usually only represented the binary H2SO4-H2O system. Several different chemicals can affect particle formation rates, even at extremely low trace concentrations, which are technically challenging to measure directly. Nucleation rates also respond to environmental changes in e.g. temperature in a highly non-linear fashion. The CERN CLOUD experiment was designed to provide the most controlled and accurate nucleation rate measurements to date, over the full range of free tropospheric temperatures and down to sulphuric acid concentrations of the order of 105 cm-3. We will present a parameterisation of inorganic nucleation rates for use in global models, based on these measurements, which includes four separate nucleation pathways: binary neutral, binary ion-induced, ternary neutral, and ternary ion-induced. Both inorganic and organic nucleation parameterisations derived from CLOUD measurements have been implemented in the GLOMAP global aerosol model. The parameterisations depend on temperature and on concentrations of sulphuric acid, ammonia, organic vapours, and ions. One of CLOUD's main original goals was to determine the sensitivity of atmospheric aerosol to changes in the nucleation rate over a solar cycle. We will show that, in a present-day atmosphere, the changes in climate-relevant aerosol (in the form of cloud-level cloud condensation nuclei) over a solar cycle are on average about 0.1%, with local changes of less than 1%. In contrast, anthropogenic changes in ammonia since pre-industrial times were estimated to have a much greater influence, resulting in a radiative forcing of between -0.62 and -0.66 W m-2. Including ternary inorganic pathways in GLOMAP improved the model's agreement with free tropospheric observations, especially aircraft measurements. The further inclusion of an organic parameterisation, which increased nucleation in the summertime boundary layer, brought our results more in line with observations made at surface stations. We therefore believe that, while the addition of other nucleation pathways (such as amine-induced nucleation) will doubtless improve agreement with local in-situ measurements, this model set-up provides a good representation of the global atmosphere as a whole. By presenting this novel parameterisation at EGU, we hope to encourage its uptake among the aerosol modelling community.

Natural Aerosols Explain Seasonal and Spatial Patterns of Southern Ocean Cloud Albedo

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCoy, Daniel; Burrows, Susannah M.; Wood, R.

2015-07-17

Small particles called aerosols act as nucleation sites for cloud drop formation, affecting clouds and cloud properties – ultimately influencing the cloud dynamics, lifetime, water path and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations not only affect cloud properties themselves, but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. Here, it is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more thanmore » half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd over regions of high biological activity is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35-45°S) and by organic matter in sea spray aerosol at higher latitudes (45-55°S). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m-2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.« less

Effect of photochemical aging on the ice nucleation properties of diesel and wood burning particles

NASA Astrophysics Data System (ADS)

Chou, C.; Stetzer, O.; Tritscher, T.; Chirico, R.; Heringa, M. F.; Kanji, Z. A.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.; Lohmann, U.

2012-06-01

A measurement campaign (IMBALANCE) was conducted in 2009 and aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC) but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro with no emission after-treatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC) at three nominal temperatures, -30 °C, -35 °C and -40 °C. Freshly emitted diesel particles showed ice formation only at -40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi) and 92% relative humidity with respect to water (RHw), and photochemical aging did not play a role in modifying their ice nucleation behavior. Only one diesel experiment where α-pinene was added, showed an ice nucleation enhancement after the aging at -35 °C. Wood burning particles also act as ice nuclei (IN) at -40 °C in the deposition mode at the same conditions as for diesel particles and photochemical aging did also not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at -35 °C with no ice nucleation observed at -30 °C for wood burning particles. Photochemical aging did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below -30 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical aging on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

Effect of photochemical ageing on the ice nucleation properties of diesel and wood burning particles

NASA Astrophysics Data System (ADS)

Chou, C.; Kanji, Z. A.; Stetzer, O.; Tritscher, T.; Chirico, R.; Heringa, M. F.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.; Lohmann, U.

2013-01-01

A measurement campaign (IMBALANCE) conducted in 2009 was aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC) but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro without emission aftertreatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC) at three nominal temperatures, -30 °C, -35 °C and -40 °C. Freshly emitted diesel particles showed ice formation only at -40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi) and 92% relative humidity with respect to water (RHw), and photochemical ageing did not play a role in modifying their ice nucleation behaviour. Only one diesel experiment where α-pinene was added for the ageing process, showed an ice nucleation enhancement at -35 °C. Wood burning particles also act as ice nuclei (IN) at -40 °C in the deposition mode at the same conditions as for diesel particles and photochemical ageing also did not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at -35 °C whereas no ice nucleation was observed at -30 °C. Photochemical ageing did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below -40 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical ageing on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

Laboratory and Cloud Chamber Studies of Formation Processes and Properties of Atmospheric Ice Particles

NASA Astrophysics Data System (ADS)

Leisner, T.; Abdelmonem, A.; Benz, S.; Brinkmann, M.; Möhler, O.; Rzesanke, D.; Saathoff, H.; Schnaiter, M.; Wagner, R.

2009-04-01

The formation of ice in tropospheric clouds controls the evolution of precipitation and thereby influences climate and weather via a complex network of dynamical and microphysical processes. At higher altitudes, ice particles in cirrus clouds or contrails modify the radiative energy budget by direct interaction with the shortwave and longwave radiation. In order to improve the parameterisation of the complex microphysical and dynamical processes leading to and controlling the evolution of tropospheric ice, laboratory experiments are performed at the IMK Karlsruhe both on a single particle level and in the aerosol and cloud chamber AIDA. Single particle experiments in electrodynamic levitation lend themselves to the study of the interaction between cloud droplets and aerosol particles under extremely well characterized and static conditions in order to obtain microphysical parameters as freezing nucleation rates for homogeneous and heterogeneous ice formation. They also allow the observation of the freezing dynamics and of secondary ice formation and multiplication processes under controlled conditions and with very high spatial and temporal resolution. The inherent droplet charge in these experiments can be varied over a wide range in order to assess the influence of the electrical state of the cloud on its microphysics. In the AIDA chamber on the other hand, these processes are observable under the realistic dynamic conditions of an expanding and cooling cloud- parcel with interacting particles and are probed simultaneously by a comprehensive set of analytical instruments. By this means, microphysical processes can be studied in their complex interplay with dynamical processes as for example coagulation or particle evaporation and growth via the Bergeron - Findeisen process. Shortwave scattering and longwave absorption properties of the nucleating and growing ice crystals are probed by in situ polarised laser light scattering measurements and infrared extinction spectroscopy. In conjunction with ex situ single particle imaging and light scattering measurements the relation between the overall extinction and depolarization properties of the ice clouds and the morphological details of the constituent ice crystals are investigated. In our contribution we will concentrate on the parameterization of homogeneous and heterogeneous ice formation processes under various atmospheric conditions and on the optical properties of the ice crystals produced under these conditions. First attempts to parameterize the observations will be presented.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mitchell, David L.

It is well known that cirrus clouds play a major role in regulating the earth’s climate, but the details of how this works are just beginning to be understood. This project targeted the main property of cirrus clouds that influence climate processes; the ice fall speed. That is, this project improves the representation of the mass-weighted ice particle fall velocity, V m, in climate models, used to predict future climate on global and regional scales. Prior to 2007, the dominant sizes of ice particles in cirrus clouds were poorly understood, making it virtually impossible to predict how cirrus clouds interactmore » with sunlight and thermal radiation. Due to several studies investigating the performance of optical probes used to measure the ice particle size distribution (PSD), as well as the remote sensing results from our last ARM project, it is now well established that the anomalously high concentrations of small ice crystals often reported prior to 2007 were measurement artifacts. Advances in the design and data processing of optical probes have greatly reduced these ice artifacts that resulted from the shattering of ice particles on the probe tips and/or inlet tube, and PSD measurements from one of these improved probes (the 2-dimensional Stereo or 2D-S probe) are utilized in this project to parameterize V m for climate models. Our original plan in the proposal was to parameterize the ice PSD (in terms of temperature and ice water content) and ice particle mass and projected area (in terms of mass- and area-dimensional power laws or m-D/A-D expressions) since these are the microphysical properties that determine V m, and then proceed to calculate V m from these parameterized properties. But the 2D-S probe directly measures ice particle projected area and indirectly estimates ice particle mass for each size bin. It soon became apparent that the original plan would introduce more uncertainty in the V m calculations than simply using the 2D-S measurements to directly calculate V m. By calculating V m directly from the measured PSD, ice particle projected area and estimated mass, more accurate estimates of V m are obtained. These V m values were then parameterized for climate models by relating them to (1) sampling temperature and ice water content (IWC) and (2) the effective diameter (D e) of the ice PSD. Parameterization (1) is appropriate for climate models having single-moment microphysical schemes whereas (2) is appropriate for double-moment microphysical schemes and yields more accurate V m estimates. These parameterizations were developed for tropical cirrus clouds, Arctic cirrus, mid-latitude synoptic cirrus and mid-latitude anvil cirrus clouds based on field campaigns in these regions. An important but unexpected result of this research was the discovery of microphysical evidence indicating the mechanisms by which ice crystals are produced in cirrus clouds. This evidence, derived from PSD measurements, indicates that homogeneous freezing ice nucleation dominates in mid-latitude synoptic cirrus clouds, whereas heterogeneous ice nucleation processes dominate in mid-latitude anvil cirrus. Based on these findings, D e was parameterized in terms of temperature (T) for conditions dominated by (1) homo- and (2) heterogeneous ice nucleation. From this, an experiment was designed for global climate models (GCMs). The net radiative forcing from cirrus clouds may be affected by the means ice is produced (homo- or heterogeneously), and this net forcing contributes to climate sensitivity (i.e. the change in mean global surface temperature resulting from a doubling of CO 2). The objective of this GCM experiment was to determine how a change in ice nucleation mode affects the predicted global radiation balance. In the first simulation (Run 1), the D e-T relationship for homogeneous nucleation is used at all latitudes, while in the second simulation (Run 2), the D e-T relationship for heterogeneous nucleation is used at all latitudes. For both runs, V m is calculated from D e. Two GCMs were used; the Community Atmosphere Model version 5 (CAM5) and a European GCM known as ECHAM5 (thanks to our European colleagues who collaborated with us). Similar results were obtained from both GCMs in the Northern Hemisphere mid-latitudes, with a net cooling of ~ 1.0 W m -2 due to heterogeneous nucleation, relative to Run 1. The mean global net cooling was 2.4 W m -2 for the ECHAM5 GCM while CAM5 produced a mean global net cooling of about 0.8 W m -2. This dependence of the radiation balance on nucleation mode is substantial when one considers the direct radiative forcing from a CO 2 doubling is 4 W m -2. The differences between GCMs in mean global net cooling estimates may demonstrate a need for improving the representation of cirrus clouds in GCMs, including the coupling between microphysical and radiative properties. Unfortunately, after completing this GCM experiment, we learned from the company that provided the 2D-S microphysical data that the data was corrupted due to a computer program coding problem. Therefore the microphysical data had to be reprocessed and reanalyzed, and the GCM experiments were redone under our current ASR project but using an improved experimental design.« less

The Cirrus Parcel Model Comparison Project. Phase 1

NASA Technical Reports Server (NTRS)

Lin, Ruei-Fong; Starr, D.; DeMott, P.; Cotten, R.; Jensen, E.; Sassen, K.

2000-01-01

The cirrus Parcel Model Comparison Project involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. In Phase 1 of the project reported here, simulated cirrus cloud microphysical properties are compared for situations of "warm" (-40 C) and "cold" (-60 C) cirrus subject to updrafts of 4, 20 and 100 centimeters per second, respectively. Five models are participating in the project. These models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins. Simulations are made including both homogeneous and heterogeneous ice nucleation mechanisms. A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. To isolate the treatment of the homogeneous freezing (of haze drops) nucleation process, the heterogeneous nucleation mechanism is disabled for a second parallel set of simulations. Qualitative agreement is found amongst the models for the homogeneous-nucleation-only simulations, e.g., the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, non-negligible quantitative differences are found. Systematic bias exists between results of a model based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each approach is constrained by critical freezing data from laboratory studies. This information is necessary, but not sufficient, to construct consistent formulae for the two approaches. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (20-100 centimeters per second) at -60 C when the commonly invoked equilibrium assumption is lifted. The resulting difference in particle-size-dependent solution concentration of haze particles may significantly affect the ice nucleation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of ice number concentration and ice crystal diffusional growth rate, partially controls the peak nucleation rate achieved in an air parcel and the duration of the active nucleation time period.

Microspectroscopic imaging and characterization of individually identified ice nucleating particles from a case field study

DOE PAGES

Knopf, Daniel A.; Alpert, P. A.; Wang, B.; ...

2014-08-11

The effect of anthropogenic and biogenic organic particles on atmospheric glaciation processes is poorly understood. We use an optical microscopy setup to identify the ice nuclei (IN) active in immersion freezing (IMF) and deposition ice nucleation within a large population of particles collected on a substrate from an ambient environment in central California dominated by urban and marine aerosols. Multimodal microspectroscopy methods are applied to characterize the physicochemical properties and mixing state of the individual IN and particle populations to identify particle-type classes. The temperature onsets of water uptake occurred between 235 and 257 K at subsaturated conditions, and themore » onsets of IMF proceeded at subsaturated and saturated conditions for 235–247 K, relevant for ice nucleation in mixed-phase clouds. Particles also took up water and nucleated ice between 226 and 235 K and acted as deposition IN with onset temperatures below 226 K, a temperature range relevant to cirrus cloud formation. The identified IN belong to the most common particle-type classes observed in the field samples: organic coated sea salt and Na-rich, secondary, and refractory carbonaceous particles. Based on these observations, we suggest that the IN are not always particles with unique chemical composition and exceptional ice nucleation propensity; rather, they are common particles in the ambient particle population. Lastly, the results suggest that particle-type abundance and total particle surface area are also crucial factors, in addition to particle-type ice nucleation efficiency, in determining ice formation within the particle population.« less

Sensitivity of warm-frontal processes to cloud-nucleating aerosol concentrations

NASA Technical Reports Server (NTRS)

Igel, Adele L.; Van Den Heever, Susan C.; Naud, Catherine M.; Saleeby, Stephen M.; Posselt, Derek J.

2013-01-01

An extratropical cyclone that crossed the United States on 9-11 April 2009 was successfully simulated at high resolution (3-km horizontal grid spacing) using the Colorado State University Regional Atmospheric Modeling System. The sensitivity of the associated warm front to increasing pollution levels was then explored by conducting the same experiment with three different background profiles of cloud-nucleating aerosol concentration. To the authors' knowledge, no study has examined the indirect effects of aerosols on warm fronts. The budgets of ice, cloud water, and rain in the simulation with the lowest aerosol concentrations were examined. The ice mass was found to be produced in equal amounts through vapor deposition and riming, and the melting of ice produced approximately 75% of the total rain. Conversion of cloud water to rain accounted for the other 25%. When cloud-nucleating aerosol concentrations were increased, significant changes were seen in the budget terms, but total precipitation remained relatively constant. Vapor deposition onto ice increased, but riming of cloud water decreased such that there was only a small change in the total ice production and hence there was no significant change in melting. These responses can be understood in terms of a buffering effect in which smaller cloud droplets in the mixed-phase region lead to both an enhanced vapor deposition and decreased riming efficiency with increasing aerosol concentrations. Overall, while large changes were seen in the microphysical structure of the frontal cloud, cloud-nucleating aerosols had little impact on the precipitation production of the warm front.

Review of Aerosol–Cloud Interactions: Mechanisms, Significance, and Challenges

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fan, Jiwen; Wang, Yuan; Rosenfeld, Daniel

2016-11-01

Over the past decade, the number of studies that investigate aerosol-cloud interactions has increased considerably. Although tremendous progress has been made to improve our understanding of basic physical mechanisms of aerosol-cloud interactions and reduce their uncertainties in climate forcing, we are still in poor understanding of (1) some of the mechanisms that interact with each other over multiple spatial and temporal scales, (2) the feedback between microphysical and dynamical processes and between local-scale processes and large-scale circulations, and (3) the significance of cloud-aerosol interactions on weather systems as well as regional and global climate. This review focuses on recent theoreticalmore » studies and important mechanisms on aerosol-cloud interactions, and discusses the significances of aerosol impacts on raditative forcing and precipitation extremes associated with different cloud systems. Despite significant understanding has been gained about aerosol impacts on the main cloud types, there are still many unknowns especially associated with various deep convective systems. Therefore, large efforts are needed to escalate our understanding. Future directions should focus on obtaining concurrent measurements of aerosol properties, cloud microphysical and dynamic properties over a range of temporal and spatial scales collected over typical climate regimes and closure studies, as well as improving understanding and parameterizations of cloud microphysics such as ice nucleation, mixed-phase properties, and hydrometeor size and fall speed« less

Physical and chemical properties of ice residuals during the 2013 and 2014 CLACE campaigns

NASA Astrophysics Data System (ADS)

Kupiszewski, Piotr; Weingartner, Ernest; Vochezer, Paul; Hammer, Emanuel; Gysel, Martin; Färber, Raphael; Fuchs, Claudia; Schnaiter, Martin; Baltensperger, Urs; Schmidt, Susan; Schneider, Johannes; Bigi, Alessandro; Toprak, Emre; Linke, Claudia; Klimach, Thomas

2014-05-01

The shortcomings in our understanding and, thus, representation of aerosol-cloud interactions are one of the major sources of uncertainty in climate model projections. Among the poorly understood processes is mixed-phase cloud formation via heterogeneous nucleation, and the subsequent spatial and temporal evolution of such clouds. Cloud glaciation augments precipitation formation, resulting in decreased cloud cover and lifetime, and affects cloud radiative properties. Meanwhile, the physical and chemical properties of atmospherically relevant ice nuclei (IN), the sub-population of aerosol particles which enable heterogeneous nucleation, are not well known. Extraction of ice residuals (IR) in mixed-phase clouds is a difficult task, requiring separation of the few small, freshly formed ice crystals (the IR within such crystals can be deemed representative of the original IN) not only from interstitial particles, but also from the numerous supercooled droplets which have aerodynamic diameters similar to those of the ice crystals. In order to address the difficulties with ice crystal sampling and IR extraction in mixed-phase clouds, the new Ice Selective Inlet (ISI) has been designed and deployed at the Jungfraujoch field site. Small ice crystals are selectively sampled via the inlet with simultaneous counting, sizing and imaging of hydrometeors contained in the cloud by a set of optical particle spectrometers, namely Welas optical particle counters (OPC) and a Particle Phase Discriminator (PPD). The heart of the ISI is a droplet evaporation unit with ice-covered inner walls, resulting in removal of droplets using the Wegener-Bergeron-Findeisen process, while transmitting a relatively high fraction of small ice crystals. The ISI was deployed in the winters of 2013 and 2014 at the high alpine Jungfraujoch site (3580 m.a.s.l) during the intensive CLACE field campaigns. The measurements focused on analysis of the physical and chemical characteristics of IR and the microphysical properties of mixed-phase clouds. A host of aerosol instrumentation was deployed downstream of the ISI, including a Grimm OPC and a scanning mobility particle sizer (SMPS) for number size distribution measurements, as well as a single particle mass spectrometer (ALABAMA; 2013 only), single particle soot photometers (SP2) and a Wideband Integrated Bioaerosol Sensor (WIBS-4) for analysis of the chemical composition, with particular focus on the content of black carbon (BC) and biological particles in IR. Corresponding instrumentation sampled through a total aerosol inlet. By comparing observations from the ISI with those from the total inlet the characteristics of ice residuals relative to the total aerosol could be established. First results from these analyses will be presented.

Contribution of feldspar and marine organic aerosols to global ice nucleating particle concentrations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vergara-Temprado, Jesús; Murray, Benjamin J.; Wilson, Theodore W.

Ice-nucleating particles (INPs) are known to affect the amount of ice in mixed-phase clouds, thereby influencing many of their properties. The atmospheric INP concentration changes by orders of magnitude from terrestrial to marine environments, which typically contain much lower concentrations. Many modelling studies use parameterizations for heterogeneous ice nucleation and cloud ice processes that do not account for this difference because they were developed based on INP measurements made predominantly in terrestrial environments without considering the aerosol composition. Errors in the assumed INP concentration will influence the simulated amount of ice in mixed-phase clouds, leading to errors in top-of-atmosphere radiativemore » flux and ultimately the climate sensitivity of the model. Here we develop a global model of INP concentrations relevant for mixed-phase clouds based on laboratory and field measurements of ice nucleation by K-feldspar (an ice-active component of desert dust) and marine organic aerosols (from sea spray). The simulated global distribution of INP concentrations based on these two species agrees much better with currently available ambient measurements than when INP concentrations are assumed to depend only on temperature or particle size. Underestimation of INP concentrations in some terrestrial locations may be due to the neglect of INPs from other terrestrial sources. Our model indicates that, on a monthly average basis, desert dusts dominate the contribution to the INP population over much of the world, but marine organics become increasingly important over remote oceans and they dominate over the Southern Ocean. However, day-to-day variability is important. Because desert dust aerosol tends to be sporadic, marine organic aerosols dominate the INP population on many days per month over much of the mid- and high-latitude Northern Hemisphere. This study advances our understanding of which aerosol species need to be included in order to adequately describe the global and regional distribution of INPs in models, which will guide ice nucleation researchers on where to focus future laboratory and field work.« less

Investigating ice nucleation in cirrus clouds with an aerosol-enabled Multiscale Modeling Framework

DOE PAGES

Zhang, Chengzhu; Wang, Minghuai; Morrison, H.; ...

2014-11-06

In this study, an aerosol-dependent ice nucleation scheme [Liu and Penner, 2005] has been implemented in an aerosol-enabled multi-scale modeling framework (PNNL MMF) to study ice formation in upper troposphere cirrus clouds through both homogeneous and heterogeneous nucleation. The MMF model represents cloud scale processes by embedding a cloud-resolving model (CRM) within each vertical column of a GCM grid. By explicitly linking ice nucleation to aerosol number concentration, CRM-scale temperature, relative humidity and vertical velocity, the new MMF model simulates the persistent high ice supersaturation and low ice number concentration (10 to 100/L) at cirrus temperatures. The low ice numbermore » is attributed to the dominance of heterogeneous nucleation in ice formation. The new model simulates the observed shift of the ice supersaturation PDF towards higher values at low temperatures following homogeneous nucleation threshold. The MMF models predict a higher frequency of midlatitude supersaturation in the Southern hemisphere and winter hemisphere, which is consistent with previous satellite and in-situ observations. It is shown that compared to a conventional GCM, the MMF is a more powerful model to emulate parameters that evolve over short time scales such as supersaturation. Sensitivity tests suggest that the simulated global distribution of ice clouds is sensitive to the ice nucleation schemes and the distribution of sulfate and dust aerosols. Simulations are also performed to test empirical parameters related to auto-conversion of ice crystals to snow. Results show that with a value of 250 μm for the critical diameter, Dcs, that distinguishes ice crystals from snow, the model can produce good agreement to the satellite retrieved products in terms of cloud ice water path and ice water content, while the total ice water is not sensitive to the specification of Dcs value.« less

The dynamics of droplets in moist Rayleigh-Benard turbulence

NASA Astrophysics Data System (ADS)

Chandrakar, Kamal Kant; van der Voort, Dennis; Kinney, Greg; Cantrell, Will; Shaw, Raymond

2017-11-01

Clouds are an intricate part of the climate, and strongly influence atmospheric dynamics and radiative balances. While properties such as cloud albedo and precipitation rate are large scale effects, these properties are determined by dynamics on the microscale, such droplet sizes, liquid water content, etc. The growth of droplets from condensation is dependent on a multitude of parameters, such as aerosol concentration (nucleation sites) and turbulence (scalar fluctuations and coalescence). However, the precise mechanism behind droplet growth and clustering in a cloud environment is still unclear. In this investigation we use a facility called the Pi Chamber to generate a (miniature) cloud in a laboratory setting with known boundary conditions, such as aerosol concentration, temperature, and humidity. Through the use of particle imaging velocimetry (PIV) on the droplets generated in the cloud, we can investigate the dynamics of these cloud droplets in the convective (Rayleigh-Benard) turbulence generated through an induced temperature gradient. We show the influence of the temperature gradient and Froude number (gravity forces) on the changing turbulence anisotropy, large scale circulation, and small-scale dissipation rates. This work was supported by National Science Foundation Grant AGS-1623429.

Experimental evidence for millisecond activation timescales using the Fast IN Chamber (FINCH) measurements

NASA Astrophysics Data System (ADS)

Bundke, U.; Jaenicke, R.; Klein, H.; Nillius, B.; Reimann, B.; Wetter, T.; Bingemer, H.

2009-04-01

Ice formation in clouds is a subject of great practical and fundamental importance since the occurrence of ice particle initializes dramatic changes in the microphysical structure of the cloud, which finally ends in the formation of precipitation. The initially step of ice formation is largely unknown. Homogenous nucleation of ice occurs only below -40 °C. If an ice nucleus (IN) is present, heterogeneous nucleation may occur at higher temperature. Here deposition freezing, condensation and immersion freezing as well as contact freezing are known. Also growth rates of ice particles are known as function of crystal surface properties, temperature and super saturation. Timescales for homogenous freezing activation in the order of 0.01 seconds and nucleation rates have been measured by Anderson et al. (1980) and Hagen et al., (1981) using their expansion cloud chamber. This contribution of deposition mode freezing measurements by the ice nucleus counter FINCH presents evidence that the activation timescale of this freezing mode is in the order of 1E-3 seconds. FINCH is an Ice Nucleus counter which activates IN in a supersaturated environment at freezing temperatures. The activation conditions are actively controlled by mixing three gas flows (aerosol, particle-free cold-dry and warm-humid flows).See Bundke et al. 2008 for details. In a special operation mode of FINCH we are able to produce a controlled peak super saturation in the order of 1 ms duration. For several test aerosols the results observed in this particular mode are comparable to normal mode operations, where the maximum super saturation remains for more than a second, thus leading to the conclusion that the time for activation is in the order of 1ms or less. References: R.J. Anderson et al, "A Study of Homogeneous Condensation Freezing Nucleation of Small Water Droplets in an Expansion Cloud Chamber, Journal of the Atmospheric Sciences, Vol. 37, 2508-2520, 1980 U.Bundke et al., "The fast Ice Nucleus chamber FINCH", Atmospheric Research, Volume 90, Issues 2-4, 180-186, DOI:10.1016/j.atmosres.2008.02.008, 2008 D.E. Hagen et al., "Homogenous Condensation Freezing Nucleation Rate Measurements for Small Water Droplets in an Expansion Cloud Chamber", Journal of the Atmospheric Sciences, Vol 38, 1236-1243, 1981 Acknowledgments: This work was supported by the German Research Foundation: SFB 641 "Tropospheric Ice Phase" TP A1, SPP1294 BU1432/3-1, JA344/12-1, by the Helmholtz Association: VI-233 "Aerosol Cloud Interactions" and by and by the EU FP6 Infastructure Project EUSAAR.

Air pollution control and decreasing new particle formation lead to strong climate warming

NASA Astrophysics Data System (ADS)

Makkonen, R.; Asmi, A.; Kerminen, V.-M.; Boy, M.; Arneth, A.; Hari, P.; Kulmala, M.

2012-02-01

The number concentration of cloud droplets determines several climatically relevant cloud properties. A major cause for the high uncertainty in the indirect aerosol forcing is the availability of cloud condensation nuclei (CCN), which in turn is highly sensitive to atmospheric new particle formation. Here we present the effect of new particle formation on anthropogenic aerosol forcing in present-day (year 2000) and future (year 2100) conditions. The present-day total aerosol forcing is increased from -1.0 W m-2 to -1.6 W m-2 when nucleation is introduced into the model. Nucleation doubles the change in aerosol forcing between years 2000 and 2100, from +0.6 W m-2 to +1.4 W m-2. Two climate feedbacks are studied, resulting in additional negative forcings of -0.1 W m-2 (+10% DMS emissions in year 2100) and -0.5 W m-2 (+50% BVOC emissions in year 2100). With the total aerosol forcing diminishing in response to air pollution control measures taking effect, warming from increased greenhouse gas concentrations can potentially increase at a very rapid rate.

GCSS Cirrus Parcel Model Comparison Project

NASA Technical Reports Server (NTRS)

Lin, Ruei-Fong; Starr, David OC.; DeMott, Paul J.; Cotton, Richard; Jensen, Eric; Sassen, Kenneth; Einaudi, Franco (Technical Monitor)

2000-01-01

The Cirrus Parcel Model Comparison Project, a project of GCSS Working Group on Cirrus Cloud Systems (WG2), involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. The goal of this project is to document and understand the factors resulting in significant inter-model differences. The intent is to foment research leading to model improvement and validation. In Phase 1 of the project reported here, simulated cirrus cloud microphysical properties are compared for situations of "warm" (-40 C) and "cold" (-60 C) cirrus subject to updrafts of 4, 20 and 100 cm/s, respectively. Five models participated. These models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins. Simulations are made including both homogeneous and heterogeneous ice nucleation mechanisms. A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. To isolate the treatment of the homogeneous freezing (of haze drops) nucleation process, the heterogeneous nucleation mechanism is disabled for a second parallel set of simulations. Qualitative agreement is found for the homogeneous-nucleation-only simulations, e.g., the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, non-negligible quantitative differences are found. Detailed analysis reveals that the homogeneous nucleation formulation, aerosol size, ice crystal growth rate (particularly the deposition coefficient), and water vapor uptake rate are critical components that lead to differences in predicted microphysics. Systematic bias exists between results based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each approach is constrained by critical freezing data from laboratory studies, but each includes assumptions that can only be justified by further laboratory data. Consequently, it is not yet clear if the two approaches can be made consistent. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (20-100 cm/s) at -60 C when the commonly invoked equilibrium assumption is lifted. The resulting difference in particle-size-dependent solution concentration of haze particles may significantly affect the ice nucleation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of ice number concentration and ice crystal diffusional growth rate, which is sensitive to the deposition coefficient when ice particles are small, partially controls the peak nucleation rate achieved in an air parcel and the duration of the active nucleation time period. The effects of heterogeneous nucleation are most pronounced in weak updraft situations. Vapor competition by the nucleated (heterogeneous) ice crystals limits the achieved ice supersaturation and thus suppresses the contribution of homogeneous nucleation. Correspondingly, ice crystal number density is markedly reduced. Definitive laboratory and atmospheric benchmark data are needed for the heterogeneous nucleation process. Inter-model differences are correspondingly greater than in the case of the homogeneous nucleation process acting alone.

A marine biogenic source of atmospheric ice-nucleating particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wilson, T. W.; Ladino, L. A.; Alpert, Peter A.

2015-09-09

The formation of ice in clouds is facilitated by the presence of airborne ice nucleating particles1,2. Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice3–11. Here we show that material in the sea surface microlayer, which is enriched in surface active organic material representative of that found in sub-micron sea- spray aerosol12–21, nucleates ice under conditions that occur in mixed-phase clouds and high-altitude ice clouds. The ice active material is likely biogenic and is less than ~0.2 ?m in size. We also showmore » that organic material (exudate) released by a common marine diatom nucleates ice when separated from cells and propose that organic material associated with phytoplankton cell exudates are a candidate for the observed ice nucleating ability of the microlayer samples. By combining our measurements with global model simulations of marine organic aerosol, we show that ice nucleating particles of marine origin are dominant in remote marine environments, such as the Southern Ocean, the North Pacific and the North Atlantic.« less

African Dust Aerosols as Atmospheric Ice Nuclei

NASA Technical Reports Server (NTRS)

DeMott, Paul J.; Brooks, Sarah D.; Prenni, Anthony J.; Kreidenweis, Sonia M.; Sassen, Kenneth; Poellot, Michael; Rogers, David C.; Baumgardner, Darrel

2003-01-01

Measurements of the ice nucleating ability of aerosol particles in air masses over Florida having sources from North Africa support the potential importance of dust aerosols for indirectly affecting cloud properties and climate. The concentrations of ice nuclei within dust layers at particle sizes below 1 pn exceeded 1/cu cm; the highest ever reported with our device at temperatures warmer than homogeneous freezing conditions. These measurements add to previous direct and indirect evidence of the ice nucleation efficiency of desert dust aerosols, but also confirm their contribution to ice nuclei populations at great distances from source regions.

Ice Cloud Formation and Dehydration in the Tropical Tropopause Layer

NASA Technical Reports Server (NTRS)

Jensen, Eric; Gore, Warren J. (Technical Monitor)

2002-01-01

Stratospheric water vapor is important not only for its greenhouse forcing, but also because it plays a significant role in stratospheric chemistry. Several recent studies have focused on the potential for dehydration due to ice cloud formation in air rising slowly through the tropical tropopause layer (TTL). Holton and Gettelman showed that temperature variations associated with horizontal transport of air in the TTL can drive ice cloud formation and dehydration, and Gettelman et al. recently examined the cloud formation and dehydration along kinematic trajectories using simple assumptions about the cloud properties. In this study, a Lagrangian, one-dimensional cloud model has been used to further investigate cloud formation and dehydration as air is transported horizontally and vertically through the TTL. Time-height curtains of temperature are extracted from meteorological analyses. The model tracks the growth, advection, and sedimentation of individual cloud particles. The regional distribution of clouds simulated in the model is comparable to the subvisible cirrus distribution indicated by SAGE II. The simulated cloud properties and cloud frequencies depend strongly on the assumed supersaturation threshold for ice nucleation. The clouds typically do not dehydrate the air along trajectories down to the temperature minimum saturation mixing ratio. Rather the water vapor mixing ratio crossing the tropopause along trajectories is 10-50% larger than the saturation mixing ratio. I will also discuss the impacts of Kelvin waves and gravity waves on cloud properties and dehydration efficiency. These simulations can be used to determine whether observed lower stratospheric water vapor mixing ratios can be explained by dehydration associated with in situ TTL cloud formation alone.

Evaluating the effect of soil dust particles from semi-arid areas on clouds and climate

NASA Astrophysics Data System (ADS)

Kristjansson, J. E.; Hummel, M.; Lewinschal, A.; Grini, A.

2016-12-01

Primary ice production in mixed-phase clouds predominantly takes place by heterogeneous freezing of mineral dust particles. Therefore, mineral dust has a large impact on cloud properties. Organic matter attached to mineral dust particles can expand their already good freezing ability further to warmer subzero temperatures. These dust particles are called "soil dust". Dusts emitted from deserts contribute most to the total dust concentration in the atmosphere and they can be transported over long distances. Soil dust is emitted from semi-arid regions, e.g. agricultural areas. Besides wind erosion, human activities like tillage or harvest might be a large source for soil dust release into the atmosphere. In this study, we analyze the influence of soil dust particles on clouds with the Norwegian Earth System Model (NorESM; Bentsen et al., 2013: GMD). The parameterization of immersion freezing on soil dust is based on findings from the AIDA cloud chamber (Steinke et al., in prep.). Contact angle and activation energy for soil dust are estimated in order to be used in the dust immersion freezing scheme of the model, which is based on classical nucleation theory. Our first results highlight the importance of soil dust for ice nucleation on a global scale. Its influence is expected to be highest in the northern hemisphere due to its higher area for soil dust emission. The immersion freezing rates due to additional soil dust can on average increase by a factor of 1.2 compared to a mineral dust-only simulation. Using a budget tool for NorESM, influences of soil dust ice nuclei on single tendencies of the cloud microphysics can be identified. For example, accretion to snow is sensitive to adding soil dust ice nuclei. This can result in changes e.g. in the ice water path and cloud radiative properties.

Nonthermal ice nucleation observed at distorted contact lines of supercooled water drops

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Fan; Cruikshank, Owen; He, Weilue

Ice nucleation is the crucial step for ice formation in atmospheric clouds and therefore underlies climatologically relevant precipitation and radiative properties. Some progress has been made in understanding the roles of temperature, supersaturation, and material properties, but an explanation for the efficient ice nucleation occurring when a particle contacts a supercooled water drop has been elusive for over half a century. Here, we explore ice nucleation initiated at constant temperature and observe that mechanical agitation induces freezing of supercooled water drops at distorted contact lines. Results show that symmetric motion of supercooled water on a vertically oscillating substrate does notmore » freeze, no matter how we agitate it. However, when the moving contact line is distorted with the help of trace amounts of oil or inhomogeneous pinning on the substrate, freezing can occur at temperatures much higher than in a static droplet, equivalent to ~1010 increase in nucleation rate. Several possible mechanisms are proposed to explain the observations. One plausible explanation among them, decreased pressure due to interface curvature, is explored theoretically and compared with the observational results quasiquantitatively. Indeed, the observed freezing-temperature increase scales with contact line speed in a manner consistent with the pressure hypothesis. Whatever the mechanism, the experiments demonstrate a strong preference for ice nucleation at three-phase contact lines compared to the two-phase interface, and they also show that movement and distortion of the contact line are necessary contributions to stimulating the nucleation process.« less

Nonthermal ice nucleation observed at distorted contact lines of supercooled water drops

DOE PAGES

Yang, Fan; Cruikshank, Owen; He, Weilue; ...

2018-02-06

Ice nucleation is the crucial step for ice formation in atmospheric clouds and therefore underlies climatologically relevant precipitation and radiative properties. Some progress has been made in understanding the roles of temperature, supersaturation, and material properties, but an explanation for the efficient ice nucleation occurring when a particle contacts a supercooled water drop has been elusive for over half a century. Here, we explore ice nucleation initiated at constant temperature and observe that mechanical agitation induces freezing of supercooled water drops at distorted contact lines. Results show that symmetric motion of supercooled water on a vertically oscillating substrate does notmore » freeze, no matter how we agitate it. However, when the moving contact line is distorted with the help of trace amounts of oil or inhomogeneous pinning on the substrate, freezing can occur at temperatures much higher than in a static droplet, equivalent to ~1010 increase in nucleation rate. Several possible mechanisms are proposed to explain the observations. One plausible explanation among them, decreased pressure due to interface curvature, is explored theoretically and compared with the observational results quasiquantitatively. Indeed, the observed freezing-temperature increase scales with contact line speed in a manner consistent with the pressure hypothesis. Whatever the mechanism, the experiments demonstrate a strong preference for ice nucleation at three-phase contact lines compared to the two-phase interface, and they also show that movement and distortion of the contact line are necessary contributions to stimulating the nucleation process.« less

Nonthermal ice nucleation observed at distorted contact lines of supercooled water drops

NASA Astrophysics Data System (ADS)

Yang, Fan; Cruikshank, Owen; He, Weilue; Kostinski, Alex; Shaw, Raymond A.

2018-02-01

Ice nucleation is the crucial step for ice formation in atmospheric clouds and therefore underlies climatologically relevant precipitation and radiative properties. Progress has been made in understanding the roles of temperature, supersaturation, and material properties, but an explanation for the efficient ice nucleation occurring when a particle contacts a supercooled water drop has been elusive for over half a century. Here, we explore ice nucleation initiated at constant temperature and observe that mechanical agitation induces freezing of supercooled water drops at distorted contact lines. Results show that symmetric motion of supercooled water on a vertically oscillating substrate does not freeze, no matter how we agitate it. However, when the moving contact line is distorted with the help of trace amounts of oil or inhomogeneous pinning on the substrate, freezing can occur at temperatures much higher than in a static droplet, equivalent to ˜1010 increase in nucleation rate. Several possible mechanisms are proposed to explain the observations. One plausible explanation among them, decreased pressure due to interface curvature, is explored theoretically and compared with the observational results quasiquantitatively. Indeed, the observed freezing-temperature increase scales with contact line speed in a manner consistent with the pressure hypothesis. Whatever the mechanism, the experiments demonstrate a strong preference for ice nucleation at three-phase contact lines compared to the two-phase interface, and they also show that movement and distortion of the contact line are necessary contributions to stimulating the nucleation process.

Nonthermal ice nucleation observed at distorted contact lines of supercooled water drops.

PubMed

Yang, Fan; Cruikshank, Owen; He, Weilue; Kostinski, Alex; Shaw, Raymond A

2018-02-01

Ice nucleation is the crucial step for ice formation in atmospheric clouds and therefore underlies climatologically relevant precipitation and radiative properties. Progress has been made in understanding the roles of temperature, supersaturation, and material properties, but an explanation for the efficient ice nucleation occurring when a particle contacts a supercooled water drop has been elusive for over half a century. Here, we explore ice nucleation initiated at constant temperature and observe that mechanical agitation induces freezing of supercooled water drops at distorted contact lines. Results show that symmetric motion of supercooled water on a vertically oscillating substrate does not freeze, no matter how we agitate it. However, when the moving contact line is distorted with the help of trace amounts of oil or inhomogeneous pinning on the substrate, freezing can occur at temperatures much higher than in a static droplet, equivalent to ∼10^{10} increase in nucleation rate. Several possible mechanisms are proposed to explain the observations. One plausible explanation among them, decreased pressure due to interface curvature, is explored theoretically and compared with the observational results quasiquantitatively. Indeed, the observed freezing-temperature increase scales with contact line speed in a manner consistent with the pressure hypothesis. Whatever the mechanism, the experiments demonstrate a strong preference for ice nucleation at three-phase contact lines compared to the two-phase interface, and they also show that movement and distortion of the contact line are necessary contributions to stimulating the nucleation process.

The relevance of nanoscale biological fragments for ice nucleation in clouds

PubMed Central

O′Sullivan, D.; Murray, B. J.; Ross, J. F.; Whale, T. F.; Price, H. C.; Atkinson, J. D.; Umo, N. S.; Webb, M. E.

2015-01-01

Most studies of the role of biological entities as atmospheric ice-nucleating particles have focused on relatively rare supermicron particles such as bacterial cells, fungal spores and pollen grains. However, it is not clear that there are sufficient numbers of these particles in the atmosphere to strongly influence clouds. Here we show that the ice-nucleating activity of a fungus from the ubiquitous genus Fusarium is related to the presence of nanometre-scale particles which are far more numerous, and therefore potentially far more important for cloud glaciation than whole intact spores or hyphae. In addition, we quantify the ice-nucleating activity of nano-ice nucleating particles (nano-INPs) washed off pollen and also show that nano-INPs are present in a soil sample. Based on these results, we suggest that there is a reservoir of biological nano-INPs present in the environment which may, for example, become aerosolised in association with fertile soil dust particles. PMID:25626414

Heterogeneous Ice Nucleation Ability of NaCl and Sea Salt Aerosol Particles at Cirrus Temperatures

NASA Astrophysics Data System (ADS)

Wagner, Robert; Kaufmann, Julia; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Ullrich, Romy; Leisner, Thomas

2018-03-01

In situ measurements of the composition of heterogeneous cirrus ice cloud residuals have indicated a substantial contribution of sea salt in sampling regions above the ocean. We have investigated the heterogeneous ice nucleation ability of sodium chloride (NaCl) and sea salt aerosol (SSA) particles at cirrus cloud temperatures between 235 and 200 K in the Aerosol Interaction and Dynamics in the Atmosphere aerosol and cloud chamber. Effloresced NaCl particles were found to act as ice nucleating particles in the deposition nucleation mode at temperatures below about 225 K, with freezing onsets in terms of the ice saturation ratio, Sice, between 1.28 and 1.40. Above 225 K, the crystalline NaCl particles deliquesced and nucleated ice homogeneously. The heterogeneous ice nucleation efficiency was rather similar for the two crystalline forms of NaCl (anhydrous NaCl and NaCl dihydrate). Mixed-phase (solid/liquid) SSA particles were found to act as ice nucleating particles in the immersion freezing mode at temperatures below about 220 K, with freezing onsets in terms of Sice between 1.24 and 1.42. Above 220 K, the SSA particles fully deliquesced and nucleated ice homogeneously. Ice nucleation active surface site densities of the SSA particles were found to be in the range between 1.0 · 1010 and 1.0 · 1011 m-2 at T < 220 K. These values are of the same order of magnitude as ice nucleation active surface site densities recently determined for desert dust, suggesting a potential contribution of SSA particles to low-temperature heterogeneous ice nucleation in the atmosphere.

Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: Future Suborbital Activities to Address Knowledge Gaps in Satellite and Model Assessments

NASA Technical Reports Server (NTRS)

Redemann, Jens; Wood, R.; Zuidema, P.; Haywood, J.; Piketh, S.; Formenti, P.; L'Ecuyer, T.; Kacenelenbogen, M.; Segal-Rosenheimer, M.; Shinozuka, Y.;

Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: Future Suborbital Activities to Address Knowledge Gaps in Satellite and Model Assessments

NASA Astrophysics Data System (ADS)

Redemann, J.; Wood, R.; Zuidema, P.; Haywood, J. M.; Piketh, S.; Formenti, P.; L'Ecuyer, T. S.; Kacenelenbogen, M. S.; Segal-Rosenhaimer, M.; Shinozuka, Y.; LeBlanc, S. E.; Vaughan, M. A.; Schmidt, S.; Flynn, C. J.; Song, S.; Schmid, B.; Luna, B.; Abel, S.

2015-12-01

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for global climate change scenarios. Our understanding of aerosol-cloud interactions in the SE Atlantic is hindered both by the lack of knowledge on aerosol and cloud properties, as well as the lack of knowledge about detailed physical processes involved. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology. We discuss the current knowledge of aerosol and cloud property distributions based on satellite observations and sparse suborbital sampling. Recent efforts to make full use of A-Train aerosol sensor synergies will be highlighted. We describe planned field campaigns in the region to address the existing knowledge gaps. Specifically, we describe the scientific objectives and implementation of the five synergistic, international research activities aimed at providing some of the key aerosol and cloud properties and a process-level understanding of aerosol-cloud interactions over the SE Atlantic: NASA's ORACLES, the UK Met Office's CLARIFY-2016, the DoE's LASIC, NSF's ONFIRE, and CNRS' AEROCLO-SA.

Simulation of the Upper Clouds and Hazes of Venus Using a Microphysical Cloud Model

NASA Astrophysics Data System (ADS)

McGouldrick, K.

2012-12-01

Several different microphysical and chemical models of the clouds of Venus have been developed in attempts to reproduce the in situ observations of the Venus clouds made by Pioneer Venus, Venera, and Vega descent probes (Turco et al., 1983 (Icarus 53:18-25), James et al, 1997 (Icarus 129:147-171), Imamura and Hashimoto, 2001 (J. Atm. Sci. 58:3597-3612), and McGouldrick and Toon, 2007 (Icarus 191:1-24)). The model of McGouldrick and Toon has successfully reproduced observations within the condensational middle and lower cloud decks of Venus (between about 48 and 57 km altitude, experiencing conditions similar to Earth's troposphere) and it now being extended to also simulate the microphysics occurring in the upper cloud deck (between altitudes of about 57 km and 70 km, experiencing conditions similar to Earth's stratosphere). In the upper clouds, aerosols composed of a solution of sulfuric acid in water are generated from the reservoir of available water vapor and sulfuric acid vapor that is photochemically produced. The manner of particle creation (e.g., activation of cloud condensation nuclei, or homogeneous or heterogeneous nucleation) is still incompletely understood, and the atmospheric environment has been measured to be not inconsistent with frozen aerosol particles (either sulfuric acid monohydrate or water ice). The material phase, viscosity, and surface tension of the aerosols (which are strongly dependent up on the local temperature and water vapor concentration) can affect the coagulation efficiencies of the aerosol, leading to variations in the size distributions, and other microphysical and radiative properties. Here, I present recent work exploring the effects of nucleation rates and coalescence efficiencies on the simulated Venus upper clouds.

Natural aerosols explain seasonal and spatial patterns of Southern Ocean cloud albedo.

PubMed

McCoy, Daniel T; Burrows, Susannah M; Wood, Robert; Grosvenor, Daniel P; Elliott, Scott M; Ma, Po-Lun; Rasch, Phillip J; Hartmann, Dennis L

2015-07-01

Atmospheric aerosols, suspended solid and liquid particles, act as nucleation sites for cloud drop formation, affecting clouds and cloud properties-ultimately influencing the cloud dynamics, lifetime, water path, and areal extent that determine the reflectivity (albedo) of clouds. The concentration N d of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations affect not only cloud properties themselves but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. It is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed N d. Enhanced N d is spatially correlated with regions of high chlorophyll a, and the spatiotemporal variability in N d is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35(o) to 45(o)S) and by organic matter in sea spray aerosol at higher latitudes (45(o) to 55(o)S). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m(-2) over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.

Fluorescent pseudomonads isolated from Hebridean cloud and rain water produce biosurfactants but do not cause ice nucleation

NASA Astrophysics Data System (ADS)

Ahern, H. E.; Walsh, K. A.; Hill, T. C. J.; Moffett, B. F.

2007-02-01

Microorganisms were discovered in clouds over 100 years ago but information on bacterial community structure and function is limited. Clouds may not only be a niche within which bacteria could thrive but they might also influence dynamic processes using ice nucleating and cloud condensing abilities. Cloud and rain samples were collected from two mountains in the Outer Hebrides, NW Scotland, UK. Community composition was determined using a combination of amplified 16S ribosomal DNA restriction analysis and sequencing. 256 clones yielded 100 operational taxonomic units (OTUs) of which half were related to bacteria from terrestrial psychrophilic environments. Cloud samples were dominated by a mixture of fluorescent Pseudomonas spp., some of which have been reported to be ice nucleators. It was therefore possible that these bacteria were using the ice nucleation (IN) gene to trigger the Bergeron-Findeisen process of raindrop formation as a mechanism for dispersal. In this study the IN gene was not detected in any of the isolates using both polymerase chain reaction (PCR) and differential scanning calorimetry (DSC). Instead 55% of the total isolates from both cloud and rain samples displayed significant biosurfactant activity when analyzed using the drop-collapse technique. All isolates were characterised as fluorescent pseudomonads. Surfactants have been found to be very important in lowering atmospheric critical supersaturations required for the activation of aerosols into cloud condensation nuclei (CCN). It is also known that surfactants influence cloud droplet size and increase cloud lifetime and albedo. Some bacteria are known to act as CCN and so it is conceivable that these fluorescent pseudomonads are using surfactants to facilitate their activation from aerosols into CCN. This would allow water scavenging,~countering desiccation, and assist in their widespread dispersal.

Ice-nucleation negative fluorescent pseudomonads isolated from Hebridean cloud and rain water produce biosurfactants

NASA Astrophysics Data System (ADS)

Ahern, H. E.; Walsh, K. A.; Hill, T. C. J.; Moffett, B. F.

2006-10-01

Microorganisms were discovered in clouds over 100 years ago but information on bacterial community structure and function is limited. Clouds may not only be a niche within which bacteria could thrive but they might also influence dynamic processes using ice nucleating and cloud condensing abilities. Cloud and rain samples were collected from two mountains in the Outer Hebrides, NW Scotland, UK. Community composition was determined using a combination of amplified 16S ribosomal DNA restriction analysis and sequencing. 256 clones yielded 100 operational taxonomic units (OTUs) of which half were related to bacteria from terrestrial psychrophilic environments. Cloud samples were dominated by a mixture of fluorescent Pseudomonas spp., some of which have been reported to be ice nucleators. It was therefore possible that these bacteria were using the ice nucleation (IN) gene to trigger the Bergeron-Findeisen process of raindrop formation as a mechanism for dispersal. In this study the IN gene was not detected in any of the isolates using both polymerase chain reaction (PCR) and differential scanning calorimetry (DSC). Instead 55% of the total isolates from both cloud and rain samples displayed significant biosurfactant activity when analyzed using the drop-collapse technique. All were characterised as fluorescent pseudomonads. Surfactants have been found to be very important in lowering atmospheric critical supersaturations required for the activation of aerosols into cloud condensation nuclei (CCN). It is also known that surfactants influence cloud droplet size and increase cloud lifetime and albedo. Some bacteria are known to act as CCN and so it is conceivable that these fluorescent pseudomonads are using surfactants to facilitate their activation from aerosols into CCN. This would allow water scavenging, countering desiccation, and assist in their widespread dispersal.

Quantifying the impact of anthropogenic pollution on cloud properties derived from ground based remote sensors at the North Slope of Alaska

NASA Astrophysics Data System (ADS)

Maahn, M.; Acquistapace, C.; de Boer, G.; Cox, C.; Feingold, G.; Marke, T.; Williams, C. R.

2017-12-01

When acting as cloud condensation nuclei (CCN) or ice nucleating particles (INPs), aerosols have a strong potential to influence cloud properties. In particular, they can impact the number, size, and phase of cloud particles and potentially cloud lifetime through aerosol indirect and semi-direct effects. In polar regions, these effects are of great importance for the radiation budget due to the shortwave albedo and longwave emissivity of mixed-phase clouds. The Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program operates two super sites equipped with state of the art ground-based remote sensing instruments in northern Alaska. The sites are both coastal and are highly correlated with respect to large scale synoptic patterns. While the site at Utqiaġvik (formerly known as Barrow) generally represents a relatively pristine Arctic environment lacking significant anthropogenic sources, the site at Oliktok Point, approximately 250 km to the east, is surrounded by the Prudhoe Bay Oil Field, which is the largest oil field in North America. Based on aircraft measurement, the authors recently showed that differences in the properties of liquid clouds properties between the sites can be attributed to local emissions associated with the industrial activities in the Prudhoe Bay region (Maahn et al. 2017, ACPD). However, aircraft measurements do not provide a representative sample of cloud properties due to temporal limitations in the amount of data. In order to investigate how frequently and to what extent liquid cloud properties and processes are modified, we use ground based remote sensing observations such as e.g., cloud radar, Doppler lidar, and microwave radiometer obtained continuously at the two sites. In this way, we are able to quantify inter-site differences with respect to cloud drizzle production, liquid water path, frequency of cloud occurrence, and cloud radiative properties. Turbulence and the coupling of clouds to the boundary layer is investigated in order to infer the potential role of locally emitted aerosols in modulating the observed differences.

Laboratory studies of stratospheric aerosol chemistry

NASA Technical Reports Server (NTRS)

Molina, Mario J.

1996-01-01

In this report we summarize the results of the two sets of projects funded by the NASA grant NAG2-632, namely investigations of various thermodynamic and nucleation properties of the aqueous acid system which makes up stratospheric aerosols, and measurements of reaction probabilities directly on ice aerosols with sizes corresponding to those of polar stratospheric cloud particles. The results of these investigations are of importance for the assessment of the potential stratospheric effects of future fleets of supersonic aircraft. In particular, the results permit to better estimate the effects of increased amounts of water vapor and nitric acid (which forms from nitrogen oxides) on polar stratospheric clouds and on the chemistry induced by these clouds.

Black carbon mixing state impacts on cloud microphysical properties: effects of aerosol plume and environmental conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ching, Ping Pui; Riemer, Nicole; West, Matthew

2016-05-27

Black carbon (BC) is usually mixed with other aerosol species within individual aerosol particles. This mixture, along with the particles' size and morphology, determines the particles' optical and cloud condensation nuclei properties, and hence black carbon's climate impacts. In this study the particle-resolved aerosol model PartMC-MOSAIC was used to quantify the importance of black carbon mixing state for predicting cloud microphysical quantities. Based on a set of about 100 cloud parcel simulations a process level analysis framework was developed to attribute the response in cloud microphysical properties to changes in the underlying aerosol population ("plume effect") and the cloud parcelmore » cooling rate ("parcel effect"). It shows that the response of cloud droplet number concentration to changes in BC emissions depends on the BC mixing state. When the aerosol population contains mainly aged BC particles an increase in BC emission results in increasing cloud droplet number concentrations ("additive effect"). In contrast, when the aerosol population contains mainly fresh BC particles they act as sinks for condensable gaseous species, resulting in a decrease in cloud droplet number concentration as BC emissions are increased ("competition effect"). Additionally, we quantified the error in cloud microphysical quantities when neglecting the information on BC mixing state, which is often done in aerosol models. The errors ranged from -12% to +45% for the cloud droplet number fraction, from 0% to +1022% for the nucleation-scavenged black carbon (BC) mass fraction, from -12% to +4% for the effective radius, and from -30% to +60% for the relative dispersion.« less

Impact of the Bergeron-Findeisen process on the release of aerosol particles during the evolution of cloud ice

NASA Astrophysics Data System (ADS)

Schwarzenböck, A.; Mertes, S.; Heintzenberg, J.; Wobrock, W.; Laj, P.

The paper focuses on the redistribution of aerosol particles (APs) during the artificial nucleation and subsequent growth of ice crystals in a supercooled cloud. A significant number of the supercooled cloud droplets during icing periods (seeding agents: C 3H 8, CO 2) did not freeze as was presumed prior to the experiment but instead evaporated. The net mass flux of water vapour from the evaporating droplets to the nucleating ice crystals (Bergeron-Findeisen mechanism) led to the release of residual particles that simultaneously appeared in the interstitial phase. The strong decrease of the droplet residuals confirms the nucleation of ice particles on seeding germs without natural aerosol particles serving as ice nuclei. As the number of residual particles during the seedings did not drop to zero, other processes such as heterogeneous ice nucleation, spontaneous freezing, entrainment of supercooled droplets and diffusion to the created particle-free ice germs must have contributed to the experimental findings. During the icing periods, residual mass concentrations in the condensed phase dropped by a factor of 1.1-6.7, as compared to the unperturbed supercooled cloud. As the Bergeron-Findeisen process also occurs without artificial seeding in the atmosphere, this study demonstrated that the hydrometeors in mixed-phase clouds might be much cleaner than anticipated for the simple freezing process of supercooled droplets in tropospheric mid latitude clouds.

The impact of gravity waves and cloud nucleation threshold on stratospheric water and tropical tropospheric cloud fraction

NASA Astrophysics Data System (ADS)

Schoeberl, Mark; Dessler, Andrew; Ye, Hao; Wang, Tao; Avery, Melody; Jensen, Eric

2016-08-01

Using the Modern Era Retrospective-Analysis for Research and Applications (MERRA) and MERRA-2 reanalysis winds, temperatures, and anvil cloud ice, we explore the impact of varying the cloud nucleation threshold relative humidity (RH) and high-frequency gravity waves on stratospheric water vapor (H2O) and upper tropical tropopause cloud fraction (TCF). Our model results are compared to 2008/2009 winter TCF derived from Cloud-Aerosol Lidar with Orthogonal Polarization and H2O observations from the Microwave Limb Sounder (MLS). The RH threshold affects both model H2O and TCF, while high-frequency gravity waves mostly impact TCF. Adjusting the nucleation RH and the amplitude of high-frequency gravity waves allows us to tune the model to observations. Reasonable observational agreement is obtained with a nucleation threshold between 130% and 150% RH consistent with airborne observations. For the MERRA reanalysis, we lower the tropopause temperature by 0.5 K roughly consistent with GPS radio occultation measurements and include ~0.1 K high-frequency gravity wave temperature oscillations in order to match TCF and H2O observations. For MERRA-2 we do not need to adjust the tropopause temperature nor add gravity waves, because there are sufficient high-frequency temperature oscillations already present in the MERRA-2 reanalysis to reproduce the observed TCF.

Parameterization of cloud glaciation by atmospheric dust

NASA Astrophysics Data System (ADS)

Nickovic, Slobodan; Cvetkovic, Bojan; Madonna, Fabio; Pejanovic, Goran; Petkovic, Slavko

2016-04-01

The exponential growth of research interest on ice nucleation (IN) is motivated, inter alias, by needs to improve generally unsatisfactory representation of cold cloud formation in atmospheric models, and therefore to increase the accuracy of weather and climate predictions, including better forecasting of precipitation. Research shows that mineral dust significantly contributes to cloud ice nucleation. Samples of residual particles in cloud ice crystals collected by aircraft measurements performed in the upper tropopause of regions distant from desert sources indicate that dust particles dominate over other known ice nuclei such as soot and biological particles. In the nucleation process, dust chemical aging had minor effects. The observational evidence on IN processes has substantially improved over the last decade and clearly shows that there is a significant correlation between IN concentrations and the concentrations of coarser aerosol at a given temperature and moisture. Most recently, due to recognition of the dominant role of dust as ice nuclei, parameterizations for immersion and deposition icing specifically due to dust have been developed. Based on these achievements, we have developed a real-time forecasting coupled atmosphere-dust modelling system capable to operationally predict occurrence of cold clouds generated by dust. We have been thoroughly validated model simulations against available remote sensing observations. We have used the CNR-IMAA Potenza lidar and cloud radar observations to explore the model capability to represent vertical features of the cloud and aerosol vertical profiles. We also utilized the MSG-SEVIRI and MODIS satellite data to examine the accuracy of the simulated horizontal distribution of cold clouds. Based on the obtained encouraging verification scores, operational experimental prediction of ice clouds nucleated by dust has been introduced in the Serbian Hydrometeorological Service as a public available product.

Global Studies of the Sulfur Cycle Including the Influence of DMS and Fossil Fuel Sulfur on Climate and Climate Change

NASA Technical Reports Server (NTRS)

Penner, Joyce E.

1998-01-01

The indirect effect of anthropogenic aerosols, wherein aerosol particles are thought to increase cloud droplet concentrations and cloud lifetime, is the most uncertain component of climate forcing over the past 100 years. Here, for the first time, we use a mechanistic treatment of droplet nucleation and a prognostic treatment of the number of cloud droplets to study the indirect aerosol effect from changes in carbonaceous and sulfate aerosols. Cloud droplet nucleation is parameterized as a function of total aerosol number concentration, updraft velocity and a shape parameter, which takes into account the mechanism, of sulfate aerosol formation, while cloud droplet number depends on the nucleation as well as on droplet sinks. Whereas previous treatments have predicted annual average indirect effects between -1 and -2 W/sq m, we obtain an indirect aerosol effect between -0.14 W/sq m and -0.42 W/sq m in the global mean.

Response of mixed-phase boundary layer clouds with rapid and slow ice nucleation processes to cloud-top temperature trend

NASA Astrophysics Data System (ADS)

Fridlind, A. M.; Avramov, A.; Ackerman, A. S.; Alpert, P. A.; Knopf, D. A.; DeMott, P. J.; Brooks, S. D.; Glen, A.

2015-12-01

It has been argued on the basis of some laboratory data sets, observed mixed-phase cloud systems, and numerical modeling studies that weakly active or slowly consumed ice forming nuclei (IFN) may be important to natural cloud systems. It has also been argued on the basis of field measurements that ice nucleation under mixed-phase conditions appears to occur predominantly via a liquid-phase mechanism, requiring the presence of liquid droplets prior to substantial ice nucleation. Here we analyze the response of quasi-Lagrangian large-eddy simulations of mixed-phase cloud layers to IFN operating via a liquid-phase mode using assumptions that result in either slow or rapid depletion of IFN from the cloudy boundary layer. Using several generalized case studies that do not exhibit riming or drizzle, based loosely on field campaign data, we vary environmental conditions such that the cloud-top temperature trend varies. One objective of this work is to identify differing patterns in ice formation intensity that may be distinguishable from ground-based or satellite platforms.

A Theory of Immersion Freezing

NASA Technical Reports Server (NTRS)

Barahona, Donifan

2017-01-01

Immersion freezing is likely involved in the initiation of precipitation and determines to large extent the phase partitioning in convective clouds. Theoretical models commonly used to describe immersion freezing in atmospheric models are based on the classical nucleation theory which however neglects important interactions near the immersed particle that may affect nucleation rates. This work introduces a new theory of immersion freezing based on two premises. First, immersion ice nucleation is mediated by the modification of the properties of water near the particle-liquid interface, rather than by the geometry of the ice germ. Second, the same mechanism that leads to the decrease in the work of germ formation also decreases the mobility of water molecules near the immersed particle. These two premises allow establishing general thermodynamic constraints to the ice nucleation rate. Analysis of the new theory shows that active sites likely trigger ice nucleation, but they do not control the overall nucleation rate nor the probability of freezing. It also suggests that materials with different ice nucleation efficiency may exhibit similar freezing temperatures under similar conditions but differ in their sensitivity to particle surface area and cooling rate. Predicted nucleation rates show good agreement with observations for a diverse set of materials including dust, black carbon and bacterial ice nucleating particles. The application of the new theory within the NASA Global Earth System Model (GEOS-5) is also discussed.

A Comparison between Airborne and Mountaintop Cloud Microphysics

NASA Astrophysics Data System (ADS)

David, R.; Lowenthal, D. H.; Hallar, A. G.; McCubbin, I.; Avallone, L. M.; Mace, G. G.; Wang, Z.

2014-12-01

Complex terrain has a large impact on cloud dynamics and microphysics. Several studies have examined the microphysical details of orographically-enhanced clouds from either an aircraft or from a mountain top location. However, further research is needed to characterize the relationships between mountain top and airborne microphysical properties. During the winter of 2011, an airborne study, the Colorado Airborne Mixed-Phase Cloud Study (CAMPS), and a ground-based field campaign, the Storm Peak Lab (SPL) Cloud Property Validation Experiment (StormVEx) were conducted in the Park Range of the Colorado Rockies. The CAMPS study utilized the University of Wyoming King Air (UWKA) to provide airborne cloud microphysical and meteorological data on 29 flights totaling 98 flight hours over the Park Range from December 15, 2010 to February 28, 2011. The UWKA was equipped with instruments that measured both cloud droplet and ice crystal size distributions, liquid water content, total water content (vapor, liquid, and ice), and 3-dimensional wind speed and direction. The Wyoming Cloud Radar and Lidar were also deployed during the campaign. These measurements are used to characterize cloud structure upwind and above the Park Range. StormVEx measured cloud droplet, ice crystal, and aerosol size distributions at SPL, located on the west summit of Mt. Werner at 3220m MSL. The observations from SPL are used to determine mountain top cloud microphysical properties at elevations lower than the UWKA was able to sample in-situ. Comparisons showed that cloud microphysics aloft and at the surface were consistent with respect to snow growth processes while small crystal concentrations were routinely higher at the surface, suggesting ice nucleation near cloud base. The effects of aerosol concentrations and upwind stability on mountain top and downwind microphysics are considered.

Comparative study of ice nucleating efficiency of K-feldspar in immersion and deposition freezing modes

NASA Astrophysics Data System (ADS)

Hiron, T.; Hoffmann, N.; Peckhaus, A.; Kiselev, A. A.; Leisner, T.; Flossmann, A. I.

2016-12-01

One of the main challenges in understanding the evolution of Earth's climate resides in the understanding the role of ice nucleation on the development of tropospheric clouds as well as its initiation. K-feldspar is known to be a very active ice nucleating particle and this study focuses on the characterization of its activity in two heterogeneous nucleation modes, immersion and deposition freezing.We use a newly built humidity-controlled cold stage allowing the simultaneous observation of up to 2000 identical 0.6-nanoliter droplets containing suspension of mineral dust particles. The droplets are first cooled down to observe immersion freezing, the obtained ice crystals are then evaporated and finally, the residual particles are exposed to the water vapor supersaturated with respect to ice.The ice nucleation abilities for the individual residual particles are then compared for the different freezing modes and correlation between immersion ice nuclei and deposition ice nuclei is investigated.Based on the electron microscopy analysis of the residual particles, we discuss the possible relationship between the ice nucleation properties of feldspar and its microstructure. Finally, we discuss the atmospheric implications of our experimental results, using DESCAM, a 1.5D bin-resolved microphysics model.

Laboratory measurements of heterogeneous CO2 ice nucleation on nanoparticles under conditions relevant to the Martian mesosphere

NASA Astrophysics Data System (ADS)

Nachbar, Mario; Duft, Denis; Mangan, Thomas Peter; Martin, Juan Carlos Gomez; Plane, John M. C.; Leisner, Thomas

2016-05-01

Clouds of CO2 ice particles have been observed in the Martian mesosphere. These clouds are believed to be formed through heterogeneous nucleation of CO2 on nanometer-sized meteoric smoke particles (MSPs) or upward propagated Martian dust particles (MDPs). Large uncertainties still exist in parameterizing the microphysical formation process of these clouds as key physicochemical parameters are not well known. We present measurements on the nucleation and growth of CO2 ice on sub-4 nm radius iron oxide and silica particles representing MSPs at conditions close to the mesosphere of Mars. For both particle materials we determine the desorption energy of CO2 to be ΔFdes = (18.5 ± 0.2) kJ mol-1 corresponding to ΔFdes = (0.192 ± 0.002) eV and obtain m = 0.78 ± 0.02 for the contact parameter that governs heterogeneous nucleation by analyzing the measurements using classical heterogeneous nucleation theory. We did not find any temperature dependence for the contact parameter in the temperature range examined (64 K to 73 K). By applying these values for MSPs in the Martian mesosphere, we derive characteristic temperatures for the onset of CO2 ice nucleation, which are 8-18 K below the CO2 frost point temperature, depending on particle size. This is in line with the occurrence of highly supersaturated conditions extending to 20 K below frost point temperature without the observation of clouds. Moreover, the sticking coefficient of CO2 on solid CO2 was determined to be near unity. We further argue that the same parameters can be applied to CO2 nucleation on upward propagated MDPs.

Radiative-dynamical and microphysical processes of thin cirrus clouds controlling humidity of air entering the stratosphere

NASA Astrophysics Data System (ADS)

Dinh, Tra; Fueglistaler, Stephan

2016-04-01

Thin cirrus clouds in the tropical tropopause layer (TTL) are of great interest due to their role in the control of water vapor and temperature in the TTL. Previous research on TTL cirrus clouds has focussed mainly on microphysical processes, specifically the ice nucleation mechanism and dehydration efficiency. Here, we use a cloud resolving model to analyse the sensitivity of TTL cirrus characteristics and impacts with respect to microphysical and radiative processes. A steady-state TTL cirrus cloud field is obtained in the model forced with dynamical conditions typical for the TTL (2-dimensional setup with a Kelvin-wave temperature perturbation). Our model results show that the dehydration efficiency (as given by the domain average relative humidity in the layer of cloud occurrence) is relatively insensitive to the ice nucleation mechanism, i.e. homogeneous versus heterogeneous nucleation. Rather, TTL cirrus affect the water vapor entering the stratosphere via an indirect effect associated with the cloud radiative heating and dynamics. Resolving the cloud radiative heating and the radiatively induced circulations approximately doubles the domain average ice mass. The cloud radiative heating is proportional to the domain average ice mass, and the observed increase in domain average ice mass induces a domain average temperature increase of a few Kelvin. The corresponding increase in water vapor entering the stratosphere is estimated to be about 30 to 40%.

Surface structure, crystallographic and ice-nucleating properties of cellulose

NASA Astrophysics Data System (ADS)

Hiranuma, Naruki; Möhler, Ottmar; Kiselev, Alexei; Saathoff, Harald; Weidler, Peter; Shutthanandan, Shuttha; Kulkarni, Gourihar; Jantsch, Evelyn; Koop, Thomas

2015-04-01

Increasing evidence of the high diversity and efficient freezing ability of biological ice-nucleating particles is driving a reevaluation of their impact upon climate. Despite their potential importance, little is known about their atmospheric abundance and ice nucleation efficiency, especially non-proteinaceous ones, in comparison to non-biological materials (e.g., mineral dust). Recently, microcrystalline cellulose (MCC; non-proteinaceous plant structural polymer) has been identified as a potential biological ice-nucleating particle. However, it is still uncertain if the ice-nucleating activity is specific to the MCC structure or generally relevant to all cellulose materials, such that the results of MCC can be representatively scaled up to the total cellulose content in the atmosphere to address its role in clouds and the climate system. Here we use the helium ion microscopy (HIM) imaging and the X-ray diffraction (XRD) technique to characterize the nanoscale surface structure and crystalline properties of the two different types of cellulose (MCC and fibrous cellulose extracted from natural wood pulp) as model proxies for atmospheric cellulose particles and to assess their potential accessibility for water molecules. To complement these structural characterizations, we also present the results of immersion freezing experiments using the cold stage-based droplet freezing BINARY (Bielefeld Ice Nucleation ARaY) technique. The HIM results suggest that both cellulose types have a complex porous morphology with capillary spaces between the nanoscale fibrils over the microfiber surface. These surface structures may make cellulose accessible to water. The XRD results suggest that the structural properties of both cellulose materials are in agreement (i.e., P21 space group; a=7.96 Å, b=8.35 Å, c=10.28 Å) and comparable to the crystallographic properties of general monoclinic cellulose (i.e., Cellulose Iβ). The results obtained from the BINARY measurements suggest that there is no significant difference of the immersion ice nucleation activity of MCC and fibrous cellulose in supercooled water. Overall, our findings support the view that MCC may be a good proxy for inferring water uptake, wettability and ice nucleating properties of various cellulose materials. In addition, we discuss the ice-nucleating efficiencies of both cellulose samples and plant debris from the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) chamber experiments in comparison to the BINARY results. The influence of the acid processing of cellulose on its ice nucleation propensity may also be discussed to further demonstrate their atmospheric relevancy. Acknowledgement: We acknowledge support by German Research Society (DFG) and Ice Nuclei research UnIT (FOR 1525 INUIT).

Advances in heterogeneous ice nucleation research: Theoretical modeling and measurements

NASA Astrophysics Data System (ADS)

Beydoun, Hassan

In the atmosphere, cloud droplets can remain in a supercooled liquid phase at temperatures as low as -40 °C. Above this temperature, cloud droplets freeze via heterogeneous ice nucleation whereby a rare and poorly understood subset of atmospheric particles catalyze the ice phase transition. As the phase state of clouds is critical in determining their radiative properties and lifetime, deficiencies in our understanding of heterogeneous ice nucleation poses a large uncertainty on our efforts to predict human induced global climate change. Experimental challenges in properly simulating particle-induced freezing processes under atmospherically relevant conditions have largely contributed to the absence of a well-established model and parameterizations that accurately predict heterogeneous ice nucleation. Conversely, the sparsity of reliable measurement techniques available struggle to be interpreted by a single consistent theoretical or empirical framework, which results in layers of uncertainty when attempting to extrapolate useful information regarding ice nucleation for use in atmospheric cloud models. In this dissertation a new framework for describing heterogeneous ice nucleation is developed. Starting from classical nucleation theory, the surface of an ice nucleating particle is treated as a continuum of heterogeneous ice nucleating activity and a particle specific distribution of this activity g is derived. It is hypothesized that an individual particle species exhibits a critical surface area. Above this critical area the ice nucleating activity of a particle species can be described by one g distribution, g, while below it g expresses itself expresses externally resulting in particle to particle variability in ice nucleating activity. The framework is supported by cold plate droplet freezing measurements for dust and biological particles in which the total surface area of particle material available is varied. Freezing spectra above a certain surface area are shown to be successfully fitted with g while a process of random sampling from g can predict the freezing behavior below the identified critical surface area threshold. The framework is then extended to account for droplets composed of multiple particle species and successfully applied to predict the freezing spectra of a mixed proxy for an atmospheric dust-biological particle system. The contact freezing mode of ice nucleation, whereby a particle induces freezing upon collision with a droplet, is thought to be more efficient than particle initiated immersion freezing from within the droplet bulk. However, it has been a decades' long challenge to accurately measure this ice nucleation mode, since it necessitates reliably measuring the rate at which particles hit a droplet surface combined with direct determination of freezing onset. In an effort to remedy this longstanding deficiency a temperature controlled chilled aerosol optical tweezers capable of stably isolating water droplets in air at subzero temperatures has been designed and implemented. The new temperature controlled system retains the powerful capabilities of traditional aerosol optical tweezers: retrieval of a cavity enhanced Raman spectrum which could be used to accurately determine the size and refractive index of a trapped droplet. With these capabilities, it is estimated that the design can achieve ice supersaturation conditions at the droplet surface. It was also found that a KCl aqueous droplet simultaneously cooling and evaporating exhibited a significantly higher measured refractive index at its surface than when it was held at a steady state temperature. This implies the potential of a "salting out" process. Sensitivity of the cavity enhanced Raman spectrum as well as the visual image of a trapped droplet to dust particle collisions is shown, an important step in measuring collision frequencies of dust particles with a trapped droplet. These results may pave the way for future experiments of the exceptionally poorly understood contact freezing mode of ice nucleation.

Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: Results from the ORACLES-2016 Deployment and a First Look at ORACLES-2017 and Beyond

NASA Technical Reports Server (NTRS)

Redemann, Jens; Wood, R.; Zuidema, P.

2018-01-01

Seasonal biomass burning (BB) in Southern Africa during the Southern hemisphere spring produces almost a third of the Earth's BB aerosol particles. These particles are lofted into the mid-troposphere and transported westward over the South-East (SE) Atlantic, where they interact with one of the three semi-permanent subtropical stratocumulus (Sc) cloud decks in the world. These interactions include adjustments to aerosol-induced solar heating and microphysical effects. The representation of these interactions in climate models remains highly uncertain, because of the scarcity of observational constraints on both, the aerosol and cloud properties, and the governing physical processes. The first deployment of the NASA P-3 and ER-2 aircraft in the ORACLES (ObseRvations of Aerosols Above Clouds and Their IntEractionS) project in August/September of 2016 has started to fill this observational gap by providing an unprecedented look at the SE Atlantic cloud-aerosol system. We provide an overview of the first deployment, highlighting aerosol absorptive and cloud-nucleating properties, their vertical distribution relative to clouds, the locations and degree of aerosol mixing into clouds, cloud changes in response to such mixing, and cloud top stability relationships to the aerosol. We also expect to describe preliminary results of the second ORACLES deployment from Sao Tome and Pri­ncipe in August 2017. We will make an initial assessment of the differences and similarities of the BB plume and cloud properties as observed from a deployment site near the plume's northern edge. We will conclude with an outlook for the third ORACLES deployment in October 2018.

Ice nucleating particle concentration during a combustion aerosol event

NASA Astrophysics Data System (ADS)

Adams, Mike; O'Sullivan, Daniel; Porter, Grace; Sanchez-Marroquin, Alberto; Tarn, Mark; Harrison, Alex; McQuaid, Jim; Murray, Benjamin

2017-04-01

The formation of ice in supercooled clouds is important for cloud radiative properties, their lifetime and the formation of precipitation. Cloud water droplets can supercool to below -33oC, but in the presence of Ice Nucleating Particles (INPs) freezing can be initiated at much higher temperatures. The concentration of atmospheric aerosols that are active as INPs depends on a number of factors, such as temperature and aerosol composition and concentration. However, our knowledge of which aerosol types serve as INPs is limited. For example, there has been much discussion over whether aerosol from combustion processes are important as INP. This is significant because combustion aerosol have increased in concentration dramatically since pre-industrial times and therefore have the potential to exert a significant anthropogenic impact on clouds and climate. In this study we made measurements of INP concentrations in Leeds over a specific combustion aerosol event in order to test if there was a correlation between INP concentrations and combustion aerosol. The combustion aerosol event was on the 5th November which is a major bonfire and firework event celebrated throughout the UK. During the event we observed a factor of five increase in aerosol and a factor of 10 increase in black carbon, but observed no significant increase in INP concentration. This implies that black carbon and combustion aerosol did not compete with the background INP during this event.

Dynamical States of Low Temperature Cirrus

NASA Technical Reports Server (NTRS)

Barahona, D.; Nenes, A.

2011-01-01

Low ice crystal concentration and sustained in-cloud supersaturation, commonly found in cloud observations at low temperature, challenge our understanding of cirrus formation. Heterogeneous freezing from effloresced ammonium sulfate, glassy aerosol, dust and black carbon are proposed to cause these phenomena; this requires low updrafts for cirrus characteristics to agree with observations and is at odds with the gravity wave spectrum in the upper troposphere. Background temperature fluctuations however can establish a dynamical equilibrium between ice production and sedimentation loss (as opposed to ice crystal formation during the first stages of cloud evolution and subsequent slow cloud decay) that explains low temperature cirrus properties. This newly-discovered state is favored at low temperatures and does not require heterogeneous nucleation to occur (the presence of ice nuclei can however facilitate its onset). Our understanding of cirrus clouds and their role in anthropogenic climate change is reshaped, as the type of dynamical forcing will set these clouds in one of two preferred microphysical regimes with very different susceptibility to aerosol.

Small particles big effect? - Investigating ice nucleation abilities of soot particles

NASA Astrophysics Data System (ADS)

Mahrt, Fabian; David, Robert O.; Lohmann, Ulrike; Stopford, Chris; Wu, Zhijun; Kanji, Zamin A.

2017-04-01

Atmospheric soot particles are primary particles produced by incomplete combustion of biomass and/or fossil fuels. Thus soot mainly originates from anthropogenic emissions, stemming from combustion related processes in transport vehicles, industrial and residential uses. Such soot particles are generally complex mixtures of black carbon (BC) and organic matter (OM) (Bond et al., 2013; Petzold et al., 2013), depending on the sources and the interaction of the primary particles with other atmospheric matter and/or gases BC absorbs solar radiation having a warming effect on global climate. It can also act as a heterogeneous ice nucleating particle (INP) and thus impact cloud-radiation interactions, potentially cooling the climate (Lohmann, 2002). Previous studies, however, have shown conflicting results concerning the ice nucleation ability of soot, limiting the ability to predict its effects on Earth's radiation budget. Here we present a laboratory study where we systematically investigate the ice nucleation behavior of different soot particles. Commercial soot samples are used, including an amorphous, industrial carbon frequently used in coatings and coloring (FW 200, Orion Engineered Carbons) and a fullerene soot (572497 ALDRICH), e.g. used as catalyst. In addition, we use soot generated from a propane flame Combustion Aerosol Standard Generator (miniCAST, JING AG), as a proxy for atmospheric soot particles. The ice nucleation ability of these soot types is tested on size-selected particles for a wide temperature range from 253 K to 218 K, using the Horizontal Ice Nucleation Chamber (HINC), a Continuous Flow Diffusion Chamber (CFDC) (Kanji and Abbatt, 2009). Ice nucleation results from these soot surrogates will be compared to chemically more complex real world samples, collected on filters. Filters will be collected during the 2016/2017 winter haze periods in Beijing, China and represent atmospheric soot particles with sources from both industrial and residential emissions. Collected particles will be re-suspended and aerosolized using an atomizer (TSI, model 3076) and dried by a diffusion drier prior to ice nucleation experiments. A Particle Phase Discriminator (PPD) coupled to HINC will allow discrimination of size-resolved liquid and ice hydrometeors formed on the atmospheric soot particles injected into the CFDC. This will allow to more precisely quantify the microphysical properties of these particles in cloud processes for the conditions tested. To our knowledge this is the first time such a coupling is done for atmospheric soot particles. Results show different activation behavior of the soot over the temperature range investigated. While CAST-brown soot needs conditions above water saturation to show any freezing, some of the commercial soot samples show heterogeneous ice nucleation well below water saturation for the cirrus conditions. For the mixed-phase cloud conditions all soot types show droplet activation for high water supersaturation.

Ice nucleation activity of polysaccharides

NASA Astrophysics Data System (ADS)

Bichler, Magdalena; Felgitsch, Laura; Haeusler, Thomas; Seidl-Seiboth, Verena; Grothe, Hinrich

2015-04-01

Heterogeneous ice nucleation is an important process in the atmosphere. It shows direct impact on our climate by triggering ice cloud formation and therefore it has much influence on the radiation balance of our planet (Lohmann et al. 2002; Mishchenko et al. 1996). The process itself is not completely understood so far and many questions remain open. Different substances have been found to exhibit ice nucleation activity (INA). Due to their vast differences in chemistry and morphology it is difficult to predict what substance will make good ice nuclei and which will not. Hence simple model substances must be found and be tested regarding INA. Our work aims at gaining to a deeper understanding of heterogeneous ice nucleation. We intend to find some reference standards with defined chemistry, which may explain the mechanisms of heterogeneous ice nucleation. A particular focus lies on biological carbohydrates in regards to their INA. Biological carbohydrates are widely distributed in all kingdoms of life. Mostly they are specific for certain organisms and have well defined purposes, e.g. structural polysaccharides like chitin (in fungi and insects) and pectin (in plants), which has also water-binding properties. Since they are widely distributed throughout our biosphere and mostly safe to use for nutrition purposes, they are well studied and easily accessible, rendering them ideal candidates as proxies. In our experiments we examined various carbohydrates, like the already mentioned chitin and pectin, as well as their chemical modifications. Lohmann U.; A Glaciation Indirect Aerosol Effect Caused by Soot Aerosols; J. Geoph. Res.; Vol. 24 No.4; pp 11-1 - 11-4; 2002 Mishchenko M.I., Rossow W.B., Macke A., Lacis A. A.; Sensitivity of Cirrus Cloud Albedo, Bidirectional Reflectance and Optical Thickness Retrieval Accuracy to Ice Particle Shape, J. Geoph. Res.; Vol. 101, No D12; pp. 16,973 - 16,985; 1996

Ice nucleating particles over the Eastern Mediterranean measured by unmanned aircraft systems

NASA Astrophysics Data System (ADS)

Schrod, Jann; Weber, Daniel; Drücke, Jaqueline; Keleshis, Christos; Pikridas, Michael; Ebert, Martin; Cvetković, Bojan; Nickovic, Slobodan; Marinou, Eleni; Baars, Holger; Ansmann, Albert; Vrekoussis, Mihalis; Mihalopoulos, Nikos; Sciare, Jean; Curtius, Joachim; Bingemer, Heinz G.

2017-04-01

During an intensive field campaign on aerosol, clouds, and ice nucleation in the Eastern Mediterranean in April 2016, we measured the abundance of ice nucleating particles (INPs) in the lower troposphere from unmanned aircraft systems (UASs). Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UASs at altitudes up to 2.5 km. The number of INPs in these samples, which are active in the deposition and condensation modes at temperatures from -20 to -30 °C, were analyzed immediately after collection on site using the ice nucleus counter FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment). During the 1-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers' altitude. Here we present INP data from 42 individual flights, together with aerosol number concentrations, observations of lidar backscattering, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INPs with the particulate matter (PM), the lidar signal, and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INPs std L-1 were measured at -30 °C. The INP concentration in elevated plumes was on average a factor of 10 higher than at ground level. Since desert dust is transported for long distances over wide areas of the globe predominantly at several kilometers' altitude, we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation.

Oxidation stability of ice nuclei from plants

NASA Astrophysics Data System (ADS)

Felgitsch, Laura; Häusler, Thomas; Grothe, Hinrich

2017-04-01

Heterogeneous ice nucleation is an important process in cloud formation and therefore has direct influence on the radiation budget of the Earth. Biological ice nuclei (IN) are highly abundant in nature. Many plants have been found to produce IN. These IN are of special interest, since several have been found to be in a nano-particular/macromolecular size range (Pummer et al. 2015, Felgitsch et al. 2016). Particles of such a small size should show a high lifespan in the atmosphere. Further the substances can easily be attached to mineral dusts. Very little is known about the atmospheric fate of plant derived ice nuclei (IN) in case they become airborne. While they inherit the possibility to influence ice cloud formation, this property depends highly on the expected lifespan of the substance and of its ice nucleation activity in the atmosphere. For our experiment we exposed plant IN derived from black currant (berry juice) and birch (pollen washing water) to high concentrations of highly oxidative substances typically present in the atmosphere. The exposure lasted several hours and allowed us to monitor the changes in ice nucleation activity. Our results suggest a high stability towards oxidation leading to a high atmospheric life span of the ice nucleation activity if airborne. Pummer, B.G., Budke, C., Augustin-Bauditz, S., Niedermeier, D., Felgitsch, L., Kampf, C.J., Huber, R.G., Liedl, K.R., Loerting, T., Moschen, T., Schauperl, M., Tollinger, M., Morris, C.E., Wex, H., Grothe, H., Pöschl, U., Koop, T., and Fröhlich-Nowoisky, J.: Ice nucleation by water-soluble macromolecules, Atmos. Chem. Phys., 15, 4077-4091, 2015. Felgitsch , L., Bichler, M., Häusler, T., Hitzenberger, R., and Grothe, H.: Heterogeneous freezing of water triggered by berry juices from perenneal plants, submitted, 2016.

Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation.

PubMed

Ehrhart, Sebastian; Ickes, Luisa; Almeida, Joao; Amorim, Antonio; Barmet, Peter; Bianchi, Federico; Dommen, Josef; Dunne, Eimear M; Duplissy, Jonathan; Franchin, Alessandro; Kangasluoma, Juha; Kirkby, Jasper; Kürten, Andreas; Kupc, Agnieszka; Lehtipalo, Katrianne; Nieminen, Tuomo; Riccobono, Francesco; Rondo, Linda; Schobesberger, Siegfried; Steiner, Gerhard; Tomé, António; Wimmer, Daniela; Baltensperger, Urs; Wagner, Paul E; Curtius, Joachim

2016-10-27

Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of the binding energies of sulphuric acid and water in charged and neutral clusters. Predictions of SAWNUC are compared for the first time comprehensively with experimental binary nucleation data from the CLOUD chamber at European Organization for Nuclear Research. The experimental measurements span a temperature range of 208-292 K, sulphuric acid concentrations from 1·10 6 to 1·10 9  cm -3 , and distinguish between ion-induced and neutral nucleation. Good agreement, within a factor of 5, is found between the experimental and modeled formation rates for ion-induced nucleation at 278 K and below and for neutral nucleation at 208 and 223 K. Differences at warm temperatures are attributed to ammonia contamination which was indicated by the presence of ammonia-sulphuric acid clusters, detected by an Atmospheric Pressure Interface Time of Flight (APi-TOF) mass spectrometer. APi-TOF measurements of the sulphuric acid ion cluster distributions ( (H2SO4)i·HSO4- with i = 0, 1, ..., 10) show qualitative agreement with the SAWNUC ion cluster distributions. Remaining differences between the measured and modeled distributions are most likely due to fragmentation in the APi-TOF. The CLOUD results are in good agreement with previously measured cluster binding energies and show the SAWNUC model to be a good representation of ion-induced and neutral binary nucleation of sulphuric acid-water clusters in the middle and upper troposphere.

Ice Nucleation in Deep Convection

NASA Technical Reports Server (NTRS)

Jensen, Eric; Ackerman, Andrew; Stevens, David; Gore, Warren J. (Technical Monitor)

2001-01-01

The processes controlling production of ice crystals in deep, rapidly ascending convective columns are poorly understood due to the difficulties involved with either modeling or in situ sampling of these violent clouds. A large number of ice crystals are no doubt generated when droplets freeze at about -40 C. However, at higher levels, these crystals are likely depleted due to precipitation and detrainment. As the ice surface area decreases, the relative humidity can increase well above ice saturation, resulting in bursts of ice nucleation. We will present simulations of these processes using a large-eddy simulation model with detailed microphysics. Size bins are included for aerosols, liquid droplets, ice crystals, and mixed-phase (ice/liquid) hydrometers. Microphysical processes simulated include droplet activation, freezing, melting, homogeneous freezing of sulfate aerosols, and heterogeneous ice nucleation. We are focusing on the importance of ice nucleation events in the upper part of the cloud at temperatures below -40 C. We will show that the ultimate evolution of the cloud in this region (and the anvil produced by the convection) is sensitive to these ice nucleation events, and hence to the composition of upper tropospheric aerosols that get entrained into the convective column.

On the usage of classical nucleation theory in predicting the impact of bacteria on weather and climate

NASA Astrophysics Data System (ADS)

Sahyoun, Maher; Woetmann Nielsen, Niels; Havskov Sørensen, Jens; Finster, Kai; Bay Gosewinkel Karlson, Ulrich; Šantl-Temkiv, Tina; Smith Korsholm, Ulrik

2014-05-01

Bacteria, e.g. Pseudomonas syringae, have previously been found efficient in nucleating ice heterogeneously at temperatures close to -2°C in laboratory tests. Therefore, ice nucleation active (INA) bacteria may be involved in the formation of precipitation in mixed phase clouds, and could potentially influence weather and climate. Investigations into the impact of INA bacteria on climate have shown that emissions were too low to significantly impact the climate (Hoose et al., 2010). The goal of this study is to clarify the reason for finding the marginal impact on climate when INA bacteria were considered, by investigating the usability of ice nucleation rate parameterization based on classical nucleation theory (CNT). For this purpose, two parameterizations of heterogeneous ice nucleation were compared. Both parameterizations were implemented and tested in a 1-d version of the operational weather model (HIRLAM) (Lynch et al., 2000; Unden et al., 2002) in two different meteorological cases. The first parameterization is based on CNT and denoted CH08 (Chen et al., 2008). This parameterization is a function of temperature and the size of the IN. The second parameterization, denoted HAR13, was derived from nucleation measurements of SnomaxTM (Hartmann et al., 2013). It is a function of temperature and the number of protein complexes on the outer membranes of the cell. The fraction of cloud droplets containing each type of IN as percentage in the cloud droplets population were used and the sensitivity of cloud ice production in each parameterization was compared. In this study, HAR13 produces more cloud ice and precipitation than CH08 when the bacteria fraction increases. In CH08, the increase of the bacteria fraction leads to decreasing the cloud ice mixing ratio. The ice production using HAR13 was found to be more sensitive to the change of the bacterial fraction than CH08 which did not show a similar sensitivity. As a result, this may explain the marginal impact of IN bacteria in climate models when CH08 was used. The number of cell fragments containing proteins appears to be a more important parameter to consider than the size of the cell when parameterizing the heterogeneous freezing of bacteria.

Do detailed simulations with size-resolved microphysics reproduce basic features of observed cirrus ice size distributions?

NASA Astrophysics Data System (ADS)

Fridlind, A. M.; Atlas, R.; van Diedenhoven, B.; Ackerman, A. S.; Rind, D. H.; Harrington, J. Y.; McFarquhar, G. M.; Um, J.; Jackson, R.; Lawson, P.

2017-12-01

It has recently been suggested that seeding synoptic cirrus could have desirable characteristics as a geoengineering approach, but surprisingly large uncertainties remain in the fundamental parameters that govern cirrus properties, such as mass accommodation coefficient, ice crystal physical properties, aggregation efficiency, and ice nucleation rate from typical upper tropospheric aerosol. Only one synoptic cirrus model intercomparison study has been published to date, and studies that compare the shapes of observed and simulated ice size distributions remain sparse. Here we amend a recent model intercomparison setup using observations during two 2010 SPARTICUS campaign flights. We take a quasi-Lagrangian column approach and introduce an ensemble of gravity wave scenarios derived from collocated Doppler cloud radar retrievals of vertical wind speed. We use ice crystal properties derived from in situ cloud particle images, for the first time allowing smoothly varying and internally consistent treatments of nonspherical ice capacitance, fall speed, gravitational collection, and optical properties over all particle sizes in our model. We test two new parameterizations for mass accommodation coefficient as a function of size, temperature and water vapor supersaturation, and several ice nucleation scenarios. Comparison of results with in situ ice particle size distribution data, corrected using state-of-the-art algorithms to remove shattering artifacts, indicate that poorly constrained uncertainties in the number concentration of crystals smaller than 100 µm in maximum dimension still prohibit distinguishing which parameter combinations are more realistic. When projected area is concentrated at such sizes, the only parameter combination that reproduces observed size distribution properties uses a fixed mass accommodation coefficient of 0.01, on the low end of recently reported values. No simulations reproduce the observed abundance of such small crystals when the projected area is concentrated at larger sizes. Simulations across the parameter space are also compared with MODIS collection 6 retrievals and forward simulations of cloud radar reflectivity and mean Doppler velocity. Results motivate further in situ and laboratory measurements to narrow parameter uncertainties in models.

A short overview of the microbial population in clouds: Potential roles in atmospheric chemistry and nucleation processes

NASA Astrophysics Data System (ADS)

Delort, Anne-Marie; Vaïtilingom, Mickael; Amato, Pierre; Sancelme, Martine; Parazols, Marius; Mailhot, Gilles; Laj, Paolo; Deguillaume, Laurent

2010-11-01

Recent studies showed that living microorganisms, including bacteria, fungi and yeasts, are present in the atmospheric water phase (fog and clouds) and their role in chemical processes may have been underestimated. At the interface between atmospheric science and microbiology, information about this field of science suffers from the fact that not all recent findings are efficiently conveyed to both scientific communities. The purpose of this paper is therefore to provide a short overview of recent work linked to living organisms in the atmospheric water phase, from their activation to cloud droplets and ice crystal, to their potential impact on atmospheric chemical processes. This paper is focused on the microorganisms present in clouds and on the role they could play in atmospheric chemistry and nucleation processes. First, the life cycle of microorganisms via the atmosphere is examined, including their aerosolization from sources, their integration into clouds and their wet deposition on the ground. Second, special attention is paid to the possible impacts of microorganisms on liquid and ice nucleation processes. Third, a short description of the microorganisms that have been found in clouds and their variability in numbers and diversity is presented, emphasizing some specific characteristics that could favour their occurrence in cloud droplets. In the last section, the potential role of microbial activity as an alternative route to photochemical reaction pathways in cloud chemistry is discussed.

A Theory of Heterogeneous Ice Nucleation in the Immersion Mode

NASA Astrophysics Data System (ADS)

Barahona, D.

2017-12-01

Immersion ice nucleation is likely involved in the initiation of precipitation and determines to a large extent the phase partitioning in convective clouds. Theoretical models commonly used to describe immersion freezing in atmospheric models are based on the classical nucleation theory. CNT however neglects important interactions near the immersed particle that may affect nucleation rates. This work introduces a new theory of immersion freezing based on two premises. First, immersion ice nucleation is mediated by the modification of the properties of water near the particle-liquid interface rather than by the geometry of the ice germ. Second, the same mechanism that leads to the decrease in the work of germ formation also decreases the mobility of water molecules near the immersed particle. These two premises allow establishing general thermodynamic constraints to the ice nucleation rate. Analysis of the new theory shows that active sites likely trigger ice nucleation, but they do not control the overall nucleation rate nor the probability of freezing. It also suggests that materials with different ice nucleation efficiency may exhibit similar freezing temperatures under similar conditions but differ in their sensitivity to particle surface area and cooling rate. The theory suggests that many species are very efficient at nucleating ice and it is likely that highly effective INP are not uncommon in the atmosphere; however ice nucleation rates may be slower than currently believed. Predicted nucleation rates show good agreement with experimental results for a diverse set of atmospheric relevant materials including dust, black carbon and bacterial ice nucleating particles. The application of the new theory within the NASA Global Earth System Model (GEOS-5) is also discussed.

Urediospores of rust fungi are ice nucleation active at > -10 °C and harbor ice nucleation active bacteria

NASA Astrophysics Data System (ADS)

Morris, C. E.; Sands, D. C.; Glaux, C.; Samsatly, J.; Asaad, S.; Moukahel, A. R.; Gonçalves, F. L. T.; Bigg, E. K.

2013-04-01

Various features of the biology of the rust fungi and of the epidemiology of the plant diseases they cause illustrate the important role of rainfall in their life history. Based on this insight we have characterized the ice nucleation activity (INA) of the aerially disseminated spores (urediospores) of this group of fungi. Urediospores of this obligate plant parasite were collected from natural infections of 7 species of weeds in France, from coffee in Brazil and from field and greenhouse-grown wheat in France, the USA, Turkey and Syria. Immersion freezing was used to determine freezing onset temperatures and the abundance of ice nuclei in suspensions of washed spores. Microbiological analyses of spores from France, the USA and Brazil, and subsequent tests of the ice nucleation activity of the bacteria associated with spores were deployed to quantify the contribution of bacteria to the ice nucleation activity of the spores. All samples of spores were ice nucleation active, having freezing onset temperatures as high as -4 °C. Spores in most of the samples carried cells of ice nucleation-active strains of the bacterium Pseudomonas syringae (at rates of less than 1 bacterial cell per 100 urediospores), but bacterial INA accounted for only a small fraction of the INA observed in spore suspensions. Changes in the INA of spore suspensions after treatment with lysozyme suggest that the INA of urediospores involves a polysaccharide. Based on data from the literature, we have estimated the concentrations of urediospores in air at cloud height and in rainfall. These quantities are very similar to those reported for other biological ice nucleators in these same substrates. However, at cloud level convective activity leads to widely varying concentrations of particles of surface origin, so that mean concentrations can underestimate their possible effects on clouds. We propose that spatial and temporal concentrations of biological ice nucleators active at temperatures > -10 °C and the specific conditions under which they can influence cloud glaciation need to be further evaluated so as to understand how evolutionary processes could have positively selected for INA.

Saharan Dust Event Impacts on Cloud Formation and Radiation over Western Europe

NASA Technical Reports Server (NTRS)

Bangert, M.; Nenes, A.; Vogel, B.; Vogel, H.; Barahona, D.; Karydis, V. A.; Kumar, P.; Kottmeier, C.; Blahak, U.

2013-01-01

We investigated the impact of mineral dust particles on clouds, radiation and atmospheric state during a strong Saharan dust event over Europe in May 2008, applying a comprehensive online-coupled regional model framework that explicitly treats particle-microphysics and chemical composition. Sophisticated parameterizations for aerosol activation and ice nucleation, together with two-moment cloud microphysics are used to calculate the interaction of the different particles with clouds depending on their physical and chemical properties. The impact of dust on cloud droplet number concentration was found to be low, with just a slight increase in cloud droplet number concentration for both uncoated and coated dust. For temperatures lower than the level of homogeneous freezing, no significant impact of dust on the number and mass concentration of ice crystals was found, though the concentration of frozen dust particles reached up to 100 l-1 during the ice nucleation events. Mineral dust particles were found to have the largest impact on clouds in a temperature range between freezing level and the level of homogeneous freezing, where they determined the number concentration of ice crystals due to efficient heterogeneous freezing of the dust particles and modified the glaciation of mixed phase clouds. Our simulations show that during the dust events, ice crystals concentrations were increased twofold in this temperature range (compared to if dust interactions are neglected). This had a significant impact on the cloud optical properties, causing a reduction in the incoming short-wave radiation at the surface up to -75Wm-2. Including the direct interaction of dust with radiation caused an additional reduction in the incoming short-wave radiation by 40 to 80Wm-2, and the incoming long-wave radiation at the surface was increased significantly in the order of +10Wm-2. The strong radiative forcings associated with dust caused a reduction in surface temperature in the order of -0.2 to -0.5K for most parts of France, Germany, and Italy during the dust event. The maximum difference in surface temperature was found in the East of France, the Benelux, and Western Germany with up to -1 K. This magnitude of temperature change was sufficient to explain a systematic bias in numerical weather forecasts during the period of the dust event.

Microphysical Model Studies of Venus Clouds

NASA Astrophysics Data System (ADS)

Meade, P. E.; Bullock, M. A.; Grinspoon, D. H.

2004-11-01

We have adapted a standard cloud microphysics model to construct a self-consistent microphysical model of Venus' cloud layer which reproduces and extends previous studies (e.g. James et al. 1997). Our model is based on the Community Aerosol and Radiation Model Atmosphere (CARMA), which is a widely used computer code for terrestrial cloud microphysics, derived from the work of Toon et al. (1988). The standard code has been adapted to treat H2O and H2SO4 as co-condensing vapor species onto aqueous H2SO4 cloud droplets, as well as the nucleation of condensation nuclei to droplets. Vapor condensation and evaporation follows the method of James et al. (1997). Microphysical processes included in this model include nucleation of condensation nuclei, condensation and evaporation of H2O and H2SO4 vapor, and droplet coagulation. Vertical transport occurs though advection, eddy diffusion, sedimentation for both droplets and condensation nuclei. The cloud model is used to explore the sensitivity of Venus' cloud layer to environmental changes. Observations of the Venus' lower cloud from the Pioneer Venus, Venera, and Galileo spacecraft have suggested that the properties of the lower cloud may be time-variable, and at times may be entirely absent (Carlson et al. 1993, Grinspoon et al. 1993, Esposito et al. 1997). Our model explores the dependence of such behavior on environment factors such as variations in water or SO2 abundance. We have also calculated the optical properties of the model atmosphere using both the conventional optical constants for H2SO4 (Palmer and Williams, 1975), and the new data of Tisdale et al. (1998). This work has been supported by NASA's Exobiology Program. References Carlson, R.W., et al., 1993. Planetary and Space Science, 41, 477-486. Esposito, L.W., et al., 1997. In Venus II, eds. S.W. Bougher et al., pp. 415-458, University of Arizona Press, Tucson. Grinspoon, D.H., et al., 1993. Planetary and Space Science, 41 (July 1993), 515-542. James, E. P., et al., 1997. Icarus, 129, 147-171. Palmer, K.F., and D. Williams, 1975. Applied Optics, 14, 208-219. Tisdale, R.T., et al., 1998. Journal of Geophysical Research, 103, 25,353-25,370. Toon , O. B., et al., 1988. J. Atmos. Sci., 45, 2123-2143.

Deposition and immersion-mode nucleation of ice by three distinct samples of volcanic ash

NASA Astrophysics Data System (ADS)

Schill, G. P.; Genareau, K.; Tolbert, M. A.

2015-07-01

Ice nucleation of volcanic ash controls both ash aggregation and cloud glaciation, which affect atmospheric transport and global climate. Previously, it has been suggested that there is one characteristic ice nucleation efficiency for all volcanic ash, regardless of its composition, when accounting for surface area; however, this claim is derived from data from only two volcanic eruptions. In this work, we have studied the depositional and immersion freezing efficiency of three distinct samples of volcanic ash using Raman microscopy coupled to an environmental cell. Ash from the Fuego (basaltic ash, Guatemala), Soufrière Hills (andesitic ash, Montserrat), and Taupo (Oruanui eruption, rhyolitic ash, New Zealand) volcanoes were chosen to represent different geographical locations and silica content. All ash samples were quantitatively analyzed for both percent crystallinity and mineralogy using X-ray diffraction. In the present study, we find that all three samples of volcanic ash are excellent depositional ice nuclei, nucleating ice from 225 to 235 K at ice saturation ratios of 1.05 ± 0.01, comparable to the mineral dust proxy kaolinite. Since depositional ice nucleation will be more important at colder temperatures, fine volcanic ash may represent a global source of cold-cloud ice nuclei. For immersion freezing relevant to mixed-phase clouds, however, only the Oruanui ash exhibited appreciable heterogeneous ice nucleation activity. Similar to recent studies on mineral dust, we suggest that the mineralogy of volcanic ash may dictate its ice nucleation activity in the immersion mode.

Biological ice nucleation initiates hailstone formation

NASA Astrophysics Data System (ADS)

Michaud, Alexander B.; Dore, John E.; Leslie, Deborah; Lyons, W. Berry; Sands, David C.; Priscu, John C.

2014-11-01

Cloud condensation and ice nuclei in the troposphere are required precursors to cloud and precipitation formation, both of which influence the radiative balance of Earth. The initial stage of hailstone formation (i.e., the embryo) and the subsequent layered growth allow hail to be used as a model for the study of nucleation processes in precipitation. By virtue of the preserved particle and isotopic record captured by hailstones, they represent a unique form of precipitation that allows direct characterization of the particles present during atmospheric ice nucleation. Despite the ecological and economic consequences of hail storms, the dynamics of hailstone nucleation, and thus their formation, are not well understood. Our experiments show that hailstone embryos from three Rocky Mountain storms contained biological ice nuclei capable of freezing water at warm, subzero (°C) temperatures, indicating that biological particles can act as nucleation sites for hailstone formation. These results are corroborated by analysis of δD and δ18O from melted hailstone embryos, which show that the hailstones formed at similarly warm temperatures in situ. Low densities of ice nucleation active abiotic particles were also present in hailstone embryos, but their low concentration indicates they were not likely to have catalyzed ice formation at the warm temperatures determined from water stable isotope analysis. Our study provides new data on ice nucleation occurring at the bottom of clouds, an atmospheric region whose processes are critical to global climate models but which has challenged instrument-based measurements.

Sensitivity of Homogeneous Ice Nucleation to Aerosol Perturbations and Its Implications for Aerosol Indirect Effects Through Cirrus Clouds

NASA Astrophysics Data System (ADS)

Liu, X.; Shi, X.

2018-02-01

The magnitude and sign of anthropogenic aerosol impacts on cirrus clouds through ice nucleation are still very uncertain. In this study, aerosol sensitivity (ηα), defined as the sensitivity of the number concentration (Ni) of ice crystals formed from homogeneous ice nucleation to aerosol number concentration (Na), is examined based on simulations from a cloud parcel model. The model represents the fundamental process of ice crystal formation that results from homogeneous nucleation. We find that the geometric dispersion (σ) of the aerosol size distribution used in the model is a key factor for ηα. For a monodisperse size distribution, ηα is close to zero in vertical updrafts (V < 50 cm s-1) typical of cirrus clouds. However, ηα increases to 0.1-0.3 (i.e., Ni increases by a factor of 1.3-2.0 for a tenfold increase in Na) if aerosol particles follow lognormal size distributions with a σ of 1.6-2.3 in the upper troposphere. By varying the input aerosol and environmental parameters, our model reproduces a large range of ηα values derived from homogeneous ice nucleation parameterizations widely used in global climate models (GCMs). The differences in ηα from these parameterizations can translate into a range of anthropogenic aerosol longwave indirect forcings through cirrus clouds from 0.05 to 0.36 W m-2 with a GCM. Our study suggests that a larger ηα (0.1-0.3) is more plausible and the homogeneous nucleation parameterizations should include a realistic aerosol size distribution to accurately quantify anthropogenic aerosol indirect effects.

Sensitivity of Cirrus and Mixed-phase Clouds to the Ice Nuclei Spectra in McRAS-AC: Single Column Model Simulations

NASA Technical Reports Server (NTRS)

Betancourt, R. Morales; Lee, D.; Oreopoulos, L.; Sud, Y. C.; Barahona, D.; Nenes, A.

2012-01-01

The salient features of mixed-phase and ice clouds in a GCM cloud scheme are examined using the ice formation parameterizations of Liu and Penner (LP) and Barahona and Nenes (BN). The performance of LP and BN ice nucleation parameterizations were assessed in the GEOS-5 AGCM using the McRAS-AC cloud microphysics framework in single column mode. Four dimensional assimilated data from the intensive observation period of ARM TWP-ICE campaign was used to drive the fluxes and lateral forcing. Simulation experiments where established to test the impact of each parameterization in the resulting cloud fields. Three commonly used IN spectra were utilized in the BN parameterization to described the availability of IN for heterogeneous ice nucleation. The results show large similarities in the cirrus cloud regime between all the schemes tested, in which ice crystal concentrations were within a factor of 10 regardless of the parameterization used. In mixed-phase clouds there are some persistent differences in cloud particle number concentration and size, as well as in cloud fraction, ice water mixing ratio, and ice water path. Contact freezing in the simulated mixed-phase clouds contributed to transfer liquid to ice efficiently, so that on average, the clouds were fully glaciated at T approximately 260K, irrespective of the ice nucleation parameterization used. Comparison of simulated ice water path to available satellite derived observations were also performed, finding that all the schemes tested with the BN parameterization predicted 20 average values of IWP within plus or minus 15% of the observations.

Ice nucleation active particles are efficiently removed by precipitating clouds.

PubMed

Stopelli, Emiliano; Conen, Franz; Morris, Cindy E; Herrmann, Erik; Bukowiecki, Nicolas; Alewell, Christine

2015-11-10

Ice nucleation in cold clouds is a decisive step in the formation of rain and snow. Observations and modelling suggest that variations in the concentrations of ice nucleating particles (INPs) affect timing, location and amount of precipitation. A quantitative description of the abundance and variability of INPs is crucial to assess and predict their influence on precipitation. Here we used the hydrological indicator δ(18)O to derive the fraction of water vapour lost from precipitating clouds and correlated it with the abundance of INPs in freshly fallen snow. Results show that the number of INPs active at temperatures ≥ -10 °C (INPs-10) halves for every 10% of vapour lost through precipitation. Particles of similar size (>0.5 μm) halve in number for only every 20% of vapour lost, suggesting effective microphysical processing of INPs during precipitation. We show that INPs active at moderate supercooling are rapidly depleted by precipitating clouds, limiting their impact on subsequent rainfall development in time and space.

Understanding Cirrus Ice Crystal Number Variability for Different Heterogeneous Ice Nucleation Spectra

NASA Technical Reports Server (NTRS)

Sullivan, Sylvia C.; Betancourt, Ricardo Morales; Barahona, Donifan; Nenes, Athanasios

2016-01-01

Along with minimizing parameter uncertainty, understanding the cause of temporal and spatial variability of the nucleated ice crystal number, Ni, is key to improving the representation of cirrus clouds in climate models. To this end, sensitivities of Ni to input variables like aerosol number and diameter provide valuable information about nucleation regime and efficiency for a given model formulation. Here we use the adjoint model of the adjoint of a cirrus formation parameterization (Barahona and Nenes, 2009b) to understand Ni variability for various ice-nucleating particle (INP) spectra. Inputs are generated with the Community Atmosphere Model version 5, and simulations are done with a theoretically derived spectrum, an empirical lab-based spectrum and two field-based empirical spectra that differ in the nucleation threshold for black carbon particles and in the active site density for dust. The magnitude and sign of Ni sensitivity to insoluble aerosol number can be directly linked to nucleation regime and efficiency of various INP. The lab-based spectrum calculates much higher INP efficiencies than field-based ones, which reveals a disparity in aerosol surface properties. Ni sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters; this low temperature sensitivity regime has been experimentally reported before but never deconstructed as done here.

Aerosol and nucleation research in support of NASA cloud physics experiments in space. [ice nuclei generator for the atmospheric cloud physics laboratory on Spacelab

NASA Technical Reports Server (NTRS)

Vali, G.; Rogers, D.; Gordon, G.; Saunders, C. P. R.; Reischel, M.; Black, R.

1978-01-01

Tasks performed in the development of an ice nucleus generator which, within the facility concept of the ACPL, would provide a test aerosol suitable for a large number and variety of potential experiments are described. The impact of Atmospheric Cloud Physics Laboratory scientific functional requirements on ice nuclei generation and characterization subsystems was established. Potential aerosol generating systems were evaluated with special emphasis on reliability, repeatability and general suitability for application in Spacelab. Possible contamination problems associated with aerosol generation techniques were examined. The ice nucleating abilities of candidate test aerosols were examined and the possible impact of impurities on the nucleating abilities of those aerosols were assessed as well as the relative merits of various methods of aerosol size and number density measurements.

Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere.

PubMed

Almeida, João; Schobesberger, Siegfried; Kürten, Andreas; Ortega, Ismael K; Kupiainen-Määttä, Oona; Praplan, Arnaud P; Adamov, Alexey; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; David, André; Dommen, Josef; Donahue, Neil M; Downard, Andrew; Dunne, Eimear; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C; Franchin, Alessandro; Guida, Roberto; Hakala, Jani; Hansel, Armin; Heinritzi, Martin; Henschel, Henning; Jokinen, Tuija; Junninen, Heikki; Kajos, Maija; Kangasluoma, Juha; Keskinen, Helmi; Kupc, Agnieszka; Kurtén, Theo; Kvashin, Alexander N; Laaksonen, Ari; Lehtipalo, Katrianne; Leiminger, Markus; Leppä, Johannes; Loukonen, Ville; Makhmutov, Vladimir; Mathot, Serge; McGrath, Matthew J; Nieminen, Tuomo; Olenius, Tinja; Onnela, Antti; Petäjä, Tuukka; Riccobono, Francesco; Riipinen, Ilona; Rissanen, Matti; Rondo, Linda; Ruuskanen, Taina; Santos, Filipe D; Sarnela, Nina; Schallhart, Simon; Schnitzhofer, Ralf; Seinfeld, John H; Simon, Mario; Sipilä, Mikko; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Tröstl, Jasmin; Tsagkogeorgas, Georgios; Vaattovaara, Petri; Viisanen, Yrjo; Virtanen, Annele; Vrtala, Aron; Wagner, Paul E; Weingartner, Ernest; Wex, Heike; Williamson, Christina; Wimmer, Daniela; Ye, Penglin; Yli-Juuti, Taina; Carslaw, Kenneth S; Kulmala, Markku; Curtius, Joachim; Baltensperger, Urs; Worsnop, Douglas R; Vehkamäki, Hanna; Kirkby, Jasper

2013-10-17

Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei. Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes. Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases. However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere. It is thought that amines may enhance nucleation, but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid-amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid-dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.

Biological aerosol particles in the atmosphere and their impact on clouds (BIOCLOUDS)

NASA Astrophysics Data System (ADS)

Amato, Pierre; Attard, Eleonore; Deguillaume, Laurent; Delort, Anne-Marie; Flossmann, Andrea; Good, Nicholas; Joly, Muriel; Koop, Thomas; Möhler, Ottmar; Monier, Marie; Morris, Cindy; Oehm, Caroline; Pöschl, Ulrich; Sancelme, Martine

2015-04-01

The project BIOCLOUDS aimed at investigating and quantifying the role of bioaerosols in tropospheric clouds. We focused on the studies on microorganisms, mainly bacteria. To reach our objective we (1) isolated and identified INA bacterial strains in cloud waters, (2) studied in more details IN properties of bacteria isolated from cloud waters in laboratories and cloud chamber, (3) used new data as input to cloud models. 1. Isolation and Identification of INA bacterial strains in cloud waters Cloud water samples were collected at the puy de Dôme station under sterile conditions, microorganisms were cultured on agar plates and further identified by DNA sequencing coding for16SrRNA. 257 bacterial strains isolated from 25 cloud events were screened and 44 isolates were selected as they belonged to Pseudomonas, Xanthomonas and Erwinia genera which are potential INA candidates. Using the classical "Droplet Freezing method" as ice nucleation test, 7 strains were shown INA+. Their cumulative IN frequency profiles were established and showed that some of them are very efficient, for example the strain Pseudomonas syringae 13b74 started to nucleate a t-3°C and 4% of the cells were active at- 5°C. 2. Further laboratory investigations of IN properties of cloud bacterial strains All the experiments presented in this section were carried out with 3 Pseudomonas syringae strains. We tested the influence of O3, NO, UV and pH, which are atmospheric markers of anthropogenic activity, on the IN activity of the Pseudomonas strains. It was clearly shown that pH had a main influence, acidic pHs decreased the IN activity of the strains. This suggests a negative impact of human emissions on the natural capacity of bacteria to precipitate with rain. The 3 Pseudomas strains were sprayed in the AIDA cloud chamber. The survival of these strains with time before cloud formation was measured and will be used in the future to parameterize models for bacterial transport. After cloud formation, IN activity of bacteria was followed with time, our results suggest that bacteria are precipitated in the cloud chamber as a result of their IN activity. Also the coating of bacteria with sulfates decreased their IN activity, pointing out the negative potential anthropogenic influence on IN bacteria activity. 3. Modeling study to see if any impact of bacteria on cloud development and/or precipitation is realistic. Modeling studies were performed with DESCAM (Detailed SCAvenging Model) using as an input the new data from the different campaigns in AIDA. M. VAÏTILINGOM et al. Atmospheric Environment, 2012, 56, 88-100. E. ATTARD et al. Atmospheric Chemistry and Physics, 2012, 12, 10667-10677. M. JOLY et al. Atmospheric Environment, 2013, 70, 392-400.

ESPC Coupled Global Prediction System

DTIC Science & Technology

2014-09-30

active, and cloud- nucleating aerosols into NAVGEM for use in long-term simulations and forecasts and for use in the full coupled system. APPROACH...cloud- nucleating aerosols into NAVGEM for use in long-term simulations and forecasts for ESPC applications. We are relying on approaches, findings...function. For sea salt we follow NAAPS and use a source that depends on ocean surface winds and relative humidity . In lieu of the relevant

Airborne observations of the microphysical structure of two contrasting cirrus clouds

NASA Astrophysics Data System (ADS)

O'Shea, S. J.; Choularton, T. W.; Lloyd, G.; Crosier, J.; Bower, K. N.; Gallagher, M.; Abel, S. J.; Cotton, R. J.; Brown, P. R. A.; Fugal, J. P.; Schlenczek, O.; Borrmann, S.; Pickering, J. C.

2016-11-01

We present detailed airborne in situ measurements of cloud microphysics in two midlatitude cirrus clouds, collected as part of the Cirrus Coupled Cloud-Radiation Experiment. A new habit recognition algorithm for sorting cloud particle images using a neural network is introduced. Both flights observed clouds that were related to frontal systems, but one was actively developing while the other dissipated as it was sampled. The two clouds showed distinct differences in particle number, habit, and size. However, a number of common features were observed in the 2-D stereo data set, including a distinct bimodal size distribution within the higher-temperature regions of the clouds. This may result from a combination of local heterogeneous nucleation and large particles sedimenting from aloft. Both clouds had small ice crystals (<100 µm) present at all levels However, this small ice mode is not present in observations from a holographic probe. This raises the possibility that the small ice observed by optical array probes may at least be in part an instrument artifact due to the counting of out-of-focus large particles as small ice. The concentrations of ice crystals were a factor 10 higher in the actively growing cloud with the stronger updrafts, with a mean concentration of 261 L-1 compared to 29 L-1 in the decaying case. Particles larger than 700 µm were largely absent from the decaying cirrus case. A comparison with ice-nucleating particle parameterizations suggests that for the developing case the ice concentrations at the lowest temperatures are best explained by homogenous nucleation.

The implications of dust ice nuclei effect on cloud top temperature in a complex mesoscale convective system.

PubMed

Li, Rui; Dong, Xue; Guo, Jingchao; Fu, Yunfei; Zhao, Chun; Wang, Yu; Min, Qilong

2017-10-23

Mineral dust is the most important natural source of atmospheric ice nuclei (IN) which may significantly mediate the properties of ice cloud through heterogeneous nucleation and lead to crucial impacts on hydrological and energy cycle. The potential dust IN effect on cloud top temperature (CTT) in a well-developed mesoscale convective system (MCS) was studied using both satellite observations and cloud resolving model (CRM) simulations. We combined satellite observations from passive spectrometer, active cloud radar, lidar, and wind field simulations from CRM to identify the place where ice cloud mixed with dust particles. For given ice water path, the CTT of dust-mixed cloud is warmer than that in relatively pristine cloud. The probability distribution function (PDF) of CTT for dust-mixed clouds shifted to the warmer end and showed two peaks at about -45 °C and -25 °C. The PDF for relatively pristine cloud only show one peak at -55 °C. Cloud simulations with different microphysical schemes agreed well with each other and showed better agreement with satellite observations in pristine clouds, but they showed large discrepancies in dust-mixed clouds. Some microphysical schemes failed to predict the warm peak of CTT related to heterogeneous ice formation.

Competition for water vapour results in suppression of ice formation in mixed-phase clouds

NASA Astrophysics Data System (ADS)

Simpson, Emma L.; Connolly, Paul J.; McFiggans, Gordon

2018-05-01

The formation of ice in clouds can initiate precipitation and influence a cloud's reflectivity and lifetime, affecting climate to a highly uncertain degree. Nucleation of ice at elevated temperatures requires an ice nucleating particle (INP), which results in so-called heterogeneous freezing. Previously reported measurements for the ability of a particle to nucleate ice have been made in the absence of other aerosol which will act as cloud condensation nuclei (CCN) and are ubiquitous in the atmosphere. Here we show that CCN can outcompete INPs for available water vapour thus suppressing ice formation, which has the potential to significantly affect the Earth's radiation budget. The magnitude of this suppression is shown to be dependent on the mass of condensed water required for freezing. Here we show that ice formation in a state-of-the-art cloud parcel model is strongly dependent on the criteria for heterogeneous freezing selected from those previously hypothesised. We have developed an alternative criteria which agrees well with observations from cloud chamber experiments. This study demonstrates the dominant role that competition for water vapour can play in ice formation, highlighting both a need for clarity in the requirements for heterogeneous freezing and for measurements under atmospherically appropriate conditions.

The influence of organic-containing soil dust on ice nucleation and cloud properties

NASA Astrophysics Data System (ADS)

Hummel, Matthias; Grini, Alf; Berntsen, Terje K.; Ekman, Annica

2017-04-01

Natural mineral dust from desert regions is known to be the most important contributor to atmospheric ice-nucleating particles (INP) which induce heterogeneous ice nucleation in mixed-phase clouds. Its ability to nucleate ice effectively is shown by various laboratory (Hoose and Möhler 2012) and field results (DeMott et al. 2015) and its abundance in ice crystal residuals has also been shown (Cziczo et al. 2013). Thus it is an important player when representing mixed-phase clouds in climate models. MODIS satellite data indicate that 1 /4 of the global dust emission originates from semi-arid areas rather than from arid deserts (Ginoux et al. 2012). Here, organic components can mix with minerals within the soil and get into the atmosphere. These so-called 'soil dust' particles are ice-nucleating active at high sub-zero temperatures, i.e. at higher temperatures than pure desert dust (Steinke et al. 2016). In this study, soil dust is incorporated into the Norwegian Earth System Model (NorESM, Bentsen et al. 2013) and applied to a modified ice nucleation parameterization (Steinke et al. 2016). Its influence on the cloud ice phase is evaluated by comparing a control run, where only pure desert dust is considered, and a sensitivity experiment, where a fraction of the dust emissions are classified as soil dust. Both simulations are nudged to ERA-interim meteorology and they have the same loading of dust emissions. NorESM gives a lower annual soil dust emission flux compared to Ginoux et al. (2012), but the desert dust flux is similar to the MODIS-retrieved data. Although soil dust concentrations are much lower than desert dust, the NorESM simulations indicate that the annual INP concentrations from soil dust are on average lower by a just a factor of 4 than INP concentrations from pure desert dust. The highest soil dust INP concentrations occur at a lower height than for desert dust, i.e at warmer temperatures inside mixed-phase clouds. Furthermore, soil dust INP distributes only to a small extent towards subtropical regions, but does not expand further poleward than desert dust INP. Due to the current setup, with simulations nudged to ERA-Interim meteorology, only small changes in the cloud variables are possible. However, the experiment still shows clear influences of soil dust INP on the cloud ice phase. Due to an increased number of ice particles in regions with T<-15˚ C, the formation of precipitation particles is larger. Bentsen, M., Bethke, I., Debernard, J. B., Iversen, T., Kirkevåg, A., Seland, Ø., Drange, H., Roelandt, C., Seierstad, I. A., Hoose, C., and Kristjánsson, J. E.: The Norwegian Earth System Model, NorESM1-M - Part 1: Description and basic evaluation of the physical climate, Geosci. Model Dev., 6, 687-720, 10.5194/gmd-6-687-2013, 2013. Cziczo, D. J., Froyd, K. D., Hoose, C., Jensen, E. J., Diao, M., Zondlo, M. A., Smith, J. B., Twohy, C. H., and Murphy, D. M.: Clarifying the Dominant Sources and Mechanisms of Cirrus Cloud Formation, Science, 340, 1320-1324, 10.1126/science.1234145, 2013. DeMott, P. J., Prenni, A. J., McMeeking, G. R., Sullivan, R. C., Petters, M. D., Tobo, Y., Niemand, M., Möhler, O., Snider, J. R., Wang, Z., and Kreidenweis, S. M.: Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles, Atmos. Chem. Phys., 15, 393-409, 10.5194/acp-15-393-2015, 2015. Ginoux, P., Prospero, J. M., Gill, T. E., Hsu, N. C., and Zhao, M.: Global-scale attribution of anthropogenic and natural dust sources and their emission rates based on MODIS Deep Blue aerosol products, Reviews of Geophysics, 50, RG3005, 10.1029/2012RG000388, 2012. Hoose, C., and Möhler, O.: Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments, Atmos. Chem. Phys., 12, 9817-9854, 10.5194/acp-12-9817-2012, 2012. Steinke, I., Funk, R., Busse, J., Iturri, A., Kirchen, S., Leue, M., Möhler, O., Schwartz, T., Schnaiter, M., Sierau, B., Toprak, E., Ullrich, R., Ulrich, A., Hoose, C., and Leisner, T.: Ice nucleation activity of agricultural soil dust aerosols from Mongolia, Argentina, and Germany, Journal of Geophysical Research: Atmospheres, n/a-n/a, 10.1002/2016JD025160, 2016.

EDITORIAL: Aerosol cloud interactions—a challenge for measurements and modeling at the cutting edge of cloud climate interactions

NASA Astrophysics Data System (ADS)

Spichtinger, Peter; Cziczo, Daniel J.

2008-04-01

Research in aerosol properties and cloud characteristics have historically been considered two separate disciplines within the field of atmospheric science. As such, it has been uncommon for a single researcher, or even research group, to have considerable expertise in both subject areas. The recent attention paid to global climate change has shown that clouds can have a considerable effect on the Earth's climate and that one of the most uncertain aspects in their formation, persistence, and ultimate dissipation is the role played by aerosols. This highlights the need for researchers in both disciplines to interact more closely than they have in the past. This is the vision behind this focus issue of Environmental Research Letters. Certain interactions between aerosols and clouds are relatively well studied and understood. For example, it is known that an increase in the aerosol concentration will increase the number of droplets in warm clouds, decrease their average size, reduce the rate of precipitation, and extend the lifetime. Other effects are not as well known. For example, persistent ice super-saturated conditions are observed in the upper troposphere that appear to exceed our understanding of the conditions required for cirrus cloud formation. Further, the interplay of dynamics versus effects purely attributed to aerosols remains highly uncertain. The purpose of this focus issue is to consider the current state of knowledge of aerosol/cloud interactions, to define the contemporary uncertainties, and to outline research foci as we strive to better understand the Earth's climate system. This focus issue brings together laboratory experiments, field data, and model studies. The authors address issues associated with warm liquid water, cold ice, and intermediate temperature mixed-phase clouds. The topics include the uncertainty associated with the effect of black carbon and organics, aerosol types of anthropogenic interest, on droplet and ice formation. Phases of water which have not yet been fully defined, for example cubic ice, are considered. The impact of natural aerosols on clouds, for example mineral dust, is also discussed, as well as other natural but highly sensitive effects such as the Wegener Bergeron Findeisen process. It is our belief that this focus issue represents a leap forward not only in reducing the uncertainty associated with the interaction of aerosols and clouds but also a new link between groups that must work together to continue progress in this important area of climate science. Focus on Aerosol Cloud Interactions Contents The articles below represent the first accepted contributions and further additions will appear in the near future. The global influence of dust mineralogical composition on heterogeneous ice nucleation in mixed-phase clouds C Hoose, U Lohmann, R Erdin and I Tegen Ice formation via deposition nucleation on mineral dust and organics: dependence of onset relative humidity on total particulate surface area Zamin A Kanji, Octavian Florea and Jonathan P D Abbatt The Explicit-Cloud Parameterized-Pollutant hybrid approach for aerosol cloud interactions in multiscale modeling framework models: tracer transport results William I Gustafson Jr, Larry K Berg, Richard C Easter and Steven J Ghan Cloud effects from boreal forest fire smoke: evidence for ice nucleation from polarization lidar data and cloud model simulations Kenneth Sassen and Vitaly I Khvorostyanov The effect of organic coating on the heterogeneous ice nucleation efficiency of mineral dust aerosols O Möhler, S Benz, H Saathoff, M Schnaiter, R Wagner, J Schneider, S Walter, V Ebert and S Wagner Enhanced formation of cubic ice in aqueous organic acid droplets Benjamin J Murray Quantification of water uptake by soot particles O B Popovicheva, N M Persiantseva, V Tishkova, N K Shonija and N A Zubareva Meridional gradients of light absorbing carbon over northern Europe D Baumgardner, G Kok, M Krämer and F Weidle

Biases in field measurements of ice nuclei concentrations

NASA Astrophysics Data System (ADS)

Garimella, S.; Voigtländer, J.; Kulkarni, G.; Stratmann, F.; Cziczo, D. J.

2015-12-01

Ice nuclei (IN) play an important role in the climate system by influencing cloud properties, precipitation, and radiative transfer. Despite their importance, there are significant uncertainties in estimating IN concentrations because of the complexities of atmospheric ice nucleation processes. Field measurements of IN concentrations with Continuous Flow Diffusion Chamber (CFDC) IN counters have been vital to constrain IN number concentrations and have led to various parameterizations of IN number vs. temperature and particle concentration. These parameterizations are used in many global climate models, which are very sensitive to the treatment of cloud microphysics. However, due to non-idealities in CFDC behavior, especially at high relative humidity, many of these measurements are likely biased too low. In this study, the extent of this low bias is examined with laboratory experiments at a variety of instrument conditions using the SPectrometer for Ice Nucleation, a commercially-available CFDC-style chamber. These laboratory results are compared to theoretical calculations and computational fluid dynamics models to map the variability of this bias as a function of chamber temperature and relative humidity.

Can Hail and Rain Nucleate Cloud Droplets?

NASA Astrophysics Data System (ADS)

Weiss, S.; Prabhakaran, P.; Krekhov, A.; Pumir, A.; Bodenschatz, E.

2017-12-01

We present results from a laboratory scale moist convection experiment composed of a mixture of pressurized sulphur hexafluoride (SF6 - liquid and vapor phase) and helium (He - gas phase) to mimic the wet (saturated water vapor) and dry components (nitrogen, oxygen etc.) of the earth's atmosphere. We operate the experiments close to critical conditions to allow for homogeneous nucleation of sulphur hexafluoride droplets. The liquid SF6 pool is heated from below and the warm SF6 vapor from the liquid-vapor interface rise and condense underneath the cold top plate. We observe the nucleation of microdroplets in the wake of cold drops falling through the SF6-He atmosphere. Using classical nucleation theory, we show that the nucleation is caused by isobaric cooling of SF6 vapor in the wake of the cold drop. Furthermore, we argue that in an atmospheric cloud, falling hail and large cold raindrops may induce heterogeneous nucleation of microdroplets in their wake. We also observe that under appropriate conditions these microdroplets form a stable horizontal layer, thus separating regions of super and sub-critical saturation.

Can hail and rain nucleate cloud droplets?

NASA Astrophysics Data System (ADS)

Prabhakaran, Prasanth; Weiss, Stephan; Krekhov, Alexei; Pumir, Alain; Bodenschatz, Eberhard

2017-11-01

We present results from a laboratory scale moist convection experiment composed of a mixture of pressurized sulphur hexafluoride (SF6 - liquid and vapor phase) and helium (He - gas phase) to mimic the wet (saturated water vapor) and dry components (nitrogen, oxygen etc.) of the earth's atmosphere. We operate the experiments close to critical conditions to allow for homogeneous nucleation of sulphur hexafluoride droplets. The liquid SF6 pool is heated from below and the warm SF6 vapor from the liquid-vapor interface rise and condense underneath the cold top plate. We observe the nucleation of microdroplets in the wake of cold drops falling through the SF6-He atmosphere. Using classical nucleation theory, we show that the nucleation is caused by isobaric cooling of SF6 vapor in the wake of the cold drop. Furthermore, we argue that in an atmospheric cloud, falling hail and large cold raindrops may induce heterogeneous nucleation of microdroplets in their wake. We also observe that under appropriate conditions these microdroplets form a stable horizontal layer, thus separating regions of super and sub-critical saturation.

Evaluating Ice Nucleating Particle Concentrations From Prognostic Dust Minerals in an Earth System Model

NASA Astrophysics Data System (ADS)

Perlwitz, J. P.; Knopf, D. A.; Fridlind, A. M.; Miller, R. L.; Pérez García-Pando, C.; DeMott, P. J.

2016-12-01

The effect of aerosol particles on the radiative properties of clouds, the so-called, indirect effect of aerosols, is recognized as one of the largest sources of uncertainty in climate prediction. The distribution of water vapor, precipitation, and ice cloud formation are influenced by the atmospheric ice formation, thereby modulating cloud albedo and thus climate. It is well known that different particle types possess different ice formation propensities with mineral dust being a superior ice nucleating particle (INP) compared to soot particles. Furthermore, some dust mineral types are more proficient INP than others, depending on temperature and relative humidity.In recent work, we have presented an improved dust aerosol module in the NASA GISS Earth System ModelE2 with prognostic mineral composition of the dust aerosols. Thus, there are regional variations in dust composition. We evaluated the predicted mineral fractions of dust aerosols by comparing them to measurements from a compilation of about 60 published literature references. Additionally, the capability of the model to reproduce the elemental composition of the simulated dusthas been tested at Izana Observatory at Tenerife, Canary Islands, which is located off-shore of Africa and where frequent dust events are observed. We have been able to show that the new approach delivers a robust improvement of the predicted mineral fractions and elemental composition of dust.In the current study, we use three-dimensional dust mineral fields and thermodynamic conditions, which are simulated using GISS ModelE, to calculate offline the INP concentrations derived using different ice nucleation parameterizations that are currently discussed. We evaluate the calculated INP concentrations from the different parameterizations by comparing them to INP concentrations from field measurements.

Warming ancient Mars with water clouds

NASA Astrophysics Data System (ADS)

Hartwick, V.; Toon, B.

2017-12-01

High clouds in the present day Mars atmosphere nucleate on interplanetary dust particles (IDPs) that burn up on entry into the Mars atmosphere. Clouds form when superstaturated water vapor condenses on suspended aerosols. Radiatively active water ice clouds may play a crucial role in warming the early Mars climate. Urata and Toon (2011) simulate a stable warm paleo-climate for Mars if clouds form high in the atmosphere and if particles are sufficiently large (r > 10 μm). The annual fluence of micrometeoroids at Mars was larger early on in the evolution of our solar system. Additionally, the water vapor budget throughout the middle and high atmosphere was likely heightened . Both factors should contribute to enhanced nucleation and growth of water ice cloud particles at high altitudes. Here, we use the MarsCAM-CARMA general circulation model (GCM) to examine the radiative impact of high altitude water ice clouds on the early Mars climate and as a possible solution to the faint young sun problem for Mars.

Ice nucleating particles in the high Arctic at the beginning of the melt season

NASA Astrophysics Data System (ADS)

Hartmann, M.; Gong, X.; Van Pinxteren, M.; Welti, A.; Zeppenfeld, S.; Herrmann, H.; Stratmann, F.

2017-12-01

Ice nucleating particles (INPs) initiate the ice crystal formation in persistent Arctic mixed-phase clouds and are important for the formation of precipitation, which affects the radiative properties of the Arctic pack ice as well as the radiative properties of clouds. Sources of Arctic INP have been suggested to be local emissions from the marine boundary and long-range transport. To what extent local marine sources contribute to the INP population or if the majority of INPs originate from long-range transport is not yet known. Ship-based INP measurements in the PASCAL framework are reported. The field campaign took place from May 24 to July 20 2017 around and north of Svalbard (up to 84°N, between 0° and 35°E) onboard the RV Polarstern. INP concentrations were determined applying in-situ measurements (DMT Spectrometer for Ice Nuclei, SPIN) and offline filter techniques (filter sampling on both quartz fiber and polycarbonate filters with subsequent analysis of filter pieces and water suspension from particles collected on filters by means of immersion freezing experiments on cold stage setups). Additionally the compartments sea-surface micro layer (SML), bulk sea water, snow, sea ice and fog water were sampled and their ice nucleation potential quantified, also utilizing cold stages. The measurements yield comprehensive picture of the spatial and temporal distribution of INPs around Svalbard for the different compartments. The dependence of the INP concentration on meteorological conditions (e.g. wind speed) and the geographical situation (sea ice cover, distance to the ice edge) are investigated. Potential sources of INP are identified by the comparison of INP concentrations in the compartments and by back trajectory analysis.

Investigation of Polar Stratospheric Cloud Solid Particle Formation Mechanisms Using ILAS and AVHRR Observations in the Arctic

NASA Technical Reports Server (NTRS)

Irie, H.; Pagan, K. L.; Tabazadeh, A.; Legg, M. J.; Sugita, T.

2004-01-01

Satellite observations of denitrification and ice clouds in the Arctic lower stratosphere in February 1997 are used with Lagrangian microphysical box model calculations to evaluate nucleation mechanisms of solid polar stratospheric cloud (PSC) particles. The occurrences of ice clouds are not correlated in time and space with the locations of back trajectories of denitrified air masses, indicating that ice particle surfaces are not always a prerequisite for the formation of solid PSCs that lead to denitrification. In contrast, the model calculations incorporating a pseudoheterogeneous freezing process occurring at the vapor-liquid interface can quantitatively explain most of the observed denitrification when the nucleation activation free energy for nitric acid dihydrate formation is raised by only approx.10% relative to the current published values. Once nucleated, the conversion of nitric acid dihydrate to the stable trihydrate phase brings the computed levels of denitrification closer to the measurements. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and SblctureC: loud physics and chemistry; 0340 Atmospheric Composition and Structure: Middle atmosphere-composition and chemistry

A review of our understanding of the aerosol-cloud interaction from the perspective of a bin resolved cloud scale modelling

NASA Astrophysics Data System (ADS)

Flossmann, Andrea I.; Wobrock, Wolfram

2010-09-01

This review compiles the main results obtained using a mesoscale cloud model with bin resolved cloud micophysics and aerosol particle scavenging, as developed by our group over the years and applied to the simulation of shallow and deep convective clouds. The main features of the model are reviewed in different dynamical frameworks covering parcel model dynamics, as well as 1.5D, 2D and 3D dynamics. The main findings are summarized to yield a digested presentation which completes the general understanding of cloud-aerosol interaction, as currently available from textbook knowledge. Furthermore, it should provide support for general cloud model development, as it will suggest potentially minor processes that might be neglected with respect to more important ones and can support development of parameterizations for air quality, chemical transport and climate models. Our work has shown that in order to analyse dedicated campaign results, the supersaturation field and the complex dynamics of the specific clouds needs to be reproduced. Only 3D dynamics represents the variation of the supersaturation over the entire cloud, the continuous nucleation and deactivation of hydrometeors, and the dependence upon initial particle size distribution and solubility. However, general statements on certain processes can be obtained also by simpler dynamics. In particular, we found: Nucleation incorporates about 90% of the initial aerosol particle mass inside the cloud drops. Collision and coalescence redistributes the scavenged aerosol particle mass in such a way that the particle mass follows the main water mass. Small drops are more polluted than larger ones, as pollutant mass mixing ratio decreases with drops size. Collision and coalescence mixes the chemical composition of the generated drops. Their complete evaporation will release processed particles that are mostly larger and more hygroscopic than the initial particles. An interstitial aerosol is left unactivated between the cloud drops which is reduced in number and almost devoid of large particles. Consequently, impaction scavenging can probably be neglected inside clouds. Below clouds, impaction scavenging contributes around 30% to the particle mass reaching the ground by a rainfall event. The exact amount depends on the precise case studied. Nucleation and impaction scavenging directly by the ice phase in mixed phase clouds seems to play a minor role with respect to the particle mass that enters the ice particles via freezing of the liquid phase.The aerosol scavenging efficiency generally follows rather closely the precipitation scavenging value. The nucleation scavenging efficiency is around 90% for the liquid phase clouds and impaction scavenging generally contributed to about 30% of the particle mass in the rain. Clouds are very efficient in pumping up the boundary layer aerosol which essentially determines the cloud properties. For a marine case studied the net pumping depleted about 70% of the aerosol from the section of the boundary layer considered. The larger particles (and thus 70% of the mass vented up) got activated inside the cloud. A weak net import through cloud top and the upwind side was found, as well as a larger net export at the downwind side. The outside cloud subsidence can add to the replenishment of the boundary layer and eventually cause a recycling of the particles into the cloud. The results of the parcel model studies seem to indicate that increasing particulate pollution and decreasing solubility suppresses rain formation. In individual and short time cloud simulations this behaviour was even confirmed in our 3D model studies. However, taking into account entire cloud fields over longer periods of time yields the strong spatial and temporal variability of the results with isolated regions of inverse correlation of the effects. Even though in general initially the expected behaviour was found, after several hours of simulation, the overall precipitation amounts of the more polluted cases caught up. This suggests that a changing pollution will affect the spatial and temporal pattern of precipitation, but will probably not reduce the overall long term precipitation amount which might be entirely governed by the moisture state of the atmosphere. Our results regarding mixed phase precipitation with respect to "all liquid" cases seem to confirm this idea, as with increasing modelling time the precipitation mass of both cases also become similar.

O the Size Dependence of the Chemical Properties of Cloud Droplets: Exploratory Studies by Aircraft

NASA Astrophysics Data System (ADS)

Twohy, Cynthia H.

1992-09-01

Clouds play an important role in the climate of the earth and in the transport and transformation of chemical species, but many questions about clouds remain unanswered. In particular, the chemical properties of droplets may vary with droplet size, with potentially important consequences. The counterflow virtual impactor (CVI) separates droplets from interstitial particles and gases in a cloud and also can collect droplets in discrete size ranges. As such, the CVI is a useful tool for investigating the chemical components present in droplets of different sizes and their potential interactions with cloud processes. The purpose of this work is twofold. First, the sampling characteristics of the airborne CVI are investigated, using data from a variety of experiments. A thorough understanding of CVI properties is necessary in order to utilize the acquired data judiciously and effectively. Although the impaction characteristics of the CVI seem to be predictable by theory, the airborne instrument is subject to influences that may result in a reduced transmission efficiency for droplets, particularly if the inlet is not properly aligned. Ways to alleviate this problem are being investigated, but currently the imperfect sampling efficiency must be taken into account during data interpretation. Relationships between the physical and chemical properties of residual particles from droplets collected by the CVI and droplet size are then explored in both stratiform and cumulus clouds. The effects of various cloud processes and measurement limitations upon these relationships are discussed. In one study, chemical analysis of different -sized droplets sampled in stratiform clouds showed a dependence of chemical composition on droplet size, with larger droplets containing higher proportions of sodium than non-sea-salt sulfate and ammonium. Larger droplets were also associated with larger residual particles, as expected from simple cloud nucleation theory. In a study of marine cumulus clouds, the CVI was combined with a cloud condensation nucleus spectrometer to study the supersaturation spectra of residual particles from droplets. The median critical supersaturation of the droplet residual particles was consistently less than or equal to the median critical supersaturation of ambient particles except at cloud top, where residual particles exhibited a variety of critical supersaturations.

Cloud condensation nuclei and ice nucleation activity of hydrophobic and hydrophilic soot particles.

PubMed

Koehler, Kirsten A; DeMott, Paul J; Kreidenweis, Sonia M; Popovicheva, Olga B; Petters, Markus D; Carrico, Christian M; Kireeva, Elena D; Khokhlova, Tatiana D; Shonija, Natalia K

2009-09-28

Cloud condensation nuclei (CCN) activity and ice nucleation behavior (for temperatures

Stratospheric ion and aerosol chemistry and possible links with cirrus cloud microphysics - A critical assessment

NASA Technical Reports Server (NTRS)

Mohnen, Volker A.

1990-01-01

Aspects of stratospheric ion chemistry and physics are assessed as they relate to aerosol formation and the transport of aerosols to upper tropospheric regions to create conditions favorable for cirrus cloud formation. It is found that ion-induced nucleation and other known phase transitions involving ions and sulfuric acid vapor are probably not efficient processes for stratospheric aerosol formation, and cannot compete with condensation of sulfuric acid on preexisting particles of volcanic or meteoritic origin which are larger than about 0.15 micron in radius. Thus, galactic cosmic rays cannot have a significant impact on stratospheric aerosol population. Changes in the stratospheric aerosol burden due to volcanos are up to two orders of magnitude larger than changes in ion densities. Thus, volcanic activity may modulate the radiative properties of cirrus clouds.

Ice Cloud Formation and Dehydration in the Tropical Tropopause Layer

NASA Technical Reports Server (NTRS)

Jensen, Eric; Pfister, Leonhard; Gore, Warren J. (Technical Monitor)

2002-01-01

Stratospheric water vapor is important not only for its greenhouse forcing, but also because it plays a significant role in stratospheric chemistry. several recent studies have focused on the potential for dehydration due to ice cloud formation in air rising slowly through the tropical tropopause layer. Holton and Gettelman showed that temperature variations associated with horizontal transport of air in the tropopause layer can drive ice cloud formation and dehydration, and Gettelman et al. recently examined the cloud formation and dehydration along kinematic trajectories using simple assumptions about the cloud properties. In this study, we use a Lagrangian, one-dimensional cloud model to further investigate cloud formation and dehydration as air is transported horizontally and vertically through the tropical tropopause layer. Time-height curtains of temperature are extracted from meteorological analyses. The model tracks the growth and sedimentation of individual cloud particles. The regional distribution of clouds simulated in the model is comparable to the subvisible cirrus distribution indicated by SAGE II. The simulated cloud properties depend strongly on the assumed ice supersaturation threshold for ice nucleation. with effective nuclei present (low supersaturation threshold), ice number densities are high (0.1--10 cm(circumflex)-3), and ice crystals do not grow large enough to fall very far, resulting in limited dehydration. With higher supersaturation thresholds, ice number densities are much lower (less than 0.01 cm(circumflex)-3), and ice crystals grow large enough to fall substantially; however, supersaturated air often crosses the tropopause without cloud formation. The clouds typically do not dehydrate the air along trajectories down to the temperature minimum saturation mixing ratio. Rather the water vapor mixing ratio crossing the tropopause along trajectories is typically 10-50% larger than the saturation mixing ratio.

Simulating the Effects of Semivolatile Compounds on Cloud Processing of Aerosol

NASA Astrophysics Data System (ADS)

Kokkola, H.; Kudzotsa, I.; Tonttila, J.; Raatikainen, T.; Romakkaniemi, S.

2017-12-01

Aerosol removal processes largely dictate how well aerosol is transported in the atmosphere and thus the aerosol load over remote regions depends on how effectively aerosol is removed during its transport from the source regions. This means that in order to model the global distribution aerosol, both in vertical and horizontal, wet deposition processes have to be properly modelled. However, in large scale models, the description of wet removal and the vertical redistribution of aerosol by cloud processes is often extremely simplified.Here we present a novel aerosol-cloud model SALSA, where the aerosol properties are tracked through different cloud processes. These processes include: cloud droplet activation, precipitation formation, ice nucleation, melting, and evaporation. It is a sectional model that includes separate size sections for non-activated aerosol, cloud droplets, precipitation droplets, and ice crystals. The aerosol-cloud model was coupled to a large eddy model UCLALES which simulates the boundary-layer dynamics. In this study, the model has been applied in studying the wet removal as well as interactions between aerosol, clouds, and semi-volatile compounds, ammonia and nitric acid. These semi-volative compounds are special in the sense that they co-condense together with water during cloud activation and have been suggested to form droplets that can be considered cloud-droplet-like already in subsaturated conditions. In our model, we calculate the kinetic partitioning of ammonia and sulfate thus explicitly taking into account the effect of ammonia and nitric acid in the cloud formation. Our simulations indicate that especially in polluted conditions, these compounds significantly affect the properties of cloud droplets thus significantly affecting the lifecycle of different aerosol compounds.

The carrier gas pressure effect in a laminar flow diffusion chamber, homogeneous nucleation of n-butanol in helium.

PubMed

Hyvärinen, Antti-Pekka; Brus, David; Zdímal, Vladimír; Smolík, Jiri; Kulmala, Markku; Viisanen, Yrjö; Lihavainen, Heikki

2006-06-14

Homogeneous nucleation rate isotherms of n-butanol+helium were measured in a laminar flow diffusion chamber at total pressures ranging from 50 to 210 kPa to investigate the effect of carrier gas pressure on nucleation. Nucleation temperatures ranged from 265 to 280 K and the measured nucleation rates were between 10(2) and 10(6) cm(-3) s(-1). The measured nucleation rates decreased as a function of increasing pressure. The pressure effect was strongest at pressures below 100 kPa. This negative carrier gas effect was also temperature dependent. At nucleation temperature of 280 K and at the same saturation ratio, the maximum deviation between nucleation rates measured at 50 and 210 kPa was about three orders of magnitude. At nucleation temperature of 265 K, the effect was negligible. Qualitatively the results resemble those measured in a thermal diffusion cloud chamber. Also the slopes of the isothermal nucleation rates as a function of saturation ratio were different as a function of total pressure, 50 kPa isotherms yielded the steepest slopes, and 210 kPa isotherms the shallowest slopes. Several sources of inaccuracies were considered in the interpretation of the results: uncertainties in the transport properties, nonideal behavior of the vapor-carrier gas mixture, and shortcomings of the used mathematical model. Operation characteristics of the laminar flow diffusion chamber at both under-and over-pressure were determined to verify a correct and stable operation of the device. We conclude that a negative carrier gas pressure effect is seen in the laminar flow diffusion chamber and it cannot be totally explained with the aforementioned reasons.

Intercomparison study and optical asphericity measurements of small ice particles in the CERN CLOUD experiment

NASA Astrophysics Data System (ADS)

Nichman, Leonid; Järvinen, Emma; Dorsey, James; Connolly, Paul; Duplissy, Jonathan; Fuchs, Claudia; Ignatius, Karoliina; Sengupta, Kamalika; Stratmann, Frank; Möhler, Ottmar; Schnaiter, Martin; Gallagher, Martin

2017-09-01

Optical probes are frequently used for the detection of microphysical cloud particle properties such as liquid and ice phase, size and morphology. These properties can eventually influence the angular light scattering properties of cirrus clouds as well as the growth and accretion mechanisms of single cloud particles. In this study we compare four commonly used optical probes to examine their response to small cloud particles of different phase and asphericity. Cloud simulation experiments were conducted at the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at European Organisation for Nuclear Research (CERN). The chamber was operated in a series of multi-step adiabatic expansions to produce growth and sublimation of ice particles at super- and subsaturated ice conditions and for initial temperatures of -30, -40 and -50 °C. The experiments were performed for ice cloud formation via homogeneous ice nucleation. We report the optical observations of small ice particles in deep convection and in situ cirrus simulations. Ice crystal asphericity deduced from measurements of spatially resolved single particle light scattering patterns by the Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition) were compared with Cloud and Aerosol Spectrometer with Polarisation (CASPOL) measurements and image roundness captured by the 3View Cloud Particle Imager (3V-CPI). Averaged path light scattering properties of the simulated ice clouds were measured using the Scattering Intensity Measurements for the Optical detectioN of icE (SIMONE) and single particle scattering properties were measured by the CASPOL. We show the ambiguity of several optical measurements in ice fraction determination of homogeneously frozen ice in the case where sublimating quasi-spherical ice particles are present. Moreover, most of the instruments have difficulties of producing reliable ice fraction if small aspherical ice particles are present, and all of the instruments cannot separate perfectly spherical ice particles from supercooled droplets. Correlation analysis of bulk averaged path depolarisation measurements and single particle measurements of these clouds showed higher R2 values at high concentrations and small diameters, but these results require further confirmation. We find that none of these instruments were able to determine unambiguously the phase of the small particles. These results have implications for the interpretation of atmospheric measurements and parametrisations for modelling, particularly for low particle number concentration clouds.

Aerosol nucleation and growth in the TTL, due to tropical convection, during the ACTIVE campaign

NASA Astrophysics Data System (ADS)

Waddicor, D.; Vaughan, G.; Choularton, T.

2009-04-01

The Aerosol and Chemical Transport In tropical convection (ACTIVE) campaign took place between October 2005 and February 2006. This investigation involved the sampling of deep convective storms that occur in the Tropics; the campaign was based in Darwin, Northern Territory, Australia - the latter half of the campaign coincided with the monsoon season. A range of scientific equipment was used to sample the inflow and outflow air from these storms; of particular importance were the NERC Dornier (low-level) and ARA Egrett (high-level outflow) aircraft. The Dornier held a range of aerosol, particle and chemical detectors for the purpose of analysing the planetary boundary layer (PBL), in the vicinity of tropical convection. The Egrett contained detection instrumentation for a range of sizes of aerosol and cloud particles (2 Condensation Particle Counters (CPC), CAPS, CIP, CPI) in the storm outflow. This allowed a quantifiable measurement to be made of the effect of deep tropical convection on the aerosol population in the Tropical Tropopause Layer (TTL). The ACTIVE campaign found that there were large numbers of aerosol particles in the 10 - 100 nm (up to 25,000 /cm3 STP) and 100 - 1000 nm (up to 600 /cm3) size ranges. These values, in many instances, surpassed those found in the PBL. The higher levels of aerosol found in the TTL compared to the PBL could indicate that aerosol nucleation was occurring in the TTL as a direct result of convective activity. Furthermore, the Egrett aircraft found distinct boundaries between the high levels of aerosol, which were found in cloud free regions, and very low numbers of aerosol, which were found in the cloudy regions (storm anvil). The air masses were determined, from back trajectories, to have been through convective uplift and were formerly part of the anvil cloud. The cloudy regions would have contained high levels of entrapped precursor gases. Reduced nucleation and cloud particle scavenging of aerosol and gases would give a much reduced aerosol number concentration in cloud. The high aerosol (cloud free) areas would appear after the cloud began to evaporate through the process of aerosol nucleation. The evaporating cloud particles and reduced cloud surface area would allow aerosol nucleation to occur - typically involving sulphuric acid and water, released from ice crystals. The time scales for the particle production have also been investigated using satellite and wind projections/ECMWF back trajectories.

Observed Aerosol Influence on Ice Water Content of Arctic Mixed-Phase Clouds

NASA Astrophysics Data System (ADS)

Norgren, M.; de Boer, G.; Shupe, M.

2016-12-01

The response of ice water content (IWC) in Arctic mixed-phase stratocumulus to atmospheric aerosols is observed. IWC retrievals from ground based radars operated by the Atmospheric Radiation Measurement (ARM) program in Barrow, Alaska are used to construct composite profiles of cloud IWC from a 9-year radar record starting in January of 2000. The IWC profiles for high (polluted) and low (clean) aerosol loadings are compared. Generally, we find that clean clouds exhibit statistically significant higher levels of IWC than do polluted clouds by a factor of 2-4 at cloud base. For springtime clouds, with a maximum relative humidity with respect to ice (RHI) above 110% in the cloud layer, the IWC at cloud base was a factor of 3.25 times higher in clean clouds than it was in polluted clouds. We infer that the aerosol loading of the cloud environment alters the liquid drop size distribution within the cloud, with larger drops being more frequent in clean clouds. Larger cloud drops promote riming within the cloud layer, which is one explanation for the higher IWC levels in clean clouds. The drop size distribution may also be a significant control of ice nucleation events within mixed-phase clouds. Whether the high IWC levels in clean clouds are due to increased riming or nucleation events is unclear at this time.

Developing a new parameterization framework for the heterogeneous ice nucleation of atmospheric aerosol particles

NASA Astrophysics Data System (ADS)

Ullrich, Romy; Hiranuma, Naruki; Hoose, Corinna; Möhler, Ottmar; Niemand, Monika; Steinke, Isabelle; Wagner, Robert

2014-05-01

Developing a new parameterization framework for the heterogeneous ice nucleation of atmospheric aerosol particles Ullrich, R., Hiranuma, N., Hoose, C., Möhler, O., Niemand, M., Steinke, I., Wagner, R. Aerosols of different nature induce microphysical processes of importance for the Earth's atmosphere. They affect not only directly the radiative budget, more importantly they essentially influence the formation and life cycles of clouds. Hence, aerosols and their ice nucleating ability are a fundamental input parameter for weather and climate models. During the previous years, the AIDA (Aerosol Interactions and Dynamics in the Atmosphere) cloud chamber was used to extensively measure, under nearly realistic conditions, the ice nucleating properties of different aerosols. Numerous experiments were performed with a broad variety of aerosol types and under different freezing conditions. A reanalysis of these experiments offers the opportunity to develop a uniform parameterization framework of ice formation for many atmospherically relevant aerosols in a broad temperature and humidity range. The analysis includes both deposition nucleation and immersion freezing. The aim of this study is to develop this comprehensive parameterization for heterogeneous ice formation mainly by using the ice nucleation active site (INAS) approach. Niemand et al. (2012) already developed a temperature dependent parameterization for the INAS- density for immersion freezing on desert dust particles. In addition to a reanalysis of the ice nucleation behaviour of desert dust (Niemand et al. (2012)), volcanic ash (Steinke et al. (2010)) and organic particles (Wagner et al. (2010,2011)) this contribution will also show new results for the immersion freezing and deposition nucleation of soot aerosols. The next step will be the implementation of the parameterizations into the COSMO- ART model in order to test and demonstrate the usability of the framework. Hoose, C. and Möhler, O. (2012) Atmos. Chem. Phys. 12, 9817-9854 Niemand, M., Möhler, O., Vogel, B., Hoose, C., Connolly, P., Klein, H., Bingemer, H., DeMott, P.J., Skrotzki, J. and Leisner, T. (2012) J. Atmos. Sci. 69, 3077-3092 Steinke, I., Möhler, O., Kiselev, A., Niemand, M., Saathoff, H., Schnaiter, M., Skrotzki, J., Hoose, C. and Leisner, T. (2011) Atmos. Chem. Phys. 11, 12945-12958 Wagner, R., Möhler, O., Saathoff, H., Schnaiter, M. and Leisner, T. (2010) Atmos. Chem. Phys. 10, 7617-7641 Wagner, R., Möhler, O., Saathoff, H., Schnaiter, M. and Leisner, T. (2011) Atmos. Chem. Phys. 11, 2083-2110

Effect of particle surface area on ice active site densities retrieved from droplet freezing spectra

NASA Astrophysics Data System (ADS)

Beydoun, Hassan; Polen, Michael; Sullivan, Ryan C.

2016-10-01

Heterogeneous ice nucleation remains one of the outstanding problems in cloud physics and atmospheric science. Experimental challenges in properly simulating particle-induced freezing processes under atmospherically relevant conditions have largely contributed to the absence of a well-established parameterization of immersion freezing properties. Here, we formulate an ice active, surface-site-based stochastic model of heterogeneous freezing with the unique feature of invoking a continuum assumption on the ice nucleating activity (contact angle) of an aerosol particle's surface that requires no assumptions about the size or number of active sites. The result is a particle-specific property g that defines a distribution of local ice nucleation rates. Upon integration, this yields a full freezing probability function for an ice nucleating particle. Current cold plate droplet freezing measurements provide a valuable and inexpensive resource for studying the freezing properties of many atmospheric aerosol systems. We apply our g framework to explain the observed dependence of the freezing temperature of droplets in a cold plate on the concentration of the particle species investigated. Normalizing to the total particle mass or surface area present to derive the commonly used ice nuclei active surface (INAS) density (ns) often cannot account for the effects of particle concentration, yet concentration is typically varied to span a wider measurable freezing temperature range. A method based on determining what is denoted an ice nucleating species' specific critical surface area is presented and explains the concentration dependence as a result of increasing the variability in ice nucleating active sites between droplets. By applying this method to experimental droplet freezing data from four different systems, we demonstrate its ability to interpret immersion freezing temperature spectra of droplets containing variable particle concentrations. It is shown that general active site density functions, such as the popular ns parameterization, cannot be reliably extrapolated below this critical surface area threshold to describe freezing curves for lower particle surface area concentrations. Freezing curves obtained below this threshold translate to higher ns values, while the ns values are essentially the same from curves obtained above the critical area threshold; ns should remain the same for a system as concentration is varied. However, we can successfully predict the lower concentration freezing curves, which are more atmospherically relevant, through a process of random sampling from g distributions obtained from high particle concentration data. Our analysis is applied to cold plate freezing measurements of droplets containing variable concentrations of particles from NX illite minerals, MCC cellulose, and commercial Snomax bacterial particles. Parameterizations that can predict the temporal evolution of the frozen fraction of cloud droplets in larger atmospheric models are also derived from this new framework.

Homogeneous Freezing of Water Droplets and its Dependence on Droplet Size

NASA Astrophysics Data System (ADS)

Schmitt, Thea; Möhler, Ottmar; Höhler, Kristina; Leisner, Thomas

2014-05-01

The formulation and parameterisation of microphysical processes in tropospheric clouds, such as phase transitions, is still a challenge for weather and climate models. This includes the homogeneous freezing of supercooled water droplets, since this is an important process in deep convective systems, where almost pure water droplets may stay liquid until homogeneous freezing occurs at temperatures around 238 K. Though the homogeneous ice nucleation in supercooled water is considered to be well understood, recent laboratory experiments with typical cloud droplet sizes showed one to two orders of magnitude smaller nucleation rate coefficients than previous literature results, including earlier results from experiments with single levitated water droplets and from cloud simulation experiments at the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) facility. This motivated us to re-analyse homogeneous droplet freezing experiments conducted during the previous years at the AIDA cloud chamber. This cloud chamber has a volume of 84m3 and operates under atmospherically relevant conditions within wide ranges of temperature, pressure and humidity, whereby investigations of both tropospheric mixed-phase clouds and cirrus clouds can be realised. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. According to our new results and their comparison to the results from single levitated droplet experiments, the homogeneous freezing of water droplets seems to be a volume-dependent process, at least for droplets as small as a few micrometers in diameter. A contribution of surface induced freezing can be ruled out, in agreement to previous conclusions from the single droplet experiments. The obtained volume nucleation rate coefficients are in good agreement, within error bars, with some previous literature data, including our own results from earlier AIDA experiments, but they do not agree with recently published lower volume nucleation rate coefficients. This contribution will show the results from the re-analysis of AIDA homogeneous freezing experiments with pure water droplets and will discuss the comparison to the literature data.

Use of the Single Particle Soot Photometer (SP2) as a pre-filter for ice nucleation measurements: effect of particle mixing state and determination of SP2 conditions to fully vaporize refractory black carbon

NASA Astrophysics Data System (ADS)

Schill, Gregory P.; DeMott, Paul J.; Levin, Ezra J. T.; Kreidenweis, Sonia M.

2018-05-01

Ice nucleation is a fundamental atmospheric process that impacts precipitation, cloud lifetimes, and climate. Challenges remain to identify and quantify the compositions and sources of ice-nucleating particles (INPs). Assessment of the role of black carbon (BC) as an INP is particularly important due to its anthropogenic sources and abundance at upper-tropospheric cloud levels. The role of BC as an INP, however, is unclear. This is, in part, driven by a lack of techniques that directly determine the contribution of refractory BC (rBC) to INP concentrations. One previously developed technique to measure this contribution uses the Single Particle Soot Photometer (SP2) as a pre-filter to an online ice-nucleating particle counter. In this technique, rBC particles are selectively heated to their vaporization temperature in the SP2 cavity by a 1064 nm laser. From previous work, however, it is unclear under what SP2 conditions, if any, the original rBC particles were fully vaporized. Furthermore, previous work also left questions about the effect of the SP2 laser on the ice-nucleating properties of several INP proxies and their mixtures with rBC.To answer these questions, we sampled the exhaust of an SP2 with a Scanning Mobility Particle Sizer and a Continuous Flow Diffusion Chamber. Using Aquadag® as an rBC proxy, the effect of several SP2 instrument parameters on the size distribution and physical properties of particles in rBC SP2 exhaust were explored. We found that a high SP2 laser power (930 nW/(220 nm PSL)) is required to fully vaporize a ˜ 0.76 fg rBC particle. We also found that the exhaust particle size distribution is minimally affected by the SP2 sheath-to-sample ratio; the size of the original rBC particle, however, greatly influences the size distribution of the SP2 exhaust. The effect of the SP2 laser on the ice nucleation efficiency of Snomax®, NX-illite, and Suwannee River Fulvic Acid was studied; these particles acted as proxies for biological, illite-rich mineral dust, and brown carbon INPs, respectively. The original size distribution and ice nucleation efficiency of all non-rBC proxies were unaffected by the SP2 laser. Furthermore, the ice nucleation efficiencies of all proxies were not affected when externally mixed with rBC. These proxies, however, always show a reduction in ice-nucleating ability when internally mixed with rBC. We end this work with recommendations for users who wish to use the SP2 as a pre-filter to remove large rBC particles from an aerosol stream.

Understanding cirrus ice crystal number variability for different heterogeneous ice nucleation spectra

DOE PAGES

Sullivan, Sylvia C.; Morales Betancourt, Ricardo; Barahona, Donifan; ...

2016-03-03

Along with minimizing parameter uncertainty, understanding the cause of temporal and spatial variability of the nucleated ice crystal number, N i, is key to improving the representation of cirrus clouds in climate models. To this end, sensitivities of N i to input variables like aerosol number and diameter provide valuable information about nucleation regime and efficiency for a given model formulation. Here we use the adjoint model of the adjoint of a cirrus formation parameterization (Barahona and Nenes, 2009b) to understand N i variability for various ice-nucleating particle (INP) spectra. Inputs are generated with the Community Atmosphere Model version 5, andmore » simulations are done with a theoretically derived spectrum, an empirical lab-based spectrum and two field-based empirical spectra that differ in the nucleation threshold for black carbon particles and in the active site density for dust. The magnitude and sign of N i sensitivity to insoluble aerosol number can be directly linked to nucleation regime and efficiency of various INP. The lab-based spectrum calculates much higher INP efficiencies than field-based ones, which reveals a disparity in aerosol surface properties. In conclusion, N i sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters; this low temperature sensitivity regime has been experimentally reported before but never deconstructed as done here.« less

Aerosol-radiation-cloud interactions in the South-East Atlantic: first results from the ORACLES-2016 deployment and plans for future activities

NASA Astrophysics Data System (ADS)

Redemann, J.; Wood, R.; Zuidema, P.; Haywood, J. M.; Piketh, S.; Formenti, P.; Abel, S.

2016-12-01

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for regional and global climate change predictions. Our understanding of aerosol-cloud interactions in the SE Atlantic is severely limited. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology. We describe first results from various synergistic, international research activities aimed at studying aerosol-cloud interactions in the region: NASA's airborne ORACLES (ObseRvations of Aerosols Above Clouds and Their IntEractionS) deployment in August/September of 2016, the DoE's LASIC (Layered Atlantic Smoke Interactions with Clouds) deployment of the ARM Mobile Facility to Ascension Island (June 2016 - October 2017), the ground-based components of CNRS' AEROCLO-sA (Aerosols Clouds and Fog over the west coast of southern Africa), and ongoing regional-scale integrative, process-oriented science efforts as part of SEALS-sA (Sea Earth Atmosphere Linkages Study in southern Africa). We expect to describe experimental setups as well as showcase initial aerosol and cloud property distributions. Furthermore, we discuss the implementation of future activities in these programs in coordination with the UK Met Office's CLARIFY (CLoud-Aerosol-Radiation Interactions and Forcing) experiment in 2017.

The Modification of Orographic Snow Growth Processes by Cloud Nucleating Aerosols

NASA Astrophysics Data System (ADS)

Cotton, W. R.; Saleeby, S.

2011-12-01

Cloud nucleating aerosols have been found to modify the amount and spatial distribution of snowfall in mountainous areas where riming growth of snow crystals is known to contribute substantially to the total snow water equivalent precipitation. In the Park Range of Colorado, a 2km deep supercooled liquid water orographic cloud frequently enshrouds the mountaintop during snowfall events. This leads to a seeder-feeder growth regime in which snow falls through the orographic cloud and collects cloud water prior to surface deposition. The addition of higher concentrations of cloud condensation nuclei (CCN) modifies the cloud droplet spectrum toward smaller size droplets and suppresses riming growth. Without rime growth, the density of snow crystals remains low and horizontal trajectories carry them further downwind due to slower vertical fall speeds. This leads to a downwind shift in snowfall accumulation at high CCN concentrations. Cloud resolving model simulations were performed (at 600m horizontal grid spacing) for six snowfall events over the Park Range. The chosen events were well simulated and occurred during intensive observations periods as part of two winter field campaigns in 2007 and 2010 based at Storm Peak Laboratory in Steamboat Springs, CO. For each event, sensitivity simulations were run with various initial CCN concentration vertical profiles that represent clean to polluted aerosol environments. Microphysical budget analyses were performed for these simulations in order to determine the relative importance of the various cloud properties and growth processes that contribute to precipitation production. Observations and modeling results indicate that initial vapor depositional growth of snow tends to be maximized within about 1km of mountaintop above the windward slope while the majority of riming growth occurs within 500m of mountaintop. This suggests that precipitation production is predominantly driven by locally enhanced orography. The large scale synoptic flow simply provides the background dynamics and moisture that impinge upon the steep terrain. The addition of cloud nucleating aerosols to this scenario tends to reduce the amount of riming and leads to greater snow vapor growth. Increased vapor growth leads to larger snow crystals but does not necessarily increase their density or fall speed. There is frequently a zone on the periphery of the orographic cloud where water saturation is low and ice saturation remains high. Here the Bergeron process allows for snow to continue growing at the expense of the cloud water. Furthermore, since less cloud water is removed by riming, and droplets are smaller in polluted conditions, there is an increase in cloud water evaporation along the lee slope. This enhanced droplet evaporation in polluted conditions allows for more saturated air to persist to the lee of the ridge. Higher saturation reduces the amount of snow crystal sublimation prior to surface deposition. In very moist winter events, the lee slope evaporation relative to the primary mountain barrier can saturate the air relative to a downstream ridge and aid in further orographic cloud development. The combination of reduced riming, the Bergeron process, and reduced lee-side sublimation leads to the snowfall spillover effect under polluted conditions.

Prognostic parameterization of cloud ice with a single category in the aerosol-climate model ECHAM(v6.3.0)-HAM(v2.3)

NASA Astrophysics Data System (ADS)

Dietlicher, Remo; Neubauer, David; Lohmann, Ulrike

2018-04-01

A new scheme for stratiform cloud microphysics has been implemented in the ECHAM6-HAM2 general circulation model. It features a widely used description of cloud water with two categories for cloud droplets and raindrops. The unique aspect of the new scheme is the break with the traditional approach to describe cloud ice analogously. Here we parameterize cloud ice by a single category that predicts bulk particle properties (P3). This method has already been applied in a regional model and most recently also in the Community Atmosphere Model 5 (CAM5). A single cloud ice category does not rely on heuristic conversion rates from one category to another. Therefore, it is conceptually easier and closer to first principles. This work shows that a single category is a viable approach to describe cloud ice in climate models. Prognostic representation of sedimentation is achieved by a nested approach for sub-stepping the cloud microphysics scheme. This yields good results in terms of accuracy and performance as compared to simulations with high temporal resolution. Furthermore, the new scheme allows for a competition between various cloud processes and is thus able to unbiasedly represent the ice formation pathway from nucleation to growth by vapor deposition and collisions to sedimentation. Specific aspects of the P3 method are evaluated. We could not produce a purely stratiform cloud where rime growth dominates growth by vapor deposition and conclude that the lack of appropriate conditions renders the prognostic parameters associated with the rime properties unnecessary. Limitations inherent in a single category are examined.

Sea spray as a source of ice nucleating particles - results from the AIDA Ocean03 campaign

NASA Astrophysics Data System (ADS)

Salter, M. E.; Ickes, L.; Adams, M.; Bierbauer, S.; Bilde, M.; Christiansen, S.; Ekman, A.; Gorokhova, E.; Höhler, K.; Kiselev, A. A.; Leck, C.; Mohr, C.; Mohler, O.; Murray, B. J.; Porter, G.; Ullrich, R.; Wagner, R.

2017-12-01

Clouds and their radiative effects are one of the major influences on the radiative fluxes in the atmosphere, but at the same time they remain the largest uncertainty in climate models. This lack of understanding is especially pronounced in the high Arctic. Summertime clouds can persist over long periods in this region, which is difficult to replicate in models based on our current understanding. The clouds most often encountered in the summertime high Arctic consist of a mixture of ice crystals and super-cooled water droplets, so-called mixed-phase clouds. This cloud type is sensitive to the availability of aerosol particles, which can act as cloud condensation nuclei and ice nuclei. However, since the high Arctic is a pristine region, aerosol particles are not very abundant, and the hypothesis of open leads in the Arctic as a potentially important source of cloud and ice nucleating particles via bubble bursting has emerged. In this context, we have conducted a series of experiments at the AIDA chamber at KIT, designed to investigate the mechanisms linking marine biology, seawater chemistry and aerosol physics/potential cloud impacts. During this campaign, two marine diatom species (Melosira arctica and Skeletonema marinoi) as well as sea surface microlayer samples collected during several Arctic Ocean research cruises were investigated. To aerosolize the samples, a variety of methods were used including a sea spray simulation chamber to mimic the process of bubble-bursting. The ice nucleating efficiency (mixed-phase cloud regime) of the samples was determined either directly in the AIDA chamber during adiabatic expansions, or using the INKA continuous flow diffusion chamber, or a cold stage. Results from the campaign along with the potential implications are presented.

Oxidative Processing Lowers the Ice Nucleation Activity of Birch and Alder Pollen

NASA Astrophysics Data System (ADS)

Gute, Ellen; Abbatt, Jonathan P. D.

2018-02-01

Pollen carry water extractable compounds with ice nucleating (IN) activity. This study investigates whether the hydroxyl radical, as the major atmospheric oxidant, can affect the IN activity of silver birch and grey alder subpollen particles under in-cloud conditions for deposition freezing mode conditions at 234 K. It is found that oxidation increases the supersaturation ratio with respect to ice necessary for the onset of ice nucleation and decreases the fraction of particles which initiate ice nucleation. This reduction of IN activity under equivalent oxidation conditions does not occur with a mineral dust sample (Arizona Test Dust). Chemical analysis of fresh and oxidized pollen material indicates a change of molecular structure with a loss of conjugation and an increase in oxidized functional groups, such as carbonyls. This is the first demonstration that in-cloud oxidation may lower the IN abilities of biological particles such as pollen.

Global atmospheric particle formation from CERN CLOUD measurements.

PubMed

Dunne, Eimear M; Gordon, Hamish; Kürten, Andreas; Almeida, João; Duplissy, Jonathan; Williamson, Christina; Ortega, Ismael K; Pringle, Kirsty J; Adamov, Alexey; Baltensperger, Urs; Barmet, Peter; Benduhn, Francois; Bianchi, Federico; Breitenlechner, Martin; Clarke, Antony; Curtius, Joachim; Dommen, Josef; Donahue, Neil M; Ehrhart, Sebastian; Flagan, Richard C; Franchin, Alessandro; Guida, Roberto; Hakala, Jani; Hansel, Armin; Heinritzi, Martin; Jokinen, Tuija; Kangasluoma, Juha; Kirkby, Jasper; Kulmala, Markku; Kupc, Agnieszka; Lawler, Michael J; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mann, Graham; Mathot, Serge; Merikanto, Joonas; Miettinen, Pasi; Nenes, Athanasios; Onnela, Antti; Rap, Alexandru; Reddington, Carly L S; Riccobono, Francesco; Richards, Nigel A D; Rissanen, Matti P; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Sengupta, Kamalika; Simon, Mario; Sipilä, Mikko; Smith, James N; Stozkhov, Yuri; Tomé, Antonio; Tröstl, Jasmin; Wagner, Paul E; Wimmer, Daniela; Winkler, Paul M; Worsnop, Douglas R; Carslaw, Kenneth S

2016-12-02

Fundamental questions remain about the origin of newly formed atmospheric aerosol particles because data from laboratory measurements have been insufficient to build global models. In contrast, gas-phase chemistry models have been based on laboratory kinetics measurements for decades. We built a global model of aerosol formation by using extensive laboratory measurements of rates of nucleation involving sulfuric acid, ammonia, ions, and organic compounds conducted in the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber. The simulations and a comparison with atmospheric observations show that nearly all nucleation throughout the present-day atmosphere involves ammonia or biogenic organic compounds, in addition to sulfuric acid. A considerable fraction of nucleation involves ions, but the relatively weak dependence on ion concentrations indicates that for the processes studied, variations in cosmic ray intensity do not appreciably affect climate through nucleation in the present-day atmosphere. Copyright © 2016, American Association for the Advancement of Science.

Modeling the clouds on Venus: model development and improvement of a nucleation parameterization

NASA Astrophysics Data System (ADS)

Määttänen, Anni; Bekki, Slimane; Vehkamäki, Hanna; Julin, Jan; Montmessin, Franck; Ortega, Ismael K.; Lebonnois, Sébastien

2014-05-01

As both the clouds of Venus and aerosols in the Earth's stratosphere are composed of sulfuric acid droplets, we use the 1-D version of a model [1,4] developed for stratospheric aerosols and clouds to study the clouds on Venus. We have removed processes and compounds related to the stratospheric clouds so that the only species remaining are water and sulfuric acid, corresponding to the stratospheric sulfate aerosols, and we have added some key processes. The model describes microphysical processes including condensation/evaporation, and sedimentation. Coagulation, turbulent diffusion, and a parameterization for two-component nucleation [8] of water and sulfuric acid have been added in the model. Since the model describes explicitly the size distribution with a large number of size bins (50-500), it can handle multiple particle modes. The validity ranges of the existing nucleation parameterization [7] have been improved to cover a larger temperature range, and the very low relative humidity (RH) and high sulfuric acid concentrations found in the atmosphere of Venus. We have made several modifications to improve the 2002 nucleation parameterization [7], most notably ensuring that the two-component nucleation model behaves as predicted by the analytical studies at the one-component limit reached at extremely low RH. We have also chosen to use a self-consistent cluster distribution [9], constrained by scaling it to recent quantum chemistry calculations [3]. First tests of the cloud model have been carried out with temperature profiles from VIRA [2] and from the LMD Venus GCM [5], and with a compilation of water vapor and sulfuric acid profiles, as in [6]. The temperature and pressure profiles do not evolve with time, but the vapour profiles naturally change with the cloud. However, no chemistry is included for the moment, so the vapor concentrations are only dependent on the microphysical processes. The model has been run for several hundreds of Earth days to reach a steady state. Preliminary results are evaluated against observations. [1] Jumelet et al., JGR, 2009. [2] Kliore et al., 1986. [3] Kurtén et al., BER, 2007 [4] Larsen et al., JGR, 2000. [5] Lebonnois et al. JGR, 2010. [6] McGouldrick and Toon, Icarus 191, 2007. [7] Vehkamäki et al. JGR, 2002 [9] Wilemski and Wyslouzil, J.Chem.Phys. 1995.

Potential origin of organic CNN observed at a marine site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andrews, E.; Kreidenweis, S.M.; Penner, J.E.

1995-12-31

Observations by Novakov and Penner (1993) suggest that organic aerosol particles may make up a significant portion of cloud condensation nuclei (CCN) comparable, perhaps, to the sulfate aerosol contribution to CCN. Because organic CCN would influence the albedo and radiative properties of clouds and play a role in climate change, it is important to identify the sources of these aerosols. In their research Novakov and Penner assumed that particles larger than 0.05 {mu}m could act as CCN. Therefore the origins of nucleation mode aerosol (0.03 < dp < 0.1 {mu}m) are the focus of our research. In our research, wemore » apply a dynamic aerosol model (MAEROS) to explore potential sources of the nucleation mode organic aerosol observed at a marine site in Puerto Rico. Novakov and Penner measured the size segregated mass and composition of the atmospheric aerosol at this site and found that organic aerosol mass dominated the sulfate mass in the nucleation size range. The presence of organics in this size range suggests that these organic aerosol particles were generated by nucleation of a gas phase organic followed by condensational processes, i.e., identifying sources of the gas phase precursors is important to determining the organic CCN origins. Back trajectory analysis shows that the air mass was without continental contact for 12 days prior to being sampled. This implicates two possible sources for the gas phase organic: biogenic emissions from the Puerto Rican forest and emissions from the ocean surface. In this research we explore both the forest and ocean source scenarios, showing that the forest is more likely to be the ultimate source of the observed organic aerosol particles. Using MAEROS (modified to include nucleation) and reasonable input parameters taken from the literature we were able to show that an organic vapor flux very similar to the measured biogenic fluxes reported by Zimmerman et al. generated size distributions similar to the observed aerosol.« less

Natural aerosols explain seasonal and spatial patterns of Southern Ocean cloud albedo

PubMed Central

McCoy, Daniel T.; Burrows, Susannah M.; Wood, Robert; Grosvenor, Daniel P.; Elliott, Scott M.; Ma, Po-Lun; Rasch, Phillip J.; Hartmann, Dennis L.

2015-01-01

Atmospheric aerosols, suspended solid and liquid particles, act as nucleation sites for cloud drop formation, affecting clouds and cloud properties—ultimately influencing the cloud dynamics, lifetime, water path, and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations affect not only cloud properties themselves but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. It is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd is spatially correlated with regions of high chlorophyll a, and the spatiotemporal variability in Nd is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35o to 45oS) and by organic matter in sea spray aerosol at higher latitudes (45o to 55oS). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m–2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere. PMID:26601216

Surface Crystallization of Cloud Droplets: Implications for Climate Change and Ozone Depletion

NASA Technical Reports Server (NTRS)

Tabazadeh, A.; Djikaev, Y. S.; Reiss, H.; Gore, Warren J. (Technical Monitor)

2002-01-01

The process of supercooled liquid water crystallization into ice is still not well understood. Current experimental data on homogeneous freezing rates of ice nucleation in supercooled water droplets show considerable scatter. For example, at -33 C, the reported freezing nucleation rates vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Until now, experimental data on the freezing of supercooled water has been analyzed under the assumption that nucleation of ice took place in the interior volume of a water droplet. Here, the same data is reanalyzed assuming that the nucleation occurred "pseudoheterogeneously" at the air (or oil)-liquid water interface of the droplet. Our analysis suggest that the scatter in the nucleation data can be explained by two main factors. First, the current assumption that nucleation occurs solely inside the volume of a water droplet is incorrect. Second, because the nucleation process most likely occurs on the surface, the rates of nuclei formation could differ vastly when oil or air interfaces are involved. Our results suggest that ice freezing in clouds may initiate on droplet surfaces and such a process can allow for low amounts of liquid water (approx. 0.002 g per cubic meters) to remain supercooled down to -40 C as observed in the atmosphere.

Heterogeneous nucleation of nitric acid trihydrate on clay minerals: relevance to type ia polar stratospheric clouds.

PubMed

Hatch, Courtney D; Gough, Raina V; Toon, Owen B; Tolbert, Margaret A

2008-01-17

Although critical to atmospheric modeling of stratospheric ozone depletion, selective heterogeneous nuclei that promote the formation of Type Ia polar stratospheric clouds (PSCs) are largely unknown. While mineral particles are known to be good ice nuclei, it is currently not clear whether they are also good nuclei for PSCs. In the present study, a high-vacuum chamber equipped with transmission Fourier transform infrared spectroscopy and a quadrupole mass spectrometer was used to study heterogeneous nucleation of nitric acid trihydrate (NAT) on two clay minerals-Na-montmorillonite and kaolinite-as analogs of atmospheric terrestrial and extraterrestrial minerals. The minerals are first coated with a 3:1 supercooled H2O/HNO3 solution prior to the observed nucleation of crystalline NAT. At 220 K, NAT formation was observed at low SNAT values of 12 and 7 on kaolinite and montmorillonite clays, respectively. These are the lowest SNAT values reported in the literature on any substrate. However, NAT nucleation exhibited significant temperature dependence. At lower temperatures, representative of typical polar stratospheric conditions, much higher supersaturations were required before nucleation was observed. Our results suggest that NAT nucleation on mineral particles, not previously treated with sulfuric acid, may not be an important nucleation platform for Type Ia PSCs under normal polar stratospheric conditions.

A Model Simulation of Pinatubo Volcanic Aerosols in the Stratosphere

NASA Technical Reports Server (NTRS)

Zhao , Jing-xia; Turco, Richard P.; Toon, Owen B.

1995-01-01

A one-dimensional, time-dependent model is used to study the chemical, microphysical, and radiative properties of volcanic aerosols produced by the Mount Pinatubo eruption on June 15, 1991. Our model treats gas-phase sulfur photochemistry, gas-to-particle conversion of sulfur, and the microphysics of sulfate aerosols and ash particles under stratospheric conditions. The dilution and diffusion of the volcanic eruption clouds are also accounted for in these conditions. Heteromolecular homogeneous and heterogeneous binary H2SO4/H2O nucleation, acid and water condensational growth, coagulation, and gravitational sedimentation are treated in detail in the model. Simulations suggested that after several weeks, the volcanic cloud was composed mainly of sulfuric acid/water droplets produced in situ from the SO2 emissions. The large amounts of SO2 (around 20 Mt) injected into the stratosphere by the Pinatubo eruption initiated homogeneous nucleation which generated a high concentration of small H2SO4/H2O droplets. These newly formed particles grew rapidly by condensation and coagulation in the first few months and then reach their stabilized sizes with effective radii in a range between 0.3 and 0.5 micron approximately one-half year after the eruption. The predicted volcanic cloud parameters reasonably agree with measurements in term of the vertical distribution and lifetime of the volcanic aerosols, their basic microphysical structures (e.g., size distribution, concentration, mass ratio, and surface area) and radiative properties. The persistent volcanic aerosols can produce significant anomalies in the radiation field, which have important climatic consequences. The large enhancement in aerosol surface area can result in measurable global stratospheric ozone depletion.

On the usage of classical nucleation theory in quantification of the impact of bacterial INP on weather and climate

NASA Astrophysics Data System (ADS)

Sahyoun, Maher; Wex, Heike; Gosewinkel, Ulrich; Šantl-Temkiv, Tina; Nielsen, Niels W.; Finster, Kai; Sørensen, Jens H.; Stratmann, Frank; Korsholm, Ulrik S.

2016-08-01

Bacterial ice-nucleating particles (INP) are present in the atmosphere and efficient in heterogeneous ice-nucleation at temperatures up to -2 °C in mixed-phase clouds. However, due to their low emission rates, their climatic impact was considered insignificant in previous modeling studies. In view of uncertainties about the actual atmospheric emission rates and concentrations of bacterial INP, it is important to re-investigate the threshold fraction of cloud droplets containing bacterial INP for a pronounced effect on ice-nucleation, by using a suitable parameterization that describes the ice-nucleation process by bacterial INP properly. Therefore, we compared two heterogeneous ice-nucleation rate parameterizations, denoted CH08 and HOO10 herein, both of which are based on classical-nucleation-theory and measurements, and use similar equations, but different parameters, to an empirical parameterization, denoted HAR13 herein, which considers implicitly the number of bacterial INP. All parameterizations were used to calculate the ice-nucleation probability offline. HAR13 and HOO10 were implemented and tested in a one-dimensional version of a weather-forecast-model in two meteorological cases. Ice-nucleation-probabilities based on HAR13 and CH08 were similar, in spite of their different derivation, and were higher than those based on HOO10. This study shows the importance of the method of parameterization and of the input variable, number of bacterial INP, for accurately assessing their role in meteorological and climatic processes.

Saharan dust, convective lofting, aerosol enhancement zones, and potential impacts on ice nucleation in the tropical upper troposphere

NASA Astrophysics Data System (ADS)

Twohy, C. H.; Anderson, B. E.; Ferrare, R. A.; Sauter, K. E.; L'Ecuyer, T. S.; van den Heever, S. C.; Heymsfield, A. J.; Ismail, S.; Diskin, G. S.

2017-08-01

Dry aerosol size distributions and scattering coefficients were measured on 10 flights in 32 clear-air regions adjacent to tropical storm anvils over the eastern Atlantic Ocean. Aerosol properties in these regions were compared with those from background air in the upper troposphere at least 40 km from clouds. Median values for aerosol scattering coefficient and particle number concentration >0.3 μm diameter were higher at the anvil edges than in background air, showing that convective clouds loft particles from the lower troposphere to the upper troposphere. These differences are statistically significant. The aerosol enhancement zones extended 10-15 km horizontally and 0.25 km vertically below anvil cloud edges but were not due to hygroscopic growth since particles were measured under dry conditions. Number concentrations of particles >0.3 μm diameter were enhanced more for the cases where Saharan dust layers were identified below the clouds with airborne lidar. Median number concentrations in this size range increased from 100 l-1 in background air to 400 l-1 adjacent to cloud edges with dust below, with larger enhancements for stronger storm systems. Integration with satellite cloud frequency data indicates that this transfer of large particles from low to high altitudes by convection has little impact on dust concentrations within the Saharan Air Layer itself. However, it can lead to substantial enhancement in large dust particles and, therefore, heterogeneous ice nuclei in the upper troposphere over the Atlantic. This may induce a cloud/aerosol feedback effect that could impact cloud properties in the region and downwind.

Measurements of ice nucleating particle concentrations at 242 K in the free troposphere

NASA Astrophysics Data System (ADS)

Lacher, L.; Lohmann, U.; Boose, Y.; Zipori, A.; Herrmann, E.; Bukowiecki, N.; Steinbacher, M.; Gute, E.; Kanji, Z. A.

2017-12-01

Clouds containing ice play an important role in the Earth's system, but some fundamental knowledge on their formation and further development is still missing. The phase change from vapor or liquid to ice in the atmosphere can occur heterogeneously in the presence of ice nucleating particles (INPs) at temperatures warmer, and supersaturations lower than required for homogeneous freezing. Only a small fraction of particles in an environment relevant for the occurrence of ice- and mixed-phase clouds are INPs, and their identification and quantification remains challenging. We measure INP concentrations with the ETH Horizontal Ice Nucleation Chamber (HINC) at the High Altitude Research Station Jungfraujoch (JFJ) during several field campaigns in different seasons and years. The measurements are performed at 242 K and above water saturation, representing ice- and mixed-phase clouds conditions. Due to its elevation of 3580 m a.s.l. the site encounters mostly free tropospheric conditions, and is influenced by boundary layer injections up to 80% of the time in summer. JFJ regularly encounters Saharan dust events and receives air masses of marine origin, which can both occur within the free troposphere. Our measurements show that INP concentrations in the free troposphere do not follow a seasonal cycle. They are remarkably constant, with concentrations from 0.5 - 8 L-1 (interquartile range), which compares well to measurements performed under the same conditions at another location within the free troposphere, the Izaña Atmospheric Research Station in Tenerife. At JFJ, correlations with parameters of physical properties of ambient particles, meteorology and air mass characteristics do not show a single best estimator to predict INP concentrations, emphasizing the complexity of ice nucleation in the free troposphere. Increases in INP concentrations of a temporary nature were observed in the free troposphere during Saharan dust events and marine air mass influence, which indicate the potential role of mineral dust and marine aerosol to the INP population. However, average free tropospheric INP concentrations are not sensitive to these transient high numbers suggesting their overall contribution may be minor for seasonal or annual trends.

Ion-induced nucleation of pure biogenic particles.

PubMed

Kirkby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika; Frege, Carla; Gordon, Hamish; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K; Wagner, Robert; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill; Dias, Antonio; Ehrhart, Sebastian; Flagan, Richard C; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P; Pringle, Kirsty; Rap, Alexandru; Richards, Nigel A D; Riipinen, Ilona; Rissanen, Matti P; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E; Seinfeld, John H; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander L; Wagner, Andrea C; Wagner, Paul E; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M; Worsnop, Douglas R; Baltensperger, Urs; Kulmala, Markku; Carslaw, Kenneth S; Curtius, Joachim

2016-05-26

Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.

Development of Two-Moment Cloud Microphysics for Liquid and Ice Within the NASA Goddard Earth Observing System Model (GEOS-5)

NASA Technical Reports Server (NTRS)

Barahona, Donifan; Molod, Andrea M.; Bacmeister, Julio; Nenes, Athanasios; Gettelman, Andrew; Morrison, Hugh; Phillips, Vaughan,; Eichmann, Andrew F.

2013-01-01

This work presents the development of a two-moment cloud microphysics scheme within the version 5 of the NASA Goddard Earth Observing System (GEOS-5). The scheme includes the implementation of a comprehensive stratiform microphysics module, a new cloud coverage scheme that allows ice supersaturation and a new microphysics module embedded within the moist convection parameterization of GEOS-5. Comprehensive physically-based descriptions of ice nucleation, including homogeneous and heterogeneous freezing, and liquid droplet activation are implemented to describe the formation of cloud particles in stratiform clouds and convective cumulus. The effect of preexisting ice crystals on the formation of cirrus clouds is also accounted for. A new parameterization of the subgrid scale vertical velocity distribution accounting for turbulence and gravity wave motion is developed. The implementation of the new microphysics significantly improves the representation of liquid water and ice in GEOS-5. Evaluation of the model shows agreement of the simulated droplet and ice crystal effective and volumetric radius with satellite retrievals and in situ observations. The simulated global distribution of supersaturation is also in agreement with observations. It was found that when using the new microphysics the fraction of condensate that remains as liquid follows a sigmoidal increase with temperature which differs from the linear increase assumed in most models and is in better agreement with available observations. The performance of the new microphysics in reproducing the observed total cloud fraction, longwave and shortwave cloud forcing, and total precipitation is similar to the operational version of GEOS-5 and in agreement with satellite retrievals. However the new microphysics tends to underestimate the coverage of persistent low level stratocumulus. Sensitivity studies showed that the simulated cloud properties are robust to moderate variation in cloud microphysical parameters. However significant sensitivity in ice cloud properties was found to variation in the dispersion of the ice crystal size distribution and the critical size for ice autoconversion. The implementation of the new microphysics leads to a more realistic representation of cloud processes in GEOS-5 and allows the linkage of cloud properties to aerosol emissions.

Ship trail/cloud dynamic effects from Apollo-Soyuz photograph July 16, 1975

DOE Office of Scientific and Technical Information (OSTI.GOV)

Porch, W.M.; Kao, Chih-yue J.; Kyle, T.G.

1988-01-01

We describe in this paper the results of a preliminary analysis of a ship trail photograph taken by the Apollo-Soyuz crew at 22:21 GMT on 16 July 1975. The photograph was taken from an altitude of 174 km and shows three separate ship trails with two of the trails intersecting. Because these photographs were taken from a non-geosynchronous satellite with a high-resolution camera, the quality of the photograph provides more detail than is usually obtained from meteorological satellites (minimum spatial resolution 14 m compared to 57 m from Landsat). The photograph not only shows enhanced detail of the ship trailsmore » themselves, but also cloud free bands generated by the ship trails. The ship trails have maximum photographed widths of 3--6 km. These cloud free bands are an obvious indication of the importance of ship trail cloud dynamics to ship trial development. These cloud dynamical effects are driven both by the initial energy release of the ship's power plant and by latent heat release from the aerosol nucleation process. Since the aerosol nucleation process is the key to understanding ocean aerosol/cloud interactions, it is important to partition these two processes in the ship trial development. We will describe in this paper preliminary numerical modeling efforts to simulate the ship trails using only the energy release from the ship and thereby give an indication of how much more energy input may be required from the nucleation process. 12 refs., 6 figs.« less

Role of stacking disorder in ice nucleation

NASA Astrophysics Data System (ADS)

Lupi, Laura; Hudait, Arpa; Peters, Baron; Grünwald, Michael; Gotchy Mullen, Ryan; Nguyen, Andrew H.; Molinero, Valeria

2017-11-01

The freezing of water affects the processes that determine Earth’s climate. Therefore, accurate weather and climate forecasts hinge on good predictions of ice nucleation rates. Such rate predictions are based on extrapolations using classical nucleation theory, which assumes that the structure of nanometre-sized ice crystallites corresponds to that of hexagonal ice, the thermodynamically stable form of bulk ice. However, simulations with various water models find that ice nucleated and grown under atmospheric temperatures is at all sizes stacking-disordered, consisting of random sequences of cubic and hexagonal ice layers. This implies that stacking-disordered ice crystallites either are more stable than hexagonal ice crystallites or form because of non-equilibrium dynamical effects. Both scenarios challenge central tenets of classical nucleation theory. Here we use rare-event sampling and free energy calculations with the mW water model to show that the entropy of mixing cubic and hexagonal layers makes stacking-disordered ice the stable phase for crystallites up to a size of at least 100,000 molecules. We find that stacking-disordered critical crystallites at 230 kelvin are about 14 kilojoules per mole of crystallite more stable than hexagonal crystallites, making their ice nucleation rates more than three orders of magnitude higher than predicted by classical nucleation theory. This effect on nucleation rates is temperature dependent, being the most pronounced at the warmest conditions, and should affect the modelling of cloud formation and ice particle numbers, which are very sensitive to the temperature dependence of ice nucleation rates. We conclude that classical nucleation theory needs to be corrected to include the dependence of the crystallization driving force on the size of the ice crystallite when interpreting and extrapolating ice nucleation rates from experimental laboratory conditions to the temperatures that occur in clouds.

Role of stacking disorder in ice nucleation.

PubMed

Lupi, Laura; Hudait, Arpa; Peters, Baron; Grünwald, Michael; Gotchy Mullen, Ryan; Nguyen, Andrew H; Molinero, Valeria

2017-11-08

The freezing of water affects the processes that determine Earth's climate. Therefore, accurate weather and climate forecasts hinge on good predictions of ice nucleation rates. Such rate predictions are based on extrapolations using classical nucleation theory, which assumes that the structure of nanometre-sized ice crystallites corresponds to that of hexagonal ice, the thermodynamically stable form of bulk ice. However, simulations with various water models find that ice nucleated and grown under atmospheric temperatures is at all sizes stacking-disordered, consisting of random sequences of cubic and hexagonal ice layers. This implies that stacking-disordered ice crystallites either are more stable than hexagonal ice crystallites or form because of non-equilibrium dynamical effects. Both scenarios challenge central tenets of classical nucleation theory. Here we use rare-event sampling and free energy calculations with the mW water model to show that the entropy of mixing cubic and hexagonal layers makes stacking-disordered ice the stable phase for crystallites up to a size of at least 100,000 molecules. We find that stacking-disordered critical crystallites at 230 kelvin are about 14 kilojoules per mole of crystallite more stable than hexagonal crystallites, making their ice nucleation rates more than three orders of magnitude higher than predicted by classical nucleation theory. This effect on nucleation rates is temperature dependent, being the most pronounced at the warmest conditions, and should affect the modelling of cloud formation and ice particle numbers, which are very sensitive to the temperature dependence of ice nucleation rates. We conclude that classical nucleation theory needs to be corrected to include the dependence of the crystallization driving force on the size of the ice crystallite when interpreting and extrapolating ice nucleation rates from experimental laboratory conditions to the temperatures that occur in clouds.

Comparisons of cirrus cloud microphysical properties between polluted and pristine air

NASA Astrophysics Data System (ADS)

Diao, Minghui; Schumann, Ulrich; Minikin, Andreas; Jensen, Jorgen

2015-04-01

Cirrus clouds occur in the upper troposphere at altitudes where atmospheric radiative forcing is most sensitive to perturbations of water vapor concentration and water phase. The formation of cirrus clouds influences the distributions of water in both vapor and ice forms. The radiative properties of cirrus depend strongly on particle sizes. Currently it is still unclear how the formation of cirrus clouds and their microphysical properties are influenced by anthropogenic emissions (e.g., industrial emission and biomass burning). If anthropogenic emissions influence cirrus formation in a significant manner, then one should expect a systematic difference in cirrus properties between pristine (clean) air and polluted air. Because of the pollution contrasts between the Southern (SH) and Northern Hemispheres (NH), cirrus properties could have hemispheric differences as well. Therefore, we study high-resolution (~200 m), in-situ observations from two global flight campaigns: 1) the HIAPER Pole-to-Pole Observations (HIPPO) global campaign in 2009-2011 funded by the US National Science Foundation (NSF), and 2) the Interhemispheric Differences In Cirrus Properties from Anthropogenic Emissions (INCA) campaign in 2000 funded by the European Union and participating research institutions. To investigate the changes of cirrus clouds by anthropogenic emissions, we compare ice crystal distributions in polluted and pristine air, in terms of their frequency occurrence, number concentration (Nc) and mean diameter (i.e., effective-mean Deff and volume-mean Dc). Total aerosol concentration is used to represent the combined influence of natural and anthropogenic aerosols. In addition, measured carbon monoxide (CO) mixing ratio is used to discriminate between polluted and pristine air masses. All analyses are restricted to temperatures ≤ -40°C to exclude mixed-phased clouds. The HIPPO campaign observations were obtained over the North America continent and the central Pacific Ocean from 87°N to 67°S. Ice crystals are measured by a Fast-2DC probe, and the analyses are restricted to particles ≥ 87.5 µm to minimize the shattering effects and optical uncertainties. When analyzing ice crystals distribution in the HIPPO campaign, the occurrence frequency of in-cloud conditions increases with both total aerosol and CO concentrations. On the other hand, the changes of ice crystal sizes are not the same for increases of total aerosol and CO concentrations, that is, Dc increases with higher total aerosol concentration but decreases with higher CO concentration. These results suggest that ice crystal formation is likely facilitated when the air parcel is under influence of both natural and anthropogenic emissions, but the anthropogenic emission is likely to decrease the sizes of ice crystals. During the INCA campaign, cirrus clouds were sampled with optical particle counters in the size range of about 1 to 800 μm at midlatitudes, mainly over the Pacific west of Punta Arenas and over the North Atlantic west of Great Britain. Simultaneous measurements of trace gases (CO, NOx and O3) and a suite of aerosols properties show that the INCA measurements in the SH occurred in air masses which were far cleaner than those measured in the NH. Previous INCA data analysis revealed differences between SH and NH cirrus: a lower Nc, a larger Deff, and a larger extinction in the cirrus in the SH compared to the NH (Gayet et al., JGR, 2004). We now recompiled the INCA data and performed a further analysis of the cirrus properties in correlation with simultaneous CO measurements. Based on in-situ sampling of ice crystals of different lower cut-off sizes ( ≥1, 3 and 6 µm) from the INCA campaign, Nc is found to have weak positive correlation with CO concentration (r2 within a range of 0.2 to 0.6). The correlation appears to be significant (95% level) based on a limited set of tests with different data subsets. The correlation is strongest for the smallest ice particles. The correlation persists when restricting the data to temperatures below -45°C. The data also reveal higher ice supersaturation in air masses with low CO concentration. The correlations suggest stronger ice nucleation in polluted air masses. Still, further measurements are desirably to exclude possible artifacts and to confirm these results. Possibly due to the larger cutoff size (≥ 87.5 µm), such correlations between Nc and CO are not captured in the HIPPO data. But the increasing Nc observed from INCA campaign is consistent with the decreasing Dc from the HIPPO campaign, since Nc and Dc are generally anti-correlated during ice crystal formation. The influence of dynamical conditions (e.g. nearby convection) and aerosol contents on the observed cirrus cloud perturbations has still to be investigated. The comparison between data from SH and NH or from different pollution regions may be affected by sampling biases over different cirrus evolution phases. Diao et al. (GRL, 2013) suggested a method to identify the occurrence frequencies of five different phases of ice crystal evolution: (1) Clear-sky ice supersaturated region, (2) Nucleation, (3) Early growth of ice crystals, (4) Late growth of ice crystals, (5) Sedimentation/sublimation. "Nucleation" events in this analysis are partially cloudy segments in ice supersaturated air masses. The HIPPO and INCA data show different frequencies for these evolution phases. The full analysis of the data is still ongoing, but the INCA FSSP data (> 1 µm) seem to show more "clear-sky ice supersaturated region" and "nucleation" events to occur in the SH than in the NH.

Factors Influencing Aerosol Concentrations and Properties over the Tropical Eastern Pacific: Observations from TC4

NASA Astrophysics Data System (ADS)

Anderson, B. E.; Chen, G.; Thornhill, K. L.; Winstead, E. L.; Dibb, J.; Scheuer, E.; Lathem, T.

2007-12-01

The NASA Tropical Composition Cloud and Climate Coupling (TC4) mission was conducted during summer 2007 and had the primary objective of gaining a better understanding of composition and dynamics of the upper troposphere over the tropical eastern pacific region. Based in San Jose, Costa Rica, the mission employed instrumented aircraft along with ground, balloon, and satellite borne sensors to determine the spatial distribution of trace gas and aerosol species as well as moisture and clouds between the surface and roughly 16 km altitude over Central America, the eastern Pacific, the western Caribbean and northern South America. Because of its heavy payload and long endurance capability, the NASA DC-8 aircraft was the primary sampling platform for the lower-tropospheric altitude regime (i.e., below 12 km). It carried both remote and in situ instruments and was used to characterize cloud inflow and outflow as well as the microphysical properties of maritime convective systems. Because of their roles in regulating atmospheric radiation transfer and cloud formation and microphysics, flight plans placed particular emphasis on determining the sources and properties of the aerosol particles present within the region. A preliminary analysis of the DC-8 data set suggests that the following sources/processes had the greatest impact on aerosol number and mass loading: dust transport from Africa; sea salt production over the ocean; urban and biogenic emissions over the continent; secondary aerosol formation in volcanic plumes; nucleation in cloud outflow; and cloud scavenging. In this presentation, we will examine the microphysical, optical and hydration properties of each aerosol type and assess the overall impact of the source/sink processes to the regional aerosol budget. We will also contrast the microphysical properties of the Saharan Dust sampled over the Caribbean with those measured in fresh dust layers over the eastern Atlantic from the DC-8 during the summer 2006, NASA African Monsoon Multidisciplinary Activity (NAMMA).

Ice Nucleation of Soot Particles in the Cirrus Regime: Is Pore Condensation and Freezing Relevant for Soot?

NASA Astrophysics Data System (ADS)

Kanji, Z. A.; Mahrt, F.; David, R.; Marcolli, C.; Lohmann, U.; Fahrni, J.; Brühwiler, D.

2017-12-01

Heterogeneous ice nucleation (HIN) onto soot particles from previous studies have produced inconsistent results of temperature and relative humidity conditions required for freezing depending on the source of soot particle investigated. The ability of soot to act as HIN depended on the type of soot and size of particle. Often homogenous freezing conditions or water saturation conditions were required to freeze soot particles, rendering HIN irrelevant. Using synthesised mesoporous silica particles, we show pore condensation and freezing works with experiments performed in the Zurich Ice Nucleation Chamber (ZINC). By testing a variety of soot particles in parallel in the Horizontal Ice Nucleation Chamber (HINC), we suggest that previously observed HIN on soot particles is not the responsible mechanism for ice formation. Laboratory generated CAST brown and black soot, commercially available soot and acid treated soot were investigated for their ice nucleation abilities in the mixed-phase and cirrus cloud temperature regimes. No heterogeneous ice nucleation activity is inferred at T > -38 °C (mixed-phase cloud regime), however depending on particle size and soot type, HIN was observed for T < -38 °C (cirrus could regime). Nevertheless, we question if this is caused by a heterogeneous phase change due the presence of a so called active site or due to pore-condensation of water as predicted by the inverse Kelvin effect followed by homogeneous nucleation of ice in the pores or cavities that are ubiquitous in soot particles between the primary spherules. The ability of some particles to freeze at lower relative humidity compared to others demonstrates why hydrophobicity plays a role in ice nucleation, i.e. controlling the conditions at which these cavities fill with water. Thus for more hydrophobic particles pore filling occurs at higher relative humidity, and therefore freezing of pore water and ice crystal growth. Future work focusses on testing the cloud processing ability of soot particles and water adsorption isotherms of the different soot samples to support the hydrophobicity inferences from the ice nucleation results.

Importance of including ammonium sulfate ((NH4)2SO4) aerosols for ice cloud parameterization in GCMs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bhattacharjee, P. S.; Sud, Yogesh C.; Liu, Xiaohong

2010-02-22

A common deficiency of many cloud-physics parameterizations including the NASA’s microphysics of clouds with aerosol- cloud interactions (hereafter called McRAS-AC) is that they simulate less (larger) than the observed ice cloud particle number (size). A single column model (SCM) of McRAS-AC and Global Circulation Model (GCM) physics together with an adiabatic parcel model (APM) for ice-cloud nucleation (IN) of aerosols were used to systematically examine the influence of ammonium sulfate ((NH4)2SO4) aerosols, not included in the present formulations of McRAS-AC. Specifically, the influence of (NH4)2SO4 aerosols on the optical properties of both liquid and ice clouds were analyzed. First anmore » (NH4)2SO4 parameterization was included in the APM to assess its effect vis-à-vis that of the other aerosols. Subsequently, several evaluation tests were conducted over the ARM-SGP and thirteen other locations (sorted into pristine and polluted conditions) distributed over marine and continental sites with the SCM. The statistics of the simulated cloud climatology were evaluated against the available ground and satellite data. The results showed that inclusion of (NH4)2SO4 in the SCM made a remarkable improvement in the simulated effective radius of ice clouds. However, the corresponding ice-cloud optical thickness increased more than is observed. This can be caused by lack of cloud advection and evaporation. We argue that this deficiency can be mitigated by adjusting the other tunable parameters of McRAS-AC such as precipitation efficiency. Inclusion of ice cloud particle splintering introduced through well- established empirical equations is found to further improve the results. Preliminary tests show that these changes make a substantial improvement in simulating the cloud optical properties in the GCM, particularly by simulating a far more realistic cloud distribution over the ITCZ.« less

Observed aerosol effects on marine cloud nucleation and supersaturation

NASA Astrophysics Data System (ADS)

Russell, Lynn M.; Sorooshian, Armin; Seinfeld, John H.; Albrecht, Bruce A.; Nenes, Athanasios; Leaitch, W. Richard; Macdonald, Anne Marie; Ahlm, Lars; Chen, Yi-Chun; Coggon, Matthew; Corrigan, Ashley; Craven, Jill S.; Flagan, Richard C.; Frossard, Amanda A.; Hawkins, Lelia N.; Jonsson, Haflidi; Jung, Eunsil; Lin, Jack J.; Metcalf, Andrew R.; Modini, Robin; Mülmenstädt, Johannes; Roberts, Greg C.; Shingler, Taylor; Song, Siwon; Wang, Zhen; Wonaschütz, Anna

2013-05-01

Aerosol particles in the marine boundary layer include primary organic and salt particles from sea spray and combustion-derived particles from ships and coastal cities. These particle types serve as nuclei for marine cloud droplet activation, although the particles that activate depend on the particle size and composition as well as the supersaturation that results from cloud updraft velocities. The Eastern Pacific Emitted Aerosol Cloud Experiment (EPEACE) 2011 was a targeted aircraft campaign to assess how different particle types nucleate cloud droplets. As part of E-PEACE 2011, we studied the role of marine particles as cloud droplet nuclei and used emitted particle sources to separate particle-induced feedbacks from dynamical variability. The emitted particle sources included shipboard smoke-generated particles with 0.05-1 μm diameters (which produced tracks measured by satellite and had drop composition characteristic of organic smoke) and combustion particles from container ships with 0.05-0.2 μm diameters (which were measured in a variety of conditions with droplets containing both organic and sulfate components) [1]. Three central aspects of the collaborative E-PEACE results are: (1) the size and chemical composition of the emitted smoke particles compared to ship-track-forming cargo ship emissions as well as background marine particles, with particular attention to the role of organic particles, (2) the characteristics of cloud track formation for smoke and cargo ships, as well as the role of multi-layered low clouds, and (3) the implications of these findings for quantifying aerosol indirect effects. For comparison with the E-PEACE results, the preliminary results of the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) 2012 provided evidence of the cloud-nucleating roles of both marine organic particles and coastal urban pollution, with simultaneous measurements of the effective supersaturations of the clouds in the California coastal region.

Microbial production of ice crystals in clouds as a novel atmospheric biosignature

NASA Astrophysics Data System (ADS)

Santl-Temkiv, T.; Sahyoun, M.; Kjeldsen, H.; Ling, M.; Boesen, T.; Karlson, U. G.; Finster, K.

2014-03-01

A diverse assembly of exoplanets has been discovered during recent decades (Howard 2013), their atmospheres providing some of the most accessible evidence for the presence of biological activity on these planets. Metabolic gases have been commonly proposed as atmospheric biosignatures (Seager et al 2012). However, airborne microbes are also involved in cloud- and precipitation formation on Earth. Thus, meteorological phenomena may serve as alternative atmospheric biosignatures, for which appropriate observational techniques have yet to be developed. The atmospheric part of the Earth's water cycle heavily relies on the presence of nucleating particles, which promote the condensation and freezing of atmospheric water, both potentially leading to precipitation. While cloud condensation nuclei are diverse and relatively common, ice nuclei are poorly understood and comparably rare airborne particles. According to current knowledge, most ice nucleation below ñ15∞C is driven by the presence of inorganic dust particles, which are considered inactive at higher temperatures. Biogenic IN are the only reported particles that promote ice formation above ñ10∞C. Some bacteria, e.g. Pseudomonas syringae, produce Ice Nucleation Active (INA) proteins that are most efficient ice nuclei currently known. These INA bacteria are common in the atmosphere, and may thus be involved in precipitation processes of mixed phase clouds (Möhler et al 2007). We investigate the relevance of bacterial INA proteins for atmospheric processes using three approaches: (i) study of the presence of INA bacteria and their INA proteins in the atmosphere, (ii) a detailed molecular and physical study of isolated INA proteins, and finally (iii) a modeling study of the importance of INA proteins for ice-path in clouds as well as their importance for precipitation. During 14 precipitation events, we observed that 12% of isolated bacteria carried INA genes. INA bacteria had likely been emitted to the atmosphere from terrestrial surfaces, e.g. by convective transport. Additionally, we found INA biological fragments <220 nm in two precipitation samples (199, 482 INA per L), which indicates that in addition to intact cells, bacterial fragments that are more abundant than cells could also impact atmospheric processes. In order to study isolated INA proteins, we sequenced the INA gene from one of the isolated bacteria, Pseudomonas sp. R10.79. The INA gene will be expressed, purified and introduced into nano-discs. These INA nano-discs will facilitate a detailed molecular and physical study of INA proteins and its ice active properties. Most of modeling approaches rely on parameterizations based on classical nucleation theory, e.g. CH08 (Chen et al 2008), when introducing INA bacteria into climate models. Instead, we used an experimentally derived parameterization HAR13 (Hartmann et al 2013), when introducing bacteria into a 1-d operational weather forecast model HIRLAM (Unden et al 2002). By comparison HAR13 yields more ice and is more sensitive to the change of bacterial densities than CH08. While CH08 is a function of the size of the ice nuclei, HAR13 is a function of the number of INA protein complexes. INA protein complexes are the locations where the nucleation occurs and their number appears to be a more important parameter than cell size. We suggest that the study of individual INA proteins complexes both alone and on cell surfaces will lead to a better understanding of ice nucleation by INA bacteria.

Immersion Freezing of Aluminas: The Effect of Crystallographic Properties on Ice Nucleation

NASA Astrophysics Data System (ADS)

King, M.; Chong, E.; Freedman, M. A.

2017-12-01

Atmospheric aerosol particles serve as the nuclei for heterogeneous ice nucleation, a process that allows for ice to form at higher temperatures and lower supersaturations with respect to ice. This process is essential to the formation of ice in cirrus clouds. Heterogeneous ice nucleation is affected by many factors including the composition, crystal structure, porosity, and surface area of the particles. However, these factors are not well understood and, as such, are difficult to account for in climate models. To test the effects of crystal structure on ice nucleation, a system of transition aluminas (Al2O3) that differ only in their crystal structure, despite being compositionally similar, were tested using immersion freezing. Particles were immersed in water and placed into a temperature controlled chamber. Freezing events were then recorded as the chamber was cooled to negative 30 °. Alpha-alumina, which is a member of the hexagonal crystal system, showed a significantly higher temperature at which all particles froze in comparison to other samples. This supports the hypothesis that, since a hexagonal crystal structure is the lowest energy state for ice, hexagonal surface structures would best facilitate ice nucleation. However, a similar sample of hexagonal chi-alumina did not show the same results. Further analysis of the samples will be done to characterize surface structures and composition. These conflicting data sets raise interesting questions about the effect of other surface features, such as surface area and porosity, on ice nucleation.

Investigations on the physical and optical properties of cirrus clouds and their relationship with ice nuclei concentration using LIDAR at Gadanki, India (13.5°N, 79.2°E)

NASA Astrophysics Data System (ADS)

Krishnakumar, Vasudevannair; Satyanarayana, Malladi; Radhakrishnan, Soman R.; Dhaman, Reji K.; Pillai, Vellara P. Mahadevan; Raghunath, Karnam; Ratnam, Madineni Venkat; Rao, Duggirala Ramakrishna; Sudhakar, Pindlodi

2011-01-01

Cirrus cloud measurements over the tropics are receiving much attention recently due to their role in the Earth's radiation budget. The interaction of water vapor and aerosols plays a major role in phase formation of cirrus clouds. Many factors control the ice supersaturation and microphysical properties in cirrus clouds and, as such, investigations on these properties of cirrus clouds are critical for proper understanding and simulating the climate. In this paper we report on the evolution, microphysical, and optical properties of cirrus clouds using the Mie LIDAR operation at the National Atmospheric Research Laboratory, Gadanki, India (13.5°N, 79.2°E), an inland tropical station. The occurrence statistics, height, optical depth, depolarization ratio of the cirrus clouds, and their relationship with ice nuclei concentration were investigated over 29 days of observation during the year 2002. Cirrus clouds with a base altitude as low as 8.4 km are observed during the month of January and clouds with a maximum top height of 17.1 km are observed during the month of May. The cirrus has a mean thickness of 2 km during the period of study. The LIDAR ratio varies from 30 to 36 sr during the summer days of observation and 25 to 31 sr during the winter days of observation. Depolarization values range from 0.1 to 0.58 during the period of observation. The ice nuclei concentration has been calculated using the De Motts equation. It is observed that during the monsoon months of June, July, and August, there appears to be an increase in the ice nuclei number concentration. From the depolarization data an attempt is made to derive the ice crystal orientation and their structure of the cirrus. Crystal structures such as thin plates, thick plates, regular hexagons, and hexagonal columns are observed in the study. From the observed crystal structure and ice nuclei concentration, the possible nucleation mechanism is suggested.

Cirrus Parcel Model Comparison Project. Phase 1

NASA Technical Reports Server (NTRS)

Lin, Ruei-Fong; Starr, David O'C.; DeMott, Paul J.; Cotton, Richard; Jensen, Eric; Sassen, Kenneth

2000-01-01

The Cirrus Parcel Model Comparison (CPMC) is a project of the GEWEX Cloud System Study Working Group on Cirrus Cloud Systems (GCSS WG2). The primary goal of this project is to identify cirrus model sensitivities to the state of our knowledge of nucleation and microphysics. Furthermore, the common ground of the findings may provide guidelines for models with simpler cirrus microphysics modules. We focus on the nucleation regimes of the warm (parcel starting at -40 C and 340 hPa) and cold (-60 C and 170 hPa) cases studied in the GCSS WG2 Idealized Cirrus Model Comparison Project. Nucleation and ice crystal growth were forced through an externally imposed rate of lift and consequent adiabatic cooling. The background haze particles are assumed to be lognormally-distributed H2SO4 particles. Only the homogeneous nucleation mode is allowed to form ice crystals in the HN-ONLY runs; all nucleation modes are switched on in the ALL-MODE runs. Participants were asked to run the HN-lambda-fixed runs by setting lambda = 2 (lambda is further discussed in section 2) or tailoring the nucleation rate calculation in agreement with lambda = 2 (exp 1). The depth of parcel lift (800 m) was set to assure that parcels underwent complete transition through the nucleation regime to a stage of approximate equilibrium between ice mass growth and vapor supplied by the specified updrafts.

Response of Cloud Condensation Nuclei (> 50 nm) to changes in ion-nucleation

NASA Astrophysics Data System (ADS)

Pedersen, J. O.; Enghoff, M. B.; Svensmark, H.

2012-12-01

The role of ionization in the formation of clouds and aerosols has been debated for many years. A body of evidence exists that correlates cloud properties to galactic cosmic ray ionization; however these results are still contested. In recent years experimental evidence has also been produced showing that ionization can promote the nucleation of small aerosols at atmospheric conditions. The experiments showed that an increase in ionization leads to an increase in the formation of ultrafine aerosols (~3 nm), but in the real atmosphere such small particles have to grow by coagulation and condensation to become cloud condensation nuclei (CCN) in order to have an effect on clouds. However, numerical studies predict that variations in the count of ultra-fine aerosols will lead only to an insignificant change in the count of CCN. This is due to 1) the competition between the additional ultra-fine aerosols for the limited supply of condensable gases leading to a slower growth and 2) the increased loss rates of the additional particles during the longer growth-time. We investigated the growth of aerosols to CCN sizes using an 8 m3 reaction chamber made from electro-polished stainless steel. One side was fitted with a Teflon foil to allow ultraviolet light to illuminate the chamber, which was continuously flushed with dry purified air. Variable concentrations of water vapor, ozone, and sulfur dioxide could be added to the chamber. UV-lamps initiated photochemistry producing sulfuric acid. Ionization could be enhanced with two Cs-137 gamma sources (30 MBq), mounted on each side of the chamber. Figure 1 shows the evolution of the aerosols, following a nucleation event induced by the gamma sources. Previous to the event the aerosols were in steady state. Each curve represents a size bin: 3-10 nm (dark purple), 10-20 nm (purple), 20-30 nm (blue), 30-40 nm (light blue), 40-50 nm (green), 50-60 nm (yellow), and 60-68 nm (red). Black curves show a ~1 hour smoothing. The initial increase in small aerosols persists all the way to the largest size bin. Similar experiments where the aerosol burst was produced with either the ionization source or an aerosol generator (neutralized aerosols) were made and compared with each other and model runs. The runs using neutral aerosol bursts agree with the model predictions, where the initial burst is dampened such that there is little or no change in the largest sizes. Thus there seems to be a fundamental difference between the bursts produced by ionization and those produced by the aerosol generator. Growth of aerosols, nucleated by ionization.

Measurements of Ice Nuclei properties at the Jungfraujoch using the Portable Ice Nucleation Chamber (PINC)

NASA Astrophysics Data System (ADS)

Chou, Cédric

2010-05-01

Ice clouds and mixed-phase clouds have different microphysical properties. Both affect the climate in various ways. Ice phase present in these clouds have the ability to scatter the incoming solar radiation and absorb terrestrial radiation differently from water droplets. Ice is also responsible for most of the precipitation in the mid-latitudes. Ice crystals can be formed via two main processes: homogeneous and heterogeneous ice nucleation. Investigation of thermodynamic conditions at which ice nuclei (IN) trigger nucleation and their number concentrations is necessary in order to understand the formation of the ice phase in the atmosphere. In order to investigate the presence of IN in the free troposphere, the Institute for Atmospheric and Climate Sciences of the ETH Zurich has recently designed a new chamber: the Portable Ice Nucleation Chamber (PINC), which is the field version of the Zurich Ice Nucleation Chamber (Stetzer et al., 2008). Both chambers follow the principle of a "continuous flow diffusion chamber" (Rogers, 1988) and can measure the number concentration of IN at different temperatures and relative humidities. Aerosols are collected through an inlet where an impactor removes larger particles that could be counted as ice crystals. The aerosol load is layered between two dry sheath air flows as it enters the main chamber. Both walls of the chamber are covered with a thin layer of ice and maintained at two different temperatures in order to create supersaturation with respect to ice (and with respect to water in case of a larger temperature difference between the walls). At the exit of the main chamber, the sample goes throught the evaporation part that is kept saturated with respect to ice. There, water droplets evaporate and only ice crystals and smaller aerosol particles are counted by the Optical Particle Counter (OPC) at the bottom of the chamber. The high alpine research station Jungfraujoch is located at 3580 m a.s.l. It is mainly in undisturbed free troposphere, but is also influenced by the Planetary Boundary Layer (PBL) especially in summer. The probability of Saharan Dust Events (SDE) at the Jungfraujoch is usually high from March to July (Collaud Coen et al., 2004). Two campaigns have been performed during this period in order to investigate the influence of a SDE on the IN number concentration and properties: PINC II took place from February 23rd to March 16th, 2009 and PINC III from June 3rd to 17th, 2009. The operating conditions inside the chamber during both campaigns were -31°C with relative humidities with respect to ice and water of 127% and 91%, respectively. During the first campaign, no SDE were detected and the average number concentration of IN was <10 particles/liter. Two SDE of different intensity occurred during the second campaign on June 15th and 16th where significantly higher IN number concentrations have been observed. We found that the larger the particles are, the more efficient they are as IN especially during SDE. References: Collaud Coen M., Weingartner E., Schaub D., Hueglin C., Corrigan C., Henning S., Schwikowski M., and Baltensperger U. (2004). Saharan dust events at the Jungfraujoch: detection by wavelength dependence of the single scattering albedo and first climatology analysis. Atmos. Chem. Phys., 4, 2465-2480, 2004 Rogers, D. C. (1988), Development of a Continuous Flow Thermal Gradient Diffusion Chamber for Ice Nucleation Studies, Atmos. Res. 22:149-181. Stetzer, O., Baschek, B., Lueoend, F., Lohmann, U. (2008), The Zurich Ice Nucleation Chamber (ZINC)-A New Instrument to Investigate Atmospheric Ice Formation, Aerosol Science and Technology, 42:64-74, 2008

Aerosol-cloud interactions in Arctic mixed-phase stratocumulus

NASA Astrophysics Data System (ADS)

Solomon, A.

2017-12-01

Reliable climate projections require realistic simulations of Arctic cloud feedbacks. Of particular importance is accurately simulating Arctic mixed-phase stratocumuli (AMPS), which are ubiquitous and play an important role in regional climate due to their impact on the surface energy budget and atmospheric boundary layer structure through cloud-driven turbulence, radiative forcing, and precipitation. AMPS are challenging to model due to uncertainties in ice microphysical processes that determine phase partitioning between ice and radiatively important cloud liquid water. Since temperatures in AMPS are too warm for homogenous ice nucleation, ice must form through heterogeneous nucleation. In this presentation we discuss a relatively unexplored source of ice production-recycling of ice nuclei in regions of ice subsaturation. AMPS frequently have ice-subsaturated air near the cloud-driven mixed-layer base where falling ice crystals can sublimate, leaving behind IN. This study provides an idealized framework to understand feedbacks between dynamics and microphysics that maintain phase-partitioning in AMPS. In addition, the results of this study provide insight into the mechanisms and feedbacks that may maintain cloud ice in AMPS even when entrainment of IN at the mixed-layer boundaries is weak.

Ice nucleation efficiency of AgI: review and new insights

NASA Astrophysics Data System (ADS)

Marcolli, Claudia; Nagare, Baban; Welti, André; Lohmann, Ulrike

2016-07-01

AgI is one of the best-investigated ice-nucleating substances. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Theoretical and experimental studies over the last 60 years provide a complex picture of silver iodide as an ice-nucleating agent with conflicting and inconsistent results. This review compares experimental ice nucleation studies in order to analyze the factors that influence the ice nucleation ability of AgI. The following picture emerges from this analysis: the ice nucleation ability of AgI seems to be enhanced when the AgI particle is on the surface of a droplet, which is indeed the position that a particle takes when it can freely move in a droplet. The ice nucleation by particles with surfaces exposed to air depends on water adsorption. AgI surfaces seem to be most efficient at nucleating ice when they are exposed to relative humidity at or even above water saturation. For AgI particles that are completely immersed in water, the freezing temperature increases with increasing AgI surface area. Higher threshold freezing temperatures seem to correlate with improved lattice matches as can be seen for AgI-AgCl solid solutions and 3AgI·NH4I·6H2O, which have slightly better lattice matches with ice than AgI and also higher threshold freezing temperatures. However, the effect of a good lattice match is annihilated when the surfaces have charges. Also, the ice nucleation ability seems to decrease during dissolution of AgI particles. This introduces an additional history and time dependence for ice nucleation in cloud chambers with short residence times.

Condensed-phase biogenic-anthropogenic interactions with implications for cold cloud formation

DOE PAGES

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew; ...

2017-01-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil-fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated by a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibitmore » a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid inducing ice nucleation. Naphthalene SOA coated soot particles acted as IN above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate further renders this even less likely. Furthermore, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during preindustrial times or in pristine areas.« less

Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation

DOE PAGES

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew T.; ...

2017-01-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA–soot biogenic–anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfatemore » mixtures exhibit a core–shell configuration (i.e.a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respectiveT gand FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.« less

Condensed-phase biogenic-anthropogenic interactions with implications for cold cloud formation.

PubMed

Charnawskas, Joseph C; Alpert, Peter A; Lambe, Andrew T; Berkemeier, Thomas; O'Brien, Rachel E; Massoli, Paola; Onasch, Timothy B; Shiraiwa, Manabu; Moffet, Ryan C; Gilles, Mary K; Davidovits, Paul; Worsnop, Douglas R; Knopf, Daniel A

2017-08-24

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles' organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g ) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.

In situ cloud and aerosol measurements over Coastal Antarctica during intensive field campaigns in 2010, 2011 and 2015

NASA Astrophysics Data System (ADS)

O'Shea, Sebastian; Choularton, Tom; Flynn, Michael; Bower, Keith; Gallagher, Martin; Fleming, Zoe; Listowski, Constantino; Kirchgaessner, Amelie; Ladkin, Russell; Lachlan-Cope, Tom; Crosier, Jonathan

2017-04-01

Few direct measurements have been made of Antarctic aerosol and cloud properties. As a result, a number of studies have suggested they are poorly represented within weather/climate models. This has important consequences for predictions of the mass balance of the Antarctic ice sheet and both weather patterns in the region and worldwide. In situ measurements of cloud and aerosol properties were collected over the Antarctic Peninsula, coastal continent and Weddell Sea during intensive observation periods in 2010, 2011 and 2015. Airborne measurements were collected using British Antarctic Survey's instrumented Twin Otter research aircraft for all 3 campaigns and additional ground based measurements were made at Halley's Clean Air Sector Laboratory in 2015. This presentation will focus on the aerosol measurements from these intensive observation periods. The aerosol in the region was found to have strong vertical gradients and to be hygroscopic in nature. The hygroscopicity parameter, κ had a mean value during the 2015 campaign of 0.69, which is consistent with other remote marine locations that are dominated by sea spray emissions. Aerosol properties will be investigated in terms of their air mass history. The relative contribution of emissions from the Antarctic Continent, sea ice and Sea/Ocean regions will be examined. The ice nucleating properties of the aerosol will also be discussed.

Characterization of Arctic ice cloud properties observed during ISDAC

NASA Astrophysics Data System (ADS)

Jouan, Caroline; Girard, Eric; Pelon, Jacques; Gultepe, Ismail; Delanoë, Julien; Blanchet, Jean-Pierre

2012-12-01

Extensive measurements from ground-based sites and satellite remote sensing (CloudSat and CALIPSO) reveal the existence of two types of ice clouds (TICs) in the Arctic during the polar night and early spring. The first type (TIC-2A), being topped by a cover of nonprecipitating very small (radar unseen) ice crystals (TIC-1), is found more frequently in pristine environment, whereas the second type (TIC-2B), detected by both sensors, is associated preferentially with a high concentration of aerosols. To further investigate the microphysical properties of TIC-1/2A and TIC-2B, airborne in situ and satellite measurements of specific cases observed during Indirect and Semi-Direct Aerosol Campaign (ISDAC) have been analyzed. For the first time, Arctic TIC-1/2A and TIC-2B microstructures are compared using in situ cloud observations. Results show that the differences between them are confined in the upper part of the clouds where ice nucleation occurs. TIC-2B clouds are characterized by fewer (by more than 1 order of magnitude) and larger (by a factor of 2 to 3) ice crystals and a larger ice supersaturation (of 15-20%) compared to TIC-1/2A. Ice crystal growth in TIC-2B clouds seems explosive, whereas it seems more gradual in TIC-1/2A. It is hypothesized that these differences are linked to the number concentration and the chemical composition of aerosols. The ice crystal growth rate in very cold conditions impinges on the precipitation efficiency, dehydration and radiation balance. These results represent an essential and important first step to relate previous modeling, remote sensing and laboratory studies with TICs cloud in situ observations.

Modeling the Hydrological Cycle in the Atmosphere of Mars: Influence of a Bimodal Size Distribution of Aerosol Nucleation Particles

NASA Astrophysics Data System (ADS)

Shaposhnikov, Dmitry S.; Rodin, Alexander V.; Medvedev, Alexander S.; Fedorova, Anna A.; Kuroda, Takeshi; Hartogh, Paul

2018-02-01

We present a new implementation of the hydrological cycle scheme into a general circulation model of the Martian atmosphere. The model includes a semi-Lagrangian transport scheme for water vapor and ice and accounts for microphysics of phase transitions between them. The hydrological scheme includes processes of saturation, nucleation, particle growth, sublimation, and sedimentation under the assumption of a variable size distribution. The scheme has been implemented into the Max Planck Institute Martian general circulation model and tested assuming monomodal and bimodal lognormal distributions of ice condensation nuclei. We present a comparison of the simulated annual variations, horizontal and vertical distributions of water vapor, and ice clouds with the available observations from instruments on board Mars orbiters. The accounting for bimodality of aerosol particle distribution improves the simulations of the annual hydrological cycle, including predicted ice clouds mass, opacity, number density, and particle radii. The increased number density and lower nucleation rates bring the simulated cloud opacities closer to observations. Simulations show a weak effect of the excess of small aerosol particles on the simulated water vapor distributions.

A Laboratory Study on the Phase Transition for Polar Stratospheric Cloud Particles

NASA Technical Reports Server (NTRS)

Teets, Edward H., Jr.

1997-01-01

The nucleation and growth of different phases of simulated polar stratospheric cloud (PSC) particles were investigated in the laboratory. Solutions and mixtures of solutions at concentrations 1 to 5 m (molality) of ammonium sulfate, ammonium bisulfate, sodium chloride, sulfuric acid, and nitric acid were supercooled to prescribed temperatures below their equilibrium melting point. These solutions were contained in small diameter glass tubing of volumes ranging from 2.6 to 0.04 ml. Samples were nucleated by insertion of an ice crystal, or in some cases by a liquid nitrogen cooled wire. Crystallization velocities were determined by timing the crystal growth front passages along the glass tubing. Solution mixtures containing aircraft exhaust (soot) were also examined. Crystallization rates increased as deltaT2, where deltaT is the supercooling for weak solutions (2 m or less). The higher concentrated solutions (greater than 3 m) showed rates significantly less than deltaT2. This reduced rate suggested an onset of a glass phase. Results were applied to the nucleation of highly concentrated solutions at various stages of polar stratospheric cloud development within the polar stratosphere.

Laboratory measurements of immersion freezing abilities of non-proteinaceous and proteinaceous biological particulate proxies

NASA Astrophysics Data System (ADS)

Cory, K.; Tobo, Y.; Murata, K.; Whiteside, C. L.; McCauley, B.; Bouma, C.; Hiranuma, N.

2017-12-01

Non-proteinaceous and proteinaceous biological aerosols are abundant within the atmosphere and have the potential to impact the climate through cloud and precipitation formation. In this study, we present the differences in the laboratory-measured freezing capabilities of the non-proteinaceous and proteinaceous biological materials to determine which has more potential to impact the ice nucleation in the clouds. As non-proteinaceous surrogates, we examined multiple cellulose materials (e.g., microcrystalline and nanocrystalline cellulose) whose sizes range from 100 nm to >100 μm (according to manufacturer report). For proteinaceous proxies, we looked at different gram-negative bacteria, such as Pseudamonas aeruginosa, Escherichia coli, Serratia marcescens, Citrobacter freundii, and Snomax, (which contains P. syringae) that can be found around the proximity of the Texas Panhandle. By using the Cryogenic Refrigeration Applied Freezing Test (CRAFT) system, we estimated immersion freezing efficiency (i.e., ice nucleation activity scaled to a unit of mass) of each sample at the temperatures greater than -30°C. We have observed that not all gram-negative bacteria has high immersion freezing activity, but the few do have a warmer temperature onset (>-20 °C) than the cellulose used. For those that did not exhibit substantial freezing efficiencies, they had similar freezing properties as the broth, in which the bacteria were incubated, as well as the cellulose materials examined. These observations suggest the presence and potential importance of bacterial cellulose in the atmospheric ice nucleation. From here, we need to conduct more in-depth investigation in the effects of a wider variety of atmospherically relevant biological aerosols to get a better understanding of the effects of said aerosols on overall aerosol-cloud interactions. Acknowledgments: K. Cory would like to acknowledge NSF-EAPSI and JSPS Summer Program for the travel fellowship support. N. Hiranuma acknowledges financial aids by the Higher Education Assistance Fund (HEAF), WTAMU Office of Graduate School and Killgore Research Center.

Promotion of Homogeneous Ice Nucleation by Soluble Molecules.

PubMed

Mochizuki, Kenji; Qiu, Yuqing; Molinero, Valeria

2017-11-29

Atmospheric aerosols nucleate ice in clouds, strongly impacting precipitation and climate. The prevailing consensus is that ice nucleation is promoted heterogeneously by the surface of ice nucleating particles in the aerosols. However, recent experiments indicate that water-soluble molecules, such as polysaccharides of pollen and poly(vinyl alcohol) (PVA), increase the ice freezing temperature. This poses the question of how do flexible soluble molecules promote the formation of water crystals, as they do not expose a well-defined surface to ice. Here we use molecular simulations to demonstrate that PVA promotes ice nucleation through a homogeneous mechanism: PVA increases the nucleation rate by destabilizing water in the solution. This work demonstrates a novel paradigm for understanding ice nucleation by soluble molecules and provides a new handle to design additives that promote crystallization.

The impact of organic vapours on warm cloud formation; characterisation of chamber setup and first experimental results

NASA Astrophysics Data System (ADS)

Frey, Wiebke; Connolly, Paul; Dorsey, James; Hu, Dawei; Alfarra, Rami; McFiggans, Gordon

2016-04-01

The Manchester Ice Cloud Chamber (MICC), consisting of a 10m high stainless steel tube and 1m in diameter, can be used to study cloud processes. MICC is housed in three separate cold rooms stacked on top of each other and warm pseudo-adiabatic expansion from controlled initial temperature and pressure is possible through chamber evacuation. Further details about the facility can be found at http://www.cas.manchester.ac.uk/restools/cloudchamber/index.html. MICC can be connected to the Manchester Aerosol Chamber (MAC, http://www.cas.manchester.ac.uk/restools/aerosolchamber/), which allows to inject specified aerosol particles into the cloud chamber for nucleation studies. The combination of MAC and MICC will be used in the CCN-Vol project, which seeks to bring the experimental evidence for co-condensation of organic and water vapour in cloud formation which leads to an increase in cloud particle numbers (see Topping et al., 2013, Nature Geoscience Letters, for details). Here, we will show a characterisation of the cloud and aerosol chamber coupling in regard to background aerosol particles and nucleation. Furthermore, we will show preliminary results from the warm CCN-Vol experiment, investigating the impact of co-condensation of organic vapours and water vapour on warm cloud droplet formation.

Incorporation of new particle formation and early growth treatments into WRF/Chem: Model improvement, evaluation, and impacts of anthropogenic aerosols over East Asia

NASA Astrophysics Data System (ADS)

Cai, Changjie; Zhang, Xin; Wang, Kai; Zhang, Yang; Wang, Litao; Zhang, Qiang; Duan, Fengkui; He, Kebin; Yu, Shao-Cai

2016-01-01

New particle formation (NPF) provides an important source of aerosol particles and cloud condensation nuclei, which may result in enhanced cloud droplet number concentration (CDNC) and cloud shortwave albedo. In this work, several nucleation parameterizations and one particle early growth parameterization are implemented into the online-coupled Weather Research and Forecasting model coupled with chemistry (WRF/Chem) to improve the model's capability in simulating NPF and early growth of ultrafine particles over East Asia. The default 8-bin over the size range of 39 nm-10 μm used in the Model for Simulating Aerosol Interactions and Chemistry aerosol module is expanded to the 12-bin over 1 nm-10 μm to explicitly track the formation and evolution of new particles. Although model biases remain in simulating H2SO4, condensation sink, growth rate, and formation rate, the evaluation of July 2008 simulation identifies a combination of three nucleation parameterizations (i.e., COMB) that can best represent the atmospheric nucleation processes in terms of both surface nucleation events and the resulting vertical distribution of ultrafine particle concentrations. COMB consists of a power law of Wang et al. (2011) based on activation theory for urban areas in planetary boundary layer (PBL), a power law of Boy et al. (2008) based on activation theory for non-urban areas in PBL, and the ion-mediated nucleation parameterization of YU10 for above PBL. The application and evaluation of the improved model with 12-bin and the COMB nucleation parameterization in East Asia during January, April, July, and October in 2001 show that the model has an overall reasonably good skill in reproducing most observed meteorological variables and surface and column chemical concentrations. Relatively large biases in simulated precipitation and wind speeds are due to inaccurate surface roughness and limitations in model treatments of cloud formation and aerosol-cloud-precipitation interactions. Large biases in the simulated surface concentrations of PM10, NOx, CO, SO2, and VOCs at some sites are due in part to possible underestimations of emissions and in part to inaccurate meteorological predictions. The simulations of 2001 show that anthropogenic aerosols can increase aerosol optical depth by 64.0-228.3%, CDNC by 40.2-76.4%, and cloud optical thickness by 14.3-25.3%; they can reduce surface net shortwave radiation by up to 42.5-52.8 W m-2, 2-m temperature by up to 0.34-0.83 °C, and PBL height by up to 76.8-125.9 m. Such effects are more significant than those previously reported for the U.S. and Europe.

Formation of a Tropopause Cirrus Layer Observed over Florida during CRYSTAL-FACE

NASA Technical Reports Server (NTRS)

Jensen, Eric; Pfister, Leonhard; Bui, Thaopaul; Weinheimer, Andrew; Weinstock, Elliot; Smith, Jessica; Pittman, Jasna; Baumgardner, Darrel; Lawson, Paul; McGill, Matthew J.

2005-01-01

On July 13, 2002 a widespread, subvisible tropopause cirrus layer occurred over the Florida region. This cloud was observed in great detail with the NASA Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) instrumentation, including in situ measurements with the WB-57 aircraft. In this paper, we use the 13 July cloud as a case study to evaluate the physical processes controlling the formation and evolution of tropopause cirrus layers. Microphysics measurements indicate that ice crystal diameters in the cloud layer ranged from about 7 to 50 microns, and the peak number mode was about 10-25 microns. In situ water vapor and temperature measurements in the cloud indicated supersaturation with respect to ice throughout, with ice saturation ratios as large as 1.8. Even when the ice surface area density was as high as about 500 sq microns/cu cm, ice supersaturations of 20-30% were observed. Trajectory analysis shows that the air sampled near the tropopause on this day generally came from the north and cooled considerably during the previous few days. Examination of infrared satellite imagery along air parcel back trajectories from the WB-57 flight track indicates that the tropopause cloud layer formation was, in general, not simply left over ice from recently generated anvil cirrus. Simulations of cloud formation using time-height curtains of temperature along the trajectory paths show that the cloud could have formed in situ near the tropopause as the air was advected into the south Florida region and cooled to unusually low temperatures. If we assume a high threshold for ice nucleation via homogeneous freezing of aqueous sulfate aerosols, the model reproduces the observed cloud structure, ice crystal size distributions, and ice supersaturation statistics. Inclusion of observed gravity wave temperature perturbations in the simulations is essential to reproduce the observed cloud properties. Without waves, crystal number densities are too low, crystal sizes are too large, and the crystals fall out too fast, leaving very little cloud persisting at the end of the simulations. In the cloud simulations, coincidence of high supersaturations and high surface areas can be produced by either recent nucleation or sedimentation of crystals into supersaturated layers. The agreement between model results and observed supersaturations is improved somewhat if we assume that the steady state relative humidity within cirrus at T<200 K is enhanced by about 30%. The WB-57 measurements and the model results suggest that the cloud layer irreversibly dehydrated air near the tropopause.

Ice forming experiment

NASA Technical Reports Server (NTRS)

Vali, G.

1982-01-01

A low gravity experiment to assess the effect of the presence of supercooled cloud droplets on the diffusional growth rate of ice crystals is described. The theoretical work and the feasibility studies are summarized. The nucleation of ice crystals in supercooled clouds is also discussed.

Comparison of ice nuclei from fruit juices and their properties

NASA Astrophysics Data System (ADS)

Fiala, Bianca; Felgitsch, Laura; Grothe, Hinrich

2017-04-01

Heterogeneous ice nucleation is a crucial process in the atmosphere. Recent findings indicate the importance of biological ice nuclei (IN) in this process. Pratt et al. (2009) sampled ice-crystal residues at approx. 8 km high altitude over Wyoming, U.S.. They found a third of the dry residues to be biological and further that 60% of the highly abundant mineral dusts to be internally mixed with biological or humic substances. Huffman et al. (2013) showed a burst of biological IN over woodlands connected to rain events. Previous investigations in our group (Pummer et al. 2012) showed that pollen and pollen washing water from several plants native to the boreal forests trigger heterogeneous ice nucleation. Recent work from our group (Felgitsch et al. 2016) showed that several juices of berries are ice nucleation active. Based on this research we examined ice nucleation activity (INA) and general properties of five juices: sea buckthorn, black currant, chokeberry, acerola, and elder berry. We elucidated particle size dependency of the ice nucleation activity to differentiate between coarse ice nucleating particles and nanoparticles or macromolecules. Investigations with different solvents and with chaotropic agents were performed in order to further clarify properties concerning chemical polarity of the IN, and the importance of hydrogen bonds and other structure forming polar interactions. The results are compared to known plant originated IN. Our results suggest similarities in terms of nucleation temperature and structure stability between different IN of plant materials. These properties show a clear differentiation to known bacterial and fungal IN. Felgitsch , L., Bichler, M., Häusler, T., Hitzenberger, R., and Grothe, H.: Heterogeneous freezing of water triggered by berry juices from perenneal plants, submitted, 2016. Huffman, J.A., Prenni, A.J., DeMott, P.J., Pöhlker, C., Mason, R.H., Robinson, N.H., Frohlich-Nowoisky, J., Tobo, Y., Després, V.R., Garcia, E., Gochis, D.J., Harris, E., Müller-Germann, I., Ruzene, C., Schmer, B., Sinha, B., Day, D.A., Andreae, M.O., Jimenez, J.L., Gallagher, M., Kreidenweis, S.M., Bertram, A.K., and Pöschl, U.: High concentrations of biological aerosol particles and ice nuclei during and after rain, Atmos. Chem. Phys., 13, 1651-1664, 2013. Pratt, K.A., DeMott, P.J., French, J.R., Wang, Z., Westphal, D.L., Heymsfield, A.J., Twohy, C.H., Prenni, A.J., and Prather, K.A.: In situ detection of biological particles in cloud ice-crystals, Nat. Geosci., 2, 298-401, 2009. Pummer, B.G., Bauer, H., Bernardi, J., Bleicher, S., and Grothe, H.: Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen, Atmos. Chem. Phys., 12, 2541-2550, 2012.

Cloud residues and interstitial aerosols from non-precipitating clouds over an industrial and urban area in northern China

NASA Astrophysics Data System (ADS)

Li, Weijun; Li, Peiren; Sun, Guode; Zhou, Shengzhen; Yuan, Qi; Wang, Wenxing

2011-05-01

Most studies of aerosol-cloud interactions have been conducted in remote locations; few have investigated the characterization of cloud condensation nuclei (CCN) over highly polluted urban and industrial areas. The present work, based on samples collected at Mt. Tai, a site in northern China affected by nearby urban and industrial air pollutant emissions, illuminates CCN properties in a polluted atmosphere. High-resolution transmission electron microscopy (TEM) was used to obtain the size, composition, and mixing state of individual cloud residues and interstitial aerosols. Most of the cloud residues displayed distinct rims which were found to consist of soluble organic matter (OM). Nearly all (91.7%) cloud residues were attributed to sulfate-related salts (the remainder was mostly coarse crustal dust particles with nitrate coatings). Half the salt particles were internally mixed with two or more refractory particles (e.g., soot, fly ash, crustal dust, CaSO 4, and OM). A comparison between cloud residues and interstitial particles shows that the former contained more salts and were of larger particle size than the latter. In addition, a somewhat high number scavenging ratio of 0.54 was observed during cloud formation. Therefore, the mixtures of salts with OMs account for most of the cloud-nucleating ability of the entire aerosol population in the polluted air of northern China. We advocate that both size and composition - the two influential, controlling factors for aerosol activation - should be built into all regional climate models of China.

Global aerosol effects on convective clouds

NASA Astrophysics Data System (ADS)

Wagner, Till; Stier, Philip

2013-04-01

Atmospheric aerosols affect cloud properties, and thereby the radiation balance of the planet and the water cycle. The influence of aerosols on clouds is dominated by increase of cloud droplet and ice crystal numbers (CDNC/ICNC) due to enhanced aerosols acting as cloud condensation and ice nuclei. In deep convective clouds this increase in CDNC/ICNC is hypothesised to increase precipitation because of cloud invigoration through enhanced freezing and associated increased latent heat release caused by delayed warm rain formation. Satellite studies robustly show an increase of cloud top height (CTH) and precipitation with increasing aerosol optical depth (AOD, as proxy for aerosol amount). To represent aerosol effects and study their influence on convective clouds in the global climate aerosol model ECHAM-HAM, we substitute the standard convection parameterisation, which uses one mean convective cloud for each grid column, with the convective cloud field model (CCFM), which simulates a spectrum of convective clouds, each with distinct values of radius, mixing ratios, vertical velocity, height and en/detrainment. Aerosol activation and droplet nucleation in convective updrafts at cloud base is the primary driver for microphysical aerosol effects. To produce realistic estimates for vertical velocity at cloud base we use an entraining dry parcel sub cloud model which is triggered by perturbations of sensible and latent heat at the surface. Aerosol activation at cloud base is modelled with a mechanistic, Köhler theory based, scheme, which couples the aerosols to the convective microphysics. Comparison of relationships between CTH and AOD, and precipitation and AOD produced by this novel model and satellite based estimates show general agreement. Through model experiments and analysis of the model cloud processes we are able to investigate the main drivers for the relationship between CTH / precipitation and AOD.

On the Importance of High Frequency Gravity Waves for Ice Nucleation in the Tropical Tropopause Layer

NASA Technical Reports Server (NTRS)

Jensen, Eric J.

2016-01-01

Recent investigations of the influence of atmospheric waves on ice nucleation in cirrus have identified a number of key processes and sensitivities: (1) ice concentrations produced by homogeneous freezing are strongly dependent on cooling rates, with gravity waves dominating upper tropospheric cooling rates; (2) rapid cooling driven by high-frequency waves are likely responsible for the rare occurrences of very high ice concentrations in cirrus; (3) sedimentation and entrainment tend to decrease ice concentrations as cirrus age; and (4) in some situations, changes in temperature tendency driven by high-frequency waves can quench ice nucleation events and limit ice concentrations. Here we use parcel-model simulations of ice nucleation driven by long-duration, constant-pressure balloon temperature time series, along with an extensive dataset of cold cirrus microphysical properties from the recent ATTREX high-altitude aircraft campaign, to statistically examine the importance of high-frequency waves as well as the consistency between our theoretical understanding of ice nucleation and observed ice concentrations. The parcel-model simulations indicate common occurrence of peak ice concentrations exceeding several hundred per liter. Sedimentation and entrainment would reduce ice concentrations as clouds age, but 1-D simulations using a wave parameterization (which underestimates rapid cooling events) still produce ice concentrations higher than indicated by observations. We find that quenching of nucleation events by high-frequency waves occurs infrequently and does not prevent occurrences of large ice concentrations in parcel simulations of homogeneous freezing. In fact, the high-frequency variability in the balloon temperature data is entirely responsible for production of these high ice concentrations in the simulations.

Landscape-precipitation feedback mediated by ice nuclei: an example from the Arctic

NASA Astrophysics Data System (ADS)

Stopelli, Emiliano; Conen, Franz; Zimmermann, Lukas; Morris, Cindy; Alewell, Christine

2016-04-01

The Arctic is one of the regions on Earth which are particularly sensitive to the effects of climate change. One of the largest uncertainties in describing climate and climate change is constituted by the characterisation of the behaviour of clouds. Specifically in the Arctic region there is a low abundance of cloud condensation nuclei (CCN) resulting in low droplet concentrations in clouds. Ice nucleating particles (INPs) in the atmosphere promote the aggregation of water molecules into ice, increasing the chance for precipitation. Therefore, a change in the absolute abundance of INPs and their relative presence compared to CCN is expected to have strong impacts on climate in the Arctic in terms of the radiative budget and of precipitation. In July 2015 we sampled particles from air at Haldde Observatory, Norway (69° 55'45" N, 22° 48'30" E, 905 m a.s.l.) on PM10 filters. We determined the number of INPs active at moderate supercooling temperatures (≥ -15 ° C, INPs-15) by immersion freezing. To identify potential sources of airborne INPs we also collected samples of soil from a highland and decaying leaf litter. Air masses passing over the land were enriched in INPs-15, with concentrations twice to three times larger than those found in air masses directly coming from the Barents Sea. Ice nucleation spectra suggest that it is mainly litter which accounts for this enrichment in INPs-15. This example helps elucidating the feedback linking landscapes and atmosphere mediated by INPs in the frame of climate change. While the snow coverage is progressively reducing in the Arctic, areas with decaying leaf litter and vegetation that are exposed to wind and grazing are expected to increase, resulting into a larger abundance of INPs in the local atmosphere. This increase in airborne INPs can promote a change in the freezing of clouds, with impact on the lifetime and on the radiative properties of clouds, and ultimately on the occurrence of precipitation in the Arctic region.

Insights Regarding Ice Nucleating Particle Measurement Capabilities from Laboratory and Field Measurements During the Fifth International Ice Nucleation Workshop

NASA Astrophysics Data System (ADS)

DeMott, P. J.; Mohler, O.; Cziczo, D. J.; Hiranuma, N.; Brooks, S. D.; Petters, M.

2017-12-01

Improvement in the ability to quantify the role of aerosols in primary ice formation in clouds is vital to improving prediction of natural and anthropogenic impacts on cold cloud properties and reducing uncertainties in climate predictions. A host of common and new methods for quantifying the atmospheric abundance of ice nucleating particles (INPs) have recently been developed. To realize the utility of such data for numerical model parameterization development and validation, it is important to understand similarities, differences, and biases in different methods. To achieve this goal, it is common to challenge instruments with a range of aerosol types in laboratory studies. Only a few comparisons have occurred in atmospheric situations. This presentation highlights comparisons made in laboratory and field phases of the Fifth International Ice Nucleation workshop (FIN) during 2015. The FIN-2 laboratory workshop was conducted at the AIDA facility of the Karlsruhe Institute of Technology, involving nine real-time INP instruments and several sampling methods for wet suspensions and filter collection and resuspension for INP measurements. The FIN-3 atmospheric activity was conducted at the Desert Research Institute's Storm Peak Laboratory (SPL), with a reduced set of participants. Lessons and insights were gained during analyses of data from both workshops regarding the capabilities and comparability of present ice nucleation measurement systems. The FIN-2 and FIN-3 results show typical one order of magnitude agreement within basic measurement types and overall for characterizing the concentrations (over several orders of magnitude dynamic range from -5 to -35 C) of a variety of INP types and ambient INPs active in the immersion-freezing mode. Discrepancies are least for lab sampling of natural soil particle INPs and greatest for materials with steep d[INP]/dT functions, such as K-feldspar or bacterial INPs processed warmer than -8 C. Varied reasons and implications for atmospheric measurements will be discussed. FIN-3 ambient studies also showed correspondence for the first time between online and offline assessment of the contrasting INP concentrations active in deposition and immersion freezing (much higher numbers) regimes. Major contributions from the FIN participant teams are acknowledged.

Increase in Ice Nucleation Efficiency of Feldspars, Kaolinite and Mica in Dilute NH3 and NH4+-containing Solutions

NASA Astrophysics Data System (ADS)

Kumar, A.; Marcolli, C.; Luo, B.; Krieger, U. K.; Peter, T.

2017-12-01

Semivolatile species present in the atmosphere are prone to adhere to mineral dust particle surfaces during long range transport, and could potentially change the particle surface properties and its ice nucleation (IN) efficiency. Immersion freezing experiments were performed with microcline (K-feldspar), known to be highly IN active, suspended in aqueous solutions of ammonia, (NH4)2SO4, NH4HSO4, NH4NO3, NH4Cl, Na2SO4, H2SO4, K2SO4 and KCl to investigate the effect of solutes on the IN efficiency. Freezing of emulsified droplets investigated with a differential scanning calorimeter (DSC) showed that the heterogeneous ice nucleation temperatures deviate from the water activity-based IN theory, describing heterogeneous ice nucleation temperatures as a function of solution water activity by a constant offset with respect to the ice melting point curve (Zobrist et al. 2008). IN temperatures enhanced up to 4.5 K were observed for very dilute NH3 and NH4+-containing solutions while a decrease was observed as the concentration was further increased. For all solutes with cations other than NH4+, the IN efficiency decreased. An increase of the IN efficiency in very dilute NH3 and NH4+-containing solutions followed by a decrease with increasing concentration was also observed for sanidine (K-feldspar) and andesine (Na/Ca-feldspar). This is an important indication towards specific chemical interactions between solutes and the feldspar surface which is not captured by the water activity-based IN theory. A similar trend is present but less pronounced in case of kaolinite and mica, while quartz is barely affected. We hypothesize that the hydrogen bonding of NH3 molecules with surface -OH groups could be the reason for the enhanced freezing temperatures in dilute ammonia and ammonium containing solutions as they could form an ice-like overlayer providing hydrogen bonding groups for ice to nucleate on top of it. This implies to possibilities of enhanced IN efficiency, especially in mixed-phase cloud regime, of ammonium sulfate coated mineral dust particles in the condensation mode when the coating dilutes during cloud droplet activation.

Ice nucleation in the upper troposphere: Sensitivity to aerosol number density, temperature, and cooling rate

NASA Technical Reports Server (NTRS)

Jensen, E. J.; Toon, O. B.

1994-01-01

We have investigated the processes that control ice crystal nucleation in the upper troposphere using a numerical model. Nucleation of ice resulting from cooling was simulated for a range of aerosol number densities, initial temperatures, and cooling rates. In contrast to observations of stratus clouds, we find that the number of ice crystals that nucleate in cirrus is relatively insensitive to the number of aerosols present. The ice crystal size distribution at the end of the nucleation process is unaffected by the assumed initial aerosol number density. Essentially, nucleation continues until enough ice crystals are present such that their deposition growth rapidly depletes the vapor and shuts off any further nucleation. However, the number of ice crystals nucleated increases rapidly with decreasing initial temperature and increasing cooling rate. This temperature dependence alone could explain the large ice crystal number density observed in very cold tropical cirrus.

Acid–base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer

PubMed Central

Chen, Modi; Titcombe, Mari; Jiang, Jingkun; Jen, Coty; Kuang, Chongai; Fischer, Marc L.; Eisele, Fred L.; Siepmann, J. Ilja; Hanson, David R.; Zhao, Jun; McMurry, Peter H.

2012-01-01

Climate models show that particles formed by nucleation can affect cloud cover and, therefore, the earth's radiation budget. Measurements worldwide show that nucleation rates in the atmospheric boundary layer are positively correlated with concentrations of sulfuric acid vapor. However, current nucleation theories do not correctly predict either the observed nucleation rates or their functional dependence on sulfuric acid concentrations. This paper develops an alternative approach for modeling nucleation rates, based on a sequence of acid–base reactions. The model uses empirical estimates of sulfuric acid evaporation rates obtained from new measurements of neutral molecular clusters. The model predicts that nucleation rates equal the sulfuric acid vapor collision rate times a prefactor that is less than unity and that depends on the concentrations of basic gaseous compounds and preexisting particles. Predicted nucleation rates and their dependence on sulfuric acid vapor concentrations are in reasonable agreement with measurements from Mexico City and Atlanta. PMID:23091030

Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer.

PubMed

Chen, Modi; Titcombe, Mari; Jiang, Jingkun; Jen, Coty; Kuang, Chongai; Fischer, Marc L; Eisele, Fred L; Siepmann, J Ilja; Hanson, David R; Zhao, Jun; McMurry, Peter H

2012-11-13

Climate models show that particles formed by nucleation can affect cloud cover and, therefore, the earth's radiation budget. Measurements worldwide show that nucleation rates in the atmospheric boundary layer are positively correlated with concentrations of sulfuric acid vapor. However, current nucleation theories do not correctly predict either the observed nucleation rates or their functional dependence on sulfuric acid concentrations. This paper develops an alternative approach for modeling nucleation rates, based on a sequence of acid-base reactions. The model uses empirical estimates of sulfuric acid evaporation rates obtained from new measurements of neutral molecular clusters. The model predicts that nucleation rates equal the sulfuric acid vapor collision rate times a prefactor that is less than unity and that depends on the concentrations of basic gaseous compounds and preexisting particles. Predicted nucleation rates and their dependence on sulfuric acid vapor concentrations are in reasonable agreement with measurements from Mexico City and Atlanta.

Measuring the CCN and IN ability of bacterial isolates: implications for the southeastern United States and Puerto Rico

NASA Astrophysics Data System (ADS)

Purdue, S.; Waters, S.; Konstantinidis, K.; Nenes, A.; DeLeon-Rodriguez, N.

2015-12-01

Ice nucleation is an important process in the climate system as it influences global precipitation processes, and can affect the vertical distribution of clouds with effects that both cool and warm the atmosphere. Of the pathways to ice nucleation, immersion mode, which occurs when ice nuclei (IN) particles are surrounded by an aqueous phase that subsequently freezes, dominates primary ice production in mixed-phase clouds. A simple but effective method to study immersion freezing is to utilize a droplet freezing assay (DFA) that consists of an aluminum plate, precisely cooled by a continuous flow of an ethylene glycol-water mixture. Using such a system we study the immersion IN characteristics of bacterial isolates (for temperatures ranging from -15oC to 0oC) isolated from rainwater and air collected in Atlanta, GA and Puerto Rico, over storms throughout the year. Despite their relatively large size and the presence of hydrophilic groups on the outer membranes of many bacteria, it is unclear if bacteria possess an inherent ability to nucleate an aqueous phase (a requirement for immersion freezing) for the wide range of supersaturations found in clouds. For this, we measure the cloud condensation nucleation (CCN) activity of each isolate (over the 0.05% to 0.6% supersaturation range) using a Continuous Flow Streamwise Thermal Gradient CCN Counter. Initial results have shown certain isolates to be very efficient CCN, allowing them to form droplets even for the very low supersaturations found in radiation fogs. In combination, these experiments provide insight into the potential dual-ability of some bacteria, isolated from the southeastern United States and Puerto Rico, to act as both efficient CCN and IN.

Direct Comparisons of Ice Cloud Microphysical Properties Simulated by the Community Atmosphere Model CAM5 with ARM SPartICus Observations

NASA Astrophysics Data System (ADS)

Wu, C.; Liu, X.; Zhang, K.; Diao, M.; Gettelman, A.

2016-12-01

Cirrus clouds in the upper troposphere play a key role in the Earth radiation budget, and their radiative forcing depends strongly on number concentration and size distribution of ice particles. In this study we evaluate the cloud microphysical properties simulated by the Community Atmosphere Model version 5.4 (CAM5) against the Small Particles in Cirrus (SPartICus) observations over the ARM South Great Plain (SGP) site between January and June 2010. Model simulation is performed using specific dynamics to preserve prognostic meteorology (U, V, and T) close to GEOS-5 analysis. Model results collocated with SPartICus flight tracks spatially and temporally are directly compared with the observations. We compare CAM5 simulated ice crystal number concentration (Ni), ice particle size distribution, ice water content (IWC), and Ni co-variances with temperature and vertical velocity with the statistics from SPartICus observations. All analyses are restricted to T ≤ -40°C and in a 6°×6° area centered at SGP. Model sensitivity tests are performed with different ice nucleation mechanisms and with the effects of pre-existing ice crystals to reflect the uncertainties in cirrus parameterizations. In addition, different threshold size for autoconversion of cloud ice to snow (Dcs) is also tested. We find that (1) a distinctly high Ni (100-1000 L-1) often occurred in the observations but is significantly underestimated in the model, which may be due to the smaller relative humidity with respect to ice (RHi) in the simulation that could suppress the homogeneous nucleation, (2) a positive correlation exists between Ni and vertical velocity variance (σw) at horizontal scales up to 50 km in the observation, and the model can reproduce this relationship but tends to underestimate Ni when σw is relatively small, (3) simulated Ni differs greatly among the sensitive experiments, and simulated IWC is also sensitive to the cirrus parameterizations but to a lesser extent. Moreover, the model produces much better ice particle sizes in terms of number-mean diameter (Dnm) but significantly underestimate Ni and IWC for all the designed sensitive experiments. Our results suggest that better representation of environmental conditions (e.g., RHi and water vapor) is needed to improve the formation and evolution of ice clouds in the model.

Possible significance of cubic water-ice, H2O-Ic, in the atmospheric water cycle of Mars

NASA Technical Reports Server (NTRS)

Gooding, James L.

1988-01-01

The possible formation and potential significance of the cubic ice polymorph on Mars is discussed. When water-ice crystallizes on Earth, the ambient conditions of temperature and pressure result in the formation of the hexagonal ice polymorph; however, on Mars, the much lower termperature and pressures may permit the crystallization of the cubic polymorph. Cubic ice has two properties of possible importance on Mars: it is an excellant nucleator of other volatiles (such as CO2), and it undergoes an exothermic transition to hexagonal ice at temperatures above 170 K. These properties may have significant implications for both martian cloud formation and the development of the seasonal polar caps.

Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model

NASA Astrophysics Data System (ADS)

Alpert, Peter A.; Knopf, Daniel A.

2016-02-01

Immersion freezing is an important ice nucleation pathway involved in the formation of cirrus and mixed-phase clouds. Laboratory immersion freezing experiments are necessary to determine the range in temperature, T, and relative humidity, RH, at which ice nucleation occurs and to quantify the associated nucleation kinetics. Typically, isothermal (applying a constant temperature) and cooling-rate-dependent immersion freezing experiments are conducted. In these experiments it is usually assumed that the droplets containing ice nucleating particles (INPs) all have the same INP surface area (ISA); however, the validity of this assumption or the impact it may have on analysis and interpretation of the experimental data is rarely questioned. Descriptions of ice active sites and variability of contact angles have been successfully formulated to describe ice nucleation experimental data in previous research; however, we consider the ability of a stochastic freezing model founded on classical nucleation theory to reproduce previous results and to explain experimental uncertainties and data scatter. A stochastic immersion freezing model based on first principles of statistics is presented, which accounts for variable ISA per droplet and uses parameters including the total number of droplets, Ntot, and the heterogeneous ice nucleation rate coefficient, Jhet(T). This model is applied to address if (i) a time and ISA-dependent stochastic immersion freezing process can explain laboratory immersion freezing data for different experimental methods and (ii) the assumption that all droplets contain identical ISA is a valid conjecture with subsequent consequences for analysis and interpretation of immersion freezing. The simple stochastic model can reproduce the observed time and surface area dependence in immersion freezing experiments for a variety of methods such as: droplets on a cold-stage exposed to air or surrounded by an oil matrix, wind and acoustically levitated droplets, droplets in a continuous-flow diffusion chamber (CFDC), the Leipzig aerosol cloud interaction simulator (LACIS), and the aerosol interaction and dynamics in the atmosphere (AIDA) cloud chamber. Observed time-dependent isothermal frozen fractions exhibiting non-exponential behavior can be readily explained by this model considering varying ISA. An apparent cooling-rate dependence of Jhet is explained by assuming identical ISA in each droplet. When accounting for ISA variability, the cooling-rate dependence of ice nucleation kinetics vanishes as expected from classical nucleation theory. The model simulations allow for a quantitative experimental uncertainty analysis for parameters Ntot, T, RH, and the ISA variability. The implications of our results for experimental analysis and interpretation of the immersion freezing process are discussed.

Double-moment Cloud Microphysics Scheme for the Deep Convection Parameterization in the GFDL AM3

NASA Astrophysics Data System (ADS)

Belochitski, A.; Donner, L.

2013-12-01

A double-moment cloud microphysical scheme originally developed by Morrision and Gettelman (2008) for the stratiform clouds and later adopted for the deep convection by Song and Zhang (2011) is being implemented in to the deep convection parameterization of Geophysical Fluid Dynamics Laboratory's atmospheric general circulation model AM3. The scheme treats cloud drop, cloud ice, rain, and snow number concentrations and mixing ratios as diagnostic variables and incorporates processes of autoconversion, self-collection, collection between hydrometeor species, sedimentation, ice nucleation, drop activation, homogeneous and heterogeneous freezing, and the Bergeron-Findeisen process. Detailed representation of microphysical processes makes the scheme suitable for studying the interactions between aerosols and convection, as well as aerosols' indirect effects on clouds and the roles of these effects in climate change. The scheme is implemented into the single column version of the GFDL AM3 and evaluated using large scale forcing data obtained at the U.S. Department of Energy Atmospheric Radiation Measurment project's Southern Great Planes and Tropical West Pacific sites. Sensitivity of the scheme to formulations for autoconversion of cloud water and its accretion by rain, self-collection of rain and self-collection of snow, as well as the formulation for heterogenous ice nucleation is investigated. In the future, tests with the full atmospheric GCM will be conducted.

Initiation of secondary ice production in clouds

NASA Astrophysics Data System (ADS)

Sullivan, Sylvia C.; Hoose, Corinna; Kiselev, Alexei; Leisner, Thomas; Nenes, Athanasios

2018-02-01

Disparities between the measured concentrations of ice-nucleating particles (INPs) and in-cloud ice crystal number concentrations (ICNCs) have led to the hypothesis that mechanisms other than primary nucleation form ice in the atmosphere. Here, we model three of these secondary production mechanisms - rime splintering, frozen droplet shattering, and ice-ice collisional breakup - with a six-hydrometeor-class parcel model. We perform three sets of simulations to understand temporal evolution of ice hydrometeor number (Nice), thermodynamic limitations, and the impact of parametric uncertainty when secondary production is active. Output is assessed in terms of the number of primarily nucleated ice crystals that must exist before secondary production initiates (NINP(lim)) as well as the ICNC enhancement from secondary production and the timing of a 100-fold enhancement. Nice evolution can be understood in terms of collision-based nonlinearity and the phasedness of the process, i.e., whether it involves ice hydrometeors, liquid ones, or both. Ice-ice collisional breakup is the only process for which a meaningful NINP(lim) exists (0.002 up to 0.15 L-1). For droplet shattering and rime splintering, a warm enough cloud base temperature and modest updraft are the more important criteria for initiation. The low values of NINP(lim) here suggest that, under appropriate thermodynamic conditions for secondary ice production, perturbations in cloud concentration nuclei concentrations are more influential in mixed-phase partitioning than those in INP concentrations.

Surface crystallization of supercooled water in clouds

PubMed Central

Tabazadeh, A.; Djikaev, Y. S.; Reiss, H.

2002-01-01

The process by which liquid cloud droplets homogeneously crystallize into ice is still not well understood. The ice nucleation process based on the standard and classical theory of homogeneous freezing initiates within the interior volume of a cloud droplet. Current experimental data on homogeneous freezing rates of ice in droplets of supercooled water, both in air and emulsion oil samples, show considerable scatter. For example, at −33°C, the reported volume-based freezing rates of ice in supercooled water vary by as many as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Here, we show that the process of ice nucleus formation at the air (or oil)-liquid water interface may help to explain why experimental results on ice nucleation rates yield different results in different ambient phases. Our results also suggest that surface crystallization of ice in cloud droplets can explain why low amounts of supercooled water have been observed in the atmosphere near −40°C. PMID:12456877

Measurements of cloud condensation nuclei spectra within maritime cumulus cloud droplets: Implications for mixing processes

NASA Technical Reports Server (NTRS)

Twohy, Cynthia H.; Hudson, James G.

1995-01-01

In a cloud formed during adiabatic expansion, the droplet size distribution will be systematically related to the critical supersaturation of the cloud condensation nuclei (CNN), but this relationship can be complicated in entraining clouds. Useful information about cloud processes, such as mixing, can be obtained from direct measurements of the CNN involved in droplet nucleation. This was accomplished by interfacing two instruments for a series of flights in maritime cumulus clouds. One instrument, the counterflow virtual impactor, collected cloud droplets, and the nonvolatile residual nuclei of the droplets was then passed to a CCN spectrometer, which measured the critical supersaturation (S(sub c)) spectrum of the droplet nuclei. The measured S(sub c) spectra of the droplet nuclei were compared with the S(sub c) spectra of ambient aerosol particles in order to identify which CCN were actually incorporated into droplets and to determine when mixing processes were active at different cloud levels. The droplet nuclei nearly always exhibited lower median S(sub c)'s than the ambient aerosol, as expected since droplets nucleate perferentially on particles with lower critical supersaturations. Critical supersaturation spectra from nuclei of droplets near cloud base were similar to those predicted for cloud regions formed adiabatically, but spectra of droplet nuclei from middle cloud levels showed some evidence that mixing had occurred. Near cloud top, the greatest variation in the spectra of the droplet nuclei was observed, and nuclei with high S(sub c)'s were sometimes present even within relatively large droplets. This suggests that the extent of mixing increases with height in cumulus clouds and that inhomogeneous mixing may be important near cloud top. These promising initial results suggest improvements to the experimental technique that will permit more quantitative results in future experiments.

The potential influence of Asian and African mineral dust on ice, mixed-phase and liquid water clouds

NASA Astrophysics Data System (ADS)

Wiacek, A.; Peter, T.; Lohmann, U.

2010-09-01

This modelling study explores the availability of mineral dust particles as ice nuclei for interactions with ice, mixed-phase and liquid water clouds, also tracking the particles' history of cloud-processing. We performed 61 320 one-week forward trajectory calculations originating near the surface of major dust emitting regions in Africa and Asia using high-resolution meteorological analysis fields for the year 2007. Dust-bearing trajectories were assumed to be those coinciding with known dust emission seasons, without explicitly modelling dust emission and deposition processes. We found that dust emissions from Asian deserts lead to a higher potential for interactions with high ice clouds, despite being the climatologically much smaller dust emission source. This is due to Asian regions experiencing significantly more ascent than African regions, with strongest ascent in the Asian Taklimakan desert at ~25%, ~40% and 10% of trajectories ascending to 300 hPa in spring, summer and fall, respectively. The specific humidity at each trajectory's starting point was transported in a Lagrangian manner and relative humidities with respect to water and ice were calculated in 6-h steps downstream, allowing us to estimate the formation of liquid, mixed-phase and ice clouds. Downstream of the investigated dust sources, practically none of the simulated air parcels reached conditions of homogeneous ice nucleation (T≲-40 °C) along trajectories that have not experienced water saturation first. By far the largest fraction of cloud forming trajectories entered conditions of mixed-phase clouds, where mineral dust will potentially exert the biggest influence. The majority of trajectories also passed through atmospheric regions supersaturated with respect to ice but subsaturated with respect to water, where so-called "warm ice clouds" (T≳-40 °C) theoretically may form prior to supercooled water or mixed-phase clouds. The importance of "warm ice clouds" and the general influence of dust in the mixed-phase cloud region are highly uncertain due to both a considerable scatter in recent laboratory data from ice nucleation experiments, which we briefly review in this work, and due to uncertainties in sub-grid scale vertical transport processes unresolved by the present trajectory analysis. For "classical" cirrus-forming temperatures (T≲-40 °C), our results show that only mineral dust ice nuclei that underwent mixed-phase cloud-processing, most likely acquiring coatings of organic or inorganic material, are likely to be relevant. While the potential paucity of deposition ice nuclei shown in this work dimishes the possibility of deposition nucleation, the absence of liquid water droplets at T≲-40 °C makes the less explored contact freezing mechanism (involving droplet collisions with bare ice nuclei) highly inefficient. These factors together indicate the necessity of further systematic studies of immersion mode ice nucleation on mineral dust suspended in atmospherically relevant coatings.

The potential influence of Asian and African mineral dust on ice, mixed-phase and liquid water clouds

NASA Astrophysics Data System (ADS)

Wiacek, A.; Peter, T.; Lohmann, U.

2010-02-01

This modelling study explores the availability of mineral dust particles as ice nuclei for interactions with ice, mixed-phase and liquid water clouds, also tracking the particles' history of cloud-processing. We performed 61 320 one-week forward trajectory calculations originating near the surface of major dust emitting regions in Africa and Asia using high-resolution meteorological analysis fields for the year 2007. Without explicitly modelling dust emission and deposition processes, dust-bearing trajectories were assumed to be those coinciding with known dust emission seasons. We found that dust emissions from Asian deserts lead to a higher potential for interactions with high clouds, despite being the climatologically much smaller dust emission source. This is due to Asian regions experiencing significantly more ascent than African regions, with strongest ascent in the Asian Taklimakan desert at ~25%, ~40% and 10% of trajectories ascending to 300 hPa in spring, summer and fall, respectively. The specific humidity at each trajectory's starting point was transported in a Lagrangian manner and relative humidities with respect to water and ice were calculated in 6-h steps downstream, allowing us to estimate the formation of liquid, mixed-phase and ice clouds. Practically none of the simulated air parcels reached regions where homogeneous ice nucleation can take place (T≲-40 °C) along trajectories that have not experienced water saturation first. By far the largest fraction of cloud forming trajectories entered conditions of mixed-phase clouds, where mineral dust will potentially exert the biggest influence. The majority of trajectories also passed through regions supersaturated with respect to ice but subsaturated with respect to water, where "warm" (T≳-40 °C) ice clouds may form prior to supercooled water or mixed-phase clouds. The importance of "warm" ice clouds and the general influence of dust in the mixed-phase cloud region are highly uncertain due to considerable scatter in recent laboratory data from ice nucleation experiments, which we briefly review in this work. For "classical" cirrus-forming temperatures, our results show that only mineral dust IN that underwent mixed-phase cloud-processing previously are likely to be relevant, and, therefore, we recommend further systematic studies of immersion mode ice nucleation on mineral dust suspended in atmospherically relevant coatings.

Global model comparison of heterogeneous ice nucleation parameterizations in mixed phase clouds

NASA Astrophysics Data System (ADS)

Yun, Yuxing; Penner, Joyce E.

2012-04-01

A new aerosol-dependent mixed phase cloud parameterization for deposition/condensation/immersion (DCI) ice nucleation and one for contact freezing are compared to the original formulations in a coupled general circulation model and aerosol transport model. The present-day cloud liquid and ice water fields and cloud radiative forcing are analyzed and compared to observations. The new DCI freezing parameterization changes the spatial distribution of the cloud water field. Significant changes are found in the cloud ice water fraction and in the middle cloud fractions. The new DCI freezing parameterization predicts less ice water path (IWP) than the original formulation, especially in the Southern Hemisphere. The smaller IWP leads to a less efficient Bergeron-Findeisen process resulting in a larger liquid water path, shortwave cloud forcing, and longwave cloud forcing. It is found that contact freezing parameterizations have a greater impact on the cloud water field and radiative forcing than the two DCI freezing parameterizations that we compared. The net solar flux at top of atmosphere and net longwave flux at the top of the atmosphere change by up to 8.73 and 3.52 W m-2, respectively, due to the use of different DCI and contact freezing parameterizations in mixed phase clouds. The total climate forcing from anthropogenic black carbon/organic matter in mixed phase clouds is estimated to be 0.16-0.93 W m-2using the aerosol-dependent parameterizations. A sensitivity test with contact ice nuclei concentration in the original parameterization fit to that recommended by Young (1974) gives results that are closer to the new contact freezing parameterization.

Analysis of isothermal and cooling rate dependent immersion freezing by a unifying stochastic ice nucleation model

NASA Astrophysics Data System (ADS)

Alpert, P. A.; Knopf, D. A.

2015-05-01

Immersion freezing is an important ice nucleation pathway involved in the formation of cirrus and mixed-phase clouds. Laboratory immersion freezing experiments are necessary to determine the range in temperature (T) and relative humidity (RH) at which ice nucleation occurs and to quantify the associated nucleation kinetics. Typically, isothermal (applying a constant temperature) and cooling rate dependent immersion freezing experiments are conducted. In these experiments it is usually assumed that the droplets containing ice nuclei (IN) all have the same IN surface area (ISA), however the validity of this assumption or the impact it may have on analysis and interpretation of the experimental data is rarely questioned. A stochastic immersion freezing model based on first principles of statistics is presented, which accounts for variable ISA per droplet and uses physically observable parameters including the total number of droplets (Ntot) and the heterogeneous ice nucleation rate coefficient, Jhet(T). This model is applied to address if (i) a time and ISA dependent stochastic immersion freezing process can explain laboratory immersion freezing data for different experimental methods and (ii) the assumption that all droplets contain identical ISA is a valid conjecture with subsequent consequences for analysis and interpretation of immersion freezing. The simple stochastic model can reproduce the observed time and surface area dependence in immersion freezing experiments for a variety of methods such as: droplets on a cold-stage exposed to air or surrounded by an oil matrix, wind and acoustically levitated droplets, droplets in a continuous flow diffusion chamber (CFDC), the Leipzig aerosol cloud interaction simulator (LACIS), and the aerosol interaction and dynamics in the atmosphere (AIDA) cloud chamber. Observed time dependent isothermal frozen fractions exhibiting non-exponential behavior with time can be readily explained by this model considering varying ISA. An apparent cooling rate dependence ofJhet is explained by assuming identical ISA in each droplet. When accounting for ISA variability, the cooling rate dependence of ice nucleation kinetics vanishes as expected from classical nucleation theory. The model simulations allow for a quantitative experimental uncertainty analysis for parameters Ntot, T, RH, and the ISA variability. In an idealized cloud parcel model applying variability in ISAs for each droplet, the model predicts enhanced immersion freezing temperatures and greater ice crystal production compared to a case when ISAs are uniform in each droplet. The implications of our results for experimental analysis and interpretation of the immersion freezing process are discussed.

Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds

PubMed Central

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H.; Rudich, Yinon

2013-01-01

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges. PMID:24297908

Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

PubMed

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

2013-12-17

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

Investigating the Sensitivity of Nucleation Parameterization on Ice Growth

NASA Astrophysics Data System (ADS)

Gaudet, L.; Sulia, K. J.

2017-12-01

The accurate prediction of precipitation from lake-effect snow events associated with the Great Lakes region depends on the parameterization of thermodynamic and microphysical processes, including the formation and subsequent growth of frozen hydrometeors. More specifically, the formation of ice hydrometeors has been represented through varying forms of ice nucleation parameterizations considering the different nucleation modes (e.g., deposition, condensation-freezing, homogeneous). These parameterizations have been developed from in-situ measurements and laboratory observations. A suite of nucleation parameterizations consisting of those published in Meyers et al. (1992) and DeMott et al. (2010) as well as varying ice nuclei data sources are coupled with the Adaptive Habit Model (AHM, Harrington et al. 2013), a microphysics module where ice crystal aspect ratio and density are predicted and evolve in time. Simulations are run with the AHM which is implemented in the Weather Research and Forecasting (WRF) model to investigate the effect of ice nucleation parameterization on the non-spherical growth and evolution of ice crystals and the subsequent effects on liquid-ice cloud-phase partitioning. Specific lake-effect storms that were observed during the Ontario Winter Lake-Effect Systems (OWLeS) field campaign (Kristovich et al. 2017) are examined to elucidate this potential microphysical effect. Analysis of these modeled events is aided by dual-polarization radar data from the WSR-88D in Montague, New York (KTYX). This enables a comparison of the modeled and observed polarmetric and microphysical profiles of the lake-effect clouds, which involves investigating signatures of reflectivity, specific differential phase, correlation coefficient, and differential reflectivity. Microphysical features of lake-effect bands, such as ice, snow, and liquid mixing ratios, ice crystal aspect ratio, and ice density are analyzed to understand signatures in the aforementioned modeled dual-polarization radar variables. Hence, this research helps to determine an ice nucleation scheme that will best model observations of lake-effect clouds producing snow off of Lake Ontario and Lake Erie, and analyses will highlight the sensitivity of the evolution of the cases to a given nucleation scheme.

Distinct Contributions of Ice Nucleation, Large-Scale Environment, and Shallow Cumulus Detrainment to Cloud Phase Partitioning With NCAR CAM5

DOE PAGES

Wang, Yong; Zhang, Damao; Liu, Xiaohong; ...

2018-01-06

Mixed-phase clouds containing both liquid droplets and ice particles occur frequently at high latitudes and in the midlatitude storm track regions. Simulations of the cloud phase partitioning between liquid and ice hydrometeors in state-of-the-art global climate models are still associated with large biases. For this study, the phase partitioning in terms of liquid mass phase ratio (MPR liq, defined as the ratio of liquid mass to total condensed water mass) simulated from the NCAR Community Atmosphere Model version 5 (CAM5) is evaluated against the observational data from A-Train satellite remote sensors. Modeled MPR liq is significantly lower than observations onmore » the global scale, especially in the Southern Hemisphere (e.g., Southern Ocean and the Antarctic). Sensitivity tests with CAM5 are conducted to investigate the distinct contributions of heterogeneous ice nucleation, shallow cumulus detrainment, and large-scale environment (e.g., winds, temperature, and water vapor) to the low MPR liq biases. Our results show that an aerosol-aware ice nucleation parameterization increases the MPR liq especially at temperatures colder than -20°C and significantly improves the model agreements with observations in the Polar regions in summer. The decrease of threshold temperature over which all detrained cloud water is liquid from 268 to 253 K enhances the MPR liq and improves the MPR liq mostly over the Southern Ocean. By constraining water vapor in CAM5 toward reanalysis, modeled low biases in many geographical regions are largely reduced through a significant decrease of cloud ice mass mixing ratio.« less

Distinct Contributions of Ice Nucleation, Large-Scale Environment, and Shallow Cumulus Detrainment to Cloud Phase Partitioning With NCAR CAM5

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Yong; Zhang, Damao; Liu, Xiaohong

Mixed-phase clouds containing both liquid droplets and ice particles occur frequently at high latitudes and in the midlatitude storm track regions. Simulations of the cloud phase partitioning between liquid and ice hydrometeors in state-of-the-art global climate models are still associated with large biases. For this study, the phase partitioning in terms of liquid mass phase ratio (MPR liq, defined as the ratio of liquid mass to total condensed water mass) simulated from the NCAR Community Atmosphere Model version 5 (CAM5) is evaluated against the observational data from A-Train satellite remote sensors. Modeled MPR liq is significantly lower than observations onmore » the global scale, especially in the Southern Hemisphere (e.g., Southern Ocean and the Antarctic). Sensitivity tests with CAM5 are conducted to investigate the distinct contributions of heterogeneous ice nucleation, shallow cumulus detrainment, and large-scale environment (e.g., winds, temperature, and water vapor) to the low MPR liq biases. Our results show that an aerosol-aware ice nucleation parameterization increases the MPR liq especially at temperatures colder than -20°C and significantly improves the model agreements with observations in the Polar regions in summer. The decrease of threshold temperature over which all detrained cloud water is liquid from 268 to 253 K enhances the MPR liq and improves the MPR liq mostly over the Southern Ocean. By constraining water vapor in CAM5 toward reanalysis, modeled low biases in many geographical regions are largely reduced through a significant decrease of cloud ice mass mixing ratio.« less

Distinct Contributions of Ice Nucleation, Large-Scale Environment, and Shallow Cumulus Detrainment to Cloud Phase Partitioning With NCAR CAM5

NASA Astrophysics Data System (ADS)

Wang, Yong; Zhang, Damao; Liu, Xiaohong; Wang, Zhien

2018-01-01

Mixed-phase clouds containing both liquid droplets and ice particles occur frequently at high latitudes and in the midlatitude storm track regions. Simulations of the cloud phase partitioning between liquid and ice hydrometeors in state-of-the-art global climate models are still associated with large biases. In this study, the phase partitioning in terms of liquid mass phase ratio (MPRliq, defined as the ratio of liquid mass to total condensed water mass) simulated from the NCAR Community Atmosphere Model version 5 (CAM5) is evaluated against the observational data from A-Train satellite remote sensors. Modeled MPRliq is significantly lower than observations on the global scale, especially in the Southern Hemisphere (e.g., Southern Ocean and the Antarctic). Sensitivity tests with CAM5 are conducted to investigate the distinct contributions of heterogeneous ice nucleation, shallow cumulus detrainment, and large-scale environment (e.g., winds, temperature, and water vapor) to the low MPRliq biases. Our results show that an aerosol-aware ice nucleation parameterization increases the MPRliq especially at temperatures colder than -20°C and significantly improves the model agreements with observations in the Polar regions in summer. The decrease of threshold temperature over which all detrained cloud water is liquid from 268 to 253 K enhances the MPRliq and improves the MPRliq mostly over the Southern Ocean. By constraining water vapor in CAM5 toward reanalysis, modeled low biases in many geographical regions are largely reduced through a significant decrease of cloud ice mass mixing ratio.

A New Method Using Single-Particle Mass Spectrometry Data to Distinguish Mineral Dust and Biological Aerosols

NASA Astrophysics Data System (ADS)

Al-Mashat, H.; Kristensen, L.; Sultana, C. M.; Prather, K. A.

2016-12-01

The ability to distinguish types of particles present within a cloud is important for determining accurate inputs to climate models. The chemical composition of particles within cloud liquid droplets and ice crystals can have a significant impact on the timing, location, and amount of precipitation that falls. Precipitation efficiency is increased by the presence of ice crystals in clouds, and both mineral dust and biological aerosols have been shown to be effective ice nucleating particles (INPs) in the atmosphere. A current challenge in aerosol science is distinguishing mineral dust and biological material in the analysis of real-time, ambient, single-particle mass spectral data. Single-particle mass spectrometers are capable of measuring the size-resolved chemical composition of individual atmospheric particles. However, there is no consistent analytical method for distinguishing dust and biological aerosols. Sampling and characterization of control samples (i.e. of known identity) of mineral dust and bacteria were performed by the Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) as part of the Fifth Ice Nucleation (FIN01) Workshop at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) facility in Karlsruhe, Germany. Using data collected by the ATOFMS of control samples, a new metric has been developed to classify single particles as dust or biological independent of spectral cluster analysis. This method, involving the use of a ratio of mass spectral peak areas for organic nitrogen and silicates, is easily reproducible and does not rely on extensive knowledge of particle chemistry or the ionization characteristics of mass spectrometers. This represents a step toward rapidly distinguishing particle types responsible for ice nucleation activity during real-time sampling in clouds. The ability to distinguish types of particles present within a cloud is important for determining accurate inputs to climate models. The chemical composition of particles within cloud liquid droplets and ice crystals can have a significant impact on the timing, location, and amount of precipitation that falls. Precipitation efficiency is increased by the presence of ice crystals in clouds, and both mineral dust and biological aerosols have been shown to be effective ice nucleating particles (INPs) in the atmosphere. A current challenge in aerosol science is distinguishing mineral dust and biological material in the analysis of real-time, ambient, single-particle mass spectral data. Single-particle mass spectrometers are capable of measuring the size-resolved chemical composition of individual atmospheric particles. However, there is no consistent analytical method for distinguishing dust and biological aerosols. Sampling and characterization of control samples (i.e. of known identity) of mineral dust and bacteria were performed by the Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) as part of the Fifth Ice Nucleation (FIN01) Workshop at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) facility in Karlsruhe, Germany. Using data collected by the ATOFMS of control samples, a new metric has been developed to classify single particles as dust or biological independent of spectral cluster analysis. This method, involving the use of a ratio of mass spectral peak areas for organic nitrogen and silicates, is easily reproducible and does not rely on extensive knowledge of particle chemistry or the ionization characteristics of mass spectrometers. This represents a step toward rapidly distinguishing particle types responsible for ice nucleation activity during real-time sampling in clouds.

Microphysical Processes Affecting the Pinatubo Volcanic Plume

NASA Technical Reports Server (NTRS)

Hamill, Patrick; Houben, Howard; Young, Richard; Turco, Richard; Zhao, Jingxia

1996-01-01

In this paper we consider microphysical processes which affect the formation of sulfate particles and their size distribution in a dispersing cloud. A model for the dispersion of the Mt. Pinatubo volcanic cloud is described. We then consider a single point in the dispersing cloud and study the effects of nucleation, condensation and coagulation on the time evolution of the particle size distribution at that point.

Ice residual properties in mixed-phase clouds at the high-alpine Jungfraujoch site.

PubMed

Kupiszewski, Piotr; Zanatta, Marco; Mertes, Stephan; Vochezer, Paul; Lloyd, Gary; Schneider, Johannes; Schenk, Ludwig; Schnaiter, Martin; Baltensperger, Urs; Weingartner, Ernest; Gysel, Martin

2016-10-27

Ice residual (IR) and total aerosol properties were measured in mixed-phase clouds (MPCs) at the high-alpine Jungfraujoch research station. Black carbon (BC) content and coating thickness of BC-containing particles were determined using single-particle soot photometers. The ice activated fraction (IAF), derived from a comparison of IR and total aerosol particle size distributions, showed an enrichment of large particles in the IR, with an increase in the IAF from values on the order of 10 -4 to 10 -3 for 100 nm (diameter) particles to 0.2 to 0.3 for 1 μm (diameter) particles. Nonetheless, due to the high number fraction of submicrometer particles with respect to total particle number, IR size distributions were still dominated by the submicrometer aerosol. A comparison of simultaneously measured number size distributions of BC-free and BC-containing IR and total aerosol particles showed depletion of BC by number in the IR, suggesting that BC does not play a significant role in ice nucleation in MPCs at the Jungfraujoch. The potential anthropogenic climate impact of BC via the glaciation effect in MPCs is therefore likely to be negligible at this site and in environments with similar meteorological conditions and a similar aerosol population. The IAF of the BC-containing particles also increased with total particle size, in a similar manner as for the BC-free particles, but on a level 1 order of magnitude lower. Furthermore, BC-containing IR were found to have a thicker coating than the BC-containing total aerosol, suggesting the importance of atmospheric aging for ice nucleation.

The Dependence of Homo- and Heterogeneously Formed Cirrus Clouds on Latitude, Season and Surface-type based on a New CALIPSO Remote Sensing Method

NASA Astrophysics Data System (ADS)

Mitchell, D. L.; Garnier, A.; Mejia, J.; Avery, M. A.; Erfani, E.

2016-12-01

A new CALIPSO infrared retrieval method sensitive to small ice crystals has been developed to measure the temperature dependence of the layer-average number concentration N, effective diameter De and ice water content in single-layer cirrus clouds (one cloud layer in the atmospheric column) that have optical depths between 0.3 and 3.0 and cloud base temperature T < 235 K. While retrievals of low N are not accurate, mid-to-high N can be retrieved with much lower uncertainty. This enables the retrieval to estimate the dominant ice nucleation mechanism (homo- or heterogeneous, henceforth hom and het) though which the cirrus formed. Based on N, hom or het cirrus can be estimated as a function of temperature, season, latitude and surface type. The retrieved properties noted above compare favorably with spatial-temporal coincident cirrus cloud in situ measurements from SPARTICUS case studies as well as the extensive in situ cirrus data set of Krämer et al. (2009, ACP). For our cirrus cloud selection, these retrievals show a pronounced seasonal cycle in the N. Hemisphere over land north of 30°N latitude in terms of both cloud amount and microphysics, with greater cloud cover, higher N and smaller De during the winter season. We postulate that this is partially due to the seasonal cycle of deep convection that replenishes the supply of ice nuclei (IN) at cirrus levels, with hom more likely when deep convection is absent. Over oceans, heterogeneous ice nucleation appears to prevail based on the lower N and higher De observed. Due to the relatively smooth ocean surface, lower amplitude atmospheric waves at cirrus cloud levels are expected. Over land outside the tropics during winter, hom cirrus tend to occur over mountainous terrain, possibly due to lower IN concentrations and stronger, more sustained updrafts in mountain-induced waves. Over pristine Antarctica, IN concentrations are minimal and the terrain near the coast is often high and rugged, allowing hom to dominate. Accordingly, over Antarctica cirrus clouds exhibit relatively high N and small De throughout the year. These retrievals allow us to parameterize De and the ice fall speed in CAM5 as a function of T, season, latitude and surface-type. Our goal is to estimate the radiative impact of hom cirrus north of 30°N latitude in winter relative to het cirrus before the AGU Fall Meeting.

A computationally efficient description of heterogeneous freezing: A simplified version of the Soccer ball model

NASA Astrophysics Data System (ADS)

Niedermeier, Dennis; Ervens, Barbara; Clauss, Tina; Voigtländer, Jens; Wex, Heike; Hartmann, Susan; Stratmann, Frank

2014-01-01

In a recent study, the Soccer ball model (SBM) was introduced for modeling and/or parameterizing heterogeneous ice nucleation processes. The model applies classical nucleation theory. It allows for a consistent description of both apparently singular and stochastic ice nucleation behavior, by distributing contact angles over the nucleation sites of a particle population assuming a Gaussian probability density function. The original SBM utilizes the Monte Carlo technique, which hampers its usage in atmospheric models, as fairly time-consuming calculations must be performed to obtain statistically significant results. Thus, we have developed a simplified and computationally more efficient version of the SBM. We successfully used the new SBM to parameterize experimental nucleation data of, e.g., bacterial ice nucleation. Both SBMs give identical results; however, the new model is computationally less expensive as confirmed by cloud parcel simulations. Therefore, it is a suitable tool for describing heterogeneous ice nucleation processes in atmospheric models.

Clouds, Aerosols, and Precipitation in the Marine Boundary Layer: An Arm Mobile Facility Deployment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wood, Robert; Wyant, Matthew; Bretherton, Christopher S.

The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) deployment at Graciosa Island in the Azores generated a 21 month (April 2009-December 2010) comprehensive dataset documenting clouds, aerosols and precipitation using the Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF). The scientific aim of the deployment is to gain improved understanding of the interactions of clouds, aerosols and precipitation in the marine boundary layer. Graciosa Island straddles the boundary between the subtropics and midlatitudes in the Northeast Atlantic Ocean, and consequently experiences a great diversity of meteorological and cloudiness conditions. Low clouds are the dominant cloud type, with stratocumulusmore » and cumulus occurring regularly. Approximately half of all clouds contained precipitation detectable as radar echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1- 11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide range of aerosol conditions was sampled during the deployment consistent with the diversity of sources as indicated by back trajectory analysis. Preliminary findings suggest important two-way interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation and cloud radiative properties while being controlled in part by precipitation scavenging. The data from at Graciosa are being compared with short-range forecasts made a variety of models. A pilot analysis with two climate and two weather forecast models shows that they reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well, but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to be a permanent fixed ARM site that became operational in October 2013.« less

Clouds, aerosol, and precipitation in the Marine Boundary Layer: An ARM mobile facility deployment

DOE PAGES

Wood, Robert; Luke, Ed; Wyant, Matthew; ...

2014-04-27

The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) deployment at Graciosa Island in the Azores generated a 21-month (April 2009-December 2010) comprehensive dataset documenting clouds, aerosols, and precipitation using the Atmospheric Radiation Measurement Program (ARM) Mobile Facility (AMF). The scientific aim of the deployment is to gain improved understanding of the interactions of clouds, aerosols, and precipitation in the marine boundary layer. Graciosa Island straddles the boundary between the subtropics and midlatitudes in the Northeast Atlantic Ocean and consequently experiences a great diversity of meteorological and cloudiness conditions. Low clouds are the dominant cloud type, with stratocumulusmore » and cumulus occurring regularly. Approximately half of all clouds contained precipitation detectable as radar echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1-11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide range of aerosol conditions was sampled during the deployment consistent with the diversity of sources as indicated by back-trajectory analysis. Preliminary findings suggest important two-way interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation and cloud radiative properties while being controlled in part by precipitation scavenging.The data from Graciosa are being compared with short-range forecasts made with a variety of models. A pilot analysis with two climate and two weather forecast models shows that they reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to be a permanent fixed ARM site that became operational in October 2013.« less

Clouds, Aerosols, and Precipitation in the Marine Boundary Layer: An Arm Mobile Facility Deployment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wood, Robert; Wyant, Matthew; Bretherton, Christopher S.

The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) 38 deployment at Graciosa Island in the Azores generated a 21 month (April 2009-December 2010) 39 comprehensive dataset documenting clouds, aerosols and precipitation using the Atmospheric 40 Radiation Measurement (ARM) Mobile Facility (AMF). The scientific aim of the deployment is 41 to gain improved understanding of the interactions of clouds, aerosols and precipitation in the 42 marine boundary layer. 43 Graciosa Island straddles the boundary between the subtropics and midlatitudes in the 44 Northeast Atlantic Ocean, and consequently experiences a great diversity of meteorological and 45 cloudiness conditions. Lowmore » clouds are the dominant cloud type, with stratocumulus and cumulus 46 occurring regularly. Approximately half of all clouds contained precipitation detectable as radar 47 echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1-48 11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide 49 range of aerosol conditions was sampled during the deployment consistent with the diversity of 50 sources as indicated by back trajectory analysis. Preliminary findings suggest important two-way 51 interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation 52 and cloud radiative properties while being controlled in part by precipitation scavenging. 53 The data from at Graciosa are being compared with short-range forecasts made a variety 54 of models. A pilot analysis with two climate and two weather forecast models shows that they 55 reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well, 56 but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to 57 be a long-term ARM site that became operational in October 2013.« less

Application of an online-coupled regional climate model, WRF-CAM5, over East Asia for examination of ice nucleation schemes: Part I. Comprehensive model evaluation and trend analysis for 2006 and 2011

DOE PAGES

Chen, Ying; Zhang, Yang; Fan, Jiwen; ...

2015-08-18

Online-coupled climate and chemistry models are necessary to realistically represent the interactions between climate variables and chemical species and accurately simulate aerosol direct and indirect effects on cloud, precipitation, and radiation. In this Part I of a two-part paper, simulations from the Weather Research and Forecasting model coupled with the physics package of Community Atmosphere Model (WRF-CAM5) are conducted with the default heterogeneous ice nucleation parameterization over East Asia for two full years: 2006 and 2011. A comprehensive model evaluation is performed using satellite and surface observations. The model shows an overall acceptable performance for major meteorological variables at themore » surface and in the boundary layer, as well as column variables (e.g., precipitation, cloud fraction, precipitating water vapor, downward longwave and shortwave radiation). Moderate to large biases exist for cloud condensation nuclei over oceanic areas, cloud variables (e.g., cloud droplet number concentration, cloud liquid and ice water paths, cloud optical depth, longwave and shortwave cloud forcing). These biases indicate a need to improve the model treatments for cloud processes, especially cloud droplets and ice nucleation, as well as to reduce uncertainty in the satellite retrievals. The model simulates well the column abundances of chemical species except for column SO 2 but relatively poor for surface concentrations of several species such as CO, NO 2, SO 2, PM 2.5, and PM 10. Several reasons could contribute to the underestimation of major chemical species in East Asia including underestimations of anthropogenic emissions and natural dust emissions, uncertainties in the spatial and vertical distributions of the anthropogenic emissions, as well as biases in meteorological, radiative, and cloud predictions. Despite moderate to large biases in the chemical predictions, the model performance is generally consistent with or even better than that reported for East Asia with only a few exceptions. The model generally reproduces the observed seasonal variations and the difference between 2006 and 2011 for most variables or chemical species. Overall, these results demonstrate promising skills of WRF-CAM5 for long-term simulations at a regional scale and suggest several areas of potential improvements.« less

Application of an Online-Coupled Regional Climate Model, WRF-CAM5, over East Asia for Examination of Ice Nucleation Schemes: Part I. Comprehensive Model Evaluation and Trend Analysis for 2006 and 2011

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, Ying; Zhang, Yang; Fan, Jiwen

Online-coupled climate and chemistry models are necessary to realistically represent the interactions between climate variables and chemical species and accurately simulate aerosol direct and indirect effects on cloud, precipitation, and radiation. In this Part I of a two-part paper, simulations from the Weather Research and Forecasting model coupled with the physics package of Community Atmosphere Model (WRF-CAM5) are conducted with the default heterogeneous ice nucleation parameterization over East Asia for two full years: 2006 and 2011. A comprehensive model evaluation is performed using satellite and surface observations. The model shows an overall acceptable performance for major meteorological variables at themore » surface and in the boundary layer, as well as column variables (e.g., precipitation, cloud fraction, precipitating water vapor, downward longwave and shortwave radiation). Moderate to large biases exist for cloud condensation nuclei over oceanic areas, cloud variables (e.g., cloud droplet number concentration, cloud liquid and ice water paths, cloud optical depth, longwave and shortwave cloud forcing). These biases indicate a need to improve the model treatments for cloud processes, especially cloud droplets and ice nucleation, as well as to reduce uncertainty in the satellite retrievals. The model simulates well the column abundances of chemical species except for column SO 2 but relatively poor for surface concentrations of several species such as CO, NO 2, SO 2, PM2.5, and PM10. Several reasons could contribute to the underestimation of major chemical species in East Asia including underestimations of anthropogenic emissions and natural dust emissions, uncertainties in the spatial and vertical distributions of the anthropogenic emissions, as well as biases in meteorological, radiative, and cloud predictions. Despite moderate to large biases in the chemical predictions, the model performance is generally consistent with or even better than that reported for East Asia with only a few exceptions. The model generally reproduces the observed seasonal variations and the difference between 2006 and 2011 for most variables or chemical species. Overall, these results demonstrate promising skills of WRF-CAM5 for long-term simulations at a regional scale and suggest several areas of potential improvements.« less

Application of an online-coupled regional climate model, WRF-CAM5, over East Asia for examination of ice nucleation schemes: Part I. Comprehensive model evaluation and trend analysis for 2006 and 2011

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, Ying; Zhang, Yang; Fan, Jiwen

Online-coupled climate and chemistry models are necessary to realistically represent the interactions between climate variables and chemical species and accurately simulate aerosol direct and indirect effects on cloud, precipitation, and radiation. In this Part I of a two-part paper, simulations from the Weather Research and Forecasting model coupled with the physics package of Community Atmosphere Model (WRF-CAM5) are conducted with the default heterogeneous ice nucleation parameterization over East Asia for two full years: 2006 and 2011. A comprehensive model evaluation is performed using satellite and surface observations. The model shows an overall acceptable performance for major meteorological variables at themore » surface and in the boundary layer, as well as column variables (e.g., precipitation, cloud fraction, precipitating water vapor, downward longwave and shortwave radiation). Moderate to large biases exist for cloud condensation nuclei over oceanic areas, cloud variables (e.g., cloud droplet number concentration, cloud liquid and ice water paths, cloud optical depth, longwave and shortwave cloud forcing). These biases indicate a need to improve the model treatments for cloud processes, especially cloud droplets and ice nucleation, as well as to reduce uncertainty in the satellite retrievals. The model simulates well the column abundances of chemical species except for column SO 2 but relatively poor for surface concentrations of several species such as CO, NO 2, SO 2, PM 2.5, and PM 10. Several reasons could contribute to the underestimation of major chemical species in East Asia including underestimations of anthropogenic emissions and natural dust emissions, uncertainties in the spatial and vertical distributions of the anthropogenic emissions, as well as biases in meteorological, radiative, and cloud predictions. Despite moderate to large biases in the chemical predictions, the model performance is generally consistent with or even better than that reported for East Asia with only a few exceptions. The model generally reproduces the observed seasonal variations and the difference between 2006 and 2011 for most variables or chemical species. Overall, these results demonstrate promising skills of WRF-CAM5 for long-term simulations at a regional scale and suggest several areas of potential improvements.« less

Contact freezing induced by biological (Snomax) and mineral dust (K-feldspar) particles

NASA Astrophysics Data System (ADS)

Hoffmann, N.; Schäfer, M.; Duft, D.; Kiselev, A. A.; Leisner, T.

2013-12-01

The contact freezing of supercooled cloud droplets is one of the potentially important and the least investigated heterogeneous mechanism of ice formation in tropospheric clouds [1]. On the time scales of cloud lifetime the freezing of supercooled water droplets via contact mechanism may occur at higher temperature compared to the same IN immersed in the droplet. In our experiment we study single water droplets freely levitated in an Electrodynamic Balance [2]. We have shown previously that the rate of freezing at given temperature is governed only by the rate of droplet -particle collision and by the properties of the contact ice nuclei [2, 3]. Recently, we have extended our experiments to feldspar, being the most abundant component of the atmospheric mineral dust particles, and Snomax, as a proxy for atmospheric biological Ice Nuclei (IN). In this contribution we show that both IN exhibits the same temperature, size and material dependency observed previously in immersion mode [4, 5]. Based on these results, we limit the number of mechanisms that could be responsible for the enhancement of contact nucleation of ice in supercooled water. [1] - Ladino, L. A., Stetzer, O., and Lohmann, U.: Contact freezing: a review, Atmos. Chem. Phys. Discuss., 13, 7811-7869, doi:10.5194/acpd-13-7811-2013, 2013. [2] - Hoffmann, N., Kiselev, A., Rzesanke, D., Duft, D., and Leisner, T.: Experimental quantification of contact freezing in an electrodynamic balance, Atmos. Meas. Tech. Discuss., 6, 3407-3437, doi:10.5194/amtd-6-3407-2013, 2013. [3] - Hoffmann, N., Duft, D., Kiselev, A., and Leisner, T.: Contact freezing efficiency of mineral dust aerosols studied in an electrodynamic balance: quantitative size and temperature dependence for illite particles, Faraday Discuss., doi: 10.1039/C3FD00033H, 2013. [4] - Atkinson, James D., Murray, Benjamin J., Woodhouse, Matthew T., Whale, Thomas F., Baustian, Kelly J., Carslaw, Kenneth S., Dobbie, Steven, O'Sullivan, Daniel, and Malkin, Tamsin L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds, Nature, 498, 355-358, doi:10.1038/nature12278, Science, 2013. [5] - Hartmann, S., Augustin, S., Clauss, T., Wex, H., Šantl-Temkiv, T., Voigtländer, J., Niedermeier, D., and Stratmann, F.: Immersion freezing of ice nucleation active protein complexes, Atmos. Chem. Phys., 13, 5751-5766, doi:10.5194/acp-13-5751-2013, 2013.

Sensitivity of aerosol loading and properties to cloudiness

NASA Astrophysics Data System (ADS)

Iversen, T.; Seland, O.; Kirkevag, A.; Kristjansson, J. E.

2005-12-01

Clouds influence aerosols in various ways. Sulfate is swiftly produced in liquid phase provided there is both sulfur dioxide and oxidants available. Nucleation and Aitken mode aerosol particles efficiently grow in size by collision and coagulation with cloud droplets. When precipitation is formed, aerosol and precursor gases may be quickly removed bay rainout. The dynamics associated with clouds in some cases may swiftly mix aerosols deeply into the troposphere. In some cases Aitken-mode particles may be formed in cloud droplets by splitting agglomerates of particulate matter such as black carbon In this presentation we will discuss how global cloudiness may influence the burden, residence time, and spatial distribution of sulfate, black carbon and particulate organic matter. A similar physico-chemical scheme for there compounds has been implemented in three generations of the NCAR community climate model (CCM3, CAM2 and CAM3). The scheme is documented in the literature and is a part of the Aerocom-intercomparison. There are many differences between these models. With respect to aerosols, a major difference is that CAM3 has a considerably higher global cloud volume and more then twice the amount of cloud water than CAM2 and CCM3. Atmospheric simulations have been made with prescribed ocean temperatures. It is slightly surprising to discover that certain aspects of the aerosols are not particularly sensitive to these differences in cloud availability. This sensitivity will be compared to sensitivities with respect to processing in deep convective clouds.

An aerosol chamber investigation of the heterogeneous ice nucleating potential of refractory nanoparticles

NASA Astrophysics Data System (ADS)

Saunders, R. W.; Möhler, O.; Schnaiter, M.; Benz, S.; Wagner, R.; Saathoff, H.; Connolly, P. J.; Burgess, R.; Gallagher, M.; Wills, R.; Murray, B. J.; Plane, J. M. C.

2009-11-01

Nanoparticles of iron oxide (crystalline and amorphous), silicon oxide and magnesium oxide were investigated for their propensity to nucleate ice over the temperature range 180-250 K, using the AIDA chamber in Karlsruhe, Germany. All samples were observed to initiate ice formation via the deposition mode at threshold ice super-saturations (RHi thresh) ranging from 105% to 140% for temperatures below 220 K. Approximately 10% of amorphous Fe2O3 particles (modal diameter = 30 nm) generated in situ from a photochemical aerosol reactor, led to ice nucleation at RHi thresh = 140% at an initial chamber temperature of 182 K. Quantitative analysis using a singular hypothesis treatment provided a fitted function [ns (190 K) = 10(3.33×sice)+8.16] for the variation in ice-active surface site density (ns: m-2) with ice saturation (sice) for Fe2O3 nanoparticles. This was implemented in an aerosol-cloud model to determine a predicted deposition (mass accommodation) coefficient for water vapour on ice of 0.1 at temperatures appropriate for the upper atmosphere. Classical nucleation theory was used to determine representative contact angles (θ) for the different particle compositions. For the in situ generated Fe2O3 particles, a slight inverse temperature dependence was observed with θ = 10.5° at 182 K, decreasing to 9.0° at 200 K (compared with 10.2° and 11.4°, respectively for the SiO2 and MgO particle samples at the higher temperature). These observations indicate that such refractory nanoparticles are relatively efficient materials for the nucleation of ice under the conditions studied in the chamber which correspond to cirrus cloud formation in the upper troposphere. The results also show that Fe2O3 particles do not act as ice nuclei under conditions pertinent for tropospheric mixed phase clouds, which necessarily form above ~233 K. At the lower temperatures (<150 K) where noctilucent clouds form during summer months in the high latitude mesosphere, higher contact angles would be expected, which may reduce the effectiveness of these particles as ice nuclei in this part of the atmosphere.

An aerosol chamber investigation of the heterogeneous ice nucleating potential of refractory nanoparticles

NASA Astrophysics Data System (ADS)

Saunders, R. W.; Möhler, O.; Schnaiter, M.; Benz, S.; Wagner, R.; Saathoff, H.; Connolly, P. J.; Burgess, R.; Murray, B. J.; Gallagher, M.; Wills, R.; Plane, J. M. C.

2010-02-01

Nanoparticles of iron oxide (crystalline and amorphous), silicon oxide and magnesium oxide were investigated for their propensity to nucleate ice over the temperature range 180-250 K, using the AIDA chamber in Karlsruhe, Germany. All samples were observed to initiate ice formation via the deposition mode at threshold ice super-saturations (RHithresh) ranging from 105% to 140% for temperatures below 220 K. Approximately 10% of amorphous Fe2O3 particles (modal diameter = 30 nm) generated in situ from a photochemical aerosol reactor, led to ice nucleation at RHithresh = 140% at an initial chamber temperature of 182 K. Quantitative analysis using a singular hypothesis treatment provided a fitted function [ns(190 K)=10(3.33×sice)+8.16] for the variation in ice-active surface site density (ns:m-2) with ice saturation (sice) for Fe2O3 nanoparticles. This was implemented in an aerosol-cloud model to determine a predicted deposition (mass accommodation) coefficient for water vapour on ice of 0.1 at temperatures appropriate for the upper atmosphere. Classical nucleation theory was used to determine representative contact angles (θ) for the different particle compositions. For the in situ generated Fe2O3 particles, a slight inverse temperature dependence was observed with θ = 10.5° at 182 K, decreasing to 9.0° at 200 K (compared with 10.2° and 11.4° respectively for the SiO2 and MgO particle samples at the higher temperature). These observations indicate that such refractory nanoparticles are relatively efficient materials for the nucleation of ice under the conditions studied in the chamber which correspond to cirrus cloud formation in the upper troposphere. The results also show that Fe2O3 particles do not act as ice nuclei under conditions pertinent for tropospheric mixed phase clouds, which necessarily form above ~233 K. At the lower temperatures (<150 K) where noctilucent clouds form during summer months in the high latitude mesosphere, higher contact angles would be expected, which may reduce the effectiveness of these particles as ice nuclei in this part of the atmosphere.

A Ground-Based Doppler Radar and Micropulse Lidar Forward Simulator for GCM Evaluation of Arctic Mixed-Phase Clouds: Moving Forward Towards an Apples-to-apples Comparison of Hydrometeor Phase

NASA Astrophysics Data System (ADS)

Lamer, K.; Fridlind, A. M.; Ackerman, A. S.; Kollias, P.; Clothiaux, E. E.

2017-12-01

An important aspect of evaluating Artic cloud representation in a general circulation model (GCM) consists of using observational benchmarks which are as equivalent as possible to model output in order to avoid methodological bias and focus on correctly diagnosing model dynamical and microphysical misrepresentations. However, current cloud observing systems are known to suffer from biases such as limited sensitivity, and stronger response to large or small hydrometeors. Fortunately, while these observational biases cannot be corrected, they are often well understood and can be reproduced in forward simulations. Here a ground-based millimeter wavelength Doppler radar and micropulse lidar forward simulator able to interface with output from the Goddard Institute for Space Studies (GISS) ModelE GCM is presented. ModelE stratiform hydrometeor fraction, mixing ratio, mass-weighted fall speed and effective radius are forward simulated to vertically-resolved profiles of radar reflectivity, Doppler velocity and spectrum width as well as lidar backscatter and depolarization ratio. These forward simulated fields are then compared to Atmospheric Radiation Measurement (ARM) North Slope of Alaska (NSA) ground-based observations to assess cloud vertical structure (CVS). Model evalution of Arctic mixed-phase cloud would also benefit from hydrometeor phase evaluation. While phase retrieval from synergetic observations often generates large uncertainties, the same retrieval algorithm can be applied to observed and forward-simulated radar-lidar fields, thereby producing retrieved hydrometeor properties with potentially the same uncertainties. Comparing hydrometeor properties retrieved in exactly the same way aims to produce the best apples-to-apples comparisons between GCM ouputs and observations. The use of a comprenhensive ground-based forward simulator coupled with a hydrometeor classification retrieval algorithm provides a new perspective for GCM evaluation of Arctic mixed-phase clouds from the ground where low-level supercooled liquid layer are more easily observed and where additional environmental properties such as cloud condensation nuclei are quantified. This should help assist in choosing between several possible diagnostic ice nucleation schemes for ModelE stratiform cloud.

North American and Asian aerosols over the eastern Pacific Ocean and their role in regulating cloud condensation nuclei

NASA Astrophysics Data System (ADS)

Roberts, G.; Mauger, G.; Hadley, O.; Ramanathan, V.

2006-07-01

Measurements of aerosol and cloud properties in the Eastern Pacific Ocean were taken during an airborne experiment on the University of Wyoming's King Air during April 2004 as part of the Cloud Indirect Forcing Experiment (CIFEX). We observed a wide variety of aerosols, including those of long-range transport from Asia, clean marine boundary layer, and North American emissions. These aerosols, classified by their size distribution and history, were found in stratified layers between 500 to 7500 m above sea level and thicknesses from 100 to 3000 m. A comparison of the aerosol size distributions to measurements of cloud condensation nuclei (CCN) provides insight to the CCN activity of the different aerosol types. The overall ratio of measured to predicted CCN concentration (NCCN) is 0.56 ± 0.41 with a relationship of NCCN,measured = NCCN,predicted0.846±0.002 for 23 research flights and 1884 comparisons. Such a relationship does not accurately describe a CCN closure; however, it is consistent with our measurements that high CCN concentrations are more influenced by anthropogenic sources, which are less CCN active. While other CCN closures have obtained results closer to the expected 1:1 relationship, the different aerosol types (and presumably differences in aerosol chemistry) are responsible for the discrepancy. The measured NCCN at 0.3% supersaturation (Sc) ranged from 20 cm-3 (pristine) to 350 cm-3 (anthropogenic) with an average of 106 ± 54 cm-3 over the experiment. The inferred supersaturation in the clouds sampled during this experiment is ˜0.3%. CCN concentrations of cloud-processed aerosol were well predicted using an ammonium sulfate approximation for Sc ≤ 0.4%. Predicted NCCN for other aerosol types (i.e., Asian and North American aerosols) were high compared to measured values indicating a less CCN active aerosol. This study highlights the importance of chemical effects on CCN measurements and introduces a CCN activation index as a method of classifying the efficiency of an aerosol to serve as CCN relative to an ammonium sulfate particle. This index ranged from close to unity for cloud processed aerosols to as low as 0.31 for aged aerosols transported from Asia. We also compare the performance of two CCN instruments (static thermal diffusion chamber and streamwise continuous flow chamber) on a 45 minute level leg where we observe an aged layer and a nucleation event. More than 50% of the aged aerosol served as CCN at 0.2% Sc, primarily owing to their large size, while CCN concentrations during the nucleation event were close to 0 cm-3. CCN concentrations from both instruments agreed within instrument errors; however, the continuous flow chamber effectively captured the rapid transition in aerosol properties.

Performance of McRAS-AC in the GEOS-5 AGCM: Part 1, Aerosol-Activated Cloud Microphysics, Precipitation, Radiative Effects, and Circulation

NASA Technical Reports Server (NTRS)

Sud, Y. C.; Lee, D.; Oreopoulos, L.; Barahona, D.; Nenes, A.; Suarez, M. J.

2012-01-01

A revised version of the Microphysics of clouds with Relaxed Arakawa-Schubert and Aerosol-Cloud interaction (McRAS-AC), including, among others, the Barahona and Nenes ice nucleation parameterization, is implemented in the GEOS-5 AGCM. Various fields from a 10-year long integration of the AGCM with McRAS-AC were compared with their counterparts from an integration of the baseline GEOS-5 AGCM, and with satellite data as observations. Generally using McRAS-AC reduced biases in cloud fields and cloud radiative effects are much better over most of the regions of the Earth. Two weaknesses are identified in the McRAS-AC runs, namely, too few cloud particles around 40S-60S, and too high cloud water path during northern hemisphere summer over the Gulf Stream and North Pacific. Sensitivity analyses showed that these biases potentially originated from biases in the aerosol input. The first bias is largely eliminated in a sensitivity test using 50% smaller aerosol particles, while the second bias is much reduced when interactive aerosol chemistry was turned on. The main drawback of McRAS-AC is dearth of low-level marine stratus clouds, probably due to lack of dry-convection, not yet implemented into the cloud scheme. Despite these biases, McRAS-AC does simulate realistic clouds and their optical properties that can improve with better aerosol-input and thereby has the potential to be a valuable tool for climate modeling research because of its aerosol indirect effect simulation capabilities involving prediction of cloud particle number concentration and effective particle size for both convective and stratiform clouds is quite realistic.

Field and Laboratory Studies of Atmospheric Organic Aerosol

NASA Astrophysics Data System (ADS)

Coggon, Matthew Mitchell

This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 < f42 < 0.15; 0.01 < f99 < 0.04), and negligible (f42 < 0.05; f99 < 0.01) ship influence. Application of these conditions to all measurements conducted during E-PEACE demonstrated that a large fraction of cloud droplet (72%) and dry aerosol mass (12%) sampled in the California coastal study region was heavily or moderately influenced by ship emissions. Another study investigated the chemical and physical evolution of a controlled organic plume emitted from the R/V Point Sur. Under sunny conditions, nucleated particles composed of oxidized organic compounds contributed nearly an order of magnitude more cloud condensation nuclei (CCN) than less oxidized particles formed under cloudy conditions. The processing time necessary for particles to become CCN active was short ( 4 hr). Laboratory chamber experiments were also conducted to evaluate particle-phase processes influencing aerosol phase and composition. In one study, ammonium sulfate seed was coated with a layer of secondary organic aerosol (SOA) from toluene oxidation followed by a layer of SOA from α-pinene oxidation. The system exhibited different evaporative properties than ammonium sulfate seed initially coated with α-pinene SOA followed by a layer of toluene SOA. This behavior is consistent with a shell-and-core model and suggests limited mixing among different SOA types. Another study investigated the reactive uptake of isoprene epoxy diols (IEPOX) onto non-acidified aerosol. It was demonstrated that particle acidity has limited influence on organic aerosol formation onto ammonium sulfate seed, and that the chemical system is limited by the availability of nucleophiles such as sulfate. Flow tube experiments were conducted to examine the role of iron in the reactive uptake and chemical oxidation of glycolaldehyde. Aerosol particles doped with iron and hydrogen peroxide were mixed with gas-phase glycolaldehyde and photochemically aged in a custom-built flow reactor. Compared to particles free of iron, iron-doped aerosols significantly enhanced the oxygen to carbon (O/C) ratio of accumulated organic mass. The primary oxidation mechanism is suggested to be a combination of Fenton and photo-Fenton reactions which enhance particle-phase OH radical concentrations.

A Numerical Study of Cirrus Clouds. Part I: Model Description.

NASA Astrophysics Data System (ADS)

Liu, Hui-Chun; Wang, Pao K.; Schlesinger, Robert E.

2003-04-01

This article, the first of a two-part series, presents a detailed description of a two-dimensional numerical cloud model directed toward elucidating the physical processes governing the evolution of cirrus clouds. The two primary scientific purposes of this work are (a) to determine the evolution and maintenance mechanisms of cirrus clouds and try to explain why some cirrus can persist for a long time; and (b) to investigate the influence of certain physical factors such as radiation, ice crystal habit, latent heat, ventilation effects, and aggregation mechanisms on the evolution of cirrus. The second part will discuss sets of model experiments that were run to address objectives (a) and (b), respectively.As set forth in this paper, the aforementioned two-dimensional numerical model, which comprises the research tool for this study, is organized into three modules that embody dynamics, microphysics, and radiation. The dynamic module develops a set of equations to describe shallow moist convection, also parameterizing turbulence by using a 1.5-order closure scheme. The microphysical module uses a double-moment scheme to simulate the evolution of the size distribution of ice particles. Heterogeneous and homogeneous nucleation of haze particles are included, along with other ice crystal processes such as diffusional growth, sedimentation, and aggregation. The radiation module uses a two-stream radiative transfer scheme to determine the radiative fluxes and heating rates, while the cloud optical properties are determined by the modified anomalous diffraction theory (MADT) for ice particles. One of the main advantages of this cirrus model is its explicit formulation of the microphysical and radiative properties as functions of ice crystal habit.

Cirrus cloud model parameterizations: Incorporating realistic ice particle generation

NASA Technical Reports Server (NTRS)

Sassen, Kenneth; Dodd, G. C.; Starr, David OC.

1990-01-01

Recent cirrus cloud modeling studies have involved the application of a time-dependent, two dimensional Eulerian model, with generalized cloud microphysical parameterizations drawn from experimental findings. For computing the ice versus vapor phase changes, the ice mass content is linked to the maintenance of a relative humidity with respect to ice (RHI) of 105 percent; ice growth occurs both with regard to the introduction of new particles and the growth of existing particles. In a simplified cloud model designed to investigate the basic role of various physical processes in the growth and maintenance of cirrus clouds, these parametric relations are justifiable. In comparison, the one dimensional cloud microphysical model recently applied to evaluating the nucleation and growth of ice crystals in cirrus clouds explicitly treated populations of haze and cloud droplets, and ice crystals. Although these two modeling approaches are clearly incompatible, the goal of the present numerical study is to develop a parametric treatment of new ice particle generation, on the basis of detailed microphysical model findings, for incorporation into improved cirrus growth models. For example, the relation between temperature and the relative humidity required to generate ice crystals from ammonium sulfate haze droplets, whose probability of freezing through the homogeneous nucleation mode are a combined function of time and droplet molality, volume, and temperature. As an example of this approach, the results of cloud microphysical simulations are presented showing the rather narrow domain in the temperature/humidity field where new ice crystals can be generated. The microphysical simulations point out the need for detailed CCN studies at cirrus altitudes and haze droplet measurements within cirrus clouds, but also suggest that a relatively simple treatment of ice particle generation, which includes cloud chemistry, can be incorporated into cirrus cloud growth.

Electroscavenging and Inferred Effects on Precipitation Efficiency

NASA Astrophysics Data System (ADS)

Tinsley, B. A.

2002-12-01

The evaporation of charged droplets leaves charged aerosol particles that can act as cloud condensation nuclei and ice forming nuclei. New calculations of scavenging of such charged particles by droplets have been made, that now include the effects of inertia and variable particle density, and variable cloud altitudes ranging into the stratosphere. They show that the Greenfield Gap closes for particles of low density, or for high altitude clouds, or for a few hundred elementary charges on the particles. A few tens of elementary charges on the particles gives collision efficiencies typically an order of magnitude greater than that due to phoretic forces alone. The numerical integrations show that electroscavenging of ice forming nuclei leading to contact ice nucleation is competitive with deposition ice nucleation, for cloud top temperatures in the range 0§C to -15§C and droplet size distributions extending past 10-15 mm radius. This implies that for marine stratocumulus or nimbostratus clouds with tops just below freezing temperature, where precipitation is initiated by the Wegener-Bergeron-Findeisen process, the precipitation efficiency can be affected by the amount of charge on the ice-forming nuclei. This in turn depends on the extent of the (weak) electrification of the cloud. Similarly, electroscavenging of condensation nuclei can increase the average droplet size in successive cycles of cloud evaporation and formation, and can also affect precipitation efficiency.

Aerosol Impacts on California Winter Clouds and Precipitation during CalWater 2011: Local Pollution versus Long-Range Transported Dust

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fan, Jiwen; Leung, Lai-Yung R.; DeMott, Paul J.

2014-01-03

Mineral dust aerosols often observed over California in winter and spring, associated with long-range transport from Asia and Sahara, have been linked to enhanced precipitation based on observations. Local anthropogenic pollution, on the other hand, was shown in previous observational and modeling studies to reduce precipitation. Here we incorporate recent developments in ice nucleation parameterizations to link aerosols with ice crystal formation in a spectral-bin cloud microphysical model coupled with the Weather Research and Forecasting (WRF) model, to examine the relative and combined impacts of dust and local pollution particles on cloud properties and precipitation type and intensity. Simulations aremore » carried out for two cloud cases with contrasting meteorology and cloud dynamics that occurred on February 16 (FEB16) and March 02 (MAR02) from the CalWater 2011 field campaign. In both cases, observations show the presence of dust and biological particles in a relative pristine environment. The simulated cloud microphysical properties and precipitation show reasonable agreement with aircraft and surface measurements. Model sensitivity experiments indicate that in the pristine environment, the dust and biological aerosol layers increase the accumulated precipitation by 10-20% from the Central Valley to the Sierra Nevada Mountains for both FEB16 and MAR02 due to a ~40% increase in snow formation, validating the observational hypothesis. Model results show that local pollution increases precipitation over the windward slope of the mountains by few percent due to increased snow formation when dust is present but reduces precipitation by 5-8% if dust is removed on FEB16. The effects of local pollution on cloud microphysics and precipitation strongly depend on meteorology including the strength of the Sierra Barrier Jet, and cloud dynamics. This study further underscores the importance of the interactions between local pollution, dust, and environmental conditions for assessing aerosol effects on cold season precipitation in California.« less

Model simulations with COSMO-SPECS: impact of heterogeneous freezing modes and ice nucleating particle types on ice formation and precipitation in a deep convective cloud

NASA Astrophysics Data System (ADS)

Diehl, Karoline; Grützun, Verena

2018-03-01

In deep convective clouds, heavy rain is often formed involving the ice phase. Simulations were performed using the 3-D cloud resolving model COSMO-SPECS with detailed spectral microphysics including parameterizations of homogeneous and three heterogeneous freezing modes. The initial conditions were selected to result in a deep convective cloud reaching 14 km of altitude with strong updrafts up to 40 m s-1. At such altitudes with corresponding temperatures below -40 °C the major fraction of liquid drops freezes homogeneously. The goal of the present model simulations was to investigate how additional heterogeneous freezing will affect ice formation and precipitation although its contribution to total ice formation may be rather low. In such a situation small perturbations that do not show significant effects at first sight may trigger cloud microphysical responses. Effects of the following small perturbations were studied: (1) additional ice formation via immersion, contact, and deposition modes in comparison to solely homogeneous freezing, (2) contact and deposition freezing in comparison to immersion freezing, and (3) small fractions of biological ice nucleating particles (INPs) in comparison to higher fractions of mineral dust INP. The results indicate that the modification of precipitation proceeds via the formation of larger ice particles, which may be supported by direct freezing of larger drops, the growth of pristine ice particles by riming, and by nucleation of larger drops by collisions with pristine ice particles. In comparison to the reference case with homogeneous freezing only, such small perturbations due to additional heterogeneous freezing rather affect the total precipitation amount. It is more likely that the temporal development and the local distribution of precipitation are affected by such perturbations. This results in a gradual increase in precipitation at early cloud stages instead of a strong increase at later cloud stages coupled with approximately 50 % more precipitation in the cloud center. The modifications depend on the active freezing modes, the fractions of active INP, and the composition of the internal mixtures in the drops.

Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alpert, Peter A.; Knopf, Daniel A.

Immersion freezing is an important ice nucleation pathway involved in the formation of cirrus and mixed-phase clouds. Laboratory immersion freezing experiments are necessary to determine the range in temperature, T, and relative humidity, RH, at which ice nucleation occurs and to quantify the associated nucleation kinetics. Typically, isothermal (applying a constant temperature) and cooling-rate-dependent immersion freezing experiments are conducted. In these experiments it is usually assumed that the droplets containing ice nucleating particles (INPs) all have the same INP surface area (ISA); however, the validity of this assumption or the impact it may have on analysis and interpretation of the experimentalmore » data is rarely questioned. Descriptions of ice active sites and variability of contact angles have been successfully formulated to describe ice nucleation experimental data in previous research; however, we consider the ability of a stochastic freezing model founded on classical nucleation theory to reproduce previous results and to explain experimental uncertainties and data scatter. A stochastic immersion freezing model based on first principles of statistics is presented, which accounts for variable ISA per droplet and uses parameters including the total number of droplets, N tot, and the heterogeneous ice nucleation rate coefficient, J het( T). This model is applied to address if (i) a time and ISA-dependent stochastic immersion freezing process can explain laboratory immersion freezing data for different experimental methods and (ii) the assumption that all droplets contain identical ISA is a valid conjecture with subsequent consequences for analysis and interpretation of immersion freezing. The simple stochastic model can reproduce the observed time and surface area dependence in immersion freezing experiments for a variety of methods such as: droplets on a cold-stage exposed to air or surrounded by an oil matrix, wind and acoustically levitated droplets, droplets in a continuous-flow diffusion chamber (CFDC), the Leipzig aerosol cloud interaction simulator (LACIS), and the aerosol interaction and dynamics in the atmosphere (AIDA) cloud chamber. Observed time-dependent isothermal frozen fractions exhibiting non-exponential behavior can be readily explained by this model considering varying ISA. An apparent cooling-rate dependence of J het is explained by assuming identical ISA in each droplet. When accounting for ISA variability, the cooling-rate dependence of ice nucleation kinetics vanishes as expected from classical nucleation theory. Finally, the model simulations allow for a quantitative experimental uncertainty analysis for parameters N tot, T, RH, and the ISA variability. We discuss the implications of our results for experimental analysis and interpretation of the immersion freezing process.« less

Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model

DOE PAGES

Alpert, Peter A.; Knopf, Daniel A.

2016-02-24

Immersion freezing is an important ice nucleation pathway involved in the formation of cirrus and mixed-phase clouds. Laboratory immersion freezing experiments are necessary to determine the range in temperature, T, and relative humidity, RH, at which ice nucleation occurs and to quantify the associated nucleation kinetics. Typically, isothermal (applying a constant temperature) and cooling-rate-dependent immersion freezing experiments are conducted. In these experiments it is usually assumed that the droplets containing ice nucleating particles (INPs) all have the same INP surface area (ISA); however, the validity of this assumption or the impact it may have on analysis and interpretation of the experimentalmore » data is rarely questioned. Descriptions of ice active sites and variability of contact angles have been successfully formulated to describe ice nucleation experimental data in previous research; however, we consider the ability of a stochastic freezing model founded on classical nucleation theory to reproduce previous results and to explain experimental uncertainties and data scatter. A stochastic immersion freezing model based on first principles of statistics is presented, which accounts for variable ISA per droplet and uses parameters including the total number of droplets, N tot, and the heterogeneous ice nucleation rate coefficient, J het( T). This model is applied to address if (i) a time and ISA-dependent stochastic immersion freezing process can explain laboratory immersion freezing data for different experimental methods and (ii) the assumption that all droplets contain identical ISA is a valid conjecture with subsequent consequences for analysis and interpretation of immersion freezing. The simple stochastic model can reproduce the observed time and surface area dependence in immersion freezing experiments for a variety of methods such as: droplets on a cold-stage exposed to air or surrounded by an oil matrix, wind and acoustically levitated droplets, droplets in a continuous-flow diffusion chamber (CFDC), the Leipzig aerosol cloud interaction simulator (LACIS), and the aerosol interaction and dynamics in the atmosphere (AIDA) cloud chamber. Observed time-dependent isothermal frozen fractions exhibiting non-exponential behavior can be readily explained by this model considering varying ISA. An apparent cooling-rate dependence of J het is explained by assuming identical ISA in each droplet. When accounting for ISA variability, the cooling-rate dependence of ice nucleation kinetics vanishes as expected from classical nucleation theory. Finally, the model simulations allow for a quantitative experimental uncertainty analysis for parameters N tot, T, RH, and the ISA variability. We discuss the implications of our results for experimental analysis and interpretation of the immersion freezing process.« less

Reconciling the aerosol-liquid water path relationship in the ECHAM6-HAM GCM and the Aerosol_cci/Cloud_cci (A)ATSR dataset by minimizing the effect of aerosol swelling

NASA Astrophysics Data System (ADS)

Neubauer, D.; Christensen, M.; Lohmann, U.; Poulsen, C. A.

2016-12-01

Studies using present day variability to assess statistical relationships between aerosol and cloud properties find different strengths of these relationships between satellite data and general circulation model (GCM) data. This discrepancy can be explained by structural uncertainties due to differences in the analysis/observational scale and the process scale or spurious relationships between aerosol and cloud properties. Such spurious relationships are the growth of aerosol particles in the humid environment surrounding clouds, misclassification of partly cloudy satellite pixels as cloud free pixels, brightening of aerosol particles by sunlight reflected at cloud edges, or effects of clouds on aerosol like processing of aerosol particles in clouds by nucleation or impact scavenging and subsequent growth by heterogeneous chemistry and release by cloud droplet evaporation or wet scavenging of aerosol particles. To minimize the effects of spatial aggregation and spurious relationships we apply a new nearest neighbour approach to high resolution (A)ATSR datasets from the Aerosol_cci and Cloud_cci projects of the Climate Change Initiative (CCI) programme of ESA. For the ECHAM6-HAM GCM we quantify the impact of using dry aerosol (without aerosol water) in the analysis to mimic the effect of the nearest neighbour approach. The aerosol-liquid water path relationship in ECHAM6-HAM is systematically stronger than in (A)ATSR data and cannot be explained by an overestimation of autoconversion when using diagnostic precipitation but rather by aerosol swelling in regions where humidity is high and clouds are present. When aerosol water is removed from the analysis in ECHAM6-HAM the strength of the aerosol-liquid water path relationship agrees much better with the ones of (A)ATSR or MODIS. We further find that while the observed relationships of different satellite sensors ((A)ATSR vs. MODIS) are not always consistent for tested environmental conditions the relationships in ECHAM6-HAM are missing a strong dependence on environmental conditions which is critical for bridging the gap between satellite and model estimates of aerosol indirect forcing.

Influence of surface morphology on the immersion mode ice nucleation efficiency of hematite particles

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Hoffmann, N.; Kiselev, A.; Dreyer, A.; Zhang, K.; Kulkarni, G.; Koop, T.; Möhler, O.

2014-03-01

In this paper, the effect of the morphological modification of aerosol particles with respect to heterogeneous ice nucleation is comprehensively investigated for laboratory-generated hematite particles as a model substrate for atmospheric dust particles. The surface-area-scaled ice nucleation efficiencies of monodisperse cubic hematite particles and milled hematite particles were measured with a series of expansion cooling experiments using the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud simulation chamber. Complementary offline characterization of physico-chemical properties of both hematite subsets were also carried out with scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, dynamic light scattering (DLS), and an electro-kinetic particle charge detector to further constrain droplet-freezing measurements of hematite particles. Additionally, an empirical parameterization derived from our laboratory measurements was implemented in the single-column version of the Community Atmospheric Model version 5 (CAM5) to investigate the model sensitivity in simulated ice crystal number concentration on different ice nucleation efficiencies. From an experimental perspective, our results show that the immersion mode ice nucleation efficiency of milled hematite particles is almost an order of magnitude higher at -35.2 °C < T < -33.5 °C than that of the cubic hematite particles, indicating a substantial effect of morphological irregularities on immersion mode freezing. Our modeling results similarly show that the increased droplet-freezing rates of milled hematite particles lead to about one order magnitude higher ice crystal number in the upper troposphere than cubic hematite particles. Overall, our results suggest that the surface irregularities and associated active sites lead to greater ice activation through droplet freezing.

Thermodynamic and Dynamic Aspects of Ice Nucleation

NASA Technical Reports Server (NTRS)

Barahona, Donifan

2018-01-01

It is known that ice nucleating particles (INP) immersed within supercooled droplets promote the formation of ice. Common theoretical models used to represent this process assume that the immersed particle lowers the work of ice nucleation without significantly affecting the dynamics of water in the vicinity of the particle. This is contrary to evidence showing that immersed surfaces significantly affect the viscosity and diffusivity of vicinal water. To study how this may affect ice formation this work introduces a model linking the ice nucleation rate to the modification of the dynamics and thermodynamics of vicinal water by immersed particles. It is shown that INP that significantly reduce the work of ice nucleation also pose strong limitations to the growth of the nascent ice germs. This leads to the onset of a new ice nucleation regime, called spinodal ice nucleation, where the dynamics of ice germ growth instead of the ice germ size determines the nucleation rate. Nucleation in this regime is characterized by an enhanced sensitivity to particle area and cooling rate. Comparison of the predicted ice nucleation rate against experimental measurements for a diverse set of species relevant to cloud formation suggests that spinodal ice nucleation may be common in nature.

Zinc Nucleation and Growth in Microgravity

NASA Technical Reports Server (NTRS)

Michael, B. Patrick; Nuth, J. A., III; Lilleleht, L. U.; Vondrak, Richard R. (Technical Monitor)

2000-01-01

We report our experiences with zinc nucleation in a microgravity environment aboard NASA's Reduced Gravity Research Facility. Zinc vapor is produced by a heater in a vacuum chamber containing argon gas. Nucleation is induced by cooling and its onset is easily detected visually by the appearance of a cloud of solid, at least partially crystalline zinc particles. Size distribution of these particles is monitored in situ by photon correlation spectroscopy. Samples of particles are also extracted for later analysis by SEM. The initially rapid increase in particle size is followed by a slower period of growth. We apply Scaled Nucleation Theory to our data and find that the derived critical temperature of zinc, the critical cluster size at nucleation, and the surface tension values are all in reasonably good agreement with their accepted literature values.

Carbon Dioxide Clouds at High Altitude in the Tropics and in an Early Dense Martian Atmosphere

NASA Technical Reports Server (NTRS)

Colaprete, Anthony; Toon, Owen B.

2001-01-01

We use a time dependent, microphysical cloud model to study the formation of carbon dioxide clouds in the Martian atmosphere. Laboratory studies by Glandor et al. show that high critical supersaturations are required for cloud particle nucleation and that surface kinetic growth is not limited. These conditions, which are similar to those for cirrus clouds on Earth, lead to the formation of carbon dioxide ice particles with radii greater than 500 micrometers and concentrations of less than 0.1 cm(exp -3) for typical atmospheric conditions. Within the current Martian atmosphere, CO2 cloud formation is possible at the poles during winter and at high altitudes in the tropics during periods of increased atmospheric dust loading. In both cases, temperature perturbations of several degrees below the CO2 saturation temperature are required to nucleate new cloud particles suggesting that dynamical processes are the most common initiators of carbon dioxide clouds rather than diabatic cooling. The microphysical cloud model, coupled to a two-stream radiative transfer model, is used to reexamine the impact of CO2 clouds on the surface temperature within a dense CO2 atmosphere. The formation of carbon dioxide clouds leads to a warmer surface than what would be expected for clear sky conditions. The amount of warming is sensitive to the presence of dust and water vapor in the atmosphere, both of which act to dampen cloud effects. The radiative warming associated with cloud formation, as well as latent heating, work to dissipate the clouds when present. Thus, clouds never last for periods much longer than several days, limiting their overall effectiveness for warming the surface. The time average cloud optical depth is approximately unity leading to a 5-10 K warming, depending on the surface pressure. However, the surface temperature does not rise about the freezing point of liquid water even for pressures as high as 5 bars, at a solar luminosity of 75% the current value.

Differences in ice nucleation behavior of arable and desert soil dust in deposition nucleation regime

NASA Astrophysics Data System (ADS)

Ullrich, Romy; Vogel, Franziska; Möhler, Ottmar; Höhler, Kristina; Schiebel, Thea

2017-04-01

Soil dust from arid and semi-arid regions is one of the most abundant aerosol types in the atmosphere with emission rates of about 1600 Tg per year (Andreae et al. (2009)). Therewith, soil dust plays an important role for the atmospheric radiative transfer and also for the formation of clouds. Soil dust refers to dust sampled from agricultural used areas, to dust from bare soil as well as to dust from desert regions. By mass-spectrometric measurements of the chemical composition of ice residuals, mineral dust as component of soil dust was found to be the major heterogeneous ice nucleating particle (INP) type (e.g. Cziczo et al. (2013)), in particular in the upper troposphere. Also in laboratory studies the ice nucleation efficiency of the different soil dusts was investigated. It was shown that desert dusts (Ullrich et al. (2017)) as well as soil dusts from arable regions (O'Sullivan et al. (2014), Tobo et al. (2014)) are efficient INP. However, there is still a lack of data for ice nucleation on soil dusts for temperatures below about 220 K. With the AIDA (Aerosol Interactions and Dynamics in the Atmosphere) cloud chamber, we are able to characterize the ice nucleation efficiency for different aerosol types to temperatures down to 180 K and high ice supersaturations. In order to extend the already existing AIDA data base for deposition nucleation on desert dusts and agricultural soil dusts, new experiments were done in the upper tropospheric temperature regime. This contribution will show the results of the new experiments with desert dust in comparison to existing data for higher temperatures. The first data analysis confirms the temperature dependent trend of the ice nucleation activity as discussed and parameterized in a recent paper by Ullrich et al. (2017). Furthermore, the update and extension of the recently published parameterization of deposition nucleation for desert dust to lower temperatures will be discussed. The experiments with agricultural soil dust will be compared to existing AIDA experiments at higher temperatures published by Steinke et al. (2016). Finally, the ice nucleation activity of both desert dust and agricultural soil dust will be compared for the upper tropospheric temperature regime. Andreae et al. (2009), Sources and Nature of Atmospheric Aerosols, in Aerosol Pollution Impact on Precipitation - A Scientific Review, Ch.3, Springer Netherlands, 45-89 Cziczo et al. (2013), Clarifying the Dominant Sources and Mechanisms of Cirrus Cloud Formation, Science, 340, 1320-1324 O'Sullivan et al. (2014), Ice nucleation by fertile soil dusts: relative importance of mineral and biogenic components, Atmos. Chem. Phys., 14, 1853-1867 Steinke et al. (2016), Ice nucleation activity of agricultural soil dust aerosols from Mongolia, Argentina and Germany, J. Geophys. Res., 121 Tobo et al. (2014), Organic matter matters for ice nuclei of agricultural soil origin, Atmos. Chem. Phys., 14, 8521-8531 Ullrich et al. (2017), A new ice nucleation active site parametrization for desert dust and soot, J. Atmos. Sci., in press

Development of a continuous flow thermal gradient diffusion chamber for ice nucleation studies

NASA Astrophysics Data System (ADS)

Rogers, David C.

A supercooled continuous flow, thermal gradient diffusion chamber has been developed to study the ice nucleating properties of natural or artificial aerosols. The chamber has concentric cylinder geometry with the cylinder axis alignment and airflow vertically downward. Sample airflow is 1 l min -1 and occupies the central 10% of the annular lamina; it is separated from the ice-covered walls by filtered sheath air. The wall temperatures are independently controlled over the range from about -4°C to -25°C, so that the vapor concentration at the location of the sample lamina can be set to a well defined value between ice saturation and a few percent water supersaturation. There is a range of temperature and supersaturation values across the sample region; for lamina center conditions of -15°C and +1% with respect to water, the range is -14.6 to -15.4°C and +0.53 to +1.31%. Errors in temperature control produce variations estimated as ±0.1°C and ±0.23%. Typical sample residence time is about 10 s. Ice crystals which form on active nuclei are detected optically at the outlet end of the chamber. To enhance the size difference between ice crystals and cloud droplets, the downstream 25% of the warm ice wall is covered with a thermally insulating vapor barrier which reduces the vapor concentration to ice saturation at the cold wall temperature, so cloud droplets evaporate. A mathematical model was developed to describe the temperature and vapor fields and to calculate the growth, evaporation, and sedimentation of water and ice particles. At 1% water supersaturation, the model predicts that ice particles will grow to about 5 μm diameter, and cloud droplets will achieve about 1 μm before they reach the evaporation section of the chamber. A different model was developed to describe the steady state airflow profile and location of the sample lamina. Experimental tests of the chamber were performed to characterize the airflow, to assess the ability of the technique to detect silver iodide ice nucleating aerosols and to distinguish ice crystals from water droplets.

TOWARDS ICE FORMATION CLOSURE IN MIXED-PHASE BOUNDARY LAYER CLOUDS DURING ISDAC

NASA Astrophysics Data System (ADS)

Avramov, A.; Ackerman, A. S.; Fridlind, A. M.; van Diedenhoven, B.; Korolev, A. V.

2009-12-01

Mixed-phase stratus clouds are ubiquitous in the Arctic during the winter and transition seasons. Despite their important role in various climate feedback mechanisms they are not well understood and are difficult to represent faithfully in cloud models. In particular, models of all types experience difficulties reproducing observed ice concentrations and liquid/ice water partitioning in these clouds. Previous studies have demonstrated that simulated ice concentrations and ice water content are critically dependent on ice nucleation modes and ice crystal habit assumed in simulations. In this study we use large-eddy simulations with size-resolved microphysics to determine whether uncertainties in ice nucleus concentrations, ice nucleation mechanisms, ice crystal habits and large-scale forcing are sufficient to account for the difference between simulated and observed quantities. We present results of simulations of two case studies based on observations taken during the recent Indirect and Semi-Direct Aerosol Campaign (ISDAC) on April 8 and 26, 2008. The model simulations are evaluated through extensive comparison with in-situ observations and ground-based remote sensing measurements.

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

NASA Astrophysics Data System (ADS)

DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.; Sullivan, R. C.; Petters, M. D.; Tobo, Y.; Niemand, M.; Möhler, O.; Snider, J. R.; Wang, Z.; Kreidenweis, S. M.

2014-06-01

Data from both laboratory studies and atmospheric measurements are used to develop a simple parametric description for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RHw) are taken to approximate the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A correction factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RHw of 105% vs. maximum fractions active at higher RHw. Instrumental factors that affect activation behavior vs. RHw in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this correction factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization to the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically-relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first order approximation in numerical modeling investigations.

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

NASA Astrophysics Data System (ADS)

DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.; Sullivan, R. C.; Petters, M. D.; Tobo, Y.; Niemand, M.; Möhler, O.; Snider, J. R.; Wang, Z.; Kreidenweis, S. M.

2015-01-01

Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RHw) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RHw of 105% vs. maximum fractions active at higher RHw. Instrumental factors that affect activation behavior vs. RHw in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

DOE PAGES

DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.; ...

2014-06-27

Data from both laboratory studies and atmospheric measurements are used to develop a simple parametric description for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RH w) are taken to approximate the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterizationmore » developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A correction factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RH w of 105% vs. maximum fractions active at higher RH w. Instrumental factors that affect activation behavior vs. RH w in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this correction factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization to the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically-relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first order approximation in numerical modeling investigations.« less

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

DOE PAGES

DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.; ...

2015-01-13

Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RH w) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. Themore » parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RH w of 105% vs. maximum fractions active at higher RH w. Instrumental factors that affect activation behavior vs. RH w in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.« less

Meteorological assessment of SRM exhaust products' environmental impact

NASA Technical Reports Server (NTRS)

Dingle, A. N.

1982-01-01

The environmental impact of solid rocket motor (SRM) exhaust products discharged into the free air stream upon the launching of space vehicles that depend upon SRM boosters to obtain large thrust was assessed. The emission of Al2O3 to the troposphere from the SRMs in each Shuttle launch is considered. The Al2O3 appears as particles suitable for heterogeneous nucleation of hydrochloric acid which under frequently occurring atmospheric conditions may form a highly acidic rain capable of damaging property and crops and of impacting upon the health of human and animal populations. The cloud processes leading to the formation of acid rain and the concentration of the acid that then reaches the ground, and the atmospheric situations that lead to the production of cloud and rain at and near a launch site, and the prediction of weather conditions that may permit or prohibit a launch operation are studied.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew T.

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA–soot biogenic–anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfatemore » mixtures exhibit a core–shell configuration (i.e.a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respectiveT gand FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Charnawskas, Joseph C.; Alpert, Peter A.; Lambe, Andrew

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil-fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without presence of sulfate or soot particles. Corresponding particle glass transition (T g) and full deliquescence relative humidity (FDRH) were estimated by a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibitmore » a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid inducing ice nucleation. Naphthalene SOA coated soot particles acted as IN above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate further renders this even less likely. Furthermore, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during preindustrial times or in pristine areas.« less

Micro-Spectroscopic Chemical Imaging of Individual Identified Marine Biogenic and Ambient Organic Ice Nuclei (Invited)

NASA Astrophysics Data System (ADS)

Knopf, D. A.; Alpert, P. A.; Wang, B.; OBrien, R. E.; Moffet, R. C.; Aller, J. Y.; Laskin, A.; Gilles, M.

2013-12-01

Atmospheric ice formation represents one of the least understood atmospheric processes with important implications for the hydrological cycle and climate. Current freezing descriptions assume that ice active sites on the particle surface initiate ice nucleation, however, the nature of these sites remains elusive. Here, we present a new experimental method that allows us to relate physical and chemical properties of individual particles with observed water uptake and ice nucleation ability using a combination of micro-spectroscopic and optical single particle analytical techniques. We apply this method to field-collected particles and particles generated via bursting of bubbles produced by glass frit aeration and plunging water impingement jets in a mesocosm containing artificial sea water and bacteria and/or phytoplankton. The most efficient ice nuclei (IN) within a particle population are identified and characterized. Single particle characterization is achieved by computer controlled scanning electron microscopy with energy dispersive analysis of X-rays (CCSEM/EDX) and scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy. A vapor controlled cooling-stage coupled to an optical microscope is used to determine the onsets of water uptake, immersion freezing, and deposition ice nucleation of the individual particles as a function of temperature (T) as low as 200 K and relative humidity (RH) up to water saturation. In addition, we perform CCSEM/EDX to obtain on a single particle level the elemental composition of the entire particle population. Thus, we can determine if the IN are exceptional in nature or belong to a major particle type class with respect to composition and size. We find that ambient and sea spray particles are coated by organic material and can induce ice formation under tropospheric relevant conditions. Micro-spectroscopic single particle analysis of the investigated particle samples invokes a potential paradigm shift: Individual ice nucleating particle composition indicates that IN are similar to the majority of particles in the population and not exceptional. This suggests that composition alone may not be a determinant for IN identification. Furthermore, the results suggest that particle abundance may be a crucial parameter for IN efficiency when predicting cloud glaciation processes. These findings would have important consequences for cloud modeling, laboratory ice nucleation experiments, and field measurements.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Jian; Krejci, Radovan; Giangrande, Scott

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- andmore » ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. Lastly, this rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.« less

The Fifth International Ice Nucleation Workshop Activities FIN-1 and FIN-2: Overview and Selected Results

NASA Astrophysics Data System (ADS)

Moehler, O.; Cziczo, D. J.; DeMott, P. J.; Hiranuma, N.; Petters, M. D.

2015-12-01

The role of aerosol particles for ice formation in clouds is one of the largest uncertainties in understanding the Earth's weather and climate systems, which is related to the poor knowledge of ice nucleation microphysics or of the nature and atmospheric abundance of ice nucleating particles (INPs). During the recent years, new mobile instruments were developed for measuring the concentration, size and chemical composition of INPs, which were tested during the three-part Fifth International Ice Nucleation (FIN) workshop. The FIN activities addressed not only instrument issues, but also important science topics like the nature of atmospheric INP and cloud ice residuals, the ice nucleation activity of relevant atmospheric aerosols, or the parameterization of ice formation in atmospheric weather and climate models. The first activity FIN-1 was conducted during November 2014 at the AIDA cloud chamber. It involved co-locating nine single particle mass spectrometers to evaluate how well they resolve the INP and ice residual composition and how spectra from different instruments compare for relevant atmospheric aerosols. We conducted about 90 experiments with mineral, carbonaceous and biological aerosol types, some also coated with organic and inorganic compounds. The second activity FIN-2 was conducted during March 2015 at the AIDA facility. A total of nine mobile INP instruments directly sampled from the AIDA aerosol chambers. Wet suspension and filter samples were also taken for offline INP processing. A refereed blind intercomparison was conducted during two days of the FIN-2 activity. The third activity FIN-3 will take place at the Desert Research Institute's Storm Peak Laboratory (SPL) in order to test the instruments' performance in the field. This contribution will introduce the FIN activities, summarize first results from the formal part of FIN-2, and discuss selected results, mainly from FIN-1 for the effect of coating on the ice nucleation (IN) by mineral aerosols. The coating with both secondary organic compounds and sulphuric acid was conducted in the AIDA chamber at relevant temperatures and precursor concentrations and was monitored with the particle mass spectrometers. Already very thin, atmospherically relevant coatings reduced deposition IN, but had little effect on immersion freezing.

Chemical Characterization of Individual Particles and Residuals of Cloud Droplets and Ice Crystals Collected On Board Research Aircraft in the ISDAC 2008 Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hiranuma, Naruki; Brooks, Sarah D.; Moffet, Ryan C.

2013-06-24

Although it has been shown that size of atmospheric particles has a direct correlation with their ability to act as cloud droplet and ice nuclei, the influence of composition of freshly emitted and aged particles in nucleation processes is poorly understood. In this work we combine data from field measurements of ice nucleation with chemical imaging of the sampled particles to link aerosol composition with ice nucleation ability. Field measurements and sampling were conducted during the Indirect and Semidirect Aerosols Campaign (ISDAC) over Barrow, Alaska, in the springtime of 2008. In-situ ice nucleation measurements were conducted using a Continuous Flowmore » Diffusion Chamber (CFDC). Measured number concentrations of ice nuclei (IN) varied from frequent values of 0.01 per liter to more than 10 per liter. Residuals of airborne droplets and ice crystals were collected through a counterflow virtual impactor (CVI). The compositions of individual atmospheric particles and the residuals were studied using Computer Controlled Scanning Electron Microscopy with Energy Dispersive X-ray analysis (CCSEM/EDX) and Scanning Transmission X-ray Microscopy coupled with Near Edge X-ray Absorption Fine Structure spectroscopy (STXM/NEXAFS). Chemical analysis of cloud particle residuals collected during an episode of high ice nucleation suggests that both size and composition may influence aerosol's ability to act as IN. The STXM/NEXAFS chemical composition maps of individual residuals have characteristic structures of either inorganic or black carbon cores coated by organic materials. In a separate flight, particle samples from a biomass burning plume were collected. Although it has previously been suggested that episodes of biomass burning contribute to increased numbers of highly effective ice nuclei, in this episode we observed that only a small fraction were effective ice nuclei. Most of the particles from the biomass plume episode were smaller in size and were composed of homogeneous organic material without identifiable cores.« less

The ice nucleation activity of biological aerosols

NASA Astrophysics Data System (ADS)

Grothe, H.; Pummer, B.; Bauer, H.; Bernardi, J.

2012-04-01

Primary Biological Aerosol Particles (PBAPs), including bacteria, spores and pollen may be important for several atmospheric processes. Particularly, the ice nucleation caused by PBAPs is a topic of growing interest, since their impact on ice cloud formation and thus on radiative forcing, an important parameter in global climate is not yet fully understood. In laboratory model studies we investigated the ice nucleation activity of selected PBAPs. We studied the immersion mode freezing using water-oil emulsion, which we observed by optical microscopy. We particularly focused on pollen. We show that pollen of different species strongly differ in their ice nucleation behavior. The average freezing temperatures in laboratory experiments range from 240 K to 255 K. As the most efficient nuclei (silver birch, Scots pine and common juniper pollen) have a distribution area up to the Northern timberline, their ice nucleation activity might be a cryoprotective mechanism. For comparison the ice nucleation activity of Snomax, fungal spores, and mushrooms will be discussed as well. In the past, pollen have been rejected as important atmospheric IN, as they are not as abundant in the atmosphere as bacteria or mineral dust and are too heavy to reach higher altitudes. However, in our experiments (Pummer et al. 2011) it turned out that water, which had been in contact with pollen and then been separated from the bodies, nucleates as good as the pollen grains themselves. So the ice nuclei have to be easily-suspendable macromolecules (100-300 kDa) located on the pollen. Once extracted, they can be distributed further through the atmosphere than the heavy pollen grains and so augment the impact of pollen on ice cloud formation even in the upper troposphere. It is widely known, that material from the pollen, like allergens and sugars, can indeed leave the pollen body and be distributed independently. The most probable mechanism is the pollen grain bursting by rain, which releases material, like allergens (Schäppi et al., 1999). As a consequence allergenic material was found in aerosol particles smaller than 5 µm, which contained no pollen or bigger fragments (Solomon et al., 1983). The release of material by bursting of wet pollen has been observed by electron microscopy (Swoboda et al., 2001). Not only allergens, but also sugars originating from pollen can be detected in the atmosphere (Yttri et al., 2007). These authors see pollen rupture and wood burning as their main sources in the atmosphere. The contrast between the hydrophilic properties of many of the surface components and the relative hydrophobia of the sporopollenin boosts the suspension of surface components in water droplets. According to that we conclude that the impact of pollen on the global atmosphere might have been underestimated. Additionally, our experiments lead to the conclusion that pollen ice nuclei, in contrast to bacterial and fungal ice nucleating proteins, are non-proteinaceous compounds.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhukhovitskii, D. I., E-mail: dmr@ihed.ras.ru

The vapor–liquid nucleation in a dense Lennard-Jones system is studied analytically and numerically. A solution of the nucleation kinetic equations, which includes the elementary processes of condensation/evaporation involving the lightest clusters, is obtained, and the nucleation rate is calculated. Based on the equation of state for the cluster vapor, the pre-exponential factor is obtained. The latter diverges as a spinodal is reached, which results in the nucleation enhancement. The work of critical cluster formation is calculated using the previously developed two-parameter model (TPM) of small clusters. A simple expression for the nucleation rate is deduced and it is shown thatmore » the work of cluster formation is reduced for a dense vapor. This results in the nucleation enhancement as well. To verify the TPM, a simulation is performed that mimics a steady-state nucleation experiments in the thermal diffusion cloud chamber. The nucleating vapor with and without a carrier gas is simulated using two different thermostats for the monomers and clusters. The TPM proves to match the simulation results of this work and of other studies.« less

Rate of Homogenous Nucleation of Ice in Supercooled Water.

PubMed

Atkinson, James D; Murray, Benjamin J; O'Sullivan, Daniel

2016-08-25

The homogeneous freezing of water is of fundamental importance to a number of fields, including that of cloud formation. However, there is considerable scatter in homogeneous nucleation rate coefficients reported in the literature. Using a cold stage droplet system designed to minimize uncertainties in temperature measurements, we examined the freezing of over 1500 pure water droplets with diameters between 4 and 24 μm. Under the assumption that nucleation occurs within the bulk of the droplet, nucleation rate coefficients fall within the spread of literature data and are in good agreement with a subset of more recent measurements. To quantify the relative importance of surface and volume nucleation in our experiments, where droplets are supported by a hydrophobic surface and surrounded by oil, comparison of droplets with different surface area to volume ratios was performed. From our experiments it is shown that in droplets larger than 6 μm diameter (between 234.6 and 236.5 K), nucleation in the interior is more important than nucleation at the surface. At smaller sizes we cannot rule out a significant contribution of surface nucleation, and in order to further constrain surface nucleation, experiments with smaller droplets are necessary. Nevertheless, in our experiments, it is dominantly volume nucleation controlling the observed nucleation rate.

Clouds, Aerosol, and Precipitation in the Marine Boundary Layer: An ARM Mobile Facility Deployment

NASA Technical Reports Server (NTRS)

Wood, Robert; Wyant, Matthew; Bretherton, Christopher S.; Remillard, Jasmine; Kollias, Pavlos; Fletcher, Jennifer; Stemmler, Jayson; de Szoeke, Simone; Yuter, Sandra; Miller, Matthew;

A Dynamic Model for Forecasting New Cloud Development

DTIC Science & Technology

1988-12-19

Fourseand Vefor cay 2,or at our0 LT~ Z7 :rZ198 -’ut l o b o u d r f ro m sh o we a ct v t na o t h o t he a lm i 13 in di c at ed Or-& I W PFA ,.M...nucleation model includes: sorption /deposition, contact nucleation by Brownian collision plus thermophoresis plus diffusiophoresis, secondary ice

Two-moment bulk stratiform cloud microphysics in the GFDL AM3 GCM: description, evaluation, and sensitivity tests

NASA Astrophysics Data System (ADS)

Salzmann, M.; Ming, Y.; Golaz, J.-C.; Ginoux, P. A.; Morrison, H.; Gettelman, A.; Krämer, M.; Donner, L. J.

2010-08-01

A new stratiform cloud scheme including a two-moment bulk microphysics module, a cloud cover parameterization allowing ice supersaturation, and an ice nucleation parameterization has been implemented into the recently developed GFDL AM3 general circulation model (GCM) as part of an effort to treat aerosol-cloud-radiation interactions more realistically. Unlike the original scheme, the new scheme facilitates the study of cloud-ice-aerosol interactions via influences of dust and sulfate on ice nucleation. While liquid and cloud ice water path associated with stratiform clouds are similar for the new and the original scheme, column integrated droplet numbers and global frequency distributions (PDFs) of droplet effective radii differ significantly. This difference is in part due to a difference in the implementation of the Wegener-Bergeron-Findeisen (WBF) mechanism, which leads to a larger contribution from super-cooled droplets in the original scheme. Clouds are more likely to be either completely glaciated or liquid due to the WBF mechanism in the new scheme. Super-saturations over ice simulated with the new scheme are in qualitative agreement with observations, and PDFs of ice numbers and effective radii appear reasonable in the light of observations. Especially, the temperature dependence of ice numbers qualitatively agrees with in-situ observations. The global average long-wave cloud forcing decreases in comparison to the original scheme as expected when super-saturation over ice is allowed. Anthropogenic aerosols lead to a larger decrease in short-wave absorption (SWABS) in the new model setup, but outgoing long-wave radiation (OLR) decreases as well, so that the net effect of including anthropogenic aerosols on the net radiation at the top of the atmosphere (netradTOA = SWABS-OLR) is of similar magnitude for the new and the original scheme.

Two-moment bulk stratiform cloud microphysics in the GFDL AM3 GCM: description, evaluation, and sensitivity tests

NASA Astrophysics Data System (ADS)

Salzmann, M.; Ming, Y.; Golaz, J.-C.; Ginoux, P. A.; Morrison, H.; Gettelman, A.; Krämer, M.; Donner, L. J.

2010-03-01

A new stratiform cloud scheme including a two-moment bulk microphysics module, a cloud cover parameterization allowing ice supersaturation, and an ice nucleation parameterization has been implemented into the recently developed GFDL AM3 general circulation model (GCM) as part of an effort to treat aerosol-cloud-radiation interactions more realistically. Unlike the original scheme, the new scheme facilitates the study of cloud-ice-aerosol interactions via influences of dust and sulfate on ice nucleation. While liquid and cloud ice water path associated with stratiform clouds are similar for the new and the original scheme, column integrated droplet numbers and global frequency distributions (PDFs) of droplet effective radii differ significantly. This difference is in part due to a difference in the implementation of the Wegener-Bergeron-Findeisen (WBF) mechanism, which leads to a larger contribution from super-cooled droplets in the original scheme. Clouds are more likely to be either completely glaciated or liquid due to the WBF mechanism in the new scheme. Super-saturations over ice simulated with the new scheme are in qualitative agreement with observations, and PDFs of ice numbers and effective radii appear reasonable in the light of observations. Especially, the temperature dependence of ice numbers qualitatively agrees with in-situ observations. The global average long-wave cloud forcing decreases in comparison to the original scheme as expected when super-saturation over ice is allowed. Anthropogenic aerosols lead to a larger decrease in short-wave absorption (SWABS) in the new model setup, but outgoing long-wave radiation (OLR) decreases as well, so that the net effect of including anthropogenic aerosols on the net radiation at the top of the atmosphere (netradTOA = SWABS-OLR) is of similar magnitude for the new and the original scheme.

The Importance of Habit Evolution for Maintaining Supercooled Liquid in Arctic Clouds

NASA Astrophysics Data System (ADS)

Sulia, K. J.; Harrington, J. Y.

2010-12-01

Low-level clouds cover large sections of the Arctic for much of the year, and these clouds are generally composed of supercooled liquid and contain regions of ice. These supercooled liquid clouds can persist for long periods of time with a large spatial extent. What are not well understood are the mechanisms whereby these clouds are able to maintain a supercooled liquid state rather than dissipating through the Bergeron mechanism, or the process by which ice crystals grow at the expense of liquid drops, with ice precipitation leading to cloud dissipation. Most prior research has focused on ice nucleation as providing a critical, first-order control on the glaciation rates of supercooled Arctic clouds. Ice nucleation is critical for its control over ice concentration, which then feeds into liquid depletion through its influence on the total ice mass growth rates. In addition, ice particle habit evolution can also strongly affect ice mass; however, the vapor growth rates based on habit evolution are routinely ignored in most mixed-phase methods. Most prior studies assume simple shapes or spheres as a proxy for ice habits. Recent studies have suggested that these simplified methods produce large uncertainties in estimates of the vapor growth rates, and hence the rate of glaciation, in supercooled clouds. Our studies show that these uncertainties are due to the inability of most models to predict ice particle aspect ratio. We therefore present results that help clarify the influence of ice habit on glaciation. We show that habit prediction is critical for estimates of glaciation in supercooled clouds, and that this is most important when ice concentrations are relatively low, as they appear to be in the Arctic.

Immersion and contact freezing experiments in the Mainz wind tunnel laboratory

NASA Astrophysics Data System (ADS)

Eppers, Oliver; Mayer, Amelie; Diehl, Karoline; Mitra, Subir; Borrmann, Stephan; Szakáll, Miklós

2016-04-01

Immersion and contact freezing are of outmost important ice nucleation processes in mixed phase clouds. Experimental studies are carried out in the Mainz vertical wind tunnel laboratory in order to characterize these nucleation processes for different ice nucleating particles (INP), such as for mineral dust or biological particles. Immersion freezing is investigated in our laboratory with two different experimental techniques, both attaining contact-free levitation of liquid droplets and cooling of the surrounding air down to about -25 °C. In an acoustic levitator placed in the cold room of our laboratory, drops with diameters of 2 mm are investigated. In the vertical air stream of the wind tunnel droplets with diameter of 700 micron are freely floated at their terminal velocities, simulating the flow conditions of the free atmosphere. Furthermore, the wind tunnel offers a unique platform for contact freezing experiments. Supercooled water droplets are floated in the vertical air stream at their terminal velocities and INP are injected into the tunnel air stream upstream of them. As soon as INP collides with the supercooled droplet the contact freezing is initiated. The first results of immersion and contact freezing experiments with cellulose particles both in the acoustic levitator and in the wind tunnel will be presented. Cellulose is considered as typical INP of biological origin and a macrotracer for plant debris. Nucleating properties of cellulose will be provided, mainly focusing on the temperature, INP concentration, and specific surface area dependences of the freezing processes. Direct comparison between the different experimental techniques (acoustic levitator and wind tunnel), as well as between nucleation modes (immersion and contact freezing) will be presented. The work is carried out within the framework of the German research unit INUIT.

A study of cloud microphysics and precipitation over the Tibetan Plateau by radar observations and cloud-resolving model simulations: Cloud Microphysics over Tibetan Plateau

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Wenhua; Sui, Chung-Hsiung; Fan, Jiwen

Cloud microphysical properties and precipitation over the Tibetan Plateau (TP) are unique because of the high terrains, clean atmosphere, and sufficient water vapor. With dual-polarization precipitation radar and cloud radar measurements during the Third Tibetan Plateau Atmospheric Scientific Experiment (TIPEX-III), the simulated microphysics and precipitation by the Weather Research and Forecasting model (WRF) with the Chinese Academy of Meteorological Sciences (CAMS) microphysics and other microphysical schemes are investigated through a typical plateau rainfall event on 22 July 2014. Results show that the WRF-CAMS simulation reasonably reproduces the spatial distribution of 24-h accumulated precipitation, but has limitations in simulating time evolutionmore » of precipitation rates. The model-calculated polarimetric radar variables have biases as well, suggesting bias in modeled hydrometeor types. The raindrop sizes in convective region are larger than those in stratiform region indicated by the small intercept of raindrop size distribution in the former. The sensitivity experiments show that precipitation processes are sensitive to the changes of warm rain processes in condensation and nucleated droplet size (but less sensitive to evaporation process). Increasing droplet condensation produces the best area-averaged rain rate during weak convection period compared with the observation, suggesting a considerable bias in thermodynamics in the baseline simulation. Increasing the initial cloud droplet size causes the rain rate reduced by half, an opposite effect to that of increasing droplet condensation.« less

Org Areo Boreal Forest Sources, compositions and properties of newly formed and regional organic aerosol in a boreal forest during the Biogenic Aerosol: Effects on Clouds and Climate Campaign

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thornton, Joel A

The major goals of this project were to make unique measurements, as part of the DOE sponsored Biogenic Aerosol Effects on Clouds and Climate (BAECC) campaign, of the volatility and molecular composition of organic aerosol, as well as gas-phase concentrations of oxygenated organic compounds that interact and affect organic aerosol. In addition, we aimed to conduct a similar set of measurements as part of a collaborative set of environmental simulation chamber experiments at PNNL, the aim of which was to simulate the atmospheric oxidation of key biogenic volatile organic compounds (BVOC) and study the associated formation and evolution of secondarymore » organic aerosol (SOA). The target BVOC were a set of monoterpenes, isoprene, and related intermediates such as IEPOX. The ultimate goal of such measurements are to develop a more detailed mechanistic understanding of the sensitivity of SOA mass formation and lifetime to precursor and environmental conditions. Molecular composition and direct volatility measurements provide robust tracers of chemical processing and properties. As such, meeting these goals will allow for stronger constraints on the types of processes and their fundamental descriptions needed to simulate aerosol particle number and size, and cloud nucleating ability in regional and global earth system models.« less

Long-Term INP Measurements within the BACCHUS project

NASA Astrophysics Data System (ADS)

Schrod, Jann; Bingemer, Heinz; Curtius, Joachim

2016-04-01

The European research project BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) studies the interactions between aerosols, clouds and the climate system, and tries to reconstruct pre-industrial aerosol and cloud conditions from data collected in pristine environments. The number concentration of Ice Nucleating Particles (INP) is an important, yet scarcely known parameter. As a partner of Work package 1 of BACCHUS we began in September 2014 to operate a globally spanned network of four INP sampling stations, which is the first of its kind. The stations are located at the ATTO observatory in the Brazilian Rainforest, the Caribbean Sea (Martinique), the Zeppelin Observatory at Svalbard in the Arctic, and in central Europe (Germany). Samples are collected routinely every day or every few days by electrostatic precipitation of aerosol particles onto Si substrates. The samples are stored in petri-slides, and shipped to our laboratory in Frankfurt, Germany. The number of ice nucleating particles on the substrate is analyzed in the isothermal static diffusion chamber FRIDGE by growing ice on the INP and photographing and counting the crystals. The measurements in the temperature range from -20°C to -30°C and relative humidities of 100-135% (with respect to ice) address primarily the deposition/condensation nucleation modes. Here we present INP and supporting aerosol data from this novel INP network for the first time.

Homogenous Surface Nucleation of Solid Polar Stratospheric Cloud Particles

NASA Technical Reports Server (NTRS)

Tabazadeh, A.; Hamill, P.; Salcedo, D.; Gore, Warren J. (Technical Monitor)

2002-01-01

A general surface nucleation rate theory is presented for the homogeneous freezing of crystalline germs on the surfaces of aqueous particles. While nucleation rates in a standard classical homogeneous freezing rate theory scale with volume, the rates in a surface-based theory scale with surface area. The theory is used to convert volume-based information on laboratory freezing rates (in units of cu cm, seconds) of nitric acid trihydrate (NAT) and nitric acid dihydrate (NAD) aerosols into surface-based values (in units of sq cm, seconds). We show that a surface-based model is capable of reproducing measured nucleation rates of NAT and NAD aerosols from concentrated aqueous HNO3 solutions in the temperature range of 165 to 205 K. Laboratory measured nucleation rates are used to derive free energies for NAT and NAD germ formation in the stratosphere. NAD germ free energies range from about 23 to 26 kcal mole, allowing for fast and efficient homogeneous NAD particle production in the stratosphere. However, NAT germ formation energies are large (greater than 26 kcal mole) enough to prevent efficient NAT particle production in the stratosphere. We show that the atmospheric NAD particle production rates based on the surface rate theory are roughly 2 orders of magnitude larger than those obtained from a standard volume-based rate theory. Atmospheric volume and surface production of NAD particles will nearly cease in the stratosphere when denitrification in the air exceeds 40 and 78%, respectively. We show that a surface-based (volume-based) homogeneous freezing rate theory gives particle production rates, which are (not) consistent with both laboratory and atmospheric data on the nucleation of solid polar stratospheric cloud particles.

Arctic sea ice melt leads to atmospheric new particle formation.

PubMed

Dall Osto, M; Beddows, D C S; Tunved, P; Krejci, R; Ström, J; Hansson, H-C; Yoon, Y J; Park, Ki-Tae; Becagli, S; Udisti, R; Onasch, T; O Dowd, C D; Simó, R; Harrison, Roy M

2017-06-12

Atmospheric new particle formation (NPF) and growth significantly influences climate by supplying new seeds for cloud condensation and brightness. Currently, there is a lack of understanding of whether and how marine biota emissions affect aerosol-cloud-climate interactions in the Arctic. Here, the aerosol population was categorised via cluster analysis of aerosol size distributions taken at Mt Zeppelin (Svalbard) during a 11 year record. The daily temporal occurrence of NPF events likely caused by nucleation in the polar marine boundary layer was quantified annually as 18%, with a peak of 51% during summer months. Air mass trajectory analysis and atmospheric nitrogen and sulphur tracers link these frequent nucleation events to biogenic precursors released by open water and melting sea ice regions. The occurrence of such events across a full decade was anti-correlated with sea ice extent. New particles originating from open water and open pack ice increased the cloud condensation nuclei concentration background by at least ca. 20%, supporting a marine biosphere-climate link through sea ice melt and low altitude clouds that may have contributed to accelerate Arctic warming. Our results prompt a better representation of biogenic aerosol sources in Arctic climate models.

Understanding ice nucleation characteristics of selective mineral dusts suspended in solution

NASA Astrophysics Data System (ADS)

Kumar, Anand; Marcolli, Claudia; Kaufmann, Lukas; Krieger, Ulrich; Peter, Thomas

2016-04-01

Introduction & Objectives Freezing of liquid droplets and subsequent ice crystal growth affects optical properties of clouds and precipitation. Field measurements show that ice formation in cumulus and stratiform clouds begins at temperatures much warmer than those associated with homogeneous ice nucleation in pure water, which is ascribed to heterogeneous ice nucleation occurring on the foreign surfaces of ice nuclei (IN). Various insoluble particles such as mineral dust, soot, metallic particles, volcanic ash, or primary biological particles have been suggested as IN. Among these the suitability of mineral dusts is best established. The ice nucleation ability of mineral dust particles may be modified when secondary organic or inorganic substances are accumulating on the dust during atmospheric transport. If the coating is completely wetting the mineral dust particles, heterogeneous ice nucleation occurs in immersion mode also below 100 % RH. A previous study by Kaufmann (PhD Thesis 2015, ETHZ) with Hoggar Mountain dust suspensions in various solutes (ammonium sulfate, PEG, malonic acid and glucose) showed reduced ice nucleation efficiency (in immersion mode) of the particles. Though it is still quite unclear of how surface modifications and coatings influence the ice nucleation activity of the components present in natural dust samples. In view of these results we run freezing experiments using a differential scanning calorimeter (DSC) with the following mineral dust particles suspended in pure water and ammonium sulfate solutions: Arizona Test Dust (ATD), microcline, and kaolinite (KGa-2, Clay Mineral Society). Methodology Suspensions of mineral dust samples (ATD: 2 weight%, microcline: 5% weight, KGa-2: 5% weight) are prepared in pure water with varying solute concentrations (ammonium sulfate: 0 - 10% weight). 20 vol% of this suspension plus 80 vol% of a mixture of 95 wt% mineral oil (Aldrich Chemical) and 5 wt% lanolin (Fluka Chemical) is emulsified with a rotor-stator homogenizer for 40 s at a rotation frequency of 7000 rpm. 4 - 10 mg of this mixture is pipetted in an aluminum pan (closed hermetically), placed in the DSC and subjected to three freezing cycles. The first and the third freezing cycles are executed at a cooling rate of 10 K/min to control the stability of the sample. The second freezing cycle is executed at a 1 K/min cooling rate and is used for evaluation. Freezing temperatures are obtained by evaluating the onset of the freezing signal in the DSC curve and plotted against water activity values corresponding to the solute concentration (obtained via Koop et al., (2000)). Observations A decrease in ice nucleation ability of the minerals (for immersion freezing) with increasing solute concentration (hence, decreasing water activity) was observed, similar as for homogeneous ice nucleation. Though the decrease was more pronounced in case of microcline and ATD as compared to kaolinite. Therefore, there seem to be specific interactions which needs to be studied further to explain the freezing behavior of minerals. The current study could be helpful in investigating the ice nucleation behavior of individual minerals when present in conjunction with a solute, viz. ammonium sulfate, which is of high atmospheric relevance. References Zobrist et al., (2008), doi: 10.1021/jp7112208. Koop et al., (2000), doi:10.1038/35020537. Kaufmann (PhD Thesis 2015, ETHZ).

Ice-nucleating bacteria control the order and dynamics of interfacial water

DOE PAGES

Pandey, Ravindra; Usui, Kota; Livingstone, Ruth A.; ...

2016-04-22

Ice-nucleating organisms play important roles in the environment. With their ability to induce ice formation at temperatures just below the ice melting point, bacteria such as Pseudomonas syringae attack plants through frost damage using specialized ice-nucleating proteins. Besides the impact on agriculture and microbial ecology, airborne P. syringae can affect atmospheric glaciation processes, with consequences for cloud evolution, precipitation, and climate. Biogenic ice nucleation is also relevant for artificial snow production and for biomimetic materials for controlled interfacial freezing. We use interface-specific sum frequency generation (SFG) spectroscopy to show that hydrogen bonding at the water-bacteria contact imposes structural ordering onmore » the adjacent water network. Experimental SFG data and molecular dynamics simulations demonstrate that ice active sites within P. syringae feature unique hydrophilic-hydrophobic patterns to enhance ice nucleation. Finally, the freezing transition is further facilitated by the highly effective removal of latent heat from the nucleation site, as apparent from time-resolved SFG spectroscopy.« less

Analysis of the Effect of Water Activity on Ice Formation Using a New Theory of Nucleation

NASA Technical Reports Server (NTRS)

Barahona, Donifan

2013-01-01

In this work a new theory of nucleation is developed and used to investigate the effect of water activity on the formation of ice within super-cooled droplets. The new theory is based on a novel concept where the interface is assumed to be made of liquid molecules trapped by the solid matrix. Using this concept new expressions are developed for the critical ice germ size and the nucleation work, with explicit dependencies on temperature and water activity. However unlike previous approaches, the new theory does not depend on the interfacial tension between liquid and ice. Comparison against experimental results shows that the new theory is able to reproduce the observed effect of water activity on nucleation rate and freezing temperature. It allows for the first time a theoretical derivation of the constant shift in water activity between melting and nucleation. The new theory offers a consistent thermodynamic view of ice nucleation, simple enough to be applied in atmospheric models of cloud formation.

Ice-nucleating bacteria control the order and dynamics of interfacial water

PubMed Central

Pandey, Ravindra; Usui, Kota; Livingstone, Ruth A.; Fischer, Sean A.; Pfaendtner, Jim; Backus, Ellen H. G.; Nagata, Yuki; Fröhlich-Nowoisky, Janine; Schmüser, Lars; Mauri, Sergio; Scheel, Jan F.; Knopf, Daniel A.; Pöschl, Ulrich; Bonn, Mischa; Weidner, Tobias

2016-01-01

Ice-nucleating organisms play important roles in the environment. With their ability to induce ice formation at temperatures just below the ice melting point, bacteria such as Pseudomonas syringae attack plants through frost damage using specialized ice-nucleating proteins. Besides the impact on agriculture and microbial ecology, airborne P. syringae can affect atmospheric glaciation processes, with consequences for cloud evolution, precipitation, and climate. Biogenic ice nucleation is also relevant for artificial snow production and for biomimetic materials for controlled interfacial freezing. We use interface-specific sum frequency generation (SFG) spectroscopy to show that hydrogen bonding at the water-bacteria contact imposes structural ordering on the adjacent water network. Experimental SFG data and molecular dynamics simulations demonstrate that ice-active sites within P. syringae feature unique hydrophilic-hydrophobic patterns to enhance ice nucleation. The freezing transition is further facilitated by the highly effective removal of latent heat from the nucleation site, as apparent from time-resolved SFG spectroscopy. PMID:27152346

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pandey, Ravindra; Usui, Kota; Livingstone, Ruth A.

Ice-nucleating organisms play important roles in the environment. With their ability to induce ice formation at temperatures just below the ice melting point, bacteria such as Pseudomonas syringae attack plants through frost damage using specialized ice-nucleating proteins. Besides the impact on agriculture and microbial ecology, airborne P. syringae can affect atmospheric glaciation processes, with consequences for cloud evolution, precipitation, and climate. Biogenic ice nucleation is also relevant for artificial snow production and for biomimetic materials for controlled interfacial freezing. We use interface-specific sum frequency generation (SFG) spectroscopy to show that hydrogen bonding at the water-bacteria contact imposes structural ordering onmore » the adjacent water network. Experimental SFG data and molecular dynamics simulations demonstrate that ice active sites within P. syringae feature unique hydrophilic-hydrophobic patterns to enhance ice nucleation. Finally, the freezing transition is further facilitated by the highly effective removal of latent heat from the nucleation site, as apparent from time-resolved SFG spectroscopy.« less

Formation of Mesospheric Clouds on Mars

NASA Astrophysics Data System (ADS)

Plane, J. M. C.; Audouard, J.; Listowski, C.; Mangan, T.; Maattanen, A. E.; Montmessin, F.; Forget, F.; Millour, E.; Spiga, A.; Crismani, M. M. J.; Schneider, N. M.

2017-12-01

Martian Mesospheric Clouds (MMCs) are observed intermittently in the Martian atmosphere between 60 and 100 km, occurring particularly at low latitudes. The clouds consist mainly of CO2-ice particles around 1 mm in radius. Explaining the nucleation and growth of these particles is challenging: it has been assumed that - by analogy with polar mesospheric clouds in the terrestrial atmosphere - nucleation occurs on meteoric smoke particles (very small metal-silicate particles resulting from the condensation of the vapor produced by cosmic dust ablation). Indeed, 1D modeling of CO2 microphysics suggests that an exogenous source of nuclei is necessary to model CO2 MMCs, in agreement with observations in cold pockets produced by the coupling of gravity waves and thermal tides. However, a recent laboratory study has shown that smoke particles, which would be around 1 nm in size - require extremely high CO2 supersaturations to nucleate CO2 ice. Here we present an alternative picture of the nucleation of CO2-ice particles. The major meteoric metals - Mg and Fe - should form MgCO3 and FeCO3 molecules in the Mars atmosphere below 90 km. These molecules have enormous electric dipole moments (11.6 and 9.3 Debye, respectively), and so will immediately form stable clusters with 3 CO2 molecules, which then slowly exchange with H2O to produce hexa-hydrated carbonate molecules. These primary particles polymerize readily to form a background population of "dirty" water-ice particles. Using MAVEN-IUVS measurements of the background Mg+ ion layer to constrain the injection rates of Mg and Fe from meteoric ablation, and a 1D model of metal chemistry coupled to an aerosol coagulation model, we show that the population of these water-ice particles with radii greater than 10 nm should be around 200 cm-3 at 80 km, thus providing a population of effective CO2-ice nuclei. When these nuclei are input in the Laboratoire de Météorologie Dynamique (LMD) Mars GCM, first results show that they can be activated in the upper mesosphere cold pockets and hence contribute to form CO­2-ice clouds whose characteristics (spatial and seasonal distribution, opacities, and particle sizes) are in agreement with observations.

Heterogeneous freezing of droplets with immersed surface modified mineral dust particles

NASA Astrophysics Data System (ADS)

Hartmann, Susan

2010-05-01

In the framework of the international measurement campaign FROST II (FReezing Of duST), the heterogeneous freezing of droplets with an immersed surface modified size-segregated mineral dust particles was investigated at LACIS (Leipzig Aerosol Cloud Interaction Simulator, Stratmann et al. 2004). The following measurements were done: LACIS, CFDC (Continuous Flow thermal gradient Diffusion Chamber, Rogers (1988)) and FINCH (Fast Ice Nucleus Chamber Counter, Bundke et al (2008)) were used to analyze the immersion freezing behavior of the treated Arizona Test Dust (ATD) particles at different temperature regimes. The ability to act as IN (Ice Nucleus) in the deposition nucleation mode was quantified by the PINC (Portable Ice Nucleation Chamber) and the CFDC instrument. AMS (Aerosol Mass Spectrometers, e.g. Schneider et al. (2005)) and ATOFMS (Aerosol Time-Of-Flight Mass Spectrometer) measurements were applied to determine particle composition. The hygroscopic growth and the critical super-saturations needed for droplet activation were determined by means of an H-TDMA (Humidity-Tandem Differential Mobility Analyzer) and CCN counter (Cloud Condensation Nucleus counter, Droplet Measurement Technologies, Roberts and Nenes (2005)). The 300 nm ATD particles were chemically and physically treated by coating with sulphuric acid (H2SO4, three different coating thicknesses) and ammonium sulphate ((NH4)2SO4) or by thermal treatment with a thermodenuder operating at 250°C. The H2SO4 coating modified the particles by reacting with particle material, forming soluble sulfates and therefore changing surface properties. AMS showed free H2SO4 only for thick H2SO4 coatings. In the heated section of the thermodenuder coating materials were evaporated partly and the surface properties of the particles were additionally altered. Uncoated particles and those coated with thin coatings of H2SO4, showed almost no hygroscopic growth. Particles coated with thicker coatings of H2SO4 and of (NH4)2SO4 grew noticeably above 95% relative humidity. All investigated particles were found to activate at atmospherically relevant super-saturations. All kinds of treatment lower the IN-ability, whereas the deposition nucleation was more sensitive to treatments than the immersion freezing mode. Considering the immersion freezing behavior, pure ATD particles and particles coated with thin coatings of H2SO4 were more efficient IN, than particles with thick H2SO4 or (NH4)2SO4 coatings. Thermal treatments of the particles led to further decrease of the IN capability except for particles coated with (NH4)2SO4, where the heating did not effect the immersion freezing behavior likely due to their already reduced IN ability. In order to specify the temperature-dependent immersion freezing, two parameterization based on either stochastic or singular hypothesis were performed. From both theoretical approaches it can be concluded that the treatments lead to particle surface modifications lowering the nucleation efficiency. References: Bundke, U., B. Nillius, et al. (2008), The fast Ice Nucleus chamber FINCH, Atmospheric Research 90(2-4): 180-186. Rader, D. J. and P. H. McMurry (1986), Application of the Tandem Differential Mobility Analyzer to studies of droplet growth or evaporation, J. Aerosol Sci., Vol. 17, No. 5, pp. 771-787. Roberts, G., and A. Nenes (2005), A continuous-flow streamwise thermal-gradient CCN chamber for atmospheric measurements, Aerosol Sci. Technol., 39, 206-221. Schneider, J., N. Hock, S. Weimer, S. Borrmann, U. Kirchner, R. Vogt, and V. Scheer (2005), Nucleation particles in Diesel exhaust: Composition inferred from in situ mass spectrometric analysis, Environ. Sci. Technol., 39, 6153-6161. Rogers,D .C. (1988), Developmenot f a continuousflow thermal gradient diffusion chamber for ice nucleation studies. Atmospheric Research, 22, 149-181. Stratmann, F., A. Kiselev, S. Wurzler, M. Wendisch, J. Heintzenberg, R. J. Charlson, K. Diehl, H. Wex, and S. Schmidt (2004), Laboratory studies and numerical simulations of cloud droplet formation under realistic super-saturation conditions, J. Atmos. Oceanic Technol., 21, 876-887.

Aircraft-Measured Indirect Cloud Effects from Biomass Burning Smoke in the Arctic and Subarctic

NASA Technical Reports Server (NTRS)

Zamora, L. M.; Kahn, R. A.; Cubison, M. J.; Diskin, G. S.; Jimenez, J. L.; Kondo, Y.; McFarquhar, G. M.; Nenes, A.; Thornhill, K. L.; Wisthaler, A.;

Aircraft-measured indirect cloud effects from biomass burning smoke in the Arctic and subarctic

DOE PAGES

Zamora, Lauren M.; Kahn, R. A.; Cubison, M. J.; ...

2016-01-21

The incidence of wildfires in the Arctic and subarctic is increasing; in boreal North America, for example, the burned area is expected to increase by 200–300% over the next 50–100 years, which previous studies suggest could have a large effect on cloud microphysics, lifetime, albedo, and precipitation. However, the interactions between smoke particles and clouds remain poorly quantified due to confounding meteorological influences and remote sensing limitations. Here, we use data from several aircraft campaigns in the Arctic and subarctic to explore cloud microphysics in liquid-phase clouds influenced by biomass burning. Median cloud droplet radii in smoky clouds were ~40–60% smallermore » than in background clouds. Based on the relationship between cloud droplet number ( N liq) and various biomass burning tracers (BB t) across the multi-campaign data set, we calculated the magnitude of subarctic and Arctic smoke aerosol–cloud interactions (ACIs, where ACI = (1/3) × d ln( N liq)/d ln(BB t)) to be ~0.16 out of a maximum possible value of 0.33 that would be obtained if all aerosols were to nucleate cloud droplets. Interestingly, in a separate subarctic case study with low liquid water content (~0.02gm –3) and very high aerosol concentrations (2000–3000 cm –3) in the most polluted clouds, the estimated ACI value was only 0.05. In this case, competition for water vapor by the high concentration of cloud condensation nuclei (CCN) strongly limited the formation of droplets and reduced the cloud albedo effect, which highlights the importance of cloud feedbacks across scales. Using our calculated ACI values, we estimate that the smoke-driven cloud albedo effect may decrease local summertime short-wave radiative flux by between 2 and 4 Wm –2 or more under some low and homogeneous cloud cover conditions in the subarctic, although the changes should be smaller in high surface albedo regions of the Arctic. Furthermore, we lastly explore evidence suggesting that numerous northern-latitude background Aitken particles can interact with combustion particles, perhaps impacting their properties as cloud condensation and ice nuclei.« less

Ice nucleation activity of agricultural soil dust aerosols from Mongolia, Argentina, and Germany

NASA Astrophysics Data System (ADS)

Steinke, I.; Funk, R.; Busse, J.; Iturri, A.; Kirchen, S.; Leue, M.; Möhler, O.; Schwartz, T.; Schnaiter, M.; Sierau, B.; Toprak, E.; Ullrich, R.; Ulrich, A.; Hoose, C.; Leisner, T.

2016-11-01

Soil dust particles emitted from agricultural areas contain considerable mass fractions of organic material. Also, soil dust particles may act as carriers for potentially ice-active biological particles. In this work, we present ice nucleation experiments conducted in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber. We investigated the ice nucleation efficiency of four types of soil dust from different regions of the world. The results are expressed as ice nucleation active surface site (INAS) densities and presented for the immersion freezing and the deposition nucleation mode. For immersion freezing occurring at 254 K, samples from Argentina, China, and Germany show ice nucleation efficiencies which are by a factor of 10 higher than desert dusts. On average, the difference in ice nucleation efficiencies between agricultural and desert dusts becomes significantly smaller at temperatures below 247 K. In the deposition mode the soil dusts showed higher ice nucleation activity than Arizona Test Dust over a temperature range between 232 and 248 K and humidities RHice up to 125%. INAS densities varied between 109 and 1011 m-2 for these thermodynamic conditions. For one soil dust sample (Argentinian Soil), the effect of treatments with heat was investigated. Heat treatments (383 K) did not affect the ice nucleation efficiency observed at 249 K. This finding presumably excludes proteinaceous ice-nucleating entities as the only source of the increased ice nucleation efficiency.

Toward Quantifying the Mass-Based Hygroscopicity of Individual Submicron Atmospheric Aerosol Particles with STXM/NEXAFS and SEM/EDX

NASA Astrophysics Data System (ADS)

Yancey Piens, D.; Kelly, S. T.; OBrien, R. E.; Wang, B.; Petters, M. D.; Laskin, A.; Gilles, M. K.

2014-12-01

The hygroscopic behavior of atmospheric aerosols influences their optical and cloud-nucleation properties, and therefore affects climate. Although changes in particle size as a function of relative humidity have often been used to quantify the hygroscopic behavior of submicron aerosol particles, it has been noted that calculations of hygroscopicity based on size contain error due to particle porosity, non-ideal volume additivity and changes in surface tension. We will present a method to quantify the hygroscopic behavior of submicron aerosol particles based on changes in mass, rather than size, as a function of relative humidity. This method results from a novel experimental approach combining scanning transmission x-ray microscopy with near-edge x-ray absorption fine spectroscopy (STXM/NEXAFS), as well as scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM/EDX) on the same individual particles. First, using STXM/NEXAFS, our methods are applied to aerosol particles of known composition ‒ for instance ammonium sulfate, sodium bromide and levoglucosan ‒ and validated by theory. Then, using STXM/NEXAFS and SEM/EDX, these methods are extended to mixed atmospheric aerosol particles collected in the field at the DOE Atmospheric Radiation Measurement (ARM) Climate Research Facility at the Southern Great Planes sampling site in Oklahoma, USA. We have observed and quantified a range of hygroscopic behaviors which are correlated to the composition and morphology of individual aerosol particles. These methods will have implications for parameterizing aerosol mixing state and cloud-nucleation activity in atmospheric models.

Investigating Type I Polar Stratospheric Cloud Formation Mechanisms with POAM Satellite Observations

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Drdla, K.; Fromm, M.; Hoppel, K.; Browell, E.; Hamill, P.; Dempsey, D.; Gore, Warren J. (Technical Monitor)

2001-01-01

Type Ia PSCs are believed to be composed of nitric acid hydrate particles. Recent results from the SOLVE/THESEO 2000 campaign showed evidence that this type of PSC was composed of a small number of very large particles capable of sedimentary denitrification of regions of the stratosphere. It is unknown whether homogeneous or heterogeneous nucleation is responsible for the formation of these PSCs. Arctic winters are tending to be colder in response to global tropospheric warming. The degree to which this influences ozone depletion will depend on the freezing mechanism of nitric acid hydrate particles. If nucleation is homogeneous it implies that the freezing process is an inherent property of the particle, while heterogeneous freezing means that the extent of PSCs will depend in part on the number of nuclei available. The Polar Ozone and Aerosol Measurement (POAM)II and III satellites have been making observations of stratospheric aerosols and Polar Stratospheric Clouds (PSCs) since 1994. Recently, we have developed a technique that can discriminate between Type Ia and Ib PSCs using these observations. A statistical approach is employed to demonstrate the robustness of this approach and results are compared with lidar measurements. The technique is used to analyze observations from POAM II and II during Northern Hemisphere winters where significant PSC formation occurred with the objective of exploring Type I PSC formation mechanisms. The different PSCs identified using this method exhibit different growth curve as expressed as extinction versus temperature.

Survival and ice nucleation activity of bacteria as aerosols in a cloud simulation chamber

NASA Astrophysics Data System (ADS)

Amato, P.; Joly, M.; Schaupp, C.; Attard, E.; Möhler, O.; Morris, C. E.; Brunet, Y..; Delort, A.-M.

2015-02-01

The residence time of bacterial cells in the atmosphere is predictable by numerical models. However, estimations of their aerial dispersion as living entities are limited by lacks of information concerning survival rates and behavior in relation to atmospheric water. Here we investigate the viability and ice nucleation (IN) activity of typical atmospheric ice nucleation active bacteria (Pseudomonas syringae and P. fluorescens) when airborne in a cloud simulation chamber (AIDA, Karlsruhe, Germany). Cell suspensions were sprayed into the chamber and aerosol samples were collected by impingement at designated times over a total duration of up to 18 h, and at some occasions after dissipation of a cloud formed by depressurization. Aerosol concentration was monitored simultaneously by online instruments. The cultivability of airborne cells decreased exponentially over time with a half-life time of 250 ± 30 min (about 3.5 to 4.5 h). In contrast, IN activity remained unchanged for several hours after aerosolization, demonstrating that IN activity was maintained after cell death. Interestingly, the relative abundance of IN active cells still airborne in the chamber was strongly decreased after cloud formation and dissipation. This illustrates the preferential precipitation of IN active cells by wet processes. Our results indicate that from 106 = cells aerosolized from a surface, one would survive the average duration of its atmospheric journey estimated at 3.4 days. Statistically, this corresponds to the emission of 1 cell that achieves dissemination every ~33 min per m2 of cultivated crops fields, a strong source of airborne bacteria. Based on the observed survival rates, depending on wind speed, the trajectory endpoint could be situated several hundreds to thousands of kilometers from the emission source. These results should improve the representation of the aerial dissemination of bacteria in numeric models.

Survival and ice nucleation activity of bacteria as aerosols in a cloud simulation chamber

NASA Astrophysics Data System (ADS)

Amato, P.; Joly, M.; Schaupp, C.; Attard, E.; Möhler, O.; Morris, C. E.; Brunet, Y.; Delort, A.-M.

2015-06-01

The residence time of bacterial cells in the atmosphere is predictable by numerical models. However, estimations of their aerial dispersion as living entities are limited by a lack of information concerning survival rates and behavior in relation to atmospheric water. Here we investigate the viability and ice nucleation (IN) activity of typical atmospheric ice nucleation active bacteria (Pseudomonas syringae and P. fluorescens) when airborne in a cloud simulation chamber (AIDA, Karlsruhe, Germany). Cell suspensions were sprayed into the chamber and aerosol samples were collected by impingement at designated times over a total duration of up to 18 h, and at some occasions after dissipation of a cloud formed by depressurization. Aerosol concentration was monitored simultaneously by online instruments. The cultivability of airborne cells decreased exponentially over time with a half-life time of 250 ± 30 min (about 3.5 to 4.5 h). In contrast, IN activity remained unchanged for several hours after aerosolization, demonstrating that IN activity was maintained after cell death. Interestingly, the relative abundance of IN active cells still airborne in the chamber was strongly decreased after cloud formation and dissipation. This illustrates the preferential precipitation of IN active cells by wet processes. Our results indicate that from 106 cells aerosolized from a surface, one would survive the average duration of its atmospheric journey estimated at 3.4 days. Statistically, this corresponds to the emission of 1 cell that achieves dissemination every ~ 33 min m-2 of cultivated crops fields, a strong source of airborne bacteria. Based on the observed survival rates, depending on wind speed, the trajectory endpoint could be situated several hundreds to thousands of kilometers from the emission source. These results should improve the representation of the aerial dissemination of bacteria in numeric models.

An overview of the Ice Nuclei Research Unit Jungfraujoch/Cloud and Aerosol Characterization Experiment 2013 (INUIT-JFJ/CLACE-2013)

NASA Astrophysics Data System (ADS)

Schneider, Johannes

2014-05-01

Ice formation in mixed phase tropospheric clouds is an essential prerequisite for the formation of precipitation at mid-latitudes. Ice formation at temperatures warmer than -35°C is only possible via heterogeneous ice nucleation, but up to now the exact pathways of heterogeneous ice formation are not sufficiently well understood. The research unit INUIT (Ice NUcleation research unIT), funded by the Deutsche Forschungsgemeinschaft (DFG FOR 1525) has been established in 2012 with the objective to investigate heterogeneous ice nucleation by combination of laboratory studies, model calculation and field experiments. The main field campaign of the INUIT project (INUIT-JFJ) was conducted at the High Alpine Research Station Jungfraujoch (Swiss Alps, 3580 m asl) during January and February 2013, in collaboration with several international partners in the framework of CLACE2013. The instrumentation included a large set of aerosol chemical and physical analysis instruments (particle counters, particle sizers, particle mass spectrometers, cloud condensation nuclei counters, ice nucleus counters etc.), that were operated inside the Sphinx laboratory and sampled in mixed phase clouds through two ice selective inlets (Ice-CVI, ISI) as well as through a total aerosol inlet that was used for out-of-cloud aerosol measurements. Besides the on-line measurements, also samples for off-line analysis (ESEM, STXM) have been taken in and out of clouds. Furthermore, several cloud microphysics instruments were operated outside the Sphinx laboratory. First results indicate that a large fraction of ice residues sampled from mixed phase clouds contain organic material, but also mineral dust. Soot and lead were not found to be enriched in ice residues. The concentration of heterogeneous ice nuclei was found to be variable (ranging between < 1 and > 100 per liter) and to be strongly dependent on the operating conditions of the respective IN counter. The number size distribution of ice residues appears to show a bimodal distribution with a smaller mode having a modal diameter around 200 nm and a coarse mode at around 2 µm. During the cloud events evaluated so far, agreement between the number concentration of ice residues sampled through the Ice-CVI and the measured concentration of small ice crystals measured outside the laboratory could be achieved. The shape of small ice crystals was found to be mainly irregular. We acknowledge the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG), the help of the custodians at the Jungfraujoch station, and the funding by DFG (FOR 1525) and the federal state Hessen ("LOEWE-Schwerpunkt AmbiProbe").

Dust in brown dwarfs. III. Formation and structure of quasi-static cloud layers

NASA Astrophysics Data System (ADS)

Woitke, P.; Helling, Ch.

2004-01-01

In this paper, first solutions of the dust moment equations developed in (Woitke & Helling \\cite{wh2003a}) for the description of dust formation and precipitation in brown dwarf and giant gas planet atmospheres are presented. We consider the special case of a static brown dwarf atmosphere, where dust particles continuously nucleate from the gas phase, grow by the accretion of molecules, settle gravitationally and re-evaporate thermally. Mixing by convective overshoot is assumed to replenish the atmosphere with condensable elements, which is necessary to counterbalance the loss of condensable elements by dust formation and gravitational settling (no dust without mixing). Applying a kinetic description of the relevant microphysical and chemical processes for TiO2-grains, the model makes predictions about the large-scale stratification of dust in the atmosphere, the depletion of molecules from the gas phase, the supersaturation of the gas in the atmosphere as well as the mean size and the mass fraction of dust grains as function of depth. Our results suggest that the presence of relevant amounts of dust is restricted to a layer, where the upper boundary (cloud deck) is related to the requirement of a minimum mixing activity (mixing time-scale τmix ≈ 10 6 s) and the lower boundary (cloud base) is determined by the thermodynamical stability of the grains. The nucleation occurs around the cloud deck where the gas is cool, strongly depleted, but nevertheless highly supersaturated (S ≫ 1). These particles settle gravitationally and populate the warmer layers below, where the in situ formation (nucleation) is ineffective or even not possible. During their descent, the particles grow and reach mean radii of ≈30 \\mum ... 400 \\mum at the cloud base, but the majority of the particles in the cloud layer remains much smaller. Finally, the dust grains sink into layers which are sufficiently hot to cause their thermal evaporation. Hence, an effective transport mechanism for condensable elements exists in brown dwarfs, which depletes the gas above and enriches the gas below the cloud base of a considered solid/liquid material. The dust-to-gas mass fraction in the cloud layer results to be approximately given by the mass fraction of condensable elements in the gas being mixed up. Only for artificially reduced mixing we find a self-regulation mechanism that approximately installs phase equilibrium (S ≈ 1) in a limited region around the cloud base.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zamora, Lauren M.; Kahn, R. A.; Cubison, M. J.

The incidence of wildfires in the Arctic and subarctic is increasing; in boreal North America, for example, the burned area is expected to increase by 200–300% over the next 50–100 years, which previous studies suggest could have a large effect on cloud microphysics, lifetime, albedo, and precipitation. However, the interactions between smoke particles and clouds remain poorly quantified due to confounding meteorological influences and remote sensing limitations. Here, we use data from several aircraft campaigns in the Arctic and subarctic to explore cloud microphysics in liquid-phase clouds influenced by biomass burning. Median cloud droplet radii in smoky clouds were ~40–60% smallermore » than in background clouds. Based on the relationship between cloud droplet number ( N liq) and various biomass burning tracers (BB t) across the multi-campaign data set, we calculated the magnitude of subarctic and Arctic smoke aerosol–cloud interactions (ACIs, where ACI = (1/3) × d ln( N liq)/d ln(BB t)) to be ~0.16 out of a maximum possible value of 0.33 that would be obtained if all aerosols were to nucleate cloud droplets. Interestingly, in a separate subarctic case study with low liquid water content (~0.02gm –3) and very high aerosol concentrations (2000–3000 cm –3) in the most polluted clouds, the estimated ACI value was only 0.05. In this case, competition for water vapor by the high concentration of cloud condensation nuclei (CCN) strongly limited the formation of droplets and reduced the cloud albedo effect, which highlights the importance of cloud feedbacks across scales. Using our calculated ACI values, we estimate that the smoke-driven cloud albedo effect may decrease local summertime short-wave radiative flux by between 2 and 4 Wm –2 or more under some low and homogeneous cloud cover conditions in the subarctic, although the changes should be smaller in high surface albedo regions of the Arctic. Furthermore, we lastly explore evidence suggesting that numerous northern-latitude background Aitken particles can interact with combustion particles, perhaps impacting their properties as cloud condensation and ice nuclei.« less

Aircraft-Measured Indirect Cloud Effects from Biomass Burning Smoke in the Arctic and Subarctic

NASA Technical Reports Server (NTRS)

Zamora, Lauren; Kahn, R. A.; Cubison, M. C.; Diskin, G. S.; Jimenez, J. L.; Kondo, Y.; McFarquhar, G. M.; Nenes, A.; Wisthaler, A.; Zelenyuk, A.;

Intercomparison of cloud model simulations of Arctic mixed-phase boundary layer clouds observed during SHEBA/FIRE-ACE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Morrison, H.; Zuidema, Paquita; Ackerman, Andrew

2011-06-16

An intercomparison of six cloud-resolving and large-eddy simulation models is presented. This case study is based on observations of a persistent mixed-phase boundary layer cloud gathered on 7 May, 1998 from the Surface Heat Budget of Arctic Ocean (SHEBA) and First ISCCP Regional Experiment - Arctic Cloud Experiment (FIRE-ACE). Ice nucleation is constrained in the simulations in a way that holds the ice crystal concentration approximately fixed, with two sets of sensitivity runs in addition to the baseline simulations utilizing different specified ice nucleus (IN) concentrations. All of the baseline and sensitivity simulations group into two distinct quasi-steady states associatedmore » with either persistent mixed-phase clouds or all-ice clouds after the first few hours of integration, implying the existence of multiple equilibria. These two states are associated with distinctly different microphysical, thermodynamic, and radiative characteristics. Most but not all of the models produce a persistent mixed-phase cloud qualitatively similar to observations using the baseline IN/crystal concentration, while small increases in the IN/crystal concentration generally lead to rapid glaciation and conversion to the all-ice state. Budget analysis indicates that larger ice deposition rates associated with increased IN/crystal concentrations have a limited direct impact on dissipation of liquid in these simulations. However, the impact of increased ice deposition is greatly enhanced by several interaction pathways that lead to an increased surface precipitation flux, weaker cloud top radiative cooling and cloud dynamics, and reduced vertical mixing, promoting rapid glaciation of the mixed-phase cloud for deposition rates in the cloud layer greater than about 1-2x10-5 g kg-1 s-1. These results indicate the critical importance of precipitation-radiative-dynamical interactions in simulating cloud phase, which have been neglected in previous fixed-dynamical parcel studies of the cloud phase parameter space. Large sensitivity to the IN/crystal concentration also suggests the need for improved understanding of ice nucleation and its parameterization in models.« less

A FIRE-ACE/SHEBA Case Study of Mixed-Phase Arctic Boundary Layer Clouds: Entrainment Rate Limitations on Rapid Primary Ice Nucleation Processes

NASA Technical Reports Server (NTRS)

Fridlin, Ann; vanDiedenhoven, Bastiaan; Ackerman, Andrew S.; Avramov, Alexander; Mrowiec, Agnieszka; Morrison, Hugh; Zuidema, Paquita; Shupe, Matthew D.

2012-01-01

Observations of long-lived mixed-phase Arctic boundary layer clouds on 7 May 1998 during the First International Satellite Cloud Climatology Project (ISCCP) Regional Experiment (FIRE)Arctic Cloud Experiment (ACE)Surface Heat Budget of the Arctic Ocean (SHEBA) campaign provide a unique opportunity to test understanding of cloud ice formation. Under the microphysically simple conditions observed (apparently negligible ice aggregation, sublimation, and multiplication), the only expected source of new ice crystals is activation of heterogeneous ice nuclei (IN) and the only sink is sedimentation. Large-eddy simulations with size-resolved microphysics are initialized with IN number concentration N(sub IN) measured above cloud top, but details of IN activation behavior are unknown. If activated rapidly (in deposition, condensation, or immersion modes), as commonly assumed, IN are depleted from the well-mixed boundary layer within minutes. Quasi-equilibrium ice number concentration N(sub i) is then limited to a small fraction of overlying N(sub IN) that is determined by the cloud-top entrainment rate w(sub e) divided by the number-weighted ice fall speed at the surface v(sub f). Because w(sub c)< 1 cm/s and v(sub f)> 10 cm/s, N(sub i)/N(sub IN)<< 1. Such conditions may be common for this cloud type, which has implications for modeling IN diagnostically, interpreting measurements, and quantifying sensitivity to increasing N(sub IN) (when w(sub e)/v(sub f)< 1, entrainment rate limitations serve to buffer cloud system response). To reproduce observed ice crystal size distributions and cloud radar reflectivities with rapidly consumed IN in this case, the measured above-cloud N(sub IN) must be multiplied by approximately 30. However, results are sensitive to assumed ice crystal properties not constrained by measurements. In addition, simulations do not reproduce the pronounced mesoscale heterogeneity in radar reflectivity that is observed.

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

DOE PAGES

Wang, Jian; Krejci, Radovan; Giangrande, Scott; ...

2016-10-24

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- andmore » ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. Lastly, this rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.« less

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

NASA Astrophysics Data System (ADS)

Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M. J.; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E.; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L.; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A. F.; Springston, Stephen R.; Tomlinson, Jason M.; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N.; Kulmala, Markku; Machado, Luiz A. T.; Artaxo, Paulo; Andreae, Meinrat O.; Petäjä, Tuukka; Martin, Scot T.

2016-11-01

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall.

PubMed

Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M J; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A F; Springston, Stephen R; Tomlinson, Jason M; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N; Kulmala, Markku; Machado, Luiz A T; Artaxo, Paulo; Andreae, Meinrat O; Petäjä, Tuukka; Martin, Scot T

2016-11-17

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

Ice formation and development in aged, wintertime cumulus over the UK : observations and modelling

NASA Astrophysics Data System (ADS)

Crawford, I.; Bower, K. N.; Choularton, T. W.; Dearden, C.; Crosier, J.; Westbrook, C.; Capes, G.; Coe, H.; Connolly, P.; Dorsey, J. R.; Gallagher, M. W.; Williams, P.; Trembath, J.; Cui, Z.; Blyth, A.

2011-11-01

In-situ high resolution aircraft measurements of cloud microphysical properties were made in coordination with ground based remote sensing observations of Radar and Lidar as part of the Aerosol Properties, PRocesses And InfluenceS on the Earth's climate (APPRAISE) project. A narrow but extensive line (~100 km long) of shallow convective clouds over the southern UK was studied. Cloud top temperatures were observed to be higher than ~-8 °C, but the clouds were seen to consist of supercooled droplets and varying concentrations of ice particles. No ice particles were observed to be falling into the cloud tops from above. Current parameterisations of ice nuclei (IN) numbers predict too few particles will be active as ice nuclei to account for ice particle concentrations at the observed near cloud top temperatures (~-7 °C). The role of biological particles, consistent with concentrations observed near the surface, acting as potential efficient high temperature IN is considered important in this case. It was found that very high concentrations of ice particles (up to 100 L-1) could be produced by powerful secondary ice particle production emphasising the importance of understanding primary ice formation in slightly supercooled clouds. Aircraft penetrations at -3.5 °C, showed peak ice crystal concentrations of up to 100 L-1 which together with the characteristic ice crystal habits observed (generally rimed ice particles and columns) suggested secondary ice production had occurred. To investigate whether the Hallett-Mossop (HM) secondary ice production process could account for these observations, ice splinter production rates were calculated. These calculated rates and observations could only be reconciled provided the constraint that only droplets >24 μm in diameter could lead to splinter production, was relaxed slightly by 2 μm. Model simulations of the case study were also performed with the WRF (Weather, Research and Forecasting) model and ACPIM (Aerosol Cloud and Precipitation Interactions Model) to investigate the likely origins of the ice phase in these slightly supercooled clouds and to assess the role played by the HM process in this and in controlling precipitation formation under these conditions. WRF results showed that while HM does act to increase the mass and number concentration of ice particles produced in the model simulations, in the absence of HM, the ice number concentration arising from primary ice nucleation alone (several L-1) was apparently sufficient to sustain precipitation although the distribution of the precipitation was changed. Thus in the WRF model the HM process was shown to be non-critical for the formation of precipitation in this particular case. However, this result is seen to be subject to an important caveat concerning the simulation of the cloud macrostructure. The model was unable to capture a sharp temperature inversion seen in the radiosonde profiles at 2 km, and consequently the cloud top temperature in the model was able to reach lower values than observed in-situ or obtained from satellite data. ACPIM simulations confirmed the HM process to be a very powerful mechanism for producing the observed high ice concentrations, provided that primary nucleation occured to initiate the ice formation, and large droplets were present which then fell collecting the primary ice particles to form instant rimer particles. However, the time to generate the observed peak ice concentrations was found to be dependant on the number of primary IN present (decreasing with increasing IN number). This became realistic (around 20 min) only when the temperature input to the existing IN parameterisation was 6 °C lower than observed at cloud top, highlighting the requirement to improve basic knowledge of the number and type of IN active at these high temperatures. In simulations where cloud droplet numbers were realistic the precipitation rate was found to be unaffected by HM, with warm rain processes dominating precipitation development in this instance.

Space Weather Connections to Clouds and Climate

NASA Astrophysics Data System (ADS)

Tinsley, B. A.

2004-12-01

There is now a considerable amount of observational data and theoretical work pointing to a link between space weather and atmospheric electricity, and then between atmospheric electricity and cloud cover and precipitation, which ultimately affect climate and the biosphere. Studies so far have been largely confined to the Earth, but may be applicable to all planets with clouds in their atmospheres. The current density Jz, that is the return current flowing downward through clouds in the global circuit, is modulated by the galactic cosmic ray flux; by solar energetic particles; by the dawn-dusk polar cap potential difference; and by the precipitation of relativistic electrons from the radiation belts. The flow of Jz through clouds generates unipolar space charge, which is positive at cloud tops and negative at cloud base. This charge attaches to aerosol particles, and affects their interaction with other particles and droplets. Ultrafine aerosol particles are formed around ions and are preserved from scavenging on background aerosols, and preserved for growth by vapor deposition, by space charge at the bases and tops of layer clouds. There is electro-preservation of both ultrafines and of existing CCN that leads to increases in CCN concentration, and increases in cloud cover and reduction in both droplet size and precipitation by the `indirect aerosol effect'. For cold clouds and larger aerosol particles that act as ice forming nuclei, the rate of scavenging of the IFN by large supercooled droplets varies with space charge. Changes in space weather affect both ion production and Jz in planetary atmospheres. In addition, changes in cosmic ray flux affect conductivity within thunderclouds and may affect the output of the thundercloud generators in the global circuit. Thus all four processes, (a) ion-induced nucleation, (b) electro-preservation of leading to increases in CCN concentration and the indirect aerosol effect, (c) contact ice nucleation affecting the production of ices, (d) cosmic ray effects on the generators of the global circuit, are potential links between space weather and life on planets.

Solar Effects on Global Climate Due to Cosmic Rays and Solar Energetic Particles

NASA Technical Reports Server (NTRS)

Turco, R. P.; Raeder, J.; DAuria, R.

2005-01-01

Although the work reported here does not directly connect solar variability with global climate change, this research establishes a plausible quantitative causative link between observed solar activity and apparently correlated variations in terrestrial climate parameters. Specifically, we have demonstrated that ion-mediated nucleation of atmospheric particles is a likely, and likely widespread, phenomenon that relates solar variability to changes in the microphysical properties of clouds. To investigate this relationship, we have constructed and applied a new model describing the formation and evolution of ionic clusters under a range of atmospheric conditions throughout the lower atmosphere. The activation of large ionic clusters into cloud nuclei is predicted to be favorable in the upper troposphere and mesosphere, and possibly in the lower stratosphere. The model developed under this grant needs to be extended to include additional cluster families, and should be incorporated into microphysical models to further test the cause-and-effect linkages that may ultimately explain key aspects of the connections between solar variability and climate.

Why do Tornados and Hail Storms Rest on Weekends?

NASA Technical Reports Server (NTRS)

Rosenfeld, Daniel; Bell, Thomas L.

2010-01-01

When anthropogenic aerosols over the eastern USA during summertime are at their weekly mid-week peak, tornado and hail storm activity there is also near its weekly maximum. The weekly cycle in storm activity is statistically significant and unlikely to be due to natural variability. The pattern of variability supports the hypothesis that air pollution aerosols invigorate deep convective clouds in a moist, unstable atmosphere, to the extent of inducing production of large hailstones and tornados. This is caused by the effect of aerosols on cloud-drop nucleation, making cloud drops smaller, delaying precipitation-forming processes and their evaporation, and hence affecting cloud dynamics.

Insights on the Feasibility, Modeling and Field Testing of Cirrus Cloud Thinning from Satellite Remote Sensing

NASA Astrophysics Data System (ADS)

Mitchell, D. L.; Garnier, A.; Mejia, J.; Avery, M. A.; Erfani, E.

2016-12-01

To date, it is not clear whether the climate intervention method known as cirrus cloud thinning (CCT) can be viable since it requires cirrus clouds to form through homogeneous ice nucleation (henceforth hom) and some recent GCM studies predict cirrus are formed primarily through heterogeneous ice nucleation (henceforth het). A new CALIPSO infrared retrieval method has been developed for single-layer cirrus cloud that measures the temperature dependence of their layer-averaged number concentration N, effective diameter De and ice water content for optical depths (OD) between 0.3 and 3.0. Based on N, the prevailing ice nucleation mechanism (hom or het) can be estimated as a function of temperature, season, latitude and surface type. These satellite results indicate that seeding cirrus clouds at high latitudes during winter may produce significant global surface cooling. This is because hom often appears to dominate over land during winter north of 30°N latitude while the same appears true for most of the Southern Hemisphere (south of 30°S) during all seasons. Moreover, the sampled cirrus cloud frequency of occurrence in the Arctic is at least twice as large during winter relative to other seasons, while frequency of occurrence in the Antarctic peaks in the spring and is second-highest during winter. During Arctic winter, a combination of frequent hom cirrus, maximum cirrus coverage and an extreme or absent sun angle produces the maximum seasonal cirrus net radiative forcing (warming). Thus a reduction in OD and coverage (via CCT) for these cirrus clouds could yield a significant net cooling effect. From these CALIPSO retrievals, De-T relationships are generated as a function of season, latitude and surface type (land vs. ocean). These will be used in CAM5 to estimate De and the ice fall speed, from which the cirrus radiative forcing will be estimated during winter north of 30°latitude, where hom cirrus are common. Another CAM5 simulation will replace the hom cirrus De-T relationships with those corresponding to het cirrus (at similar latitudes). In this way the potential cooling from CCT in the Northern Hemisphere will be estimated. If a field campaign was ever conducted for testing the efficacy of CCT, this CALIPSO retrieval could be used to help determine whether the seeded hom cirrus were transformed into het cirrus.

The potential effects of volcanic aerosols on cirrus cloud microphysics

NASA Technical Reports Server (NTRS)

Jensen, Eric J.; Toon, Owen B.

1992-01-01

The potential impact of volcanic aerosols on nucleation of ice crystals in upper tropospheric cirrus clouds is examined from a microphysical perspective. The sulfuric acid aerosols which form in the stratosphere are presumably transported into the troposphere by sedimentation and tropopause folding. The tropospheric volcanic aerosol size distribution is estimated from 10-micron lidar backscatter and in situ measurements. Microphysical simulations suggest that at temperatures below about -50 C the concentration of ice crystals which nucleate may be as much as a factor of 5 larger when volcanic aerosols are present. The simulations suggest that the presence of volcanic aerosols may increase the net radiative forcing (surface warming) of certain types of cirrus near the tropopause by as much as 8 W/sq m. Further observations are required to determine whether these effects actually occur, and their global impact.

Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel

How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20°C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that depositionmore » plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm -3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm -3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces supercooled water content and increases the cloud glaciation temperature, while increasing CCN has the opposite effect with much smaller significance.« less

Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

DOE PAGES

Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel; ...

2017-01-23

How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20°C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that depositionmore » plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm -3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm -3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces supercooled water content and increases the cloud glaciation temperature, while increasing CCN has the opposite effect with much smaller significance.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

None, None

This 3-year project has studied how aerosol pollution influences glaciated clouds. The tool applied has been an 'aerosol-cloud model'. It is a type of Cloud-System Resolving Model (CSRM) modified to include 2-moment bulk microphysics and 7 aerosol species, as described by Phillips et al. (2009, 2013). The study has been done by, first, improving the model and then performing sensitivity studies with validated simulations of a couple of observed cases from ARM. These are namely the Tropical Warm Pool International Cloud Experiment (TWP-ICE) over the tropical west Pacific and the Cloud and Land Surface Interaction Campaign (CLASIC) over Oklahoma. Duringmore » the project, sensitivity tests with the model showed that in continental clouds, extra liquid aerosols (soluble aerosol material) from pollution inhibited warm rain processes for precipitation production. This promoted homogeneous freezing of cloud droplets and aerosols. Mass and number concentrations of cloud-ice particles were boosted. The mean sizes of cloud-ice particles were reduced by the pollution. Hence, the lifetime of glaciated clouds, especially ice-only clouds, was augmented due to inhibition of sedimentation and ice-ice aggregation. Latent heat released from extra homogeneous freezing invigorated convective updrafts, and raised their maximum cloud-tops, when aerosol pollution was included. In the particular cases simulated in the project, the aerosol indirect effect of glaciated clouds was twice than of (warm) water clouds. This was because glaciated clouds are higher in the troposphere than water clouds and have the first interaction with incoming solar radiation. Ice-only clouds caused solar cooling by becoming more extensive as a result of aerosol pollution. This 'lifetime indirect effect' of ice-only clouds was due to higher numbers of homogeneously nucleated ice crystals causing a reduction in their mean size, slowing the ice-crystal process of snow production and slowing sedimentation. In addition to the known indirect effects (glaciation, riming and thermodynamic), new indirect effects were discovered and quantified due to responses of sedimentation, aggregation and coalescence in glaciated clouds to changing aerosol conditions. In summary, the change in horizontal extent of the glaciated clouds ('lifetime indirect effects'), especially of ice-only clouds, was seen to be of higher importance in regulating aerosol indirect effects than changes in cloud properties ('cloud albedo indirect effects').« less

Using depolarization to quantify ice nucleating particle concentrations: a new method

NASA Astrophysics Data System (ADS)

Zenker, Jake; Collier, Kristen N.; Xu, Guanglang; Yang, Ping; Levin, Ezra J. T.; Suski, Kaitlyn J.; DeMott, Paul J.; Brooks, Sarah D.

2017-12-01

We have developed a new method to determine ice nucleating particle (INP) concentrations observed by the Texas A&M University continuous flow diffusion chamber (CFDC) under a wide range of operating conditions. In this study, we evaluate differences in particle optical properties detected by the Cloud and Aerosol Spectrometer with POLarization (CASPOL) to differentiate between ice crystals, droplets, and aerosols. The depolarization signal from the CASPOL instrument is used to determine the occurrence of water droplet breakthrough (WDBT) conditions in the CFDC. The standard procedure for determining INP concentration is to count all particles that have grown beyond a nominal size cutoff as ice crystals. During WDBT this procedure overestimates INP concentration, because large droplets are miscounted as ice crystals. Here we design a new analysis method based on depolarization ratio that can extend the range of operating conditions of the CFDC. The method agrees reasonably well with the traditional method under non-WDBT conditions with a mean percent error of ±32.1 %. Additionally, a comparison with the Colorado State University CFDC shows that the new analysis method can be used reliably during WDBT conditions.

The Horizontal Ice Nucleation Chamber (HINC): INP measurements at conditions relevant for mixed-phase clouds at the High Altitude Research Station Jungfraujoch

NASA Astrophysics Data System (ADS)

Lacher, Larissa; Lohmann, Ulrike; Boose, Yvonne; Zipori, Assaf; Herrmann, Erik; Bukowiecki, Nicolas; Steinbacher, Martin; Kanji, Zamin A.

2017-12-01

In this work we describe the Horizontal Ice Nucleation Chamber (HINC) as a new instrument to measure ambient ice-nucleating particle (INP) concentrations for conditions relevant to mixed-phase clouds. Laboratory verification and validation experiments confirm the accuracy of the thermodynamic conditions of temperature (T) and relative humidity (RH) in HINC with uncertainties in T of ±0.4 K and in RH with respect to water (RHw) of ±1.5 %, which translates into an uncertainty in RH with respect to ice (RHi) of ±3.0 % at T > 235 K. For further validation of HINC as a field instrument, two measurement campaigns were conducted in winters 2015 and 2016 at the High Altitude Research Station Jungfraujoch (JFJ; Switzerland, 3580 m a. s. l. ) to sample ambient INPs. During winters 2015 and 2016 the site encountered free-tropospheric conditions 92 and 79 % of the time, respectively. We measured INP concentrations at 242 K at water-subsaturated conditions (RHw = 94 %), relevant for the formation of ice clouds, and in the water-supersaturated regime (RHw = 104 %) to represent ice formation occurring under mixed-phase cloud conditions. In winters 2015 and 2016 the median INP concentrations at RHw = 94 % was below the minimum detectable concentration. At RHw = 104 %, INP concentrations were an order of magnitude higher, with median concentrations in winter 2015 of 2.8 per standard liter (std L-1; normalized to standard T of 273 K and pressure, p, of 1013 hPa) and 4.7 std L-1 in winter 2016. The measurements are in agreement with previous winter measurements obtained with the Portable Ice Nucleation Chamber (PINC) of 2.2 std L-1 at the same location. During winter 2015, two events caused the INP concentrations at RHw = 104 % to significantly increase above the campaign average. First, an increase to 72.1 std L-1 was measured during an event influenced by marine air, arriving at the JFJ from the North Sea and the Norwegian Sea. The contribution from anthropogenic or other sources can thereby not be ruled out. Second, INP concentrations up to 146.2 std L-1 were observed during a Saharan dust event. To our knowledge this is the first time that a clear enrichment in ambient INP concentration in remote regions of the atmosphere is observed during a time of marine air mass influence, suggesting the importance of marine particles on ice nucleation in the free troposphere.

Polar winter cloud depolarization measurements with the CANDAC Rayleigh-Mie-Raman Lidar

NASA Astrophysics Data System (ADS)

McCullough, E. M.; Nott, G. J.; Duck, T. J.; Sica, R. J.; Doyle, J. G.; Pike-thackray, C.; Drummond, J. R.

2011-12-01

Clouds introduce a significant positive forcing to the Arctic radiation budget and this is strongest during the polar winter when shortwave radiation is absent (Intrieri et al., 2002). The amount of forcing depends on the occurrence probability and optical depth of the clouds as well as the cloud particle phase (Ebert and Curry 1992). Mixed-phase clouds are particularly complex as they involve interactions between three phases of water (vapour, liquid and ice) coexisting in the same cloud. Although significant progress has been made in characterizing wintertime Arctic clouds (de Boer et al., 2009 and 2011), there is considerable variability in the relative abundance of particles of each phase, in the morphology of solid particles, and in precipitation rates depending on the meteorology at the time. The Canadian Network for the Detection of Atmospheric Change (CANDAC) Rayleigh-Mie-Raman Lidar (CRL) was installed in the Canadian High Arctic at Eureka, Nunavut (80°N, 86°W) in 2008-2009. The remotely-operated system began with measurement capabilities for multi-wavelength aerosol extinction, water vapour mixing ratio, and tropospheric temperature profiles, as well as backscatter cross section coefficient and colour ratio. In 2010, a new depolarization channel was added. The capability to measure the polarization state of the return signal allows the characterization of the cloud in terms of liquid and ice water content, enabling the lidar to probe all three phases of water in these clouds. Lidar depolarization results from 2010 and 2011 winter clouds at Eureka will be presented, with a focus on differences in downwelling radiation between mixed phase clouds and ice clouds. de Boer, G., E.W. Eloranta, and M.D. Shupe (2009), Arctic mixed-phase stratiform cloud properties from multiple years of surface-based measurements at two high-latitude locations, Journal of Atmospheric Sciences, 66 (9), 2874-2887. de Boer, G., H. Morrison, M. D. Shupe, and R. Hildner (2011), Evidence of liquid dependent ice nucleation in high-latitude stratiform clouds from surface remote sensors, Geophysical Research Letters, 38, L01803. Ebert, EE and J.A .Curry (1992), A parameterization of ice cloud optical properties for climate models, Journal of Geophysical Research 97:3831-3836. Intrieri JM, Fairall CW, Shupe MD, Persson POG, Andreas EL, Guest PS, Moritz RE. 2002. An annual cycle of Arctic surface cloud forcing at SHEBA. Journal of Geophysical Research 107 NO. C10, 8039 . Noel, V., H. Chepfer, M. Haeffelin, and Y. Morille (2006), Classification of ice crystal shapes in midlatitude ice clouds from three years of lidar observations over the SIRTA observatory. Journal of the Atmospheric Sciences, 63:2978 - 2991.

Assessment of the first indirect radiative effect of ammonium-sulfate-nitrate aerosols in East Asia

NASA Astrophysics Data System (ADS)

Han, Xiao; Zhang, Meigen; Skorokhod, Andrei

2017-11-01

A physically based cloud nucleation parameterization was introduced into an optical properties/radiative transfer module incorporated with the off-line air quality modeling system Regional Atmospheric Modeling System (RAMS)-Models-3 Community Multi Scale Air Quality (CMAQ) to investigate the distribution features of the first indirect radiative effects of sulfate, nitrate, and ammonium-sulfate-nitrate (ASN) over East Asia for the years of 2005, 2010, and 2013. The relationship between aerosol particles and cloud droplet number concentration could be properly described by this parameterization because the simulated cloud fraction and cloud liquid water path were generally reliable compared with Moderate Resolution Imaging Spectroradiometer (MODIS) retrieved data. Simulation results showed that the strong effect of indirect forcing was mainly concentrated in Southeast China, the East China Sea, the Yellow Sea, and the Sea of Japan. The highest indirect radiative forcing of ASN reached -3.47 W m-2 over Southeast China and was obviously larger than the global mean of the indirect forcing of all anthropogenic aerosols. In addition, sulfate provided about half of the contribution to the ASN indirect forcing effect. However, the effect caused by nitrate was weak because the mass burden of nitrate was very low during summer, whereas the cloud fraction was the highest. The analysis indicated that even though the interannual variation of indirect forcing magnitude generally followed the trend of aerosol mass burden from 2005 to 2013, the cloud fraction was an important factor that determined the distribution pattern of indirect forcing. The heaviest aerosol loading in North China did not cause a strong radiative effect because of the low cloud fraction over this region.

Heterogeneous Ice Nucleation: Interplay of Surface Properties and Their Impact on Water Orientations.

PubMed

Glatz, Brittany; Sarupria, Sapna

2018-01-23

Ice is ubiquitous in nature, and heterogeneous ice nucleation is the most common pathway of ice formation. How surface properties affect the propensity to observe ice nucleation on that surface remains an open question. We present results of molecular dynamics studies of heterogeneous ice nucleation on model surfaces. The models surfaces considered emulate the chemistry of kaolinite, an abundant component of mineral dust. We investigate the interplay of surface lattice and hydrogen bonding properties in affecting ice nucleation. We find that lattice matching and hydrogen bonding are necessary but not sufficient conditions for observing ice nucleation at these surfaces. We correlate this behavior to the orientations sampled by the metastable supercooled water in contact with the surfaces. We find that ice is observed in cases where water molecules not only sample orientations favorable for bilayer formation but also do not sample unfavorable orientations. This distribution depends on both surface-water and water-water interactions and can change with subtle modifications to the surface properties. Our results provide insights into the diverse behavior of ice nucleation observed at different surfaces and highlight the complexity in elucidating heterogeneous ice nucleation.

The composition of nucleation and Aitken modes particles during coastal nucleation events: evidence for marine secondary organic contribution

NASA Astrophysics Data System (ADS)

Vaattovaara, P.; Huttunen, P. E.; Yoon, Y. J.; Joutsensaari, J.; Lehtinen, K. E. J.; O'Dowd, C. D.; Laaksonen, A.

2006-04-01

Newly-formed nanometer-sized particles have been observed at coastal and marine environments worldwide. Interestingly, organic species have so far not been detected in those newly-formed nucleation mode particles. In this study, we applied the UFO-TDMA (ultrafine organic tandem differential mobility analyzer) method to study the possible existence of an organic fraction in recently formed coastal nucleation mode particles (d<20 nm) at the Mace Head research station. Furthermore, effects of those nucleation events to potential CCN (cloud condensation nuclei) were studied. The coastal events were typical for the Mace Head region and they occurred at low tide conditions during efficient solar radiation and high biological activity (HBA, i.e. a high mass concentration of chlorophyll a of the ocean) in spring 2002. Additionally, a PHA-UCPC (pulse height analyzer ultrafine condensation particle counter) technique was used to study the composition of newly-formed particles formed in low tide conditions during a lower biological activity (LBA, i.e. a lower mass concentration of chlorophyll a of the ocean) in October 2002. The overall results of the UFO-TDMA and the PHA-UCPC measurements indicate that those coastally/marinely formed nucleation mode particles include a remarkable fraction of secondary organic products, beside iodine oxides, which are likely to be responsible for the nucleation. During clean marine air mass conditions, the origin of those secondary organic oxidation compounds can be related to marine/coastal biota and thus a major fraction of the organics may originate from biosynthetic production of alkenes such as isoprene and their oxidation by iodine, hydroxyl radical, and ozone. During modified marine conditions, also anthropogenic secondary organic compounds may contribute to the nucleation mode organic mass, in addition to biogenic secondary organic compounds. Thus, the UFO-TDMA results suggest that the secondary organic compounds may, in addition to being significant contributors to the nucleation mode processes, accelerate the growth of freshly nucleated particles and increase their survival probability to CCN and even larger radiatively active particle sizes. The results give new insights to the coastal/marine particle formation, growth, and properties. The marine biota driven secondary organic contributions to coastal/marine particle formation and composition can be anticipated in other species specific biologically active oceans and fresh-waters areas around the world and thus, they may be significant also to the global radiative bugdet, atmosphere-biosphere feedbacks, and climate change.

Effects of Atmospheric Dynamics and Aerosols on the Fraction of Supercooled Water Clouds

NASA Astrophysics Data System (ADS)

Li, J.

2016-12-01

Based on the 8 years (2007-2015) of data of cloud phase information from the GCM-Oriented Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) Cloud Product (GOCCP), aerosol products from CALIPSO, and meteorological parameters from the ERA-Interim products, this study investigates the effects of atmospheric dynamics on the supercooled liquid cloud fraction (SCF) under different aerosol loadings at a global scale in order to better understand the conditions under which supercooled liquid water will gradually transform to ice phase. Statistical results indicate that aerosols' effect on nucleation cannot fully explain all SCF changes, especially in those regions where aerosols' effect on nucleation is not a first-order influence (e.g., due to low IN aerosol frequency). By performing the temporal and spatial correlations between SCFs and different meteorological factors, we find that the impacts of different meteorological factors on SCFs contain obvious regional differences. In the tropics, obvious positive correlations between SCFs and vertical velocity and relative humidity indicate that high vertical velocity and relative humidity suppress ice formation. However, the impacts of LTSS, skin temperature and horizontal wind on SCFs are relatively complex than those of vertical velocity and humidity. But, their effects are predominantly located in middle and high latitudes, and the temporal correlations with SCFs depend on latitude or surface type. In addition, this study also indicates that strong horizontal wind inhibits the glaciation of supercooled droplets in the middle and high latitudes. Our results verify the importance and regional of dynamical factors on the changes of supercooled water cloud fraction, thus have potential implications for further improving the parameterization of the cloud phase and determining the climate feedbacks.

Heterogeneous nucleation and its relationship to precipitation type. Technical memo

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smith, G.

1995-04-01

The purpose of this study is to present important elements of cloud microphysics that will be useful to the operational meteorologist in determining precipitation type. Synoptic-scale environments and vertical atmospheric structures of cases, where freezing precipitation occurred, will be examined. Furthermore, only cases in which the entire depth of the troposphere was below freezing are studied. The absences of lower tropospheric warm layers (above freezing) suggest that the primary atmospheric process that influenced precipitation type was heterogeneous nucleation rather than melting.

Importance of the mixing state for ice nucleating capabilities of individual aerosol particles

NASA Astrophysics Data System (ADS)

Ebert, Martin; Worringen, Annette; Benker, Nathalie; Weinbruch, Stephan

2010-05-01

The effects of aerosol particles on heterogeneous ice formation are currently insufficiently understood. Modelling studies have shown that the type and quantity of atmospheric aerosol particles acting as ice nuclei (IN) can influence ice cloud microphysical and radiative properties as well as their precipitation efficiency. Therefore, the physicochemical identification of IN and a quantitative description of the ice nucleation processes are crucial for a better understanding of formation, life cycles, and the optical properties of clouds as well as for numerical precipitation forecast. During the CLACE 5 campaign in 2006 at the high alpine research station Jungfraujoch (3580 m asl), Switzerland, the physicochemical parameters of IN within mixed-phase clouds were studied. By the use of special Ice-Counterflow Virtual Impactor, residual particles of small ice nuclei (IN) and the interstitial aerosol fraction were sampled seperately within mixed-phase clouds. The size, morphology, elemental composition and mixing state of more than 7000 particles of selected IN- and interstitial-samples were analyzed by scanning electron microscopy (SEM) combined with energy-dispersive X-ray analysis (EDX). For selected particles, the mineralogical phase composition was determined by transmission electron microscopy. In order to receive detailed information about the mixing state (coatings, agglomerates, heterogeneous inclusions) of the IN- and interstitial-samples, the complete individual particle analysis was performed operator controlled. Four different particle types were identified to act as IN. 1) Carbonaceous particles, which were identified to be a complex mixture of soot (main component), sulfate and nitrate. 2) Complex mixtures of two or more diverse particle groups. In almost 75% of these particles silicates or metal oxides are the main-component. 3) Aluminium oxide particles, which were internally mixed with calcium and sulphate rich material and 4) Pb bearing particles. The high abundance of Pb-bearing particles in the IN-samples (up to 24% by number) was an unexpected finding. Besides a smaller content of larger PbO and PbCl2-particles the main component of the particles within this type are predominantly sea salt, soot or silicates, while Pb in these particles is only present as small (50 - 500 nm) heterogeneous Pb or PbS inclusions. In all 4 particle types identified as IN, the mixing state seems to play an essential role. Therefore it can be concluded that the determination of the main-component of a particle is not sufficient for the prediction of its IN-capability.

Fungal spores as potential ice nuclei in fog/cloud water and snow

NASA Astrophysics Data System (ADS)

Bauer, Heidi; Goncalves, Fabio L. T.; Schueller, Elisabeth; Puxbaum, Hans

2010-05-01

INTRODUCTION: In discussions about climate change and precipitation frequency biological ice nucleation has become an issue. While bacterial ice nucleation (IN) is already well characterized and even utilized in industrial processes such as the production of artificial snow or to improve freezing processes in food industry, less is known about the IN potential of fungal spores which are also ubiquitous in the atmosphere. A recent study performed at a mountain top in the Rocky Mountains suggests that fungal spores and/or pollen might play a role in increased IN abundance during periods of cloud cover (Bowers et al. 2009). In the present work concentrations of fungal spores in fog/cloud water and snow were determined. EXPERIMENTAL: Fog samples were taken with an active fog sampler in 2008 in a traffic dominated area and in a national park in São Paulo, Brazil. The number concentrations of fungal spores were determined by microscopic by direct enumeration by epifluorescence microscopy after staining with SYBR Gold nucleic acid gel stain (Bauer et al. 2008). RESULTS: In the fog water collected in the polluted area at a junction of two highly frequented highways around 22,000 fungal spores mL-1 were counted. Fog in the national park contained 35,000 spores mL-1. These results were compared with cloud water and snow samples from Mt. Rax, situated at the eastern rim of the Austrian Alps. Clouds contained on average 5,900 fungal spores mL-1 cloud water (1,300 - 11,000) or 2,200 spores m-3 (304 - 5,000). In freshly fallen snow spore concentrations were lower than in cloud water, around 1,000 fungal spores mL-1 were counted (Bauer et al. 2002). In both sets of samples representatives of the ice nucleating genus Fusarium could be observed. REFERENCES: Bauer, H., Kasper-Giebl, A., Löflund, M., Giebl, H., Hitzenberger, R., Zibuschka, F., Puxbaum, H. (2002). The contribution of bacteria and fungal spores to the organic carbon content of cloud water, precipitation and aerosols. Atmos. Res. 64, 109-119. Bauer, H., Schueller, E., Weinke, G. Berger, A., Hitzenberger, R., Marr, I.L., Puxbaum, H. (2008). Significant contributions of fungal spores to the organic carbon and to the aerosol mass balance of the urban atmospheric aerosol. Atmos. Environ. 42, 5542-5549. Bowers, R.M., Lauber, C.L., Wiedinmyer, C., Hamady, M., Hallar, A.G., Fall, R., Knight, R., Fierer, N. (2009). Characterization of airborne microbial communities at a high-elevation site and their potential to act as atmospheric ice nuclei. Appl. Environ. Microbiol: 75, 5121-5130.

In situ measurements of cloud microphysics and aerosol over coastal Antarctica during the MAC campaign

NASA Astrophysics Data System (ADS)

O'Shea, Sebastian J.; Choularton, Thomas W.; Flynn, Michael; Bower, Keith N.; Gallagher, Martin; Crosier, Jonathan; Williams, Paul; Crawford, Ian; Fleming, Zoë L.; Listowski, Constantino; Kirchgaessner, Amélie; Ladkin, Russell S.; Lachlan-Cope, Thomas

2017-11-01

During austral summer 2015, the Microphysics of Antarctic Clouds (MAC) field campaign collected unique and detailed airborne and ground-based in situ measurements of cloud and aerosol properties over coastal Antarctica and the Weddell Sea. This paper presents the first results from the experiment and discusses the key processes important in this region, which is critical to predicting future climate change. The sampling was predominantly of stratus clouds, at temperatures between -20 and 0 °C. These clouds were dominated by supercooled liquid water droplets, which had a median concentration of 113 cm-3 and an interquartile range of 86 cm-3. Both cloud liquid water content and effective radius increased closer to cloud top. The cloud droplet effective radius increased from 4 ± 2 µm near cloud base to 8 ± 3 µm near cloud top. Cloud ice particle concentrations were highly variable with the ice tending to occur in small, isolated patches. Below approximately 1000 m, glaciated cloud regions were more common at higher temperatures; however, the clouds were still predominantly liquid throughout. When ice was present at temperatures higher than -10 °C, secondary ice production most likely through the Hallett-Mossop mechanism led to ice concentrations 1 to 3 orders of magnitude higher than the number predicted by commonly used primary ice nucleation parameterisations. The drivers of the ice crystal variability are investigated. No clear dependence on the droplet size distribution was found. The source of first ice in the clouds remains uncertain but may include contributions from biogenic particles, blowing snow or other surface ice production mechanisms. The concentration of large aerosols (diameters 0.5 to 1.6 µm) decreased with altitude and were depleted in air masses that originated over the Antarctic continent compared to those more heavily influenced by the Southern Ocean and sea ice regions. The dominant aerosol in the region was hygroscopic in nature, with the hygroscopicity parameter κ having a median value for the campaign of 0.66 (interquartile range of 0.38). This is consistent with other remote marine locations that are dominated by sea salt/sulfate.

Particle backscatter and relative humidity measured across cirrus clouds and comparison with microphysical cirrus modelling

NASA Astrophysics Data System (ADS)

Brabec, M.; Wienhold, F. G.; Luo, B. P.; Vömel, H.; Immler, F.; Steiner, P.; Hausammann, E.; Weers, U.; Peter, T.

2012-10-01

Advanced measurement and modelling techniques are employed to estimate the partitioning of atmospheric water between the gas phase and the condensed phase in and around cirrus clouds, and thus to identify in-cloud and out-of-cloud supersaturations with respect to ice. In November 2008 the newly developed balloon-borne backscatter sonde COBALD (Compact Optical Backscatter and AerosoL Detector) was flown 14 times together with a CFH (Cryogenic Frost point Hygrometer) from Lindenberg, Germany (52° N, 14° E). The case discussed here in detail shows two cirrus layers with in-cloud relative humidities with respect to ice between 50% and 130%. Global operational analysis data of ECMWF (roughly 1° × 1° horizontal and 1 km vertical resolution, 6-hourly stored fields) fail to represent ice water contents and relative humidities. Conversely, regional COSMO-7 forecasts (6.6 km × 6.6 km, 5-min stored fields) capture the measured humidities and cloud positions remarkably well. The main difference between ECMWF and COSMO data is the resolution of small-scale vertical features responsible for cirrus formation. Nevertheless, ice water contents in COSMO-7 are still off by factors 2-10, likely reflecting limitations in COSMO's ice phase bulk scheme. Significant improvements can be achieved by comprehensive size-resolved microphysical and optical modelling along backward trajectories based on COSMO-7 wind and temperature fields, which allow accurate computation of humidities, homogeneous ice nucleation, resulting ice particle size distributions and backscatter ratios at the COBALD wavelengths. However, only by superimposing small-scale temperature fluctuations, which remain unresolved by the numerical weather prediction models, can we obtain a satisfying agreement with the observations and reconcile the measured in-cloud non-equilibrium humidities with conventional ice cloud microphysics. Conversely, the model-data comparison provides no evidence that additional changes to ice-cloud microphysics - such as heterogeneous nucleation or changing the water vapour accommodation coefficient on ice - are required.

Bacteria in atmospheric waters: Detection, characteristics and implications

NASA Astrophysics Data System (ADS)

Hu, Wei; Niu, Hongya; Murata, Kotaro; Wu, Zhijun; Hu, Min; Kojima, Tomoko; Zhang, Daizhou

2018-04-01

In this review paper, we synthesize the current knowledges about bacteria in atmospheric waters, e.g., cloud, fog, rain, and snow, most of which were obtained very recently. First, we briefly describe the importance of bacteria in atmospheric waters, i.e., the essentiality of studying bacteria in atmospheric waters in understanding aerosol-cloud-precipitation-climate interactions in the Earth system. Next, approaches to collect atmospheric water samples for the detection of bacteria and methods to identify the bacteria are summarized and compared. Then the available data on the abundance, viability and community composition of bacteria in atmospheric waters are summarized. The average bacterial concentration in cloud water was usually on the order 104-105 cells mL-1, while that in precipitation on the order 103-104 cells mL-1. Most of the bacteria were viable or metabolically active. Their community composition was highly diverse and differed at various sites. Factors potentially influencing the bacteria, e.g., air pollution levels and sources, meteorological conditions, seasonal effect, and physicochemical properties of atmospheric waters, are described. After that, the implications of bacteria present in atmospheric waters, including their effect on nucleation in clouds, atmospheric chemistry, ecosystems and public health, are briefly discussed. Finally, based on the current knowledges on bacteria in atmospheric waters, which in fact remains largely unknown, we give perspectives that should be paid attention to in future studies.

Kinetics of spontaneous filament nucleation via oligomers: Insights from theory and simulation

NASA Astrophysics Data System (ADS)

Šarić, Andela; Michaels, Thomas C. T.; Zaccone, Alessio; Knowles, Tuomas P. J.; Frenkel, Daan

2016-12-01

Nucleation processes are at the heart of a large number of phenomena, from cloud formation to protein crystallization. A recently emerging area where nucleation is highly relevant is the initiation of filamentous protein self-assembly, a process that has broad implications in many research areas ranging from medicine to nanotechnology. As such, spontaneous nucleation of protein fibrils has received much attention in recent years with many theoretical and experimental studies focussing on the underlying physical principles. In this paper we make a step forward in this direction and explore the early time behaviour of filamentous protein growth in the context of nucleation theory. We first provide an overview of the thermodynamics and kinetics of spontaneous nucleation of protein filaments in the presence of one relevant degree of freedom, namely the cluster size. In this case, we review how key kinetic observables, such as the reaction order of spontaneous nucleation, are directly related to the physical size of the critical nucleus. We then focus on the increasingly prominent case of filament nucleation that includes a conformational conversion of the nucleating building-block as an additional slow step in the nucleation process. Using computer simulations, we study the concentration dependence of the nucleation rate. We find that, under these circumstances, the reaction order of spontaneous nucleation with respect to the free monomer does no longer relate to the overall physical size of the nucleating aggregate but rather to the portion of the aggregate that actively participates in the conformational conversion. Our results thus provide a novel interpretation of the common kinetic descriptors of protein filament formation, including the reaction order of the nucleation step or the scaling exponent of lag times, and put into perspective current theoretical descriptions of protein aggregation.

Kinetics of spontaneous filament nucleation via oligomers: Insights from theory and simulation.

PubMed

Šarić, Anđela; Michaels, Thomas C T; Zaccone, Alessio; Knowles, Tuomas P J; Frenkel, Daan

2016-12-07

Nucleation processes are at the heart of a large number of phenomena, from cloud formation to protein crystallization. A recently emerging area where nucleation is highly relevant is the initiation of filamentous protein self-assembly, a process that has broad implications in many research areas ranging from medicine to nanotechnology. As such, spontaneous nucleation of protein fibrils has received much attention in recent years with many theoretical and experimental studies focussing on the underlying physical principles. In this paper we make a step forward in this direction and explore the early time behaviour of filamentous protein growth in the context of nucleation theory. We first provide an overview of the thermodynamics and kinetics of spontaneous nucleation of protein filaments in the presence of one relevant degree of freedom, namely the cluster size. In this case, we review how key kinetic observables, such as the reaction order of spontaneous nucleation, are directly related to the physical size of the critical nucleus. We then focus on the increasingly prominent case of filament nucleation that includes a conformational conversion of the nucleating building-block as an additional slow step in the nucleation process. Using computer simulations, we study the concentration dependence of the nucleation rate. We find that, under these circumstances, the reaction order of spontaneous nucleation with respect to the free monomer does no longer relate to the overall physical size of the nucleating aggregate but rather to the portion of the aggregate that actively participates in the conformational conversion. Our results thus provide a novel interpretation of the common kinetic descriptors of protein filament formation, including the reaction order of the nucleation step or the scaling exponent of lag times, and put into perspective current theoretical descriptions of protein aggregation.

What Determines the Ice Polymorph in Clouds?

PubMed

Hudait, Arpa; Molinero, Valeria

2016-07-20

Ice crystals in the atmosphere nucleate from supercooled liquid water and grow by vapor uptake. The structure of the ice polymorph grown has strong impact on the morphology and light scattering of the ice crystals, modulates the amount of water vapor in ice clouds, and can impact the molecular uptake and reactivity of atmospheric aerosols. Experiments and molecular simulations indicate that ice nucleated and grown from deeply supercooled liquid water is metastable stacking disordered ice. The ice polymorph grown from vapor has not yet been determined. Here we use large-scale molecular simulations to determine the structure of ice that grows as a result of uptake of water vapor in the temperature range relevant to cirrus and mixed-phase clouds, elucidate the molecular mechanism of the formation of ice at the vapor interface, and compute the free energy difference between cubic and hexagonal ice interfaces with vapor. We find that vapor deposition results in growth of stacking disordered ice only under conditions of extreme supersaturation, for which a nonequilibrium liquid layer completely wets the surface of ice. Such extreme conditions have been used to produce stacking disordered frost ice in experiments and may be plausible in the summer polar mesosphere. Growth of ice from vapor at moderate supersaturations in the temperature range relevant to cirrus and mixed-phase clouds, from 200 to 260 K, produces exclusively the stable hexagonal ice polymorph. Cubic ice is disfavored with respect to hexagonal ice not only by a small penalty in the bulk free energy (3.6 ± 1.5 J mol(-1) at 260 K) but also by a large free energy penalty at the ice-vapor interface (89.7 ± 12.8 J mol(-1) at 260 K). The latter originates in higher vibrational entropy of the hexagonal-terminated ice-vapor interface. We predict that the free energy penalty against the cubic ice interface should decrease strongly with temperature, resulting in some degree of stacking disorder in ice grown from vapor in the tropical tropopause layer, and in polar stratospheric and noctilucent clouds. Our findings support and explain the evolution of the morphology of ice crystals from hexagonal to trigonal symmetry with decreasing temperature, as reported by experiments and in situ measurements in clouds. We conclude that selective growth of the elusive cubic ice polymorph by manipulation of the interfacial properties can likely be achieved at the ice-liquid interface but not at the ice-vapor interface.

The immersion freezing behavior of ash particles from wood and brown coal burning

NASA Astrophysics Data System (ADS)

Grawe, Sarah; Augustin-Bauditz, Stefanie; Hartmann, Susan; Hellner, Lisa; Pettersson, Jan B. C.; Prager, Andrea; Stratmann, Frank; Wex, Heike

2016-11-01

It is generally known that ash particles from coal combustion can trigger ice nucleation when they interact with water vapor and/or supercooled droplets. However, data on the ice nucleation of ash particles from different sources, including both anthropogenic and natural combustion processes, are still scarce. As fossil energy sources still fuel the largest proportion of electric power production worldwide, and biomass burning contributes significantly to the global aerosol loading, further data are needed to better assess the ice nucleating efficiency of ash particles. In the framework of this study, we found that ash particles from brown coal (i.e., lignite) burning are up to 2 orders of magnitude more ice active in the immersion mode below -32 °C than those from wood burning. Fly ash from a coal-fired power plant was shown to be the most efficient at nucleating ice. Furthermore, the influence of various particle generation methods on the freezing behavior was studied. For instance, particles were generated either by dispersion of dry sample material, or by atomization of ash-water suspensions, and then led into the Leipzig Aerosol Cloud Interaction Simulator (LACIS) where the immersion freezing behavior was examined. Whereas the immersion freezing behavior of ashes from wood burning was not affected by the particle generation method, it depended on the type of particle generation for ash from brown coal. It was also found that the common practice of treating prepared suspensions in an ultrasonic bath to avoid aggregation of particles led to an enhanced ice nucleation activity. The findings of this study suggest (a) that ash from brown coal burning may influence immersion freezing in clouds close to the source and (b) that the freezing behavior of ash particles may be altered by a change in sample preparation and/or particle generation.

New Particle Formation in the Mid-Latitude Upper Troposphere

NASA Astrophysics Data System (ADS)

Axisa, Duncan

Primary aerosol production due to new particle formation (NPF) in the upper troposphere and the impact that this might have on cloud condensation nuclei (CCN) concentration can be of sufficient magnitude to contribute to the uncertainty in radiative forcing. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Therefore, new particle formation must be accurately defined, parametrized and accounted for in models. This research involved the deployment of instruments, data analysis and interpretation of particle formation events during the Mid-latitude Airborne Cirrus Properties Experiment (MACPEX) campaign. The approach combined field measurements and observations with extensive data analysis and modeling to study the process of new particle formation and growth to CCN active sizes. Simultaneous measurements of O3, CO, ultrafine aerosol particles and surface area from a high-altitude research aircraft were used to study tropospheric-stratospheric mixing as well as the frequency and location of NPF. It was found that the upper troposphere was an active region in the production of new particles by gas-to-particle conversion, that nucleation was triggered by convective clouds and mixing processes, and that NPF occurred in regions with high relative humidity and low surface area. In certain cases, mesoscale and synoptic features enhanced mixing and facilitated the formation of new particles in the northern mid-latitudes. A modeling study of particle growth and CCN formation was done based on measured aerosol size distributions and modeled growth. The results indicate that when SO2 is of sufficient concentration NPF is a significant source of potential CCN in the upper troposphere. In conditions where convective cloud outflow eject high concentrations of SO2, a large number of new particles can form especially in the instance when the preexisting surface area is low. The fast growth of nucleated clusters produces a particle mode that becomes CCN active within 24-hours.

Ice nucleation by soil dust compared to desert dust aerosols

NASA Astrophysics Data System (ADS)

Moehler, O.; Steinke, I.; Ullrich, R.; Höhler, K.; Schiebel, T.; Hoose, C.; Funk, R.

2015-12-01

A minor fraction of atmospheric aerosol particles, so-called ice-nucleating particles (INPs), initiates the formation of the ice phase in tropospheric clouds and thereby markedly influences the Earth's weather and climate systems. Whether an aerosol particle acts as an INP depends on its size, morphology and chemical compositions. The INP fraction of certain aerosol types also strongly depends on the temperature and the relative humidity. Because both desert dust and soil dust aerosols typically comprise a variety of different particles, it is difficult to assess and predict their contribution to the atmospheric INP abundance. This requires both accurate modelling of the sources and atmospheric distribution of atmospheric dust components and detailed investigations of their ice nucleation activities. The latter can be achieved in laboratory experiments and parameterized for use in weather and climate models as a function of temperature and particle surface area, a parameter called ice-nucleation active site (INAS) density. Concerning ice nucleation activity studies, the soil dust is of particular interest because it contains a significant fraction of organics and biological components, both with the potential for contributing to the atmospheric INP abundance at relatively high temperatures compared to mineral components. First laboratory ice nucleation experiments with a few soil dust samples indicated their INP fraction to be comparable or slightly enhanced to that of desert dust. We have used the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber to study the immersion freezing ability of four different arable soil dusts, sampled in Germany, China and Argentina. For temperatures higher than about -20°C, we found the INP fraction of aerosols generated from these samples by a dry dispersion technique to be significantly higher compared to various desert dust aerosols also investigated in AIDA experiments. In this contribution, we will summarize the experimental results, introduce related INP parameterizations for use in weather and climate models, and briefly discuss possible reasons for the discrepancy between the INP fraction of desert and soil dust aerosols.

Cirrus Cloud Seeding has Potential to Cool Climate

NASA Technical Reports Server (NTRS)

Storelvmo, T.; Kristjansson, J. E.; Muri, H.; Pfeffer, M.; Barahona, D.; Nenes, A.

2013-01-01

Cirrus clouds, thin ice clouds in the upper troposphere, have a net warming effect on Earth s climate. Consequently, a reduction in cirrus cloud amount or optical thickness would cool the climate. Recent research indicates that by seeding cirrus clouds with particles that promote ice nucleation, their lifetimes and coverage could be reduced. We have tested this hypothesis in a global climate model with a state-of-the-art representation of cirrus clouds and find that cirrus cloud seeding has the potential to cancel the entire warming caused by human activity from pre-industrial times to present day. However, the desired effect is only obtained for seeding particle concentrations that lie within an optimal range. With lower than optimal particle concentrations, a seeding exercise would have no effect. Moreover, a higher than optimal concentration results in an over-seeding that could have the deleterious effect of prolonging cirrus lifetime and contributing to global warming.

Aerosol and CCN in southwest Saudi Arabia

NASA Astrophysics Data System (ADS)

Collins, Don; Li, Runjun; Axisa, Duncan; Kucera, Paul; Burger, Roelof

2010-05-01

As part of an ongoing study of the microphysical and dynamical controls on precipitation in southwest Saudi Arabia, a number of surface and aircraft-based instruments were used in summer / fall 2009 to measure the size distribution, hygroscopic properties, and cloud droplet nucleation efficiency of the local aerosol. Submicron size distributions were measured using differential mobility analyzers both on the ground and on board the aircraft, while an aerodynamic particle sizer and a forward scattering spectrometer probe were used to measure the supermicron size distributions on the ground and from on board the aircraft, respectively. Identical continuous flow cloud condensation nuclei counters were used to measure CCN spectra at the surface and aloft and a humidified tandem differential mobility analyzer was operated on the ground to measure size-resolved hygroscopicity. The aerosol in this arid environment is characterized by a persistent accumulation mode having hygroscopic and CCN efficiency properties consistent with a sulfate-rich aged aerosol. The particles in that background aerosol are generally sufficiently large and hygroscopic to activate at those supersaturations expected in the convective clouds responsible for most of the regional precipitation, which consequently acts as a lower bound on the resulting cloud droplet concentrations. Though the concentration, size distribution, and properties of the submicron aerosol generally changed very slowly over periods of several hours, abrupt ~doubling in concentration almost always accompanied the arrival of the sea breeze front that began along the Red Sea. Interestingly, the hygroscopicity and the shape of the size distribution differed little in the pre- and post-sea breeze air masses. The dust-dominated coarse mode typically contributed significantly more to the aerosol mass concentration than did the submicron mode and likely controlled the ice nuclei concentration, though no direct measurements were made to confirm this. Results of routine flight patterns designed to examine the spatial, vertical, and day-to-day variability of the aerosol will be presented and the link between the aerosol at the surface and aloft will be quantified. This presentation will emphasize the regional character of the aerosol and will assess its influence on cloud microphysics.

Grain formation in astronomical systems: A critical review of condensation processes

NASA Technical Reports Server (NTRS)

Donn, B.

1978-01-01

An analysis is presented of the assumption and the applicability of the three theoretical methods for calculating condensations in cosmic clouds where no pre-existing nuclei exist. The three procedures are: thermodynamic equilibrium calculations, nucleation theory, and a kinetic treatment which would take into account the characteristics of each individual collision. Thermodynamics provide detailed results on the composition temperature and composition of the condensate provided the system attains equilibrium. Because of the cosmic abundance mixture of elements, large supersaturations in some cases and low pressures, equilibrium is not expected in astronomical clouds. Nucleation theory, a combination of thermodynamics and kinetics, has the limitations of each scheme. Kinetics, not requiring equilibrium, avoids nearly all the thermodynamics difficulties but requires detailed knowledge of many reactions which thermodynamics avoids. It appears to be the only valid way to treat grain formation in space. A review of experimental studies is given.

Advances in Understanding the Role of Aerosols on Ice Clouds from the Fifth International Ice Nucleation (FIN) Workshops

NASA Astrophysics Data System (ADS)

Cziczo, D. J.; Moehler, O.; DeMott, P. J.

2015-12-01

The relationship of ambient aerosol particles to the formation of ice-containing clouds is one of the largest uncertainties in understanding climate. This is due to several poorly understood processes including the microphysics of how particles nucleate ice, the number of effective heterogeneous ice nuclei and their atmospheric distribution, the role of anthropogenic activities in producing or changing the behavior of ice forming particles and the interplay between effective heterogeneous ice nuclei and homogeneous ice formation. Our team recently completed a three-part international workshop to improve our understanding of atmospheric ice formation. Termed the Fifth International Ice Nucleation (FIN) Workshops, our motivation was the limited number of measurements and a lack of understanding of how to compare data acquired by different groups. The first activity, termed FIN1, addressed the characterization of ice nucleating particle size, number and chemical composition. FIN2 addressed the determination of ice nucleating particle number density. Groups modeling ice nucleation joined FIN2 to provide insight on measurements critically needed to model atmospheric ice nucleation and to understand the performance of ice chambers. FIN1 and FIN2 took place at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber at the Karlsruhe Institute of Technology. A particular emphasis of FIN1 and FIN2 was the use of 'blind' intercomparisons using a highly characterized, but unknown to the instrument operators, aerosol sample. The third activity, FIN3, took place at the Desert Research Institute's Storm Peak Laboratory (SPL). A high elevation site not subject to local emissions, SPL allowed for a comparison of ice chambers and subsequent analysis of the ice residuals under the challenging conditions of low particle loading, temperature and pressure found in the atmosphere. The presentation focuses on the improvement in understanding how mass spectra from different instruments can be compared from FIN1 and FIN3. The complementary nature of different ice chamber to access the diverse regimes of temperature and relative humidity space will also be discussed. As a result of the FIN Workshops we believe the performance of instruments in the field can now be quantified and compared.

Measurements to Fill Knowledge Gaps on Ice Nucleating Particle Sources over Oceans

NASA Astrophysics Data System (ADS)

DeMott, P. J.; Hill, T. C.; Ruppel, M. J.; Prather, K. A.; Collins, D. B.; Axson, J. L.; Lee, T.; Hwang, C. Y.; Sullivan, R. C.; McMeeking, G. R.; Mason, R.; Bertram, A. K.; Mayol-Bracero, O. L.; Lewis, E. R.

2013-12-01

Measurements of the temperature spectrum of ice nucleating particle concentrations by two methods in recent specialized laboratory sea spray studies and field campaigns in the Northern Hemisphere will be discussed and compared with historical data from over Southern Oceans. In general, new measurements of the condensation/immersion freezing activation spectra of realistically-generated laboratory sea spray particles (by wave generation or plunging water bubble production) are consistent with previous measurements made over oceans. The number concentrations of ice nuclei tend to be lower than are measured over land regions, at least for modestly supercooled cloud conditions. Certain but complex connections of ice nucleating particle production to ocean microbiological processes affecting the chemical composition of the sea surface microlayer are seen, but the nature of the ice nucleating units of particles remains to be identified. Associations of ice nucleating particle concentrations with heterotrophic bacterial concentrations were noted in some experiments, while correlation with chlorophyll-a concentration in seawater was clearly identified in laboratory simulations of phytoplankton blooms. These data may ultimately serve as the basis for parameterization development for ice initiation in numerical model simulations of mixed-phase clouds. Atmospheric measurements have been made at island sites, via aircraft, and from ship-based filter collections in the Northern Hemisphere. The immersion freezing spectra of these particles are similar to those found in recent laboratory studies and historical measurements, but show the expected natural variability by location. The majority of particles detected thus far as ice nuclei from sea spray and in marine air show minimal or episodic/variable direct participation of biological ice nucleating organisms on the basis of sensitivity to high temperatures (95°C). However, assembled measurements are still sparse, the nuclei could be a product of biological processes, and ship-collected particles from the Bering Sea showed a high labile fraction associated with the presence of a high proportion, based on pyrosequencing of DNA extracted from the collected particles, of species from the Gammaproteobacteria, the same class that contains the ice nucleating bacteria. These studies are ongoing, and new measurement plans, including ship-based aerosol collections over Southern Oceans, will be described.

Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

NASA Astrophysics Data System (ADS)

Schiebel, Thea; Höhler, Kristina; Funk, Roger; Hill, Thomas C. J.; Levin, Ezra J. T.; Nadolny, Jens; Steinke, Isabelle; Suski, Kaitlyn J.; Ullrich, Romy; Wagner, Robert; Weber, Ines; DeMott, Paul J.; Möhler, Ottmar

2016-04-01

Recent investigations at the cloud simulation chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) suggest that agricultural soil dust has an ice nucleation ability that is enhanced up to a factor of 10 compared to desert dust, especially at temperatures above -26 °C (Steinke et al., in preparation for submission). This enhancement might be caused by the contribution of very ice-active biological particles. In addition, soil dust aerosol particles often contain a considerably higher amount of organic matter compared to desert dust particles. To test agricultural soil dust as a source of ice nucleating particles, especially for ice formation in warm clouds, we conducted a series of laboratory measurements with different soil dust samples to extend the existing AIDA dataset. The AIDA has a volume of 84 m3 and operates under atmospherically relevant conditions over wide ranges of temperature, pressure and humidity. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. As a supplement to the AIDA facility, we use the INKA (Ice Nucleation Instrument of the KArlsruhe Institute of Technology) continuous flow diffusion chamber based on the design by Rogers (1988) to expose the sampled aerosol particles to a continuously increasing saturation ratio by keeping the aerosol temperature constant. For our experiments, soil dust was dry dispersed into the AIDA vessel. First, fast saturation ratio scans at different temperatures were performed with INKA, sampling soil dust aerosol particles directly from the AIDA vessel. Then, we conducted the AIDA expansion experiment starting at a preset temperature. The combination of these two different methods provides a robust data set on the temperature-dependent ice activity of various agriculture soil dust aerosol particles with a special focus on relatively high temperatures. In addition, to extend the data set, we investigated the role of biological and organic matter in more detail to gain additional information on the trigger of the enhanced ice nucleation activity of soil dust. References Rogers (1988): Development of a continuous flow thermal gradient diffusion chamber for ice nucleation studies Steinke et al. (In preparation for submission): Ice nucleation activity of agricultural soil dust aerosols from Mongolia, Argentina and Germany

The Exoplanet Cloud Atlas

NASA Astrophysics Data System (ADS)

Gao, Peter; Marley, Mark S.; Morley, Caroline; Fortney, Jonathan J.

2017-10-01

Clouds have been readily inferred from observations of exoplanet atmospheres, and there exists great variability in cloudiness between planets, such that no clear trend in exoplanet cloudiness has so far been discerned. Equilibrium condensation calculations suggest a myriad of species - salts, sulfides, silicates, and metals - could condense in exoplanet atmospheres, but how they behave as clouds is uncertain. The behavior of clouds - their formation, evolution, and equilibrium size distribution - is controlled by cloud microphysics, which includes processes such as nucleation, condensation, and evaporation. In this work, we explore the cloudy exoplanet phase space by using a cloud microphysics model to simulate a suite of cloud species ranging from cooler condensates such as KCl/ZnS, to hotter condensates like perovskite and corundum. We investigate how the cloudiness and cloud particle sizes of exoplanets change due to variations in temperature, metallicity, gravity, and cloud formation mechanisms, and how these changes may be reflected in current and future observations. In particular, we will evaluate where in phase space could cloud spectral features be observable using JWST MIRI at long wavelengths, which will be dependent on the cloud particle size distribution and cloud species.

ATom observations of new particle formation in the tropical upper troposphere. The role of convection and nucleation mechanisms

NASA Astrophysics Data System (ADS)

Kupc, A.; Williamson, C.; Hodshire, A. L.; Pierce, J. R.; Ray, E. A.; Froyd, K. D.; Richardson, M.; Weinzierl, B.; Dollner, M.; Erdesz, F.; Bui, T. V.; Diskin, G. S.; Brock, C. A.

2017-12-01

Measurements of size distributions during the Atmospheric Tomography Mission (ATom) reveal high number concentrations (>>1000 cm-3) of nucleation mode particles at high altitudes in the tropics and subtropics under low condensation sink conditions and are associated with upwelling in convective clouds. The broad spatial extent of these newly formed particles shows that the upper free troposphere (FT) of the tropics and subtropics is a globally significant source. In this study, we investigate the link between convection and new particle formation (NPF) by exploring the processes that govern NPF and growth in the tropical and subtropical FT of the Pacific and Atlantic Oceans. We use measurements of the size distributions made with a suite of fast-response instruments on board of a NASA DC-8 aircraft during ATom mission. ATom maps the remote atmosphere over the Pacific and Atlantic basins ( 80 °N and 65 °S) in continuous ascents and descents (0.2 and 13 km), providing the latitudinal and vertical information on the greenhouse gases, reactive and tracer species and aerosol properties and their seasonal variability. We couple measurements of size distributions between 0.003 and 4.8 µm and potential aerosol precursor vapors measured on ATom (August 2016 and February 2017) with calculated air mass back trajectories and the TwO-Moment Aerosol Sectional (TOMAS) box model. The back trajectories identify air masses potentially influenced by recent convection. We then use TOMAS to model particle nucleation, condensation and coagulation along that trajectory to investigate the link between convection and NPF. Through TOMAS, we explore the influence of different nucleation mechanisms (such as binary, ternary or the one with organics) and gas-phase aerosol precursors (such as sulfur dioxide) on observed particle size distributions. We discuss similarities and differences in NPF over the Pacific and Atlantic Oceans and their relationship to convection, examine particle composition and volatility from in situ measurements, and examine which nucleation schemes are most consistent with the observations.

Properties of Arctic Aerosol Particles and Residuals of Warm Clouds: Cloud Activation Efficiency and the Aerosol Indirect Effect

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Imre, D. G.; Leaitch, R.; Ovchinnikov, M.; Liu, P.; Macdonald, A.; Strapp, W.; Ghan, S. J.; Earle, M. E.

2012-12-01

Single particle mass spectrometer, SPLAT II, was used to characterize the size, composition, number concentration, density, and shape of individual Arctic spring aerosol. Background particles, particles above and below the cloud, cloud droplet residuals, and interstitial particles were characterized with goal to identify the properties that separate cloud condensation nuclei (CCN) from background aerosol particles. The analysis offers a comparison between warm clouds formed on clean and polluted days, with clean days having maximum particle concentrations (Na) lower than ~250 cm-3, as compared with polluted days, in which maximum concentration was tenfold higher. On clean days, particles were composed of organics, organics mixed with sulfates, biomass burning (BB), sea salt (SS), and few soot and dust particles. On polluted days, BB, organics associated with BB, and their mixtures with sulfate dominated particle compositions. Based on the measured compositions and size distributions of cloud droplet residuals, background aerosols, and interstitial particles, we conclude that these three particle types had virtually the same compositions, which means that cloud activation probabilities were surprisingly nearly composition independent. Moreover, these conclusions hold in cases in which less than 20% or more than 90% of background particles got activated. We concluded that for the warm clouds interrogated in this study particle size played a more important factor on aerosol CCN activity. Comparative analysis of all studied clouds reveals that aerosol activation efficiency strongly depends on the aerosol concentrations, such that at Na <200 cm-3, nearly all particles activate, and at higher concentrations the activation efficiency is lower. For example, when Na was greater than 1500 cm-3, less than ~30% of particles activated. The data suggest that as the number of nucleated droplets increases, condensation on existing droplets effectively competes with particle activation, limiting maximum droplet concentrations Nd = 525 ± 50 cm-3, which is lower than the 750 cm-3 limit found by Leaitch et al. (1986) for mid-latitude continental cloud that had generally larger updraft speeds than the clouds interrogated in Arctic. These findings are important for the aerosol indirect effect, in which increase in aerosol particle number concentrations is expected to result in increase in Nd and decrease in droplet size, leading to increased cloud albedo and potentially lifetimes. Our conclusions point to limited susceptibility to changes in ambient aerosol concentrations, providing simple explanation for the finding of weaker than expected indirect effect. In summary, the data presented here show that Nd increases as the cloud base particle number concentration increases; however, they also show a limit on Nd that is in the range of 500-600 cm-3.

Immersion freezing in concentrated solution droplets for a variety of ice nucleating particles

NASA Astrophysics Data System (ADS)

Wex, Heike; Kohn, Monika; Grawe, Sarah; Hartmann, Susan; Hellner, Lisa; Herenz, Paul; Welti, Andre; Lohmann, Ulrike; Kanji, Zamin; Stratmann, Frank

2016-04-01

The measurement campaign LINC (Leipzig Ice Nucleation counter Comparison) was conducted in September 2015, during which ice nucleation measurements as obtained with the following instruments were compared: - LACIS (Leipzig Aerosol Cloud Interaction Simulator, see e.g. Wex et al., 2014) - PIMCA-PINC (Portable Immersion Mode Cooling Chamber together with PINC) - PINC (Portable Ice Nucleation Chamber, Chou et al., 2011) - SPIN (SPectrometer for Ice Nuclei, Droplet Measurement Technologies) While LACIS and PIMCA-PINC measured immersion freezing, PINC and SPIN varied the super-saturation during the measurements and collected data also for relative humidities below 100% RHw. A suite of different types of ice nucleating particles were examined, where particles were generated from suspensions, subsequently dried and size selected. For the following samples, data for all four instruments are available: K-feldspar, K-feldspar treated with nitric acid, Fluka-kaolinite and birch pollen. Immersion freezing measurements by LACIS and PIMCA-PINC were in excellent agreement. Respective parameterizations from these measurement were used to model the ice nucleation behavior below water vapor saturation, assuming that the process can be described as immersion freezing in concentrated solutions. This is equivalent to simply including a concentration dependent freezing point depression in the immersion freezing parameterization, as introduced for coated kaolinite particles in Wex et al. (2014). Overall, measurements performed below water vapor saturation were reproduced by the model, and it will be discussed in detail, why deviations were observed in some cases. Acknowledgement: Part of this work was funded by the DFG Research Unit FOR 1525 INUIT, grant WE 4722/1-2. Literature: Chou, C., O. Stetzer, E. Weingartner, Z. Juranyi, Z. A. Kanji, and U. Lohmann (2011), Ice nuclei properties within a Saharan dust event at the Jungfraujoch in the Swiss Alps, Atmos. Chem. Phys., 11(10), 4725-4738, doi:10.5194/acp-11-4725-2011. Wex, H., P. J. DeMott, Y. Tobo, S. Hartmann, M. Rösch, T. Clauss, L. Tomsche, D. Niedermeier, and F. Stratmann (2014), Kaolinite particles as ice nuclei: learning from the use of different kaolinite samples and different coatings, Atmos. Chem. Phys., 14, doi:10.5194/acp-14-5529-2014.

The Dominant Snow-forming Process in Warm and Cold Mixed-phase Orographic Clouds: Effects of Cloud Condensation Nuclei and Ice Nuclei

NASA Astrophysics Data System (ADS)

Fan, J.; Rosenfeld, D.; Leung, L. R.; DeMott, P. J.

2014-12-01

Mineral dust aerosols often observed over California in winter and spring from long-range transport can be efficient ice nuclei (IN) and enhance snow precipitation in mixed-phase orographic clouds. On the other hand, local pollution particles can serve as good CCN and suppress warm rain, but their impacts on cold rain processes are uncertain. The main snow-forming mechanism in warm and cold mixed-phase orographic clouds (refer to as WMOC and CMOC, respectively) could be very different, leading to different precipitation response to CCN and IN. We have conducted 1-km resolution model simulations using the Weather Research and Forecasting (WRF) model coupled with a spectral-bin cloud microphysical model for WMOC and CMOC cases from CalWater2011. We investigated the response of cloud microphysical processes and precipitation to CCN and IN with extremely low to extremely high concentrations using ice nucleation parameterizations that connect with dust and implemented based on observational evidences. We find that riming is the dominant process for producing snow in WMOC while deposition plays a more important role than riming in CMOC. Increasing IN leads to much more snow precipitation mainly due to an increase of deposition in CMOC and increased rimming in WMOC. Increasing CCN decreases precipitation in WMOC by efficiently suppressing warm rain, although snow is increased. In CMOC where cold rain dominates, increasing CCN significantly increases snow, leading to a net increase in precipitation. The sensitivity of supercooled liquid to CCN and IN has also been analyzed. The mechanism for the increased snow by CCN and caveats due to uncertainties in ice nucleation parameterizations will be discussed.

Single-bubble and multibubble cavitation in water triggered by laser-driven focusing shock waves

NASA Astrophysics Data System (ADS)

Veysset, D.; Gutiérrez-Hernández, U.; Dresselhaus-Cooper, L.; De Colle, F.; Kooi, S.; Nelson, K. A.; Quinto-Su, P. A.; Pezeril, T.

2018-05-01

In this study a single laser pulse spatially shaped into a ring is focused into a thin water layer, creating an annular cavitation bubble and cylindrical shock waves: an outer shock that diverges away from the excitation laser ring and an inner shock that focuses towards the center. A few nanoseconds after the converging shock reaches the focus and diverges away from the center, a single bubble nucleates at the center. The inner diverging shock then reaches the surface of the annular laser-induced bubble and reflects at the boundary, initiating nucleation of a tertiary bubble cloud. In the present experiments, we have performed time-resolved imaging of shock propagation and bubble wall motion. Our experimental observations of single-bubble cavitation and collapse and appearance of ring-shaped bubble clouds are consistent with our numerical simulations that solve a one-dimensional Euler equation in cylindrical coordinates. The numerical results agree qualitatively with the experimental observations of the appearance and growth of large bubble clouds at the smallest laser excitation rings. Our technique of shock-driven bubble cavitation opens interesting perspectives for the investigation of shock-induced single-bubble or multibubble cavitation phenomena in thin liquids.

On water in volcanic clouds

NASA Astrophysics Data System (ADS)

Durant, Adam J.

2007-12-01

Volcanic clouds and tephra fallout present a hazard to aviation, human and animal health (direct inhalation or ingestion, contamination of water supplies), and infrastructure (building collapse, burial of roads and railways, agriculture, abrasive and chemical effects on machinery). Understanding sedimentation processes is a fundamental component in the prediction of volcanic cloud lifetime and fallout at the ground, essential in the mitigation of these hazards. The majority of classical volcanic ash transport and dispersion models (VATDM) are based solely on fluid dynamics. The non-agreement between VATDM and observed regional-scale tephra deposit characteristics is especially obvious at large distances from the source volcano. In meteorology, the processes of hydrometeor nucleation, growth and collection have been long-established as playing a central role in sedimentation and precipitation. Taking this as motivation, the hypothesis that hydrometeor formation drives sedimentation from volcanic clouds was tested. The research objectives of this dissertation are: (1) To determine the effectiveness of tephra particles in the catalysis of the liquid water to ice phase transformation, with application to ice hydrometeor formation in volcanic clouds. (2) To determine the sedimentological characteristics of distal (100s km) tephra fallout from recent volcanic clouds. (3) To assess particle fallout rates from recent volcanic clouds in the context of observed deposit characteristics. (4) To assess the implications of hydrometeor formation on the enhancement of volcanic sedimentation and the potential for cloud destabilization from volcanic hydrometeor sublimation. Dissertation Overview. The following chapters present the analysis, results and conclusions of heterogeneous ice nucleation experiments and sedimentological characterization of several recent tephra deposits. The dissertation is organized in three chapters, each prepared in journal article format. In Chapter 1, single ash particle freezing experiments were carried out to investigate the effect of ash particle composition and surface area on water drop freezing temperature. In Chapter 2, the tephra deposit from the 18 May 1980 eruption of Mount St. Helens, USA, was reanalyzed using laser diffraction particle size analysis and hydrometeor-induced sedimentation mechanisms are considered. In Chapter 3, fallout from the 18 August 1992 and 16--17 September 1992 eruptions of Mount Spurr, USA, was analyzed and particle sedimentation and cloud microphysics were modeled to assess the potential for cloud destabilization from hydrometeor sublimation.

Contact freezing of supercooled cloud droplets on collision with mineral dust particles: effect of particle size

NASA Astrophysics Data System (ADS)

Hoffmann, Nadine; Duft, Denis; Kiselev, Alexei; Leisner, Thomas

2013-04-01

The contact freezing of supercooled cloud droplets is one of the potentially important and the least investigated heterogeneous mechanism of ice formation in the tropospheric clouds [1]. On the time scales of cloud lifetime the freezing of supercooled water droplets via contact mechanism may occur at higher temperature compared to the same IN immersed in the droplet. However, the laboratory experiments of contact freezing are very challenging due to the number of factors affecting the probability of ice formation. In our experiment we study single water droplets freely levitated in the laminar flow of mineral dust particles acting as the contact freezing nuclei. By repeating the freezing experiment sufficient number of times we are able to reproduce statistical freezing behavior of large ensembles of supercooled droplets and measure the average rate of freezing events. We show that the rate of freezing at given temperature is governed only by the rate of droplet -particle collision and by the properties of the contact ice nuclei. In this contribution we investigate the relationship between the freezing probability and the size of mineral dust particle (represented by illite) and show that their IN efficiency scales with the particle size. Based on this observation, we discuss the similarity between the freezing of supercooled water droplets in immersion and contact modes and possible mechanisms of apparent enhancement of the contact freezing efficiency. [1] - K.C. Young, The role of contact nucleation in ice phase initiation in clouds, Journal of the Atmospheric Sciences 31, 1974

Formation of ultra-compact dwarf galaxies from supergiant molecular clouds

NASA Astrophysics Data System (ADS)

Goodman, Morgan; Bekki, Kenji

2018-05-01

The origin of ultra-compact dwarf galaxies (UCDs) is not yet clear. One possible formation path of UCDs is the threshing of a nucleated elliptical dwarf galaxy (dE, N), however, it remains unclear how such massive nuclear stellar systems were formed in dwarf galaxies. To better establish the early history of UCDs, we investigate the formation of UCD progenitor clusters from super giant molecular clouds (SGMCs), using hydrodynamical simulations. In this study we focus on SGMCs with masses 107 - 108 M_{\\odot } that can form massive star clusters that display physical properties similar to UCDs. We find that the clusters have extended star formation histories with two phases, producing multiple distinct stellar populations, and that the star formation rate is dependent on the feedback effects of SNe and AGB stars. The later generations of stars formed in these clusters are more compact, leading to a clearly nested structure, and these stars will be more He-rich than those of the first generation, leading to a slight colour gradient. The simulated clusters demonstrate scaling relations between Reff and M and σv and M consistent with those observed in UCDs and strongly consistent with those of the original SGMC. We discuss whether SGMCs such as these can be formed through merging of self-gravitating molecular clouds in galaxies at high-z.

Understanding the ice nucleation characteristics of feldspars suspended in solution

NASA Astrophysics Data System (ADS)

Kumar, Anand; Marcolli, Claudia; Kaufmann, Lukas; Krieger, Ulrich; Peter, Thomas

2017-04-01

Freezing of liquid droplets and subsequent ice crystal growth affects optical properties of clouds and precipitation. Field measurements show that ice formation in cumulus and stratiform clouds begins at temperatures much warmer than those associated with homogeneous ice nucleation in pure water, which is ascribed to heterogeneous ice nucleation occurring on the foreign surfaces of ice nuclei (IN). Various insoluble particles such as mineral dust, soot, metallic particles, volcanic ash, or primary biological particles have been suggested as IN. Among these the suitability of mineral dusts is best established. The ice nucleation ability of mineral dust particles may be modified when secondary organic or inorganic substances are accumulating on the dust during atmospheric transport. If the coating is completely wetting the mineral dust particles, heterogeneous ice nucleation occurs in immersion mode also below 100 % RH. A previous study by Zobrist et al. (2008) Arizona test dust, silver iodide, nonadecanol and silicon dioxide suspensions in various solutes showed reduced ice nucleation efficiency (in immersion mode) of the particles. Though it is still quite unclear how surface modifications and coatings influence the ice nucleation activity of the components present in natural dust particles at a microphysical scale. To improve our understanding how solute and mineral dust particle surface interaction, we run freezing experiments using a differential scanning calorimeter (DSC) with microcline, sanidine, plagioclase, kaolinite and quartz particles suspended in pure water and solutions containing ammonia, ammonium bisulfate, ammonium sulfate, ammonium chloride, ammonium nitrate, potassium chloride, potassium sulfate, sodium sulfate and sulfuric acid. Methodology Suspensions of mineral dust samples (2 - 5 wt%) are prepared in water with varying solute concentrations (0 - 15 wt%). 20 vol% of this suspension plus 80 vol% of a mixture of 95 wt% mineral oil (Aldrich Chemical) and 5 wt% lanolin (Fluka Chemical) is emulsified with a rotor-stator homogenizer for 40 s at a rotation frequency of 7000 rpm. 4 - 10 mg of this mixture is pipetted in an aluminum pan (closed hermetically), placed in the DSC and subjected to three freezing cycles. The first and the third freezing cycles are executed at a cooling rate of 10 K/min to control the stability of the sample. The second freezing cycle is executed at a 1 K/min cooling rate and is used for evaluation. Freezing temperatures are obtained by evaluating the onset of the freezing signal in the DSC curve and plotted against water activity. Results Based on Koop et al. (2000), a general decreasing trend in ice nucleation efficiency of the mineral samples with increasing solute concentrations is expected. Interestingly, feldspars (microcline, sanidine, plagioclase) in very dilute solutions of ammonia and ammonium salts (water activity close to one) show an increase in ice nucleation efficiency of 4 to 6 K compared to that in pure water. Similar trends but less pronounced are observed for kaolinite while quartz shows barely any effect. Therefore, there seem to be specific interactions between the feldspar surface and ammonia and/or ammonium ions which result in an increase in freezing temperatures at low solute concentrations. The surface ion exchange seems to be secondary for this effect since it is also present in ammonia solution. We hypothesize that ammonia adsorbs on the aluminol/silanol groups present on feldspar (viz. aluminosilicate surface) surfaces (Nash and Marshall, 1957; Belchinskaya et al., 2013). Hence allowing one of the N-H bonds to stick outwards from the surface, facing towards the bulk water and providing a favorable template for ice to grow. The current study gives an insight into the ice nucleation behavior of aluminosilicate minerals when present in conjunction with chemical species, eg. ammonium/sulfates, which is of high atmospheric relevance. References Koop et al., (2000), doi:10.1038/35020537. Zobrist et al., (2008). J. Phys. Chem., 112:3965-3975. Nash and Marshall (1957). Proceedings Soil Sci. Society, 21:149-153. Belchinskaya et al., (2013). J. Applied Chemistry, doi:10.1155/2013/789410

A new chemistry option in WRF-Chem v. 3.4 for the simulation of direct and indirect aerosol effects using VBS: evaluation against IMPACT-EUCAARI data

NASA Astrophysics Data System (ADS)

Tuccella, P.; Curci, G.; Grell, G. A.; Visconti, G.; Crumeyrolle, S.; Schwarzenboeck, A.; Mensah, A. A.

2015-09-01

A parameterization for secondary organic aerosol (SOA) production based on the volatility basis set (VBS) approach has been coupled with microphysics and radiative schemes in the Weather Research and Forecasting model with Chemistry (WRF-Chem) model. The new chemistry option called "RACM-MADE-VBS-AQCHEM" was evaluated on a cloud resolving scale against ground-based and aircraft measurements collected during the IMPACT-EUCAARI (Intensive Cloud Aerosol Measurement Campaign - European Integrated project on Aerosol Cloud Climate and Air quality interaction) campaign, and complemented with satellite data from MODIS. The day-to-day variability and the diurnal cycle of ozone (O3) and nitrogen oxides (NOx) at the surface are captured by the model. Surface aerosol mass concentrations of sulfate (SO4), nitrate (NO3), ammonium (NH4), and organic matter (OM) are simulated with correlations larger than 0.55. WRF-Chem captures the vertical profile of the aerosol mass concentration in both the planetary boundary layer (PBL) and free troposphere (FT) as a function of the synoptic condition, but the model does not capture the full range of the measured concentrations. Predicted OM concentration is at the lower end of the observed mass concentrations. The bias may be attributable to the missing aqueous chemistry processes of organic compounds and to uncertainties in meteorological fields. A key role could be played by assumptions on the VBS approach such as the SOA formation pathways, oxidation rate, and dry deposition velocity of organic condensable vapours. Another source of error in simulating SOA is the uncertainties in the anthropogenic emissions of primary organic carbon. Aerosol particle number concentration (condensation nuclei, CN) is overestimated by a factor of 1.4 and 1.7 within the PBL and FT, respectively. Model bias is most likely attributable to the uncertainties of primary particle emissions (mostly in the PBL) and to the nucleation rate. Simulated cloud condensation nuclei (CCN) are also overestimated, but the bias is more contained with respect to that of CN. The CCN efficiency, which is a characterization of the ability of aerosol particles to nucleate cloud droplets, is underestimated by a factor of 1.5 and 3.8 in the PBL and FT, respectively. The comparison with MODIS data shows that the model overestimates the aerosol optical thickness (AOT). The domain averages (for 1 day) are 0.38 ± 0.12 and 0.42 ± 0.10 for MODIS and WRF-Chem data, respectively. The droplet effective radius (Re) in liquid-phase clouds is underestimated by a factor of 1.5; the cloud liquid water path (LWP) is overestimated by a factor of 1.1-1.6. The consequence is the overestimation of average liquid cloud optical thickness (COT) from a few percent up to 42 %. The predicted cloud water path (CWP) in all phases displays a bias in the range +41-80 %, whereas the bias of COT is about 15 %. In sensitivity tests where we excluded SOA, the skills of the model in reproducing the observed patterns and average values of the microphysical and optical properties of liquid and all phase clouds decreases. Moreover, the run without SOA (NOSOA) shows convective clouds with an enhanced content of liquid and frozen hydrometers, and stronger updrafts and downdrafts. Considering that the previous version of WRF-Chem coupled with a modal aerosol module predicted very low SOA content (secondary organic aerosol model (SORGAM) mechanism) the new proposed option may lead to a better characterization of aerosol-cloud feedbacks.

A new temperature and humidity dependent surface site density approach for deposition ice nucleation

NASA Astrophysics Data System (ADS)

Steinke, I.; Hoose, C.; Möhler, O.; Connolly, P.; Leisner, T.

2014-07-01

Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol surface area concentration. Additionally, a contact angle parameterization according to classical nucleation theory was fitted to the experimental data in order to relate the ice nucleation efficiencies to contact angle distributions. From this study it can be concluded that the INAS density formulation is a very useful tool to decribe the temperature and humidity dependent ice nucleation efficiency of ATD particles. Deposition nucleation on ATD particles can be described by a temperature and relative humidity dependent INAS density function ns(T, Sice) with ns(xtherm) = 1.88 × 105 \\centerdot exp(0.2659 \\centerdot xtherm) [m-2] (1) where the thermodynamic variable xtherm is defined as xtherm = -(T - 273.2) + (Sice-1) × 100 (2) with Sice>1 and within a temperature range between 226 and 250 K. For lower temperatures, xtherm deviates from a linear behavior with temperature and relative humidity over ice. Two different approaches for describing the time dependence of deposition nucleation initiated by ATD particles are proposed. Box model estimates suggest that the time dependent contribution is only relevant for small cooling rates and low number fractions of ice-active particles.

Modelling ice microphysics of mixed-phase clouds

NASA Astrophysics Data System (ADS)

Ahola, J.; Raatikainen, T.; Tonttila, J.; Romakkaniemi, S.; Kokkola, H.; Korhonen, H.

2017-12-01

The low-level Arctic mixed-phase clouds have a significant role for the Arctic climate due to their ability to absorb and reflect radiation. Since the climate change is amplified in polar areas, it is vital to apprehend the mixed-phase cloud processes. From a modelling point of view, this requires a high spatiotemporal resolution to capture turbulence and the relevant microphysical processes, which has shown to be difficult.In order to solve this problem about modelling mixed-phase clouds, a new ice microphysics description has been developed. The recently published large-eddy simulation cloud model UCLALES-SALSA offers a good base for a feasible solution (Tonttila et al., Geosci. Mod. Dev., 10:169-188, 2017). The model includes aerosol-cloud interactions described with a sectional SALSA module (Kokkola et al., Atmos. Chem. Phys., 8, 2469-2483, 2008), which represents a good compromise between detail and computational expense.Newly, the SALSA module has been upgraded to include also ice microphysics. The dynamical part of the model is based on well-known UCLA-LES model (Stevens et al., J. Atmos. Sci., 56, 3963-3984, 1999) which can be used to study cloud dynamics on a fine grid.The microphysical description of ice is sectional and the included processes consist of formation, growth and removal of ice and snow particles. Ice cloud particles are formed by parameterized homo- or heterogeneous nucleation. The growth mechanisms of ice particles and snow include coagulation and condensation of water vapor. Autoconversion from cloud ice particles to snow is parameterized. The removal of ice particles and snow happens by sedimentation and melting.The implementation of ice microphysics is tested by initializing the cloud simulation with atmospheric observations from the Indirect and Semi-Direct Aerosol Campaign (ISDAC). The results are compared to the model results shown in the paper of Ovchinnikov et al. (J. Adv. Model. Earth Syst., 6, 223-248, 2014) and they show a good match. One of the advantages of UCLALES-SALSA is that it can be used to quantify the effect of aerosol scavenging on cloud properties in a precise way.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mitchell, David; Erfani, Ehsan; Garnier, Anne

This project has evolved during its execution, and what follows are the key project findings. This project has arguably provided the first global view of how cirrus cloud (defined as having cloud base temperature T < 235 K) nucleation physics (evaluated through satellite retrievals of ice particle number concentration Ni, effective diameter De and ice water content IWC) evolves with the seasons for a given temperature, latitude zone and surface type (e.g. ocean vs. land), based on a new satellite remote sensing method developed for this project. The retrieval method is unique in that it is very sensitive to themore » small ice crystals that govern the number concentration Ni, allowing Ni to be retrieved. The method currently samples single-layer cirrus clouds having visible optical depth ranging from about 0.3 to 3.0, using co-located observations from the Infrared Imaging Radiometer (IIR) and from the CALIOP (Cloud and Aerosol Lidar with Orthogonal Polarization) lidar aboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) polar orbiting satellite, employing IIR channels at 10.6 μm and 12.05 μm. Retrievals of Ni are primarily used to estimate the cirrus cloud formation mechanism; that is, either homo- or heterogeneous ice nucleation (henceforth hom and het). This is possible since, in general, hom produces more than an order of magnitude more ice crystals than does het. Thus the retrievals provide insight on how these mechanisms change with the seasons for a given latitude zone or region, based on the years 2008 and 2013. Using a conservative criterion for hom cirrus, on average, the sampled cirrus clouds formed through hom occur about 43% of the time in the Arctic and 50% of the time in the Antarctic, and during winter at mid-latitudes in the Northern Hemisphere, hom cirrus occur 37% of the time. Elsewhere (and during other seasons in the Northern Hemisphere mid-latitudes), this hom cirrus fraction is lower, and it is lowest in the tropics. Thus, the microphysical properties of cirrus clouds in the Polar Regions are much different than they are in the tropics; something unknown prior to this study. Moreover, the frequency of cirrus cloud occurrence in the Polar Regions varies strongly with season, peaking during winter in the Arctic and during spring in the Antarctic. Considering these seasonal changes in microphysics and inferred cloud coverage, this leads us to speculate that the buildup of Arctic cirrus during winter may significantly contribute to tropospheric heating in that region, possibly affecting winter jet-stream dynamics and mid-latitude weather patterns through the thermal-wind balance relationship. This cirrus cloud research provides essential guidance for realistically representing cirrus clouds in climate models; guidance previously unavailable. For example, mid-latitude hom cirrus were widespread during winter over or nearby mountainous terrain, evidently due to mountain-induced waves that produce strong updrafts at cirrus cloud levels. The treatment of turbulent mountain stress and gravity waves will likely need to be improved in climate models in order to adequately represent cirrus clouds outside the tropics. Another goal of this project was to develop a ground-based 94-GHz radar retrieval for winter snowstorms, based on (1) an improved analytical framework describing the interaction of radiation from radar with snowfall and (2) the development of a steady-state snow growth model that predicts the height-evolution of the ice particle size distribution through ice particle growth by vapor diffusion, aggregation and riming (i.e. the growth of snow through collisions with supercooled cloud droplets). Although activities (1) and (2) were completed, there was insufficient time to test and finalize the radar retrieval scheme. However, activity (2) provided a new method for relating ice particle mass “m” and projected area “A” to the ice particle maximum dimension “D”. The ice cloud microphysical processes (which determine ice cloud radiative properties) in climate models are parameterized in terms of these m-D and A-D relationships. By improving these relationships, the ice cloud radiative properties in Community Atmosphere Model version 5, or CAM5 (an atmosphere global climate model, or GCM) were improved. Student funding from the University of Nevada, Reno, was combined with funds from this project to conduct some basic research on the mechanism of the North American monsoon, or NAM. Federal research on the NAM has dwindled since 2006, but atmospheric soundings taken during research vessel cruises in the Gulf of California (GC) during the North American Monsoon Experiment (NAME) were used to reveal a likely mechanism that explains the relationship between an intrusion of tropical warm water into the GC during late spring-early summer and the onset of relatively heavy NAM rainfall in northwest Mexico and the southwestern United States. These soundings, combined with reanalysis data, satellite sea surface temperatures and satellite measurements of outgoing longwave radiation were used to develop and provide evidence for a planetary-scale NAM mechanism. As far as we know, no other physical explanation has been offered for the spring-summer evolution of the NAM system.« less

Correlation of Solubility with the Metastable Limit of Nucleation Using Gauge-Cell Monte Carlo Simulations.

PubMed

Clark, Michael D; Morris, Kenneth R; Tomassone, Maria Silvina

2017-09-12

We present a novel simulation-based investigation of the nucleation of nanodroplets from solution and from vapor. Nucleation is difficult to measure or model accurately, and predicting when nucleation should occur remains an open problem. Of specific interest is the "metastable limit", the observed concentration at which nucleation occurs spontaneously, which cannot currently be estimated a priori. To investigate the nucleation process, we employ gauge-cell Monte Carlo simulations to target spontaneous nucleation and measure thermodynamic properties of the system at nucleation. Our results reveal a widespread correlation over 5 orders of magnitude of solubilities, in which the metastable limit depends exclusively on solubility and the number density of generated nuclei. This three-way correlation is independent of other parameters, including intermolecular interactions, temperature, molecular structure, system composition, and the structure of the formed nuclei. Our results have great potential to further the prediction of nucleation events using easily measurable solute properties alone and to open new doors for further investigation.

Geometrical and Mechanical Properties Control Actin Filament Organization

PubMed Central

Ennomani, Hajer; Théry, Manuel; Nedelec, Francois; Blanchoin, Laurent

2015-01-01

The different actin structures governing eukaryotic cell shape and movement are not only determined by the properties of the actin filaments and associated proteins, but also by geometrical constraints. We recently demonstrated that limiting nucleation to specific regions was sufficient to obtain actin networks with different organization. To further investigate how spatially constrained actin nucleation determines the emergent actin organization, we performed detailed simulations of the actin filament system using Cytosim. We first calibrated the steric interaction between filaments, by matching, in simulations and experiments, the bundled actin organization observed with a rectangular bar of nucleating factor. We then studied the overall organization of actin filaments generated by more complex pattern geometries used experimentally. We found that the fraction of parallel versus antiparallel bundles is determined by the mechanical properties of actin filament or bundles and the efficiency of nucleation. Thus nucleation geometry, actin filaments local interactions, bundle rigidity, and nucleation efficiency are the key parameters controlling the emergent actin architecture. We finally simulated more complex nucleation patterns and performed the corresponding experiments to confirm the predictive capabilities of the model. PMID:26016478

Properties of the seismic nucleation phase

USGS Publications Warehouse

Beroza, G.C.; Ellsworth, W.L.

1996-01-01

Near-source observations show that earthquakes begin abruptly at the P-wave arrival, but that this beginning is weak, with a low moment rate relative to the rest of the main shock. We term this initial phase of low moment rate the seismic nucleation phase. We have observed the seismic nucleation phase for a set of 48 earthquakes ranging in magnitude from 1.1-8.1. The size and duration of the seismic nucleation phase scale with the total seismic moment of the earthquake, suggesting that the process responsible for the seismic nucleation phase carries information about the eventual size of the earthquake. The seismic nucleation phase is characteristically followed by quadratic growth in the moment rate, consistent with self-similar rupture at constant stress drop. In this paper we quantify the properties of the seismic nucleation phase and offer several possible explanations for it.

Ice-Crystal Fallstreaks from Supercooled Liquid Water Parent Clouds

NASA Technical Reports Server (NTRS)

Campbell, James R.; O'C. Starr, David; Welton, Ellsworth J.; Spinhirne, James D.; Ferrare, Richard A.

2003-01-01

On 31 December 2001, ice-crystal fallstreaks (e.g., cirrus uncinus, or colloquially "Mare's Tails") from supercooled liquid water parent clouds were observed by ground-based lidars pointed vertically from the Atmospheric Radiation Measurement Southern Great Plains (SGP) facility near Lamont, Oklahoma. The incidence of liquid phase cloud with apparent ice-phase precipitation is investigated. Scenarios for mixed-phase particle nucleation, and fallstreak formation and sustenance are discussed. The observations are unique in the context of the historical reverence given to the commonly observed c h s uncinus fallstreak (wholly ice) versus this seemingly contradictory coincidence of liquid water begetting ice-crystal streaks.

Evidence of Mineral Dust Altering Cloud Microphysics and Precipitation

NASA Technical Reports Server (NTRS)

Min, Qilong; Li, Rui; Lin, Bing; Joseph, Everette; Wang, Shuyu; Hu, Yongxiang; Morris, Vernon; Chang, F.

2008-01-01

Multi-platform and multi-sensor observations are employed to investigate the impact of mineral dust on cloud microphysical and precipitation processes in mesoscale convective systems. It is clearly evident that for a given convection strength,small hydrometeors were more prevalent in the stratiform rain regions with dust than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust sector, particularly at altitudes where heterogeneous nucleation process of mineral dust prevails, further supports the observed changes of precipitation. The consequences of the microphysical effects of the dust aerosols were to shift the precipitation size spectrum from heavy precipitation to light precipitation and ultimately suppressing precipitation.

Using depolarization to quantify ice nucleating particle concentrations: a new method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zenker, Jake; Collier, Kristen N.; Xu, Guanglang

We have developed a new method to determine ice nucleating particle (INP) concentrations observed by the Texas A&M University continuous flow diffusion chamber (CFDC) under a wide range of operating conditions. In this study, we evaluate differences in particle optical properties detected by the Cloud and Aerosol Spectrometer with POLarization (CASPOL) to differentiate between ice crystals, droplets, and aerosols. The depolarization signal from the CASPOL instrument is used to determine the occurrence of water droplet breakthrough (WDBT) conditions in the CFDC. The standard procedure for determining INP concentration is to count all particles that have grown beyond a nominal sizemore » cutoff as ice crystals. During WDBT this procedure overestimates INP concentration, because large droplets are miscounted as ice crystals. Here we design a new analysis method based on depolarization ratio that can extend the range of operating conditions of the CFDC. The method agrees reasonably well with the traditional method under non-WDBT conditions with a mean percent error of ±32.1 %. Additionally, a comparison with the Colorado State University CFDC shows that the new analysis method can be used reliably during WDBT conditions.« less

Using depolarization to quantify ice nucleating particle concentrations: a new method

DOE PAGES

Zenker, Jake; Collier, Kristen N.; Xu, Guanglang; ...

2017-12-01

We have developed a new method to determine ice nucleating particle (INP) concentrations observed by the Texas A&M University continuous flow diffusion chamber (CFDC) under a wide range of operating conditions. In this study, we evaluate differences in particle optical properties detected by the Cloud and Aerosol Spectrometer with POLarization (CASPOL) to differentiate between ice crystals, droplets, and aerosols. The depolarization signal from the CASPOL instrument is used to determine the occurrence of water droplet breakthrough (WDBT) conditions in the CFDC. The standard procedure for determining INP concentration is to count all particles that have grown beyond a nominal sizemore » cutoff as ice crystals. During WDBT this procedure overestimates INP concentration, because large droplets are miscounted as ice crystals. Here we design a new analysis method based on depolarization ratio that can extend the range of operating conditions of the CFDC. The method agrees reasonably well with the traditional method under non-WDBT conditions with a mean percent error of ±32.1 %. Additionally, a comparison with the Colorado State University CFDC shows that the new analysis method can be used reliably during WDBT conditions.« less

Modeling of Cloud/Radiation Processes for Large-Scale Clouds and Tropical Anvils

DTIC Science & Technology

1994-05-31

Bergeron- Findeisen process. The saturation vapor pressure over ice is less than 2.4. Radiative transfer parameterization that over water. As a result, ice...nucleation to generate ice dN ) ’- if T>- -20 0C crystals, depositional growth to simulate the T•’= 0j At (3.7) Bergeron- Findeisen process, sublimation...and (0 if T< - 200C. melting of ice crystals, and gravitational settling to deplete the ice crystals. The Bergeron- Findeisen Here, N, +,,, and N, are

The Colorado/Missouri 1989 cirrus mini IFO

NASA Technical Reports Server (NTRS)

Heymsfield, Andrew J.; Hagen, Donald

1990-01-01

A series of experiments with aircraft were planned for Nov. and Dec. 1989 to study cirrus ice crystal nucleation mechanisms and to test new aircraft instrumentation. The measurements were conducted using the NCAR Sabreliner and King Air. Sampling was conducted near Boulder, Colorado, in lenticular (mountain wave) clouds, and over Missouri in cirrus generating cells. Field samples of aerosol and ice crystal replicas and melt water from these cirrus clouds were collected and studied. Aircraft instrumentation and sampling techniques are discussed.

New particle formation events as a source for cloud condensation nuclei in an urban environment

NASA Astrophysics Data System (ADS)

Wonaschütz, Anna; Burkart, Julia; Wagner, Robert; Reischl, Georg; Steiner, Gerhard; Hitzenberger, Regina

2014-05-01

Nucleation and growth events have been observed in many remote, urban and rural environments. The new particles can contribute significantly to cloud condensation nuclei concentrations, after growing into the appropriate size range (Kerminen et al., 2012). Several studies have attempted to quantify this contribution (e.g. Asmi et al., 2011, Matsui et al., 2013), but only a limited number of them to date have used simultaneous measurements of CCN concentrations and particle size distributions for this purpose (e.g. Levin et al., 2012). In this study, a data set from an urban background station, consisting of 22 months of size distribution and 12 months of CCN concentration measurements (Burkart et al., 2011, Burkart et al., 2012) with 10 months of overlapping measurements is combined to explore the variability of CCN concentrations, their possible causes, and the contribution of nucleation and growth events to CCN concentrations. Consistent with observations in many other locations, nucleation and growth events occur on 30% of all days in spring and summer, on 11% of days in fall and on 4% of days in winter. This suggests a potentially large source of CCN from nucleation and growth events, particularly in the warm season. We acknowledge funding from FWF (Austrian Science Fund) P19515-N20 References: Asmi E., Kivekas, N., Kerminen, V. M., Komppula, M., Hyvarinen, A. P., Hatakka, J., Viisanen, Y., and Lihavainen, H.: Secondary new particle formation in Northern Finland Pallas site between the years 2000 and 2010, Atmos. Chem. Phys., 11, 12959-12972, doi: 10.5194/acp-11-12959-2011, 2011 Burkart J., Steiner, G., Reischl, G., and Hitzenberger, R.: Long-term study of cloud condensation nuclei (CCN) acticvation of the atmospheric aerosol in Vienna, Atmos. Environ., 45, 5751-5759, doi: 10.1016/j.atmosenv.2011.07.022, 2011. Burkart J., Hitzenberger, R., Reischl, G., Bauer, H., Leder, K., and Puxbaum, H.: Activation of "synthetic ambient" aerosols - relation to chemical composition of particles < 100 nm, Atmos. Environ., 54, 583-591, doi: 10.1016/j.atmosenv.2012.01.063, 2012. Kerminen V.-M., Paramonov, M., Anttila, T., Riipinen, I., Fountoukis, C., Korhonen, H., Asmi, E., Laakso, L., Lihavainen, H., Swietlicki, E., Svenningsson, B., Asmi, A., Pandis, S. N., Kulmala, M., and Petäjä, T.: Cloud condensation nuclei production associated with atmospheric nucleation: a synthesis based on existing literature and new results, Atmos. Chem. Phys., 12, 12037-12059, doi: 10.5194/acp-12-12037-2012, 2012. Levin, E. J. T., Prenni, A. J., Petters, M. D., Kreidenweis, S. M., Sullivan, R. C., Atwood, S. A., Ortega, J., DeMott, P. J., and Smith, J. N.: An annual cycle of size-resolved aerosol hygroscopicity at a forested site in Colorado, J. Geophys. Res., 117, 06201, doi:10.1029/2011JD016854, 2012. Matsui, H., Koike, M., Kondo, Y., Takegawa, N., Wiedensohler, A., Fast, J. D., and Zaveri, R. A.: Impact of new particle formation on the concentrations of aerosols and cloud condensation nuclei around Beijing, J. Geophys. Res., 116, 19208, doi:10.1029/2011JD016025, 2011.

Effect of Terrestrial and Marine Organic Aerosol on Regional and Global Climate: Model Development, Application, and Verification with Satellite Data

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meskhidze, Nicholas; Zhang, Yang; Kamykowski, Daniel

2012-03-28

In this DOE project the improvements to parameterization of marine primary organic matter (POM) emissions, hygroscopic properties of marine POM, marine isoprene derived secondary organic aerosol (SOA) emissions, surfactant effects, new cloud droplet activation parameterization have been implemented into Community Atmosphere Model (CAM 5.0), with a seven mode aerosol module from the Pacific Northwest National Laboratory (PNNL)'s Modal Aerosol Model (MAM7). The effects of marine aerosols derived from sea spray and ocean emitted biogenic volatile organic compounds (BVOCs) on microphysical properties of clouds were explored by conducting 10 year CAM5.0-MAM7 model simulations at a grid resolution 1.9° by 2.5° withmore » 30 vertical layers. Model-predicted relationship between ocean physical and biological systems and the abundance of CCN in remote marine atmosphere was compared to data from the A-Train satellites (MODIS, CALIPSO, AMSR-E). Model simulations show that on average, primary and secondary organic aerosol emissions from the ocean can yield up to 20% increase in Cloud Condensation Nuclei (CCN) at 0.2% Supersaturation, and up to 5% increases in droplet number concentration of global maritime shallow clouds. Marine organics were treated as internally or externally mixed with sea salt. Changes associated with cloud properties reduced (absolute value) the model-predicted short wave cloud forcing from -1.35 Wm-2 to -0.25 Wm-2. By using different emission scenarios, and droplet activation parameterizations, this study suggests that addition of marine primary aerosols and biologically generated reactive gases makes an important difference in radiative forcing assessments. All baseline and sensitivity simulations for 2001 and 2050 using global-through-urban WRF/Chem (GU-WRF) were completed. The main objective of these simulations was to evaluate the capability of GU-WRF for an accurate representation of the global atmosphere by exploring the most accurate configuration of physics options in GWRF for global scale modeling in 2001 at a horizontal grid resolution of 1° x 1°. GU-WRF model output was evaluated using observational datasets from a variety of sources including surface based observations (NCDC and BSRN), model reanalysis (NCEP/ NCAR Reanalysis and CMAP), and remotely-sensed data (TRMM) to evaluate the ability of GU-WRF to simulate atmospheric variables at the surface as well as aloft. Explicit treatment of nanoparticles produced from new particle formation in GU-WRF/Chem-MADRID was achieved by expanding particle size sections from 8 to 12 to cover particles with the size range of 1.16 nm to 11.6m. Simulations with two different nucleation parameterizations were conducted for August 2002 over a global domain at a 4º by 5º horizontal resolution. The results are evaluated against field measurement data from the 2002 Aerosol Nucleation and Real Time Characterization Experiment (ANARChE) in Atlanta, Georgia, as well as satellite and reanalysis data. We have also explored the relationship between clean marine aerosol optical properties and ocean surface wind speed using remotely sensed data from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the CALIPSO satellite and the Advanced Microwave Scanning Radiometer (AMSR-E) on board the AQUA satellite. Detailed data analyses were carried out over 15 regions selected to be representative of different areas of the global ocean for the time period from June 2006 to April 2011. We show that for very low (less than 4 m s-1) and very high (more than 12 m s-1) wind speed conditions the mean CALIPSO-derived aerosol optical depth (AOD) has little dependency on the surface wind speed. For an intermediate (between 4 and 12 m s-1) marine AOD was linearly correlated with the surface wind speed values, with a slope of 0.0062 s m-1. Results of our study suggest that considerable improvements to both optical properties of marine aerosols and their production mechanisms can be achieved by discriminating clean marine aerosols (or sea salt particles) from all other types of aerosols present over the ocean.« less

Temperature characterisation of the CLOUD chamber at CERN

NASA Astrophysics Data System (ADS)

Dias, A. M.; Almeida, J.; Kirkby, J.; Mathot, S.; Onnela, A.; Vogel, A.; Ehrhart, S.

2014-12-01

Temperature stability, uniformity and absolute scale inside the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN are important for experiments on aerosol particle nucleation and ice/liquid cloud formation. In order to measure the air temperature, a comprehensive set of arrays ("strings") of platinum resistance thermometers, thermocouples and optical sensors have been installed inside the 26 m3 chamber. The thermal sensors must meet several challenging design requirements: ultra-clean materials, 0.01 K measurement sensitivity, high absolute precision (<0.1 K), 200 K - 373 K range, ability to operate in high electric fields (20 kV/m), and fast response in air (~1 s) in order to measure rapid changes of temperature during ice/liquid cloud formation in the chamber by adiabatic pressure reductions. This presentation will focus on the design of the thermometer strings and the thermal performance of the chamber during the CLOUD8 and CLOUD9 campaigns, 2013-2014, together with the planned upgrades of the CLOUD thermal system.

When is an INP not an INP?

NASA Astrophysics Data System (ADS)

Simpson, Emma; Connolly, Paul; McFiggans, Gordon

2016-04-01

Processes such as precipitation and radiation depend on the concentration and size of different hydrometeors within clouds therefore it is important to accurately predict them in weather and climate models. A large fraction of clouds present in our atmosphere are mixed phase; contain both liquid and ice particles. The number of drops and ice crystals present in mixed phase clouds strongly depends on the size distribution of aerosols. Cloud condensation nuclei (CCN), a subset of atmospheric aerosol particles, are required for liquid drops to form in the atmosphere. These particles are ubiquitous in the atmosphere. To nucleate ice particles in mixed phase clouds ice nucleating particles (INP) are required. These particles are rarer than CCN. Here we investigate the case where CCN and INPs are in direct competition with each other for water vapour within a cloud. Focusing on the immersion and condensation modes of freezing (where an INP must be immersed within a liquid drop before it can freeze) we show that the presence of CCN can suppress the formation of ice. CCN are more hydrophilic than IN and as such are better able to compete for water vapour than, typically insoluble, INPs. Therefore water is more likely to condense onto a CCN than INP, leaving the INP without enough condensed water on it to be able to freeze in the immersion or condensation mode. The magnitude of this suppression effect strongly depends on a currently unconstrained quantity. Here we refer to this quantity as the critical mass of condensed water required for freezing, Mwc. Mwc is the threshold amount of water that must be condensed onto a INP before it can freeze in the immersion or condensation mode. Using the detailed cloud parcel model, Aerosol-Cloud-Precipiation-Interaction Model (ACPIM), developed at the University of Manchester we show that if only a small amount of water is required for freezing there is little suppression effect and if a large amount of water is required there is a large suppression effect. In this poster possible ways to constrain Mwc are discussed as well as conditions where the suppression effect is likely to be greatest. Key Words: Clouds, aerosol, CCN, IN, modelling

Effects of atmospheric dynamics and aerosols on the fraction of supercooled water clouds

NASA Astrophysics Data System (ADS)

Li, Jiming; Lv, Qiaoyi; Zhang, Min; Wang, Tianhe; Kawamoto, Kazuaki; Chen, Siyu; Zhang, Beidou

2017-02-01

Based on 8 years of (January 2008-December 2015) cloud phase information from the GCM-Oriented Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) Cloud Product (GOCCP), aerosol products from CALIPSO and meteorological parameters from the ERA-Interim products, the present study investigates the effects of atmospheric dynamics on the supercooled liquid cloud fraction (SCF) during nighttime under different aerosol loadings at global scale to better understand the conditions of supercooled liquid water gradually transforming to ice phase. Statistical results indicate that aerosols' effect on nucleation cannot fully explain all SCF changes, especially in those regions where aerosols' effect on nucleation is not a first-order influence (e.g., due to low ice nuclei aerosol frequency). By performing the temporal and spatial correlations between SCFs and different meteorological factors, this study presents specifically the relationship between SCF and different meteorological parameters under different aerosol loadings on a global scale. We find that the SCFs almost decrease with increasing of aerosol loading, and the SCF variation is closely related to the meteorological parameters but their temporal relationship is not stable and varies with the different regions, seasons and isotherm levels. Obviously negative temporal correlations between SCFs versus vertical velocity and relative humidity indicate that the higher vertical velocity and relative humidity the smaller SCFs. However, the patterns of temporal correlation for lower-tropospheric static stability, skin temperature and horizontal wind are relatively more complex than those of vertical velocity and humidity. For example, their close correlations are predominantly located in middle and high latitudes and vary with latitude or surface type. Although these statistical correlations have not been used to establish a certain causal relationship, our results may provide a unique point of view on the phase change of mixed-phase cloud and have potential implications for further improving the parameterization of the cloud phase and determining the climate feedbacks.

Melt rheological properties of nucleated PET/MWCNT nanocomposites

NASA Astrophysics Data System (ADS)

Gaonkar, Amita; Murudkar, Vrishali; Deshpande, V. D.

2018-05-01

This work investigates the effect of precipitated Polyethylene Terephthalate (p-PET) and loading of Multiwalled carbon nanotubes (MWCNT) on morphology and rheology of Polyethylene Terephthalate (PET)/MWCNT nanocomposites. As received PET and Self-Nucleated PET (Nuc-PET) nanocomposites with different loadings of multi-walled carbon nanotubes (MWCNT) were prepared by melt mixing technique. Synthesized reorganized PET crystallizes rapidly from the melt and it is used in small quantities as a self-nucleating agent to make Nuc-PET. In the present study, Rheological properties of nanocomposites are obtained and results show with increase in MWCNT loading complex viscosity of nanocomposites increases. Nonterminal solid like rheological behavior of PET nanocomposites were observed at low frequencies, which indicates the formation of the network like structures of MWCNT in nanocomposites. Morphological and rheological properties of self-nucleated PET nanocomposites improved significantly may be due to self-nucleating agent p-PET. Morphological properties were studied by Scanning Electron Microscopy (SEM). SEM shows better dispersion of MWCNT in Nuc-PET nanocomposites.

Persistent Daily Aerosol Nucleation Events at Mountain-Top Location

NASA Astrophysics Data System (ADS)

Hallar, A. G.; Wiedinmyer, C.; Lowenthal, D. H.

2009-12-01

Atmospheric aerosols are of great consequence since they can impact climate through direct and indirect forcing, degrade air quality and visibility, and have detrimental effects on human health. Thus, an important phenomenon is atmospheric aerosol formation, the production of nanometer-size particles by nucleation and their growth to detectable sizes. Storm Peak Laboratory (3210 m AMSL), owned and operated by the Desert Research Institute (DRI), is located on the west summit of Mt. Werner in the Park Range near Steamboat Springs in northwestern Colorado. This site has been used in aerosol studies for more than 20 years. Daily nucleation events have been observed Storm Peak Laboratory between 2002 and 2009 with a TSI Scanning Mobility Particle Sizer (SMPS) (model 3936) coupled with a TSI model 3022 condensation particle counter (CPC). This instrument was set to measure particles with diameters between 8 and 335 nm. These events were observed during all measurement periods in the spring, summer and winter months. Nucleation was consistently seen in the mid-afternoon each day. This study includes 422 days of data; in 320 of these days nucleation events were observed. Thus, the nucleation events occurred during 76% of the measurement days, including during cloud events, and appear to be associated with elevated levels of ultraviolet radiation. This work will compare and contrast days with and without nucleation events, by investigating the radiation and meteorological conditions present. The results presented will provide further insight to the insitu production of aerosols via nucleation.

Biogenic influence on the composition and growth of summertime Arctic aerosol

NASA Astrophysics Data System (ADS)

Willis, M. D.; Burkart, J.; Thomas, J. L.; Koellner, F.; Schneider, J.; Bozem, H.; Hoor, P. M.; Aliabadi, A. A.; Schulz, H.; Herber, A. B.; Leaitch, R.; Abbatt, J.

2016-12-01

The summertime Arctic lower troposphere is a relatively pristine background aerosol environment dominated by nucleation and Aitken mode particles. Understanding the mechanisms that control the formation and growth of aerosol is crucial for our ability to predict cloud properties and therefore radiative balance and climate. We present aircraft-based observations of submicron aerosol composition from an aerosol mass spectrometer made during the NETCARE 2014 summertime arctic campaign, based in the Canadian High Arctic, at Resolute Bay, NU (74°N). Under stable and regionally influenced atmospheric conditions with low carbon monoxide and black carbon concentrations (< 100 ppbv and < 50 ng/m3, respectively), we observed organic aerosol (OA)-to-sulfate ratios ranging from 0.5 to > 6 with evidence for enhancement within the lower boundary layer. Methanesulfonic acid (MSA), a marker for the contribution of ocean-derived biogenic sulphur, was also observed in submicron aerosol. MSA-to-sulfate ratios ranged from near zero to 0.3 and tended to increase within the lower boundary layer, suggesting a contribution to aerosol loading from the ocean. In one notable case while flying in the lower boundary layer above open water in Lancaster Sound, we observed growth of small particles, <20 nm in diameter, into sizes above 50 nm. Aerosol growth was correlated with the presence of organic species, trimethylamine, and MSA in particles 80 nm and larger, where the organics were similar to those previously observed in marine settings. The organic-rich aerosol contributed significantly to particles active as cloud condensation nuclei (CCN, supersaturation = 0.6%). Our results highlight the potential importance of secondary organic aerosol formation and its role in growing nucleation mode aerosol into CCN-active sizes in this remote marine environment.

New particle formation and growth in biomass burning plumes: An important source of cloud condensation nuclei

NASA Astrophysics Data System (ADS)

Hennigan, Christopher J.; Westervelt, Daniel M.; Riipinen, Ilona; Engelhart, Gabriella J.; Lee, Taehyoung; Collett, Jeffrey L., Jr.; Pandis, Spyros N.; Adams, Peter J.; Robinson, Allen L.

2012-05-01

Experiments were performed in an environmental chamber to characterize the effects of photo-chemical aging on biomass burning emissions. Photo-oxidation of dilute exhaust from combustion of 12 different North American fuels induced significant new particle formation that increased the particle number concentration by a factor of four (median value). The production of secondary organic aerosol caused these new particles to grow rapidly, significantly enhancing cloud condensation nuclei (CCN) concentrations. Using inputs derived from these new data, global model simulations predict that nucleation in photo-chemically aging fire plumes produces dramatically higher CCN concentrations over widespread areas of the southern hemisphere during the dry, burning season (Sept.-Oct.), improving model predictions of surface CCN concentrations. The annual indirect forcing from CCN resulting from nucleation and growth in biomass burning plumes is predicted to be -0.2 W m-2, demonstrating that this effect has a significant impact on climate that has not been previously considered.

A new temperature- and humidity-dependent surface site density approach for deposition ice nucleation

NASA Astrophysics Data System (ADS)

Steinke, I.; Hoose, C.; Möhler, O.; Connolly, P.; Leisner, T.

2015-04-01

Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol surface area concentration. Additionally, a contact angle parameterization according to classical nucleation theory was fitted to the experimental data in order to relate the ice nucleation efficiencies to contact angle distributions. From this study it can be concluded that the INAS density formulation is a very useful tool to describe the temperature- and humidity-dependent ice nucleation efficiency of ATD particles. Deposition nucleation on ATD particles can be described by a temperature- and relative-humidity-dependent INAS density function ns(T, Sice) with ns(xtherm) = 1.88 ×105 · exp(0.2659 · xtherm) [m-2] , (1) where the temperature- and saturation-dependent function xtherm is defined as xtherm = -(T-273.2)+(Sice-1) ×100, (2) with the saturation ratio with respect to ice Sice >1 and within a temperature range between 226 and 250 K. For lower temperatures, xtherm deviates from a linear behavior with temperature and relative humidity over ice. Also, two different approaches for describing the time dependence of deposition nucleation initiated by ATD particles are proposed. Box model estimates suggest that the time-dependent contribution is only relevant for small cooling rates and low number fractions of ice-active particles.

Process-model simulations of cloud albedo enhancement by aerosols in the Arctic.

PubMed

Kravitz, Ben; Wang, Hailong; Rasch, Philip J; Morrison, Hugh; Solomon, Amy B

2014-12-28

A cloud-resolving model is used to simulate the effectiveness of Arctic marine cloud brightening via injection of cloud condensation nuclei (CCN), either through geoengineering or other increased sources of Arctic aerosols. An updated cloud microphysical scheme is employed, with prognostic CCN and cloud particle numbers in both liquid and mixed-phase marine low clouds. Injection of CCN into the marine boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. Albedo increases are stronger for pure liquid clouds than mixed-phase clouds. Liquid precipitation can be suppressed by CCN injection, whereas ice precipitation (snow) is affected less; thus, the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. CCN injection into a clean regime results in a greater albedo increase than injection into a polluted regime, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, dynamical changes in circulation owing to precipitation changes are small. According to these results, which are dependent upon the representation of ice nucleation processes in the employed microphysical scheme, Arctic geoengineering is unlikely to be effective as the sole means of altering the global radiation budget but could have substantial local radiative effects. © 2014 The Author(s) Published by the Royal Society. All rights reserved.

Process-model simulations of cloud albedo enhancement by aerosols in the Arctic

PubMed Central

Kravitz, Ben; Wang, Hailong; Rasch, Philip J.; Morrison, Hugh; Solomon, Amy B.

2014-01-01

A cloud-resolving model is used to simulate the effectiveness of Arctic marine cloud brightening via injection of cloud condensation nuclei (CCN), either through geoengineering or other increased sources of Arctic aerosols. An updated cloud microphysical scheme is employed, with prognostic CCN and cloud particle numbers in both liquid and mixed-phase marine low clouds. Injection of CCN into the marine boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. Albedo increases are stronger for pure liquid clouds than mixed-phase clouds. Liquid precipitation can be suppressed by CCN injection, whereas ice precipitation (snow) is affected less; thus, the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. CCN injection into a clean regime results in a greater albedo increase than injection into a polluted regime, consistent with current knowledge about aerosol–cloud interactions. Unlike previous studies investigating warm clouds, dynamical changes in circulation owing to precipitation changes are small. According to these results, which are dependent upon the representation of ice nucleation processes in the employed microphysical scheme, Arctic geoengineering is unlikely to be effective as the sole means of altering the global radiation budget but could have substantial local radiative effects. PMID:25404677

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

NASA Astrophysics Data System (ADS)

Wagner, R.; Möhler, O.; Saathoff, H.; Schnaiter, M.; Leisner, T.

2010-04-01

The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 μm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investigated species, namely sodium oxalate. Our experiments address the atmospheric scenario that coating layers of oxalic acid or its salts may be formed by physical and chemical processing on pre-existing particulates such as mineral dust and soot. Given the broad diversity of the observed heterogeneous ice nucleability of the oxalate species, it is not straightforward to predict whether an oxalate coating layer will improve or reduce the ice nucleation ability of the seed aerosol particles.

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

NASA Astrophysics Data System (ADS)

Wagner, R.; Möhler, O.; Saathoff, H.; Schnaiter, M.; Leisner, T.

2010-08-01

The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 μm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investigated species, namely sodium oxalate. Our experiments address the atmospheric scenario that coating layers of oxalic acid or its salts may be formed by physical and chemical processing on pre-existing particulates such as mineral dust and soot. Given the broad diversity of the observed heterogeneous ice nucleability of the oxalate species, it is not straightforward to predict whether an oxalate coating layer will improve or reduce the ice nucleation ability of the seed aerosol particles.

The immersion freezing behavior of size-segregated soot and kaolinite particles

NASA Astrophysics Data System (ADS)

Hartmann, S.; Augustin, S.; Clauss, T.; Niedermeier, D.; Raddatz, M.; Wex, H.; Shaw, R. A.; Stratmann, F.

2011-12-01

Heterogeneous ice nucleation plays a crucial role for ice formation in mixed-phase and cirrus clouds and has an important impact on precipitation formation, global radiation balances, and therefore Earth's climate (Cantrell and Heymsfield, 2005). Mineral dust and soot particles are found to be a major component of ice crystal residues (e.g., Pratt et al., 2009) so these substances are potential sources of atmospheric ice nuclei (IN). Experimental studies investigating the immersion freezing behavior of size-segregated soot and kaolinite particles conducted at the Leipzig Aerosol Cloud Interaction Simulator (LACIS) are presented. In our measurements only one aerosol particle is immersed in an air suspended water droplet which can trigger ice nucleation. The method facilitates very precise examinations with respect to temperature, ice nucleation time and ice nucleus size. Considering laboratory studies, the picture of the IN ability of soot particles is quite heterogeneous. Our studies show that submicron flame, spark soot particles and optionally coated with sulfuric acid to simulate chemically aging do not act as IN at temperatures higher than homogeneous freezing taking place. Therefore soot particles might not be an important source of IN for immersion freezing in the atmosphere. In contrast, kaolinite being representative for natural mineral dust with a well known composition and structure is found to be very active in forming ice for all freezing modes (e.g., Mason and Maybank, 1958). Analyzing the immersion freezing behavior of different sized kaolinite particles (300, 500 and 700 nm in diameter) the size effect was clearly observed, i.e. the ice fraction (number of frozen droplets per total number) scales with particle surface, i.e. the larger the ice nucleus surface the higher the ice fraction. The slope of the logarithm of the ice fraction as function of temperature is similar for all particle sizes investigated and fits very well with the results of Lüönd et al. (2010) and Murray et al. (2011). Heterogeneous ice nucleation rate coefficients are derived which can be used to describe the immersion freezing process size-segregated in cloud microphysical models.

A water activity based model of heterogeneous ice nucleation kinetics for freezing of water and aqueous solution droplets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Knopf, Daniel A.; Alpert, Peter A.

Immersion freezing of water and aqueous solutions by particles acting as ice nuclei (IN) is a common process of heterogeneous ice nucleation which occurs in many environments, especially in the atmosphere where it results in the glaciation of clouds. Here we experimentally show, using a variety of IN types suspended in various aqueous solutions, that immersion freezing temperatures and kinetics can be described solely by temperature, T, and solution water activity, aw, which is the ratio of the vapour pressure of the solution and the saturation water vapour pressure under the same conditions and, in equilibrium, equivalent to relative humiditymore » (RH). This allows the freezing point and corresponding heterogeneous ice nucleation rate coefficient, Jhet, to be uniquely expressed by T and aw, a result we term the aw based immersion freezing model (ABIFM). This method is independent of the nature of the solute and accounts for several varying parameters, including cooling rate and IN surface area, while providing a holistic description of immersion freezing and allowing prediction of freezing temperatures, Jhet, frozen fractions, ice particle production rates and numbers. Our findings are based on experimental freezing data collected for various IN surface areas, A, and cooling rates, r, of droplets variously containing marine biogenic material, two soil humic acids, four mineral dusts, and one organic monolayer acting as IN. For all investigated IN types we demonstrate that droplet freezing temperatures increase as A increases. Similarly, droplet freezing temperatures increase as the cooling rate decreases. The log 10(J het) values for the various IN types derived exclusively by T and aw, provide a complete description of the heterogeneous ice nucleation kinetics. Thus, the ABIFM can be applied over the entire range of T, RH, total particulate surface area, and cloud activation timescales typical of atmospheric conditions. Finally, we demonstrate that ABIFM can be used to derive frozen fractions of droplets and ice particle production for atmospheric models of cirrus and mixed phase cloud conditions.« less

A water activity based model of heterogeneous ice nucleation kinetics for freezing of water and aqueous solution droplets.

PubMed

Knopf, Daniel A; Alpert, Peter A

2013-01-01

Immersion freezing of water and aqueous solutions by particles acting as ice nuclei (IN) is a common process of heterogeneous ice nucleation which occurs in many environments, especially in the atmosphere where it results in the glaciation of clouds. Here we experimentally show, using a variety of IN types suspended in various aqueous solutions, that immersion freezing temperatures and kinetics can be described solely by temperature, T, and solution water activity, a(w), which is the ratio of the vapour pressure of the solution and the saturation water vapour pressure under the same conditions and, in equilibrium, equivalent to relative humidity (RH). This allows the freezing point and corresponding heterogeneous ice nucleation rate coefficient, J(het), to be uniquely expressed by T and a(w), a result we term the a(w) based immersion freezing model (ABIFM). This method is independent of the nature of the solute and accounts for several varying parameters, including cooling rate and IN surface area, while providing a holistic description of immersion freezing and allowing prediction of freezing temperatures, J(het), frozen fractions, ice particle production rates and numbers. Our findings are based on experimental freezing data collected for various IN surface areas, A, and cooling rates, r, of droplets variously containing marine biogenic material, two soil humic acids, four mineral dusts, and one organic monolayer acting as IN. For all investigated IN types we demonstrate that droplet freezing temperatures increase as A increases. Similarly, droplet freezing temperatures increase as the cooling rate decreases. The log10(J(het)) values for the various IN types derived exclusively by Tand a(w), provide a complete description of the heterogeneous ice nucleation kinetics. Thus, the ABIFM can be applied over the entire range of T, RH, total particulate surface area, and cloud activation timescales typical of atmospheric conditions. Lastly, we demonstrate that ABIFM can be used to derive frozen fractions of droplets and ice particle production for atmospheric models of cirrus and mixed phase cloud conditions.

A water activity based model of heterogeneous ice nucleation kinetics for freezing of water and aqueous solution droplets

DOE PAGES

Knopf, Daniel A.; Alpert, Peter A.

2013-04-24

Immersion freezing of water and aqueous solutions by particles acting as ice nuclei (IN) is a common process of heterogeneous ice nucleation which occurs in many environments, especially in the atmosphere where it results in the glaciation of clouds. Here we experimentally show, using a variety of IN types suspended in various aqueous solutions, that immersion freezing temperatures and kinetics can be described solely by temperature, T, and solution water activity, aw, which is the ratio of the vapour pressure of the solution and the saturation water vapour pressure under the same conditions and, in equilibrium, equivalent to relative humiditymore » (RH). This allows the freezing point and corresponding heterogeneous ice nucleation rate coefficient, Jhet, to be uniquely expressed by T and aw, a result we term the aw based immersion freezing model (ABIFM). This method is independent of the nature of the solute and accounts for several varying parameters, including cooling rate and IN surface area, while providing a holistic description of immersion freezing and allowing prediction of freezing temperatures, Jhet, frozen fractions, ice particle production rates and numbers. Our findings are based on experimental freezing data collected for various IN surface areas, A, and cooling rates, r, of droplets variously containing marine biogenic material, two soil humic acids, four mineral dusts, and one organic monolayer acting as IN. For all investigated IN types we demonstrate that droplet freezing temperatures increase as A increases. Similarly, droplet freezing temperatures increase as the cooling rate decreases. The log 10(J het) values for the various IN types derived exclusively by T and aw, provide a complete description of the heterogeneous ice nucleation kinetics. Thus, the ABIFM can be applied over the entire range of T, RH, total particulate surface area, and cloud activation timescales typical of atmospheric conditions. Finally, we demonstrate that ABIFM can be used to derive frozen fractions of droplets and ice particle production for atmospheric models of cirrus and mixed phase cloud conditions.« less

Contributions of Uncertainty in Droplet Nucleation to the Indirect Effect in Global Models

NASA Astrophysics Data System (ADS)

Rothenberg, D. A.; Wang, C.; Avramov, A.

2016-12-01

Anthropogenic aerosol perturbations to clouds and climate (the indirect effect, or AIE) contribute significant uncertainty towards understanding contemporary climate change. Despite refinements over the past two decades, modern global aerosol-climate models widely disagree on the magnitude of AIE, and wholly disagree with satellite estimates. Part of the spread in estimates of AIE arises from a lack of constraints on what exactly comprised the pre-industrial atmospheric aerosol burden, but another component is attributable to inter-model differences in simulating the chain of aerosol-cloud-precipitation processes which ultimately produce the indirect effect. Thus, one way to help constrain AIE is to thoroughly investigate the differences in aerosol-cloud processes and interactions occurring in these models. We have configured one model, the CESM/MARC, with a suite of parameterizations affecting droplet activation. Each configuration produces similar climatologies with respect to precipitation and cloud macrophysics, but shows different sensitivies to aerosol perturbation - up to 1 W/m^2 differences in AIE. Regional differences in simulated aerosol-cloud interactions, especially in marine regions with little anthropogenic pollution, contribute to the spread in these AIE estimates. The baseline pre-industrial droplet number concentration in marine regions dominated by natural aerosol strongly predicts the magnitude of each model's AIE, suggesting that targeted observations of cloud microphysical properties across different cloud regimes and their sensitivity to aerosol influences could help provide firm constraints and targets for models. Additionally, we have performed supplemental fully-coupled (atmosphere/ocean) simulations with each model configuration, allowing the model to relax to equilibrium following a change in aerosol emissions. These simulations allow us to assess the slower-timescale responses to aerosol perturbations. The spread in fast model responses (which produce the noted changes in indirect effect or forcing) gives rise to large differences in the equilibrium climate state of each configuration. We show that these changes in equilibrium climate state have implications for AIE estimates from model configurations tuned to the present-day climate.

Evaluation of the Physical and Chemical Properties of Eyjafjallajökull Volcanic Plume Using a Cloud-Resolving Model

NASA Astrophysics Data System (ADS)

Spiridonov, Vlado; Curic, Mladjen

2013-11-01

The Eyjafjallajökull volcanic eruption, which occurred on April 14, 2010, caused many environmental, air traffic and health problems. An attempt has been made to demonstrate for the first time that certain improvements could be made in the quantitative prediction of the volcanic ash parameters, and in the accounting of the processes in the immediate vicinity of the volcano, using a cloud-resolving model. This type of explicit modeling by treatment of volcanic ash and sulfate chemistry parameterization, with input of a number parameters describing the volcanic source, is the way forward for understanding the complex processes in plumes and in the future plume dispersion modeling. Results imply that the most significant microphysical processes are those related to accretion of cloud water, cloud ice and rainwater by snow, and accretion of rain and snow by hail. The dominant chemical conversion rates that give a great contribution to the sulfate budget are nucleation and dynamic scavenging and oxidation processes. A three-dimensional numerical experiment has shown a very realistic simulation of volcanic ash and other chemical compounds evolution, with a sloping structure strongly influenced by the meteorological conditions. In-cloud oxidation by H2O2 is the dominant pathway for SO2 oxidation and allows sulfate to be produced within the SO2 source region. The averaged cloud water pH of about 5.8 and rainwater pH of 4.5 over simulation time show quantitatively how the oxidation may strongly influence the sulfate budget and acidity of volcanic cloud. Compared to observations, model results are close in many aspects. Information on the near field volcanic plume behavior is essential for early preparedness and evacuation. This approach demonstrates a potential improvement in quantitative predictions regarding the volcanic plume distribution at different altitudes. It could be a useful tool for modeling volcanic plumes for better emergency measures planning.

Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley

NASA Astrophysics Data System (ADS)

Liggio, J.; Pierce, J. R.; Leaitch, R.; Macdonald, A.; Whistler Aerosol; Cloud Study (WACS2010) Team

2011-12-01

The Whistler Aerosol and Cloud Study (WACS 2010), included intensive measurements of trace gases and particles at two sites on Whistler Mountain. Between July 6-11, 2010 there was a sustained high-pressure system over the region with cloud-free and higher-temperature conditions. During this period, the organic aerosol concentrations rose from <1 to 6 μ g m-3. Precursor gas and aerosol composition measurements show that these organics were almost entirely of secondary biogenic nature. Throughout July 6-11, the anthropogenic influence was minimal with sulfate concentrations < 0.2 μ g m-3 and SO2 mixing ratios ≈ 0.5 ppbv. Although SO2 mixing ratios were relatively low, companion box-model simulations show that nucleation and growth may be modeled accurately if Jnuc=3x10-7[H2SO4] and the organics are treated as effectively non-volatile. Due to the low condensation sink and the fast rate of condensing organics, the nucleated particles grew rapidly (2-5 nm hr-1) with a high probability of growing to CCN sizes before being scavenged by coagulation with larger particles (>10% growing to 100 nm in the first two days). The particles were observed to ultimately grow to ~200 nm after three days. Comparisons of SMPS with DMT CCN data show that particle hygroscopicity was generally around 0.1-0.11. The concentration of particles with diameters larger than 100 nm as well as CCN at 3% supersaturation rise from about 300 cm-3 to 1200 cm-3 during the 5 days due entirely to nucleation and growth. Relatively little SO2 is necessary to generate nucleation and growth to CCN sizes when biogenic SOA is abundant. This case offers a unique look at processes that may have controlled CCN formation in the pristine pre-industrial forested continental atmosphere.

Immersion freezing by SnomaxTM particles: Comparison of results from different instruments

NASA Astrophysics Data System (ADS)

Wex, Heike; Stratmann, Frank; Rösch, Michael; Niedermeier, Dennis; Nilius, Björn; Möhler, Ottmar; Mitra, Subir K.; Koop, Thomas; Jantsch, Evelyn; Hiranuma, Naruki; Diehl, Karoline; Curtius, Joachim; Budke, Carsten; Boose, Yvonne; Augustin, Stefanie

2014-05-01

Within the DFG funded research unit INUIT (Ice Nucleation research UnIT, FOR 1525), an effort was made to compare results on immersion freezing from a suite of different instruments. Besides mineral dusts, SnomaxTM was picked as one of the substances that were examined by all participating groups. Here, the comparison of the results for SnomaxTM is presented. Every participating group used SnomaxTM from the same batch and, as far as possible, the same particle generation set-up. Instruments participating in the comparison were, in alphabetical order, an acoustic levitator (Diehl et al., 2009), AIDA (Connolly et al., 2009), BINARY (Budke et al., 2013), FINCH (Bundke et al., 2008), LACIS (Hartmann et al., 2011), PINC (Chou et al., 2011) and the Mainz vertical windtunnel (Diehl et al., 2011). Some of the instruments examined droplets directly produced from SnomaxTM suspensions, where the suspensions could have a wide range of concentrations. Other instruments used size segregated particles which were generated via atomization from a SnomaxTM suspension and subsequent drying, followed by size selection with a DMA (Differential Mobility Analyzer). These particles were then activated to droplets and cooled subsequently. For these, the number of ice nucleation active protein complexes present in the droplets depended on the original particle size (for details see e.g. Hartmann et al., 2013). Also, the different measurements spanned a range of different time scales. The shortest residence time of roughly 1 second was used for LACIS measurements, and the longest one was about 6 seconds used in the BINARY setup with a cooling rate of 1 K/min. All data were evaluated using two different approaches: 1) a time dependent approach following Classical Nucleation Theory which included the use of a contact angle distribution (see Niedermeier et al., 2014); 2) a singular approach using an active site density per mass (see Vali, 1971, Murray et al., 2012). Both approaches were found to work equally well, hence freezing by SnomaxTM can be considered to show no time dependence. Particularly data from LACIS and BINARY, i.e. from the "fastest" and "slowest" measurements, were found to agree very well. Acknowledgement: This work was done within the framework of the DFG funded Ice Nucleation research UnIT (INUIT, FOR 1525). Literature Budke et al. (2013), Investigation of Heterogeneous Ice Nucleation Using a Novel Optical Freezing Array, AIP Conference Proceedings, 1527, 949-951, doi: 10.1064/1.4803429. Bundke et al. (2008), The fast Ice Nucleus chamber FINCH, Atmos. Res. 90, 180-186. Chou et al. (2011), Ice nuclei properties within a Saharan dust event at the Jungfraujoch in the Swiss Alps, Atmos. Chem. Phys., 11, 4725-4738. Connolly, et al. (2009), Studies of heterogeneous freezing by three different desert dust samples, Atmos. Chem. Phys., 9, 2805-2824. Diehl et al. (2011), The Mainz vertical wind tunnel facility: A review of 25 years of laboratory experiments on cloud physics and chemistry. In: J.D. Pereira (Ed.), Wind tunnels: Aerodynamics, models, and experiments. Nova Science Publishers, Inc., Chapter 2. Diehl et al. (2009), Homogeneous freezing of single sulfuric and nitric acid solution drops levitated in an acoustic trap, Atm. Res., 94, 356-361, doi:10.1016/j.atmosres.2009.06.001. Hartmann et al. (2011), Homogeneous and heterogeneous ice nucleation at LACIS: Operating principle and theoretical studies, Atmos. Chem. Phys., 11, 1753-1767. Hartmann et al. (2013), Immersion freezing of ice nucleating active protein complexes, Atmos. Chem. Phys., 13, 5751-5766. Murray et al. (2012), Ice nucleation by particles immersed in supercooled cloud droplets, Chem. Soc. Rev., 41, 6519-6554. Niedermeier et al. (2014), A computationally-efficient description of heterogeneous freezing: A simplified version of the Soccer ball model, Geophys. Res. Lett., 10.1002/2013GL058684. Vali, G. (1971), Quantitative evaluation of experimental results on heterogeneous freezing nucleation of supercooled liquids, J. Atmos. Sci., 28(3), 402-409.

Marine Aerosols and Clouds.

PubMed

Brooks, Sarah D; Thornton, Daniel C O

2018-01-03

The role of marine bioaerosols in cloud formation and climate is currently so uncertain that even the sign of the climate forcing is unclear. Marine aerosols form through direct emissions and through the conversion of gas-phase emissions to aerosols in the atmosphere. The composition and size of aerosols determine how effective they are in catalyzing the formation of water droplets and ice crystals in clouds by acting as cloud condensation nuclei and ice nucleating particles, respectively. Marine organic aerosols may be sourced both from recent regional phytoplankton blooms that add labile organic matter to the surface ocean and from long-term global processes, such as the upwelling of old refractory dissolved organic matter from the deep ocean. Understanding the formation of marine aerosols and their propensity to catalyze cloud formation processes are challenges that must be addressed given the major uncertainties associated with aerosols in climate models.

Ice nucleating particles over the Eastern Mediterranean measured at ground and by unmanned aircraft systems

NASA Astrophysics Data System (ADS)

Weber, Daniel; Schrod, Jann; Drücke, Jaqueline; Keleshis, Christos; Pikridas, Michael; Ebert, Martin; Cvetkovic, Bojan; Nickovic, Slobodan; Baars, Holger; Marinou, Eleni; Vrekoussis, Mihalis; Sciare, Jean; Mihalopoulos, Nikos; Curtius, Joachim; Bingemer, Heinz G.

2017-04-01

During the intensive INUIT-BACCHUS-ACTRIS field campaign focusing on aerosols, clouds and ice nucleation in the Eastern Mediterranean in April 2016, we have measured the abundance of ice nucleating particles (INP) in the lower troposphere both with unmanned aircraft systems (UAS) as well as from the ground. Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UAS and were analyzed immediately after collection on site in the ice nucleus counter FRIDGE for INP active at -20˚ C to -30˚ C in the deposition/condensation mode (INPD). Immersion freezing INP (INPI) were sampled on membrane filters and were analysed in aqueous extracts by the drop freezing method on the cold stage of FRIDGE. Ground samples were collected at the Cyprus Atmospheric Observatory (CAO) in Agia Marina Xyliatou (Latitude; 35˚ 2' 8" N; Longitude: 33˚ 3' 26" E; Altitude: 532 m a.s.l.). During the one-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers altitude. Here we present INP data from 42 individual flights, together with OPC aerosol number concentrations, backscatter and depolarization retrievals from the Polly-XT Raman Lidar, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INP with the particulate mass (PM), the Lidar retrievals and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INP std.l-1 were measured at -30˚ C. The INPD concentration in elevated plumes was on average a factor of 10 higher than at ground level. The INPI concentration at ground also agreed with PM levels and exceeded the ground-based INPD concentration by more than one order of magnitude. Since desert dust is transported for long distances over wide areas of the globe predominantly at several km altitude, we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation. This project received funding from the European Union's Seventh Framework Programme (FP7) project BACCHUS under grant agreement no. 603445, and the European Union's Horizon 2020 research and innovation programme ACTRIS-2 under grant agreement No 654109, and the Deutsche Forschungsgemeinschaft (DFG) under the Research Unit FOR 1525 (INUIT).

Cloud condensation nuclei droplet growth kinetics of ultrafine particles during anthropogenic nucleation events

NASA Astrophysics Data System (ADS)

Shantz, N. C.; Pierce, J. R.; Chang, R. Y.-W.; Vlasenko, A.; Riipinen, I.; Sjostedt, S.; Slowik, J. G.; Wiebe, A.; Liggio, J.; Abbatt, J. P. D.; Leaitch, W. R.

2012-02-01

Evolution of the cloud condensation nucleus (CCN) activity of 36 ± 4 nm diameter anthropogenic aerosol particles at a water supersaturation of 1.0 ± 0.1% is examined for particle nucleation and growth. During the early stages of one event, relatively few of the anthropogenic particles at 36 nm were CCN active and their growth rates by water condensation were delayed relative to ammonium sulphate particles. As the event progressed, the particle size distribution evolved to larger sizes and the relative numbers of particles at 36 nm that were CCN active increased until all the 36 nm particles were activating at the end of the event. Based on the chemistry of larger particles and the results from an aerosol chemical microphysics box model, the increase in CCN activity of the particles was most likely the result of the condensation of sulphate in this case. Despite the increased CCN activity, a delay was observed in the initial growth of these particles into cloud droplets, which persisted even when the aerosol was most CCN active later in the afternoon. Simulations show that the delay in water uptake is explained by a reduction of the mass accommodation coefficient assuming that the composition of the 36 nm particles is the same as the measured composition of the 60-100 nm particles.

An experimental and numerical study of the light scattering properties of ice crystals with black carbon inclusions

NASA Astrophysics Data System (ADS)

Arienti, Marco; Geier, Manfred; Yang, Xiaoyuan; Orcutt, John; Zenker, Jake; Brooks, Sarah D.

2018-05-01

We investigate the optical properties of ice crystals nucleated on atmospheric black carbon (BC). The parameters examined in this study are the shape of the ice crystal, the volume fraction of the BC inclusion, and its location inside the crystal. We report on new spectrometer measurements of forward scattering and backward polarization from ice crystals nucleated on BC particles and grown under laboratory-controlled conditions. Data from the Cloud and Aerosol Spectrometer with Polarization (CASPOL) are used for direct comparison with single-particle calculations of the scattering phase matrix. Geometrical optics and discrete dipole approximation techniques are jointly used to provide the best compromise of flexibility and accuracy over a broad range of size parameters. Together with the interpretation of the trends revealed by the CASPOL measurements, the numerical results confirm previous reports on absorption cross-section magnification in the visible light range. Even taking into account effects of crystal shape and inclusion position, the ratio between absorption cross-section of the compound particle and the absorption cross-section of the BC inclusion alone (the absorption magnification) has a lower bound of 1.5; this value increases to 1.7 if the inclusion is centered with respect to the crystal. The simple model of BC-ice particle presented here also offers new insights on the effect of the relative position of the BC inclusion with respect to the crystal's outer surfaces, the shape of the crystal, and its size.

Visual verification and analysis of cluster detection for molecular dynamics.

PubMed

Grottel, Sebastian; Reina, Guido; Vrabec, Jadran; Ertl, Thomas

2007-01-01

A current research topic in molecular thermodynamics is the condensation of vapor to liquid and the investigation of this process at the molecular level. Condensation is found in many physical phenomena, e.g. the formation of atmospheric clouds or the processes inside steam turbines, where a detailed knowledge of the dynamics of condensation processes will help to optimize energy efficiency and avoid problems with droplets of macroscopic size. The key properties of these processes are the nucleation rate and the critical cluster size. For the calculation of these properties it is essential to make use of a meaningful definition of molecular clusters, which currently is a not completely resolved issue. In this paper a framework capable of interactively visualizing molecular datasets of such nucleation simulations is presented, with an emphasis on the detected molecular clusters. To check the quality of the results of the cluster detection, our framework introduces the concept of flow groups to highlight potential cluster evolution over time which is not detected by the employed algorithm. To confirm the findings of the visual analysis, we coupled the rendering view with a schematic view of the clusters' evolution. This allows to rapidly assess the quality of the molecular cluster detection algorithm and to identify locations in the simulation data in space as well as in time where the cluster detection fails. Thus, thermodynamics researchers can eliminate weaknesses in their cluster detection algorithms. Several examples for the effective and efficient usage of our tool are presented.

Integrating biomass, sulphate and sea-salt aerosol responses into a microphysical chemical parcel model: implications for climate studies.

PubMed

Ghosh, S; Smith, M H; Rap, A

2007-11-15

Aerosols are known to influence significantly the radiative budget of the Earth. Although the direct effect (whereby aerosols scatter and absorb solar and thermal infrared radiation) has a large perturbing influence on the radiation budget, the indirect effect (whereby aerosols modify the microphysical and hence the radiative properties and amounts of clouds) poses a greater challenge to climate modellers. This is because aerosols undergo chemical and physical changes while in the atmosphere, notably within clouds, and are removed largely by precipitation. The way in which aerosols are processed by clouds depends on the type, abundance and the mixing state of the aerosols concerned. A parametrization with sulphate and sea-salt aerosol has been successfully integrated within the Hadley Centre general circulation model (GCM). The results of this combined parametrization indicate a significantly reduced role, compared with previous estimates, for sulphate aerosol in cloud droplet nucleation and, consequently, in indirect radiative forcing. However, in this bicomponent system, the cloud droplet number concentration, N(d) (a crucial parameter that is used in GCMs for radiative transfer calculations), is a smoothly varying function of the sulphate aerosol loading. Apart from sea-salt and sulphate aerosol particles, biomass aerosol particles are also present widely in the troposphere. We find that biomass smoke can significantly perturb the activation and growth of both sulphate and sea-salt particles. For a fixed salt loading, N(d) increases linearly with modest increases in sulphate and smoke masses, but significant nonlinearities are observed at higher non-sea-salt mass loadings. This non-intuitive N(d) variation poses a fresh challenge to climate modellers.

A new laboratory facility to study the interactions of aerosols, cloud droplets/ice crystals, and trace gases in a turbulent environment: The Π Chamber

NASA Astrophysics Data System (ADS)

Cantrell, W. H., II; Chang, K.; Ciochetto, D.; Niedermeier, D.; Bench, J.; Shaw, R. A.

2014-12-01

A detailed understanding of gas-aerosol-cloud interaction within the turbulent atmosphere is of prime importance for an accurate understanding of Earth's climate system. As one example: While every cloud droplet began as an aerosol particle, not every aerosol particle becomes a cloud droplet. The particle to droplet transformation requires that the particle be exposed to some critical concentration of water vapor, which differs for different combinations of particle size and chemical composition. Similarly, the formation of ice particles in mixed phase clouds is also catalyzed by aerosol particles. Even in the simplest scenarios it is challenging to gain a full understanding of the aerosol activation and ice nucleation processes. At least two other factors contribute significantly to the complexity observed in the atmosphere. First, aerosols and cloud particles are not static entities, but are continuously interacting with their chemical environment, and therefore changing in their properties. Second, clouds are ubiquitously turbulent, so thermodynamic and compositional variables, such as water vapor or other trace gas concentrations, fluctuate in space and time. Indeed, the coupling between turbulence and microphysical processes is one of the major research challenges in cloud physics. We have developed a multiphase, turbulent reaction chamber, (dubbed the Π Chamber, after the internal volume of 3.14 cubic meters) designed to address the problems outlined above. It is capable of pressures ranging from sea level to ~ 100 mbar, and can sustain temperatures of +40 to -55 ºC. We can independently control the temperatures on the surfaces of three heat transfer zones. This allows us to establish a temperature gradient between the floor and ceiling inducing Rayleigh-Benard convection and inducing a turbulent environment. Interior surfaces are electropolished stainless steel to facilitate cleaning before and after chemistry experiments. At present, supporting instrumentation includes a suite of aerosol generation and characterization techniques, a laser Doppler interferometer, and a holographic cloud particle imaging system.We will present detailed specifications, an overview of the supporting instrumentation, and initial characterization experiments from the Π chamber.

Pre-activation of aerosol particles by ice preserved in pores

NASA Astrophysics Data System (ADS)

Marcolli, Claudia

2017-02-01

Pre-activation denotes the capability of particles or materials to nucleate ice at lower relative humidities or higher temperatures compared to their intrinsic ice nucleation efficiency after having experienced an ice nucleation event or low temperature before. This review presumes that ice preserved in pores is responsible for pre-activation and analyses pre-activation under this presumption. Idealized trajectories of air parcels are used to discuss the pore characteristics needed for ice to persist in pores and to induce macroscopic ice growth out of the pores. The pore width needed to keep pores filled with water decreases with decreasing relative humidity as described by the inverse Kelvin equation. Thus, narrow pores remain filled with ice well below ice saturation. However, the smaller the pore width, the larger the melting and freezing point depressions within the pores. Therefore, pre-activation due to pore ice is constrained by the melting of ice in narrow pores and the sublimation of ice from wide pores imposing restrictions on the temperature and relative humidity range of pre-activation for cylindrical pores. Ice is better protected in ink-bottle-shaped pores with a narrow opening leading to a large cavity. However, whether pre-activation is efficient also depends on the capability of ice to grow macroscopically, i.e. out of the pore. A strong effect of pre-activation is expected for swelling pores, because at low relative humidity (RH) their openings narrow and protect the ice within them against sublimation. At high relative humidities, they open up and the ice can grow to macroscopic size and form an ice crystal. Similarly, ice protected in pockets is perfectly sheltered against sublimation but needs the dissolution of the surrounding matrix to be effective. Pores partially filled with condensable material may also show pre-activation. In this case, complete filling occurs at lower RH than for empty pores and freezing shifts to lower temperatures.Pre-activation experiments confirm that materials susceptible to pre-activation are indeed porous. Pre-activation was observed for clay minerals like illite, kaolinite, and montmorillonite with inherent porosity. The largest effect was observed for the swelling clay mineral montmorillonite. Some materials may acquire porosity, depending on the formation and processing conditions. Particles of CaCO3, meteoritic material, and volcanic ash showed pre-activation for some samples or in some studies but not in other ones. Quartz and silver iodide were not susceptible to pre-activation.Atmospheric relevance of pre-activation by ice preserved in pores may not be generally given but depend on the atmospheric scenario. Lower-level cloud seeding by pre-activated particles released from high-level clouds crucially depends on the ability of pores to retain ice at the relative humidities and temperatures of the air masses they pass through. Porous particles that are recycled in wave clouds may show pre-activation with subsequent ice growth as soon as ice saturation is exceeded after having passed a first cloud event. Volcanic ash particles and meteoritic material likely influence ice cloud formation by pre-activation. Therefore, the possibility of pre-activation should be considered when ice crystal number densities in clouds exceed the number of ice-nucleating particles measured at the cloud forming temperature.

Modeling studying on ice formation by bacteria in warm-based convective cloud

NASA Astrophysics Data System (ADS)

Sun, J.

2005-12-01

Bacteria have been recognized as cloud condensation nuclei (CCN), and certain bacteria, commonly found in plants, have exhibited capacity to act as ice nuclei (IN) at temperatures as warm as -2 °C. These ice nucleating bacteria are readily disseminated into the atmosphere and have been observed in clouds at altitudes of several kilometres. It is noteworthy that over 20 years ago, one assumed the possibility of bacterial transport and their importance into cloud formation process, rain and precipitation, as well as causing disease in plants and animal kingdom. We used a 1-D cumulus cloud model with the CCOPE 19th July 1981 case and the observed field profile of bacterial concentration, to simulate the significance of bacteria as IN through condensation freezing mechanism. In this paper, we will present our results on the role of bacteria as active ice nuclei in the developing stage of cumulus clouds, and their potential significance in atmospheric sciences.

Characterization of Aircraft Produced Soot and Contrails Near the Tropopause

NASA Technical Reports Server (NTRS)

Hallett, John; Gudson, James G.

1997-01-01

Participation in the SUCCESS project primarily involved development and deployment of specific instruments for characterizing jet aircraft exhaust emissions as particulates and their subsequent evolution as contrail particles, either liquid or solid, as cirrus. Observations can be conveniently considered in two categories - close or distant from the aircraft. Thus close to the aircraft the exhaust is mixing through the engine turbulence with a much drier and colder environment and developing water/ ice supersaturation along the trail depending on circumstances (near field), whereas distant from the aircraft (far field) the exhaust has cooled essentially to ambient temperature, the turbulence has decayed and any particle growth or evaporation is controlled by the prevailing ambient conditions. Intermediate between these two regions the main aircraft vortices form (one on each side of the aircraft) which tend to inhibit mixing under some conditions, a region extending from a few aircraft lengths to sometimes a hundred times this distance. Our approach to the problem lay in experience gained in characterizing the smoke from hydrocarbon combustion in terms of its cloud forming properties and its potential influence on the radiation properties of the smoke and subsequent cloud from the viewpoint of reduction (absorbtion and scattering ) of solar radiation flux leading to significant global cooling (Hudson et al 1991; Hallett and Hudson 1991). Engine exhaust contains a much smaller proportion of the fuel carbon than is sometimes present in ordinary combustion (less than 0.01% compared with 10%) and influences condensation in quite different ways, to be characterized by the Cloud Condensation Nucleus, CCN - supersaturation spectrum. The transition to ice is to be related to the dilution of solution droplets to freeze by homogeneous nucleation at temperatures somewhat below -40C (Pueschel et al 1998). The subsequent growth of ice particles depends critically on temperature, supersaturation and to some extent pressure, as is demonstrated in an NSF funded project being carried out in parallel with the work reported here. As will be discussed below, nucleation processes themselves and also exhaust impurities also influence the growth of ice particles and may control some aspects of growth of ice in contrails. Instrumentation was designed to give insight into these questions and to be flown on the NASA DC- 8 as a platform. In addition a modest program was undertaken to investigate the properties of laboratory produced smoke produced under controlled conditions from the viewpoint of forming both CCN and CN. The composition of the smoke could inferred from a thermal characterization technique; larger particles were captured by formvar replicator for detailed analysis; ice particles were captured and evaporated in flight on a new instrument, the cloudscope, to give their mass, density and impurity content.

Effects Of Crystallographic Properties On The Ice Nucleation Properties Of Volcanic Ash Particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kulkarni, Gourihar R.; Nandasiri, Manjula I.; Zelenyuk, Alla

2015-04-28

Specific chemical and physical properties of volcanic ash particles that could affect their ability to induce ice formation are poorly understood. In this study, the ice nucleating properties of size-selected volcanic ash and mineral dust particles in relation to their surface chemistry and crystalline structure at temperatures ranging from –30 to –38 °C were investigated in deposition mode. Ice nucleation efficiency of dust particles was higher compared to ash particles at all temperature and relative humidity conditions. Particle characterization analysis shows that surface elemental composition of ash and dust particles was similar; however, the structural properties of ash samples weremore » different.« less

Deposition nucleation viewed as homogeneous or immersion freezing in pores and cavities

NASA Astrophysics Data System (ADS)

Marcolli, C.

2013-06-01

Heterogeneous ice nucleation is an important mechanism for the glaciation of mixed phase clouds and may also be relevant for cloud formation and dehydration at the cirrus cloud level. It is thought to proceed through different mechanisms, namely contact, condensation, immersion and deposition nucleation. Supposedly, deposition nucleation is the only pathway which does not involve liquid water but occurs by direct water vapor deposition on a surface. This study challenges this classical view by putting forward the hypothesis that what is called deposition nucleation is in fact homogeneous or immersion nucleation occurring in pores and cavities that may form between aggregated primary particles and fill with water at relative humidity RHw < 100% because of the inverse Kelvin effect. Evidence for this hypothesis of pore condensation and freezing (PCF) originates from a number of only loosely connected scientific areas. The prime example for PCF is ice nucleation in clay minerals and mineral dusts, for which the data base is best. Studies on freezing in confinement carried out on mesoporous silica materials such as SBA-15, SBA-16, MCM-41, zeolites and KIT have shown that homogeneous ice nucleation occurs abruptly at T=230-235 K in pores with diameters (D) of 3.5-4 nm or larger but only gradually at T=210-230 K in pores with D=2.5-3.5 nm. Melting temperatures in pores are depressed by an amount that can be described by the Gibbs-Thomson equation. Water adsorption isotherms of MCM-41 show that pores with D=3.5-4 nm fill with water at RHw = 56-60% in accordance with an inverse Kelvin effect. Water in such pores should freeze homogeneously for T < 235 K even before relative humidity with respect to ice (RHi) reaches ice saturation. Ice crystal growth by water vapor deposition from the gas phase is therefore expected to set in as soon as RHw > 100%. Pores with D > 7.5 nm fill with water at RHi > 100% for T < 235 K and are likely to freeze homogeneously as soon as they are filled with water. Water in pores can freeze in immersion mode at T > 235 K if the pore walls contain an active site. Pore analysis of clay minerals shows that kaolinites exhibit pore structures with pore diameters of 20-50 nm. The mesoporosity of illites and montmorillonites is characterized by pores with T = 2-5 nm. The number and size of pores is distinctly increased in acid treated montmorillonites like K10. Many clay minerals and mineral dusts show a strong increase in ice nucleation efficiency when temperature is decreased below 235 K. Such an increase is difficult to explain when ice nucleation is supposed to occur by a deposition mechanism, but evident when assuming freezing in pores, because for homogeneous ice nucleation only small pore volumes are needed, while heterogeneous ice nucleation requires larger pore structures to contain at least one active site for immersion nucleation. Together, these pieces of evidence strongly suggest that ice nucleation within pores should be the prevailing freezing mechanism of clay minerals for RHw below water saturation. Extending the analysis to other types of ice nuclei shows that freezing in pores and cracks is probably the prevailing ice nucleation mechanism for glassy and volcanic ash aerosols at RHw below water saturation. Freezing of water in carbon nanotubes might be of significance for ice nucleation by soot aerosols. No case could be identified that gives clear evidence of ice nucleation by water vapor deposition on a solid surface. Inspection of ice nuclei with a close lattice match to ice, such as silver iodide or SnomaxTM, show that for high ice nucleation efficiency below water saturation the presence of impurities or cracks on the surface may be essential. Soluble impurities promote the formation of a liquid phase below water saturation in patches on the surface or as a complete surface layer that offers an environment for immersion freezing. If porous aerosol particles come in contact with semivolatile vapors, these will condense preferentially in pores before a coating on the surface of the particles is formed. A pore partially filled with condensed species attracts water at lower RHw than an empty pore, but the aqueous solution that forms in the pore will freeze at a higher RHi than pure water. The ice nucleation ability of pores completely filled with condensed organic species might be totally impeded. Pores might also be important for preactivation, the capability of a particle to nucleate ice at lower RHi in subsequent experiments when compared to the first initial ice nucleation event. Preactivation has often been explained by persistence of ice embryos at specific sites like dislocations, steps, kinks or pores. However, it is not clear how such features can preserve an ice embryo at RHi < 100%. Rather, ice embryos could be preserved when embedded in water. To keep liquid water at RHw well below 100%, narrow pores are needed but to avoid a strong melting point depression large pores are favorable. A narrow pore opening and a large inner volume are combined in "ink bottle" pores. Such "ink bottle" pores would be suited to preserve ice at RHi < 100% and can arise e.g. in spaces between aggregated particles.

Direct in situ observation of ZnO nucleation and growth via transmission X-ray microscopy

NASA Astrophysics Data System (ADS)

Tay, S. E. R.; Goode, A. E.; Nelson Weker, J.; Cruickshank, A. A.; Heutz, S.; Porter, A. E.; Ryan, M. P.; Toney, M. F.

2016-01-01

The nucleation and growth of a nanostructure controls its size and morphology, and ultimately its functional properties. Hence it is crucial to investigate growth mechanisms under relevant growth conditions at the nanometer length scale. Here we image the nucleation and growth of electrodeposited ZnO nanostructures in situ, using a transmission X-ray microscope and specially designed electrochemical cell. We show that this imaging technique leads to new insights into the nucleation and growth mechanisms in electrodeposited ZnO including direct, in situ observations of instantaneous versus delayed nucleation.The nucleation and growth of a nanostructure controls its size and morphology, and ultimately its functional properties. Hence it is crucial to investigate growth mechanisms under relevant growth conditions at the nanometer length scale. Here we image the nucleation and growth of electrodeposited ZnO nanostructures in situ, using a transmission X-ray microscope and specially designed electrochemical cell. We show that this imaging technique leads to new insights into the nucleation and growth mechanisms in electrodeposited ZnO including direct, in situ observations of instantaneous versus delayed nucleation. Electronic supplementary information (ESI) available: Methods and videos of nanoparticle growth. See DOI: 10.1039/c5nr07019h

Effect of nucleation time on bending response of ionic polymer–metal composite actuators

DOE PAGES

Kim, Suran; Hong, Seungbum; Choi, Yoon-Young; ...

2013-07-02

We attempted an autocatalytic electro-less plating of nickel in order to replace an electroless impregnation-reduction (IR) method in ionic polymer–metal composite (IPMC) actuators to reduce cost and processing time. Because nucleation time of Pd–Sn colloids is the determining factor of overall processing time, we used the nucleation time as our control parameter. In order to optimize nucleation time and investigate its effect on the performance of IPMC actuators, we analyzed the relationship between the nucleation time, interface morphology and electrical properties. The optimized nucleation time was 10 h. Furthermore, the trends of the performance and electrical properties as a functionmore » of nucleation time were attributed to the fact that the Ni penetration depth was determined by the minimum diffusion length of either Pd–Sn colloids or reducing agent ions. The Ni-IPMC actuators can be fabricated less than 14 h processing time without deteriorating performance of the actuators, which is comparable to Pt-IPMC prepared by IR method.« less

Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

NASA Astrophysics Data System (ADS)

Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

2013-12-01

The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles <100 nm generated by means of jets were enhanced with time compared with larger sizes. In contrast, all particle sizes were equally enhanced when frits were used. Aerosolized particles were hygroscopic, a finding with significance for warm cloud formation and potential liquid-to-ice phase transformations. Aqueous and dry aerosolized particles from biologically active mesocosm water were found to efficiently nucleate ice exposed to supersaturated water vapor. The majority of particles, including those nucleating ice, consisted of a sea salt core coated with organic material dominated by the carboxyl functional group, and corresponded to a particle type commonly found in marine air. Our results provide improved estimates of marine aerosol production, chemical composition, and hygroscopicity, as well as an accurate physical and chemical representation of ice nucleation by marine biogenic aerosol particles for use in cloud and climate models.

A Comprehensive Two-moment Warm Microphysical Bulk Scheme :

NASA Astrophysics Data System (ADS)

Caro, D.; Wobrock, W.; Flossmann, A.; Chaumerliac, N.

The microphysic properties of gaz, aerosol particles, and hydrometeors have impli- cations at local scale (precipitations, pollution peak,..), at regional scale (inundation, acid rains,...), and also, at global scale (radiative forcing,...). So, a multi-scale study is necessary to understand and forecast in a good way meteorological phenomena con- cerning clouds. However, it cannot be carried with detailed microphysic model, on account of computers limitations. So, microphysical bulk schemes have to estimate the n´ large scale z properties of clouds due to smaller scale processes and charac- teristics. So, the development of such bulk scheme is rather important to go further in the knowledge of earth climate and in the forecasting of intense meteorological phenomena. Here, a quasi-spectral microphysic warm scheme has been developed to predict the concentrations and mixing ratios of aerosols, cloud droplets and raindrops. It considers, explicitely and analytically, the nucleation of droplets (Abdul-Razzak et al., 2000), condensation/evaporation (Chaumerliac et al., 1987), the breakup and collision-coalescence processes with the Long (1974) Ss kernels and the Berry and ´ Reinhardt (1974) Ss autoconversion parameterization, but also, the aerosols and gaz ´ scavenging. First, the parameterization has been estimated in the simplest dynamic framework of an air parcel model, with the results of the detailed scavenging model, DESCAM (Flossmann et al., 1985). Then, it has been tested, in the dynamic frame- work of a kinematic model (Szumowski et al., 1998) dedicated to the HaRP cam- paign (Hawaiian Rainband Project, 1990), with the observations and with the results of the two dimensional detailed microphysic scheme, DESCAM 2-D (Flossmann et al., 1988), implement in the CLARK model (Clark and Farley, 1984).

On the relationship between Arctic ice clouds and polluted air masses over the North Slope of Alaska in April 2008

NASA Astrophysics Data System (ADS)

Jouan, C.; Pelon, J.; Girard, E.; Ancellet, G.; Blanchet, J. P.; Delanoë, J.

2014-02-01

Recently, two types of ice clouds (TICs) properties have been characterized using the Indirect and Semi-Direct Aerosol Campaign (ISDAC) airborne measurements (Alaska, April 2008). TIC-2B were characterized by fewer (< 10 L-1) and larger (> 110 μm) ice crystals, and a larger ice supersaturation (> 15%) compared to TIC-1/2A. It has been hypothesized that emissions of SO2 may reduce the ice nucleating properties of ice nuclei (IN) through acidification, resulting in a smaller concentration of larger ice crystals and leading to precipitation (e.g., cloud regime TIC-2B). Here, the origin of air masses forming the ISDAC TIC-1/2A (1 April 2008) and TIC-2B (15 April 2008) is investigated using trajectory tools and satellite data. Results show that the synoptic conditions favor air masses transport from three potential SO2 emission sources into Alaska: eastern China and Siberia where anthropogenic and biomass burning emissions, respectively, are produced, and the volcanic region of the Kamchatka/Aleutians. Weather conditions allow the accumulation of pollutants from eastern China and Siberia over Alaska, most probably with the contribution of acidic volcanic aerosol during the TIC-2B period. Observation Monitoring Instrument (OMI) satellite observations reveal that SO2 concentrations in air masses forming the TIC-2B were larger than in air masses forming the TIC-1/2A. Airborne measurements show high acidity near the TIC-2B flight where humidity was low. These results support the hypothesis that acidic coating on IN could be at the origin of the formation of TIC-2B.

On the relationship between Arctic ice clouds and polluted air masses over the north slope of Alaska in April 2008

NASA Astrophysics Data System (ADS)

Jouan, C.; Pelon, J.; Girard, E.; Ancellet, G.; Blanchet, J. P.; Delanoë, J.

2013-02-01

Recently, two Types of Ice Clouds (TICs) properties have been characterized using ISDAC airborne measurements (Alaska, April 2008). TIC-2B were characterized by fewer (<10 L-1) and larger (>110 μm) ice crystals, a larger ice supersaturation (>15%) and a fewer ice nuclei (IN) concentration (<2 order of magnitude) when compared to TIC-1/2A. It has been hypothesized that emissions of SO2 may reduce the ice nucleating properties of IN through acidification, resulting to a smaller concentration of larger ice crystals and leading to precipitation (e.g. cloud regime TIC-2B) because of the reduced competition for the same available moisture. Here, the origin of air masses forming the ISDAC TIC-1/2A (1 April 2008) and TIC-2B (15 April 2008) is investigated using trajectory tools and satellite data. Results show that the synoptic conditions favor air masses transport from the three potentials SO2 emission areas to Alaska: eastern China and Siberia where anthropogenic and biomass burning emission respectively are produced and the volcanic region from the Kamchatka/Aleutians. Weather conditions allow the accumulation of pollutants from eastern China/Siberia over Alaska, most probably with the contribution of acid volcanic aerosol during the TIC-2B period. OMI observations reveal that SO2 concentrations in air masses forming the TIC-2B were larger than in air masses forming the TIC-1/2A. Airborne measurements show high acidity near the TIC-2B flight where humidity was low. These results strongly support the hypothesis that acidic coating on IN are at the origin of the formation of TIC-2B.

The clouds of Venus. II - An investigation of the influence of coagulation on the observed droplet size distribution

NASA Technical Reports Server (NTRS)

Rossow, W. B.

1977-01-01

An approximate numerical technique is used to investigate the influence of coagulation, sedimentation and turbulent motions on the observed droplet size distribution in the upper layers of the Venus clouds. If the cloud mass mixing ratio is less than 0.000001 at 250 K or the eddy diffusivity throughout the cloud is greater than 1,000,000 sq cm per sec, then coagulation is unimportant. In this case, the observed droplet size distribution is the initial size distribution produced by the condensation of the droplets. It is found that all cloud models with droplet formation near the cloud top (e.g., a photochemical model) must produce the observed droplet size distribution by condensation without subsequent modification by coagulation. However, neither meteoritic or surface dust can supply sufficient nucleating particles to account for the observed droplet number density. If the cloud droplets are formed near the cloud bottom, the observed droplet size distribution can be produced solely by the interaction of coagulation and dynamics; all information about the initial size distribution is lost. If droplet formation occurs near the cloud bottom, the lower atmosphere of Venus is oxidizing rather than reducing.

A Review of Spatial and Seasonal Changes in Condensation Clouds Observed During Aerobraking by MGS TES

NASA Technical Reports Server (NTRS)

Pearl, J. C.; Smith, M. D.; Conrath, B. J.; Bandfield, J. L.; Christensen, P. R.

1999-01-01

Successful operation of the Mars Global Surveyor spacecraft beginning in September 1997, has permitted extensive infrared observations of condensation clouds during the martian southern summer and fall seasons (184 deg

Airship measurements of aerosol size distributions, cloud droplet spectra, and trace gas concentrations in the marine boundary layers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Frick, G.M.; Hoppel, W.A.

1993-11-01

The use of an airship as a platform to conduct atmospheric chemistry, aerosol, and cloud microphysical research is described, and results from demonstration flights made off the Oregon coast are presented. The slow speed of the airship makes it an ideal platform to do high-spatial resolution profiling both vertically and horizontally, and to measure large aerosol and cloud droplet distributions without the difficulties caused by high-speed aircraft sampling. A unique set of data obtained during the demonstration flights show the effect that processing marine boundary layer aerosol through stratus clouds has on the aerosol size distribution. Evidence of new particlemore » formation (nucleation of particles) was also observed on about half the days on which flights were made. 11 refs., 9 figs., 1 tab.« less

Increased ionization supports growth of aerosols into cloud condensation nuclei.

PubMed

Svensmark, H; Enghoff, M B; Shaviv, N J; Svensmark, J

2017-12-19

Ions produced by cosmic rays have been thought to influence aerosols and clouds. In this study, the effect of ionization on the growth of aerosols into cloud condensation nuclei is investigated theoretically and experimentally. We show that the mass-flux of small ions can constitute an important addition to the growth caused by condensation of neutral molecules. Under atmospheric conditions the growth from ions can constitute several percent of the neutral growth. We performed experimental studies which quantify the effect of ions on the growth of aerosols between nucleation and sizes >20 nm and find good agreement with theory. Ion-induced condensation should be of importance not just in Earth's present day atmosphere for the growth of aerosols into cloud condensation nuclei under pristine marine conditions, but also under elevated atmospheric ionization caused by increased supernova activity.

In search of the best match: probing a multi-dimensional cloud microphysical parameter space to better understand what controls cloud thermodynamic phase

NASA Astrophysics Data System (ADS)

Tan, Ivy; Storelvmo, Trude

2015-04-01

Substantial improvements have been made to the cloud microphysical schemes used in the latest generation of global climate models (GCMs), however, an outstanding weakness of these schemes lies in the arbitrariness of their tuning parameters, which are also notoriously fraught with uncertainties. Despite the growing effort in improving the cloud microphysical schemes in GCMs, most of this effort has neglected to focus on improving the ability of GCMs to accurately simulate the present-day global distribution of thermodynamic phase partitioning in mixed-phase clouds. Liquid droplets and ice crystals not only influence the Earth's radiative budget and hence climate sensitivity via their contrasting optical properties, but also through the effects of their lifetimes in the atmosphere. The current study employs NCAR's CAM5.1, and uses observations of cloud phase obtained by NASA's CALIOP lidar over a 79-month period (November 2007 to June 2014) guide the accurate simulation of the global distribution of mixed-phase clouds in 20∘ latitudinal bands at the -10∘ C, -20∘C and -30∘C isotherms, by adjusting six relevant cloud microphysical tuning parameters in the CAM5.1 via Quasi-Monte Carlo sampling. Among the parameters include those that control the Wegener-Bergeron-Findeisen (WBF) timescale for the conversion of supercooled liquid droplets to ice and snow in mixed-phase clouds, the fraction of ice nuclei that nucleate ice in the atmosphere, ice crystal sedimentation speed, and wet scavenging in stratiform and convective clouds. Using a Generalized Linear Model as a variance-based sensitivity analysis, the relative contributions of each of the six parameters are quantified to gain a better understanding of the importance of their individual and two-way interaction effects on the liquid to ice proportion in mixed-phase clouds. Thus, the methodology implemented in the current study aims to search for the combination of cloud microphysical parameters in a GCM that produce the most accurate reproduction of observations of cloud thermodynamic phase, while simultaneously assessing the weaknesses of the parameterizations in the model. We find that the simulated proportion of liquid to ice in mixed-phase clouds is dominated by the fraction of active ice nuclei in the atmosphere and the WBF timescale. In a follow-up to this study, we apply these results to a fully-coupled GCM, CESM, and find that cloud thermodynamic phase has profound ramifications for the uncertainty associated with climate sensitivity estimates.

Global and Regional Impacts of HONO on the Chemical Composition of Clouds and Aerosols

NASA Technical Reports Server (NTRS)

Elshorbany, Y. F.; Crutzen, P. J.; Steil, B.; Pozzer, A.; Tost, H.; Lelieveld, J.

2014-01-01

Recently, realistic simulation of nitrous acid (HONO) based on the HONO / NOx ratio of 0.02 was found to have a significant impact on the global budgets of HOx (OH + HO2) and gas phase oxidation products in polluted regions, especially in winter when other photolytic sources are of minor importance. It has been reported that chemistry-transport models underestimate sulphate concentrations, mostly during winter. Here we show that simulating realistic HONO levels can significantly enhance aerosol sulphate (S(VI)) due to the increased formation of H2SO4. Even though in-cloud aqueous phase oxidation of dissolved SO2 (S(IV)) is the main source of S(VI), it appears that HONO related enhancement of H2O2 does not significantly affect sulphate because of the predominantly S(IV) limited conditions, except over eastern Asia. Nitrate is also increased via enhanced gaseous HNO3 formation and N2O5 hydrolysis on aerosol particles. Ammonium nitrate is enhanced in ammonia-rich regions but not under ammonia-limited conditions. Furthermore, particle number concentrations are also higher, accompanied by the transfer from hydrophobic to hydrophilic aerosol modes. This implies a significant impact on the particle lifetime and cloud nucleating properties. The HONO induced enhancements of all species studied are relatively strong in winter though negligible in summer. Simulating realistic HONO levels is found to improve the model measurement agreement of sulphate aerosols, most apparent over the US. Our results underscore the importance of HONO for the atmospheric oxidizing capacity and corroborate the central role of cloud chemical processing in S(IV) formation

Automation and heat transfer characterization of immersion mode spectroscopy for analysis of ice nucleating particles

NASA Astrophysics Data System (ADS)

Beall, Charlotte M.; Stokes, M. Dale; Hill, Thomas C.; DeMott, Paul J.; DeWald, Jesse T.; Prather, Kimberly A.

2017-07-01

Ice nucleating particles (INPs) influence cloud properties and can affect the overall precipitation efficiency. Developing a parameterization of INPs in global climate models has proven challenging. More INP measurements - including studies of their spatial distribution, sources and sinks, and fundamental freezing mechanisms - must be conducted in order to further improve INP parameterizations. In this paper, an immersion mode INP measurement technique is modified and automated using a software-controlled, real-time image stream designed to leverage optical changes of water droplets to detect freezing events. For the first time, heat transfer properties of the INP measurement technique are characterized using a finite-element-analysis-based heat transfer simulation to improve accuracy of INP freezing temperature measurement. The heat transfer simulation is proposed as a tool that could be used to explain the sources of bias in temperature measurements in INP measurement techniques and ultimately explain the observed discrepancies in measured INP freezing temperatures between different instruments. The simulation results show that a difference of +8.4 °C between the well base temperature and the headspace gas results in an up to 0.6 °C stratification of the aliquot, whereas a difference of +4.2 °C or less results in a thermally homogenous water volume within the error of the thermal probe, ±0.2 °C. The results also show that there is a strong temperature gradient in the immediate vicinity of the aliquot, such that without careful placement of temperature probes, or characterization of heat transfer properties of the water and cooling environment, INP measurements can be biased toward colder temperatures. Based on a modified immersion mode technique, the Automated Ice Spectrometer (AIS), measurements of the standard test dust illite NX are reported and compared against six other immersion mode droplet assay techniques featured in Hiranuma et al. (2015) that used wet suspensions. AIS measurements of illite NX INP freezing temperatures compare reasonably with others, falling within the 5 °C spread in reported spectra. The AIS as well as its characterization of heat transfer properties allows higher confidence in accuracy of freezing temperature measurement, allows higher throughput of sample analysis, and enables disentanglement of the effects of heat transfer rates on sample volumes from time dependence of ice nucleation.

Structure and wettability property of the growth and nucleation surfaces of thermally treated freestanding CVD diamond films

NASA Astrophysics Data System (ADS)

Pei, Xiaoqiang; Cheng, Shaoheng; Ma, Yibo; Wu, Danfeng; Liu, Junsong; Wang, Qiliang; Yang, Yizhou; Li, Hongdong

2015-08-01

This paper reports the surface features and wettability properties of the (1 0 0)-textured freestanding chemical vapor deposited (CVD) diamond films after thermal exposure in air at high temperature. Thermal oxidation at proper conditions eliminates selectively nanodiamonds and non-diamond carbons in the films. The growth side of the films contains (1 0 0)-oriented micrometer-sized columns, while its nucleation side is formed of nano-sized tips. The examined wettability properties of the as-treated diamond films reveal a hydrophilicity and superhydrophilicity on the growth surface and nucleation surface, respectively, which is determined by oxygen termination and geometry structure of the surface. When the surface termination is hydrogenated, the wettability of nucleation side converted from superhydrophilicity to high hydrophobicity, while the hydrophilicity of the growth side does not change significantly. The findings open a possibility for realizing freestanding diamond films having not only novel surface structures but also multifunction applications, especially proposed on the selected growth side or nucleation side in one product.

Homogeneous ice nucleation from aqueous inorganic/organic particles representative of biomass burning: water activity, freezing temperatures, nucleation rates.

PubMed

Knopf, Daniel A; Rigg, Yannick J

2011-02-10

Homogeneous ice nucleation plays an important role in the formation of cirrus clouds with subsequent effects on the global radiative budget. Here we report on homogeneous ice nucleation temperatures and corresponding nucleation rate coefficients of aqueous droplets serving as surrogates of biomass burning aerosol. Micrometer-sized (NH(4))(2)SO(4)/levoglucosan droplets with mass ratios of 10:1, 1:1, 1:5, and 1:10 and aqueous multicomponent organic droplets with and without (NH(4))(2)SO(4) under typical tropospheric temperatures and relative humidities are investigated experimentally using a droplet conditioning and ice nucleation apparatus coupled to an optical microscope with image analysis. Homogeneous freezing was determined as a function of temperature and water activity, a(w), which was set at droplet preparation conditions. The ice nucleation data indicate that minor addition of (NH(4))(2)SO(4) to the aqueous organic droplets renders the temperature dependency of water activity negligible in contrast to the case of aqueous organic solution droplets. The mean homogeneous ice nucleation rate coefficient derived from 8 different aqueous droplet compositions with average diameters of ∼60 μm for temperatures as low as 195 K and a(w) of 0.82-1 is 2.18 × 10(6) cm(-3) s(-1). The experimentally derived freezing temperatures and homogeneous ice nucleation rate coefficients are in agreement with predictions of the water activity-based homogeneous ice nucleation theory when taking predictive uncertainties into account. However, the presented ice nucleation data indicate that the water activity-based homogeneous ice nucleation theory overpredicts the freezing temperatures by up to 3 K and corresponding ice nucleation rate coefficients by up to ∼2 orders of magnitude. A shift of 0.01 in a(w), which is well within the uncertainty of typical field and laboratory relative humidity measurements, brings experimental and predicted freezing temperatures and homogeneous ice nucleation rate coefficients into agreement. The experimentally derived ice nucleation data are applied to constrain the water activity-based homogeneous ice nucleation theory to smaller than ±1 order of magnitude compared to the predictive uncertainty of larger than ±6 orders of magnitude. The atmospheric implications of these findings are discussed.

A potential regulation of jet stream behavior by changes in Arctic cirrus cloud formation mechanism and coverage

NASA Astrophysics Data System (ADS)

Mejia, J.; Mitchell, D. L.; Garnier, A.; Hosseinpour, F.; Avery, M. A.

2017-12-01

Global retrievals of cirrus cloud effective diameter De and mid-cloud temperature T were used to make the cirrus clouds simulated in CAM5 conform with the retrieved De, with the ice fall speeds in CAM5 calculated from the retrieved De. This was done by developing De-T relationships for six latitude zones. Within each latitude zone, seasonal De-T relationships were developed for cirrus over land and for cirrus over ocean (making 48 De-T relationships in total). The recently developed CALIPSO retrieval algorithm is sensitive to the ice crystal number concentration N, which is also retrieved, and it utilizes radiances from the infrared imaging radiometer and backscatter from the CALIPSO lidar. Retrieved De (N) is largest (lowest) between 30S and 30N latitude; a region dominated by anvil cirrus where pre-existing ice strongly favors heterogeneous ice nucleation (henceforth het). Therefore, the De-T relations for this region are considered representative for cirrus formed via het. Outside this region, retrieved De (N) tended to be considerably smaller (higher), presumably due to homogeneous ice nucleation (henceforth hom). Two CAM5 simulations were performed; one where cirrus cloud De is based on the CALIPSO retrievals and one where De-T for het cirrus is applied globally. Differences in net cloud radiative forcing between runs are believed due to differences in cirrus formation mechanism (hom vs. het). Such differences are typically 1.3 W m-2 in the mid-to-high latitudes in the N. Hemisphere excepting summer. These differences imply differences in cirrus cloud heating rates that affect temperatures in the underlying troposphere, which in turn affect the wind fields. The natural cirrus (mixture of hom and het) tend to trap more heat than the het cirrus. Changes in zonal wind fields between simulations suggest that heating by polar cirrus clouds have modifed meridional temperature gradients and thus zonal winds through the thermal wind balance. These changes in heating by polar cirrus clouds can modify the amplitude and meridional position of the midlatitude jet streams, which can lead to more extreme weather. Moreover, the retrievals indicate a doubling of Arctic cirrus coverage during winter, which will also result in increased heating of the underlying troposphere, likely contributing to this same phenomenon.

Climate impact of anthropogenic aerosols on cirrus clouds

NASA Astrophysics Data System (ADS)

Penner, J.; Zhou, C.

2017-12-01

Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. However, the efficacy with which particles act to form cirrus particles in a model depends on the representation of updrafts. Here, we use a representation of updrafts based on observations of gravity waves, and follow ice formation/evaporation during both updrafts and downdrafts. We examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning and from aircraft particles that have previously formed ice in contrails. Results show that fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of -0.15±0.02 Wm-2 while aircraft aerosols that have been pre-activated within contrails exert a forcing of -0.20±0.06 Wm-2, but it is possible to decrease these estimates of forcing if a larger fraction of dust particles act as heterogeneous ice nuclei. In addition aircraft aerosols may warm the climate if a large fraction of these particles act as ice nuclei. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds. This assessment could therefore support climate models with high sensitivity to greenhouse gas forcing, while still allowing the models to fit the overall historical temperature change.

Characterization of airborne ice-nucleation-active bacteria and bacterial fragments

NASA Astrophysics Data System (ADS)

Šantl-Temkiv, Tina; Sahyoun, Maher; Finster, Kai; Hartmann, Susan; Augustin-Bauditz, Stefanie; Stratmann, Frank; Wex, Heike; Clauss, Tina; Nielsen, Niels Woetmann; Sørensen, Jens Havskov; Korsholm, Ulrik Smith; Wick, Lukas Y.; Karlson, Ulrich Gosewinkel

2015-05-01

Some bacteria have the unique capacity of synthesising ice-nucleation-active (INA) proteins and exposing them at their outer membrane surface. As INA bacteria enter the atmosphere, they may impact the formation of clouds and precipitation. We studied members of airborne bacterial communities for their capacity to catalyse ice formation and we report on the excretion of INA proteins by airborne Pseudomonas sp. We also observed for the first time that INA biological fragments <220 nm were present in precipitation samples (199 and 482 INA fragments per L of precipitation), which confirms the presence of submicron INA biological fragments in the atmosphere. During 14 precipitation events, strains affiliated with the genus Pseudomonas, which are known to carry ina genes, were dominant. A screening for INA properties revealed that ∼12% of the cultivable bacteria caused ice formation at ≤-7 °C. They had likely been emitted to the atmosphere from terrestrial surfaces, e.g. by convective transport. We tested the ability of isolated INA strains to produce outer membrane vesicles and found that two isolates could do so. However, only very few INA vesicles were released per INA cell. Thus, the source of the submicron INA proteinaceous particles that we detected in the atmosphere remains to be elucidated.