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.

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.

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.

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.

Understanding the Effect of Aerosol Properties on Cloud Droplet Formation during TCAP Field Campaign Report

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

Cziczo, Daniel

2016-05-01

The formation of clouds is an essential element in understanding the Earth’s radiative budget. Liquid water clouds form when the relative humidity exceeds saturation and condensedphase water nucleates on atmospheric particulate matter. The effect of aerosol properties such as size, morphology, and composition on cloud droplet formation has been studied theoretically as well as in the laboratory and field. Almost without exception these studies have been limited to parallel measurements of aerosol properties and cloud formation or collection of material after the cloud has formed, at which point nucleation information has been lost. Studies of this sort are adequate whenmore » a large fraction of the aerosol activates, but correlations and resulting model parameterizations are much more uncertain at lower supersaturations and activated fractions.« less

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

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

Strong control of Southern Ocean cloud reflectivity by ice-nucleating particles

NASA Astrophysics Data System (ADS)

Vergara-Temprado, Jesús; Miltenberger, Annette K.; Furtado, Kalli; Grosvenor, Daniel P.; Shipway, Ben J.; Hill, Adrian A.; Wilkinson, Jonathan M.; Field, Paul R.; Murray, Benjamin J.; Carslaw, Ken S.

2018-03-01

Large biases in climate model simulations of cloud radiative properties over the Southern Ocean cause large errors in modeled sea surface temperatures, atmospheric circulation, and climate sensitivity. Here, we combine cloud-resolving model simulations with estimates of the concentration of ice-nucleating particles in this region to show that our simulated Southern Ocean clouds reflect far more radiation than predicted by global models, in agreement with satellite observations. Specifically, we show that the clouds that are most sensitive to the concentration of ice-nucleating particles are low-level mixed-phase clouds in the cold sectors of extratropical cyclones, which have previously been identified as a main contributor to the Southern Ocean radiation bias. The very low ice-nucleating particle concentrations that prevail over the Southern Ocean strongly suppress cloud droplet freezing, reduce precipitation, and enhance cloud reflectivity. The results help explain why a strong radiation bias occurs mainly in this remote region away from major sources of ice-nucleating particles. The results present a substantial challenge to climate models to be able to simulate realistic ice-nucleating particle concentrations and their effects under specific meteorological conditions.

Strong control of Southern Ocean cloud reflectivity by ice-nucleating particles

PubMed Central

Miltenberger, Annette K.; Furtado, Kalli; Grosvenor, Daniel P.; Shipway, Ben J.; Hill, Adrian A.; Wilkinson, Jonathan M.; Field, Paul R.

2018-01-01

Large biases in climate model simulations of cloud radiative properties over the Southern Ocean cause large errors in modeled sea surface temperatures, atmospheric circulation, and climate sensitivity. Here, we combine cloud-resolving model simulations with estimates of the concentration of ice-nucleating particles in this region to show that our simulated Southern Ocean clouds reflect far more radiation than predicted by global models, in agreement with satellite observations. Specifically, we show that the clouds that are most sensitive to the concentration of ice-nucleating particles are low-level mixed-phase clouds in the cold sectors of extratropical cyclones, which have previously been identified as a main contributor to the Southern Ocean radiation bias. The very low ice-nucleating particle concentrations that prevail over the Southern Ocean strongly suppress cloud droplet freezing, reduce precipitation, and enhance cloud reflectivity. The results help explain why a strong radiation bias occurs mainly in this remote region away from major sources of ice-nucleating particles. The results present a substantial challenge to climate models to be able to simulate realistic ice-nucleating particle concentrations and their effects under specific meteorological conditions. PMID:29490918

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.

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.

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.

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.

Strong control of Southern Ocean cloud reflectivity by ice-nucleating particles.

PubMed

Vergara-Temprado, Jesús; Miltenberger, Annette K; Furtado, Kalli; Grosvenor, Daniel P; Shipway, Ben J; Hill, Adrian A; Wilkinson, Jonathan M; Field, Paul R; Murray, Benjamin J; Carslaw, Ken S

2018-03-13

Large biases in climate model simulations of cloud radiative properties over the Southern Ocean cause large errors in modeled sea surface temperatures, atmospheric circulation, and climate sensitivity. Here, we combine cloud-resolving model simulations with estimates of the concentration of ice-nucleating particles in this region to show that our simulated Southern Ocean clouds reflect far more radiation than predicted by global models, in agreement with satellite observations. Specifically, we show that the clouds that are most sensitive to the concentration of ice-nucleating particles are low-level mixed-phase clouds in the cold sectors of extratropical cyclones, which have previously been identified as a main contributor to the Southern Ocean radiation bias. The very low ice-nucleating particle concentrations that prevail over the Southern Ocean strongly suppress cloud droplet freezing, reduce precipitation, and enhance cloud reflectivity. The results help explain why a strong radiation bias occurs mainly in this remote region away from major sources of ice-nucleating particles. The results present a substantial challenge to climate models to be able to simulate realistic ice-nucleating particle concentrations and their effects under specific meteorological conditions. Copyright © 2018 the Author(s). Published by PNAS.

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.

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.

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.

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.

Skylab near-infrared observations of clouds indicating supercooled liquid water droplets

NASA Technical Reports Server (NTRS)

Curran, R. J.; Wu, M.-L. C.

1982-01-01

Orographically-induced lee-wave clouds were observed over New Mexico by a multichannel scanning radiometer on Skylab during December 1973. Channels centered at 0.83, 1.61 and 2.125 microns were used to determine the cloud optical thickness, thermodynamic phase and effective particle size. An additional channel centered at 11.4 microns was used to determine cloud-top temperature, which was corroborated through comparison with the stereographically determined cloud top altitudes and conventional temperature soundings. Analysis of the measured near-infrared reflection functions at 1.61 and 2.125 microns are most easily interpreted as indicating the presence of liquid-phase water droplets. This interpretation is not conclusive even after considerable effort to understand possible sources for misinterpretation. However, if accepted the resulting phase determination is considered anomalous due to the inferred cloud-top temperatures being in the -32 to -47 C range. Theory for the homogeneous nucleation of pure supercooled liquid water droplets predicts very short lifetimes for the liquid phase at these cold temperatures. A possible explanation for the observations is that the wave-clouds are composed of solution droplets. Impurities in the cloud droplets could decrease the homogeneous freezing rate for these droplets, permitting them to exist for a longer time in the liquid phase, at the cold temperatures found.

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.

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.

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.

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.

Effect of Heterogeneous Chemical Reactions on the Köhler Activation of Aqueous Organic Aerosols.

PubMed

Djikaev, Yuri S; Ruckenstein, Eli

2018-05-03

We study some thermodynamic aspects of the activation of aqueous organic aerosols into cloud droplets considering the aerosols to consist of liquid solution of water and hydrophilic and hydrophobic organic compounds, taking into account the presence of reactive species in the air. The hydrophobic (surfactant) organic molecules on the surface of such an aerosol can be processed by chemical reactions with some atmospheric species; this affects the hygroscopicity of the aerosol and hence its ability to become a cloud droplet either via nucleation or via Köhler activation. The most probable pathway of such processing involves atmospheric hydroxyl radicals that abstract hydrogen atoms from hydrophobic organic molecules located on the aerosol surface (first step), the resulting radicals being quickly oxidized by ubiquitous atmospheric oxygen molecules to produce surface-bound peroxyl radicals (second step). These two reactions play a crucial role in the enhancement of the Köhler activation of the aerosol and its evolution into a cloud droplet. Taking them and a third reaction (next in the multistep chain of relevant heterogeneous reactions) into account, one can derive an explicit expression for the free energy of formation of a four-component aqueous droplet on a ternary aqueous organic aerosol as a function of four independent variables of state of a droplet. The results of numerical calculations suggest that the formation of cloud droplets on such (aqueous hydrophilic/hydrophobic organic) aerosols is most likely to occur as a Köhler activation-like process rather than via nucleation. The model allows one to determine the threshold parameters of the system necessary for the Köhler activation of such aerosols, which are predicted to be very sensitive to the equilibrium constant of the chain of three heterogeneous reactions involved in the chemical aging of aerosols.

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.

Free energy of formation of a crystal nucleus in incongruent solidification: Implication for modeling the crystallization of aqueous nitric acid droplets in polar stratospheric clouds

NASA Astrophysics Data System (ADS)

Djikaev, Yuri S.; Ruckenstein, Eli

2017-04-01

Using the formalism of classical thermodynamics in the framework of the classical nucleation theory, we derive an expression for the reversible work W* of formation of a binary crystal nucleus in a liquid binary solution of non-stoichiometric composition (incongruent crystallization). Applied to the crystallization of aqueous nitric acid droplets, the new expression more adequately takes account of the effects of nitric acid vapor compared to the conventional expression of MacKenzie, Kulmala, Laaksonen, and Vesala (MKLV) [J. Geophys. Res.: Atmos. 102, 19729 (1997)]. The predictions of both MKLV and modified expressions for the average liquid-solid interfacial tension σls of nitric acid dihydrate (NAD) crystals are compared by using existing experimental data on the incongruent crystallization of aqueous nitric acid droplets of composition relevant to polar stratospheric clouds (PSCs). The predictions for σls based on the MKLV expression are higher by about 5% compared to predictions based on our modified expression. This results in similar differences between the predictions of both expressions for the solid-vapor interfacial tension σsv of NAD crystal nuclei. The latter can be obtained by using the method based on the analysis of experimental data on crystal nucleation rates in aqueous nitric acid droplets; it exploits the dominance of the surface-stimulated mode of crystal nucleation in small droplets and its negligibility in large ones. Applying that method to existing experimental data, our expression for the free energy of formation provides an estimate for σsv of NAD in the range ≈92 dyn/cm to ≈100 dyn/cm, while the MKLV expression predicts it in the range ≈95 dyn/cm to ≈105 dyn/cm. The predictions of both expressions for W* become identical for the case of congruent crystallization; this was also demonstrated by applying our method for determining σsv to the nucleation of nitric acid trihydrate crystals in PSC droplets of stoichiometric composition.

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

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.

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.

Contrasting cloud composition between coupled and decoupled marine boundary layer clouds

NASA Astrophysics Data System (ADS)

Wang, Zhen; Mora Ramirez, Marco; Dadashazar, Hossein; MacDonald, Alex B.; Crosbie, Ewan; Bates, Kelvin H.; Coggon, Matthew M.; Craven, Jill S.; Lynch, Peng; Campbell, James R.; Azadi Aghdam, Mojtaba; Woods, Roy K.; Jonsson, Haflidi; Flagan, Richard C.; Seinfeld, John H.; Sorooshian, Armin

2016-10-01

Marine stratocumulus clouds often become decoupled from the vertical layer immediately above the ocean surface. This study contrasts cloud chemical composition between coupled and decoupled marine stratocumulus clouds for dissolved nonwater substances. Cloud water and droplet residual particle composition were measured in clouds off the California coast during three airborne experiments in July-August of separate years (Eastern Pacific Emitted Aerosol Cloud Experiment 2011, Nucleation in California Experiment 2013, and Biological and Oceanic Atmospheric Study 2015). Decoupled clouds exhibited significantly lower air-equivalent mass concentrations in both cloud water and droplet residual particles, consistent with reduced cloud droplet number concentration and subcloud aerosol (Dp > 100 nm) number concentration, owing to detachment from surface sources. Nonrefractory submicrometer aerosol measurements show that coupled clouds exhibit higher sulfate mass fractions in droplet residual particles, owing to more abundant precursor emissions from the ocean and ships. Consequently, decoupled clouds exhibited higher mass fractions of organics, nitrate, and ammonium in droplet residual particles, owing to effects of long-range transport from more distant sources. Sodium and chloride dominated in terms of air-equivalent concentration in cloud water for coupled clouds, and their mass fractions and concentrations exceeded those in decoupled clouds. Conversely, with the exception of sea-salt constituents (e.g., Cl, Na, Mg, and K), cloud water mass fractions of all species examined were higher in decoupled clouds relative to coupled clouds. Satellite and Navy Aerosol Analysis and Prediction System-based reanalysis data are compared with each other, and the airborne data to conclude that limitations in resolving boundary layer processes in a global model prevent it from accurately quantifying observed differences between coupled and decoupled cloud composition.

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.

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

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.

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.

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.

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.

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 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.

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.

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.

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.

Immersion freezing of ice nucleation active protein complexes

NASA Astrophysics Data System (ADS)

Hartmann, S.; Augustin, S.; Clauss, T.; Wex, H.; Šantl-Temkiv, T.; Voigtländer, J.; Niedermeier, D.; Stratmann, F.

2013-06-01

Utilising the Leipzig Aerosol Cloud Interaction Simulator (LACIS), the immersion freezing behaviour of droplet ensembles containing monodisperse particles, generated from a Snomax™ solution/suspension, was investigated. Thereto ice fractions were measured in the temperature range between -5 °C to -38 °C. Snomax™ is an industrial product applied for artificial snow production and contains Pseudomonas syringae} bacteria which have long been used as model organism for atmospheric relevant ice nucleation active (INA) bacteria. The ice nucleation activity of such bacteria is controlled by INA protein complexes in their outer membrane. In our experiments, ice fractions increased steeply in the temperature range from about -6 °C to about -10 °C and then levelled off at ice fractions smaller than one. The plateau implies that not all examined droplets contained an INA protein complex. Assuming the INA protein complexes to be Poisson distributed over the investigated droplet populations, we developed the CHESS model (stoCHastic modEl of similar and poiSSon distributed ice nuclei) which allows for the calculation of ice fractions as function of temperature and time for a given nucleation rate. Matching calculated and measured ice fractions, we determined and parameterised the nucleation rate of INA protein complexes exhibiting class III ice nucleation behaviour. Utilising the CHESS model, together with the determined nucleation rate, we compared predictions from the model to experimental data from the literature and found good agreement. We found that (a) the heterogeneous ice nucleation rate expression quantifying the ice nucleation behaviour of the INA protein complex is capable of describing the ice nucleation behaviour observed in various experiments for both, Snomax™ and P. syringae bacteria, (b) the ice nucleation rate, and its temperature dependence, seem to be very similar regardless of whether the INA protein complexes inducing ice nucleation are attached to the outer membrane of intact bacteria or membrane fragments, (c) the temperature range in which heterogeneous droplet freezing occurs, and the fraction of droplets being able to freeze, both depend on the actual number of INA protein complexes present in the droplet ensemble, and (d) possible artifacts suspected to occur in connection with the drop freezing method, i.e., the method frequently used by biologist for quantifying ice nucleation behaviour, are of minor importance, at least for substances such as P. syringae, which induce freezing at comparably high temperatures. The last statement implies that for single ice nucleation entities such as INA protein complexes, it is the number of entities present in the droplet population, and the entities' nucleation rate, which control the freezing behaviour of the droplet population. Quantities such as ice active surface site density are not suitable in this context. The results obtained in this study allow a different perspective on the quantification of the immersion freezing behaviour of bacterial ice nucleation.

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 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.

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

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.

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.

Cloud Processed CCN Suppress Stratus Cloud Drizzle

NASA Astrophysics Data System (ADS)

Hudson, J. G.; Noble, S. R., Jr.

2017-12-01

Conversion of sulfur dioxide to sulfate within cloud droplets increases the sizes and decreases the critical supersaturation, Sc, of cloud residual particles that had nucleated the droplets. Since other particles remain at the same sizes and Sc a size and Sc gap is often observed. Hudson et al. (2015) showed higher cloud droplet concentrations (Nc) in stratus clouds associated with bimodal high-resolution CCN spectra from the DRI CCN spectrometer compared to clouds associated with unimodal CCN spectra (not cloud processed). Here we show that CCN spectral shape (bimodal or unimodal) affects all aspects of stratus cloud microphysics and drizzle. Panel A shows mean differential cloud droplet spectra that have been divided according to traditional slopes, k, of the 131 measured CCN spectra in the Marine Stratus/Stratocumulus Experiment (MASE) off the Central California coast. K is generally high within the supersaturation, S, range of stratus clouds (< 0.5%). Because cloud processing decreases Sc of some particles, it reduces k. Panel A shows higher concentrations of small cloud droplets apparently grown on lower k CCN than clouds grown on higher k CCN. At small droplet sizes the concentrations follow the k order of the legend, black, red, green, blue (lowest to highest k). Above 13 µm diameter the lines cross and the hierarchy reverses so that blue (highest k) has the highest concentrations followed by green, red and black (lowest k). This reversed hierarchy continues into the drizzle size range (panel B) where the most drizzle drops, Nd, are in clouds grown on the least cloud-processed CCN (blue), while clouds grown on the most processed CCN (black) have the lowest Nd. Suppression of stratus cloud drizzle by cloud processing is an additional 2nd indirect aerosol effect (IAE) that along with the enhancement of 1st IAE by higher Nc (panel A) are above and beyond original IAE. However, further similar analysis is needed in other cloud regimes to determine if MASE was typical. Hudson, J.G., S. Noble, and S. Tabor, 2015: J. Geophys. Res., Atmos., 120, 3436-3452, doi:10.1002/2014JD022669.

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.

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.

Influence of Solar Wind on the Global Electric Circuit, and Inferred Effects on Cloud Microphysics, Temperature, and Dynamics in the Troposphere

NASA Astrophysics Data System (ADS)

Tinsley, Brian A.

2000-11-01

There are at least three independent ways in which the solar wind modulates the flow of current density (Jz) in the global electric circuit. These are (A) changes in the galactic cosmic ray energy spectrum, (B) changes in the precipitation of relativistic electrons from the magnetosphere, and (C) changes in the ionospheric potential distribution in the polar caps due to magnetosphere-ionosphere coupling. The current density J_z flows between the ionosphere and the surface, and as it passes through conductivity gradients it generates space charge concentrations dependent on J_z and the conductivity gradient. The gradients are large at the surfaces of clouds and space charge concentrations of order 1000 to 10,000 elementary charges per cm^3 can be generated at cloud tops. The charge transfers to droplets, many of which are evaporating at the cloud-clear air interface. The charge remains on the residual evaporation nuclei with a lifetime against leakage of order 1000 sec, and for a longer period the nuclei also retain coatings of sulfate and organic compounds adsorbed by the droplet while in the cloud. The charged evaporation nuclei become well mixed with more droplets in many types of clouds with penetrative mixing. The processes of entrainment and evaporation are also efficient for these clouds. The collection of such nuclei by nearby droplets is greatly increased by the electrical attraction between the charge on the particle and the image charge that it creates on the droplet. This process is called electroscavenging. Because the charge on the evaporation nuclei is derived from the original space charge, it depends on J_z, giving a rate of electroscavenging responsive to the solar wind inputs. There may be a number of ways in which the electroscavenging has consequences for weather and climate. One possibility is enhanced production of ice. The charged evaporation nuclei have been found to be good ice forming nuclei because of their coatings, and so in supercooled clouds droplet freezing can occur by contact ice nucleation, as the evaporation nuclei are electroscavenged. Although quantitative models for the all the cloud microphysical processes that may be involved have not yet been produced, we show that for many clouds, especially those with broad droplet size distributions, relatively high droplet concentrations, and cloud top temperatures just below freezing, this process is likely to dominate over other primary ice nucleation processes. In these cases there are likely to be effects on cloud albedo and rates of sedimentation of ice, and these will depend on J_z. For an increase in ice production in thin clouds such as altocumulus or stratocumulus the main effect is a decrease in albedo to incoming solar radiation, and in opacity to outgoing longwave radiation. At low latitudes the surface and troposphere heat, and at high latitudes in winter they cool. The change in meridional temperature gradient affects the rate of cyclogenesis, and the amplitude of planetary waves. For storm clouds, as in winter cyclones, the effect of increased ice formation is mainly to increase the rate of glaciation of lower level clouds by the seeder-feeder process. The increase in precipitation efficiency increases the rate of transfer of latent heat between the air mass and the surface. In most cyclones this is likely to result in intensification, producing changes in the vorticity area index as observed. Cyclone intensification also increases the amplitude of planetary waves, and shifts storm tracks, as observed. In this paper we first describe the production of space charge and the way in which it may influence the rate of ice nucleation. Then we review theory and observations of the solar wind modulation of J_z, and the correlated changes in atmospheric temperature and dynamics in the troposphere. The correlations are present for each input, (A, B, and C), and the detailed patterns of responses provide support for the inferred electrical effects on the physics of clouds, affecting precipitation, temperature and dynamics.

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.

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.

Intercomparison between Individual Particles Scavenged as CCN and Those Collected at Ground-based Site on West Coast of Japan During Asian Dust Storm

NASA Astrophysics Data System (ADS)

Ma, C. J.; Tohno, S.; Kasahara, M.; Hayakawa, S.

2002-12-01

Asian dust storm particles can affect precipitation composition because they are either incorporated into cloud via condensation of water vapour (nucleation) or due to the uptake of particles by existing droplets. And subsequently they affect aquatic and terrestrial ecosystems. In order to study the intercorrelation between the chemical natures of both the particles collected at ground-based site and those scavenged as CCN, the intensive field measurement was carried out on west coast of Japan (Yasaka, Tango Peninsula, 35.62°N; 135.07°E) during dense Asian dust storm event on March 22, 2002. Due to the size dependence of the chemical composition of aerosol particle, size-segregated aerosol particles were collect using Low pressure Andersen impactor sampler. Also, to collect cloud droplets individually, a particular method for the cloud droplet replication was newly applied using collodion (nitrocellulose) film. Sampling of cloud droplets was performed at summit of a mountain (680 m) in Yasaka. To analyze the ambient individual aerosol particles and individual retained particles in cloud droplet, X-ray fluorescence (XRF) analytical method set at SPring-8 on BL39XU was applied. Analytical result enables us not only to compare the characteristics of individual particles scavenged as CCN and those collected at ground-based site, but also to estimate the influence of long-range transport.

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).

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.

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

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

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.

Cloud microphysics and aerosol indirect effects in the global climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Lohmann, U.; Stier, P.; Hoose, C.; Ferrachat, S.; Kloster, S.; Roeckner, E.; Zhang, J.

2007-07-01

The double-moment cloud microphysics scheme from ECHAM4 that predicts both the mass mixing ratios and number concentrations of cloud droplets and ice crystals has been coupled to the size-resolved aerosol scheme ECHAM5-HAM. ECHAM5-HAM predicts the aerosol mass, number concentrations and mixing state. The simulated liquid, ice and total water content and the cloud droplet and ice crystal number concentrations as a function of temperature in stratiform mixed-phase clouds between 0 and -35° C agree much better with aircraft observations in the ECHAM5 simulations. ECHAM5 performs better because more realistic aerosol concentrations are available for cloud droplet nucleation and because the Bergeron-Findeisen process is parameterized as being more efficient. The total anthropogenic aerosol effect includes the direct, semi-direct and indirect effects and is defined as the difference in the top-of-the-atmosphere net radiation between present-day and pre-industrial times. It amounts to -1.9 W m-2 in ECHAM5, when a relative humidity dependent cloud cover scheme and aerosol emissions representative for the years 1750 and 2000 from the AeroCom emission inventory are used. The contribution of the cloud albedo effect amounts to -0.7 W m-2. The total anthropogenic aerosol effect is larger when either a statistical cloud cover scheme or a different aerosol emission inventory are employed because the cloud lifetime effect increases.

A laboratory study of the nucleation kinetics of nitric acid hydrates under stratospheric conditions

NASA Astrophysics Data System (ADS)

James, Alexander D.; Murray, Benjamin J.; Plane, John M. C.

2016-04-01

Measurements of the kinetics of crystallisation of ternary H2O-H2SO4-HNO3 mixtures to produce nitric acid hydrate phases, as occurs in the lower stratosphere, have been a long-standing challenge for investigators in the laboratory. Understanding polar stratospheric chlorine chemistry and thereby ozone depletion is increasingly limited by descriptions of nucleation processes. Meteoric smoke particles have been considered in the past as heterogeneous nuclei, however recent studies suggest that these particles will largely dissolve, leaving mainly silica and alumina as solid inclusions. In this study the nucleation kinetics of nitric acid hydrate phases have been measured in microliter droplets at polar stratospheric cloud (PSC) temperatures, using a droplet freezing assay. A clear heterogeneous effect was observed when silica particles were added. A parameterisation based on the number of droplets activated per nuclei surface area (ns) has been developed and compared to global model data. Nucleation experiments on identical droplets have been performed in an X-Ray Diffractometer (XRD) to determine the nature of the phase which formed. β-Nitric Acid Trihydrate (NAT) was observed alongside a mixture of Nitric Acid Dihydrate (NAD) phases. It is not possible to determine whether NAT nucleates directly or is formed by a phase transition from NAD (likely requiring the presence of a mediating liquid phase). Regardless, these results demonstrate the possibility of forming NAT on laboratory timescales. In the polar stratosphere, sulfuric acid (present at several weight percent of the liquid under equilibrium conditions) could provide such a liquid phase. This study therefor provides insight into previous discrepancies between phases formed in the laboratory and those observed in the atmosphere. It also provides a basis for future studies into atmospheric nucleation of solid PSCs.

Microphysical modeling of cirrus. 2: Sensitivity studies

NASA Technical Reports Server (NTRS)

Jensen, Eric J.; Toon, Owen B.; Westphal, Douglas L.; Kinne, Stefan; Heymsfield, Andrew J.

1994-01-01

The one-dimensional cirrus model described in part 1 of this issue has been used to study the sensitivity of simulated cirrus microphysical and radiative properties to poorly known model parameters, poorly understood physical processes, and environmental conditions. Model parameters and physical processes investigated include nucleation rate, mode of nucleation (e.g., homogeneous freezing of aerosols and liquid droplets or heterogeneous deposition), ice crystal shape, and coagulation. These studies suggest that the leading sources of uncertainty in the model are the phase change (liquid-solid) energy barrier and the ice-water surface energy which dominate the homogeneous freezing nucleation rate and the coagulation sticking efficiency at low temperatures which controls the production of large ice crystals (radii greater than 100 mcirons). Environmental conditions considered in sensitivity tests were CN size distribution, vertical wind speed, and cloud height. We found that (unlike stratus clouds) variations in the total number of condensation nuclei (NC) have little effect on cirrus microphysical and radiative properties, since nucleation occurs only on the largest CN at the tail of the size distribution. The total number of ice crystals which nucleate has little or no relationship to the number of CN present and depends primarily on the temperature and the cooling rate. Stronger updrafts (more rapid cooling) generate higher ice number densities, ice water content, cloud optical depth, and net radiative forcing. Increasing the height of the clouds in the model leads to an increase in ice number density, a decrease in effective radius, and a decrease in ice water content. The most prominent effect of increasing cloud height was a rapid increase in the net cloud radiative forcing which can be attributed to the change in cloud temperature as well as change in cloud ice size distributions. It has long been recognized that changes in cloud height or cloud area have the greatest potential for causing feedbacks on climate change. Our results suggest that variations in vertical velocity or cloud microphysical changes associatd with cloud height changes may also be important.

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.

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.

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

Fan, Jiwen; Rosenfeld, Daniel; Zhang, Yuwei

Aerosol-cloud interaction remains the largest uncertainty in climate projections. Ultrafine aerosol particles (UAP; size <50nm) are considered too small to serve as cloud condensation nuclei conventionally. However, this study provides observational evidence to accompany insights from numerical simulations to support that deep convective clouds (DCCs) over Amazon have strong capability of nucleating UAP from an urban source and forming greater numbers of droplets, because fast drop coalescence in these DCCs reduces drop surface area available for condensation, leading to high vapor supersaturation. The additional droplets subsequently decrease supersaturation and release more condensational latent heating, a dominant contributor to convection intensification,more » whereas enhanced latent heat from ice-related processes plays a secondary role. Therefore, the addition of anthropogenic UAP may play a much greater role in modulating clouds than previously believed over the Amazon region and possibly in other relatively pristine regions such as maritime and forest locations.« less

Heterogeneous freezing of super cooled water droplets in micrometre range- freezing on a chip

NASA Astrophysics Data System (ADS)

Häusler, Thomas; Witek, Lorenz; Felgitsch, Laura; Hitzenberger, Regina; Grothe, Hinrich

2017-04-01

A new setup to analyse the freezing behaviour of ice nucleation particles (INPs) dispersed in aqueous droplets has been developed with the aim to analyse ensembles of droplets with sizes in the micrometre range, in which INPs are immersed. Major disadvantages of conventional drop-freezing experiments like varying drop sizes or interactions between the water- oil mixture and the INP, were solved by introducing a unique freezing- chip consisting of an etched and sputtered 15x15x1 mm gold-plated silicon or pure gold film (Pummer et al., 2012; Zolles et al., 2015). Using this chip, isolated micrometre-sized droplets can be generated with sizes similar to droplets in real world clouds. The experimental set-up for drop-freezing experiments was revised and improved by establishing automated process control and image evaluation. We were able to show the efficiency and accuracy of our setup by comparing measured freezing temperatures of different INPs (Snomax®, K- feldspar, birch pollen (Betula pendula) washing water, juniper pollen suspension (Juniperus communis) and ultrapure water) with already published results (Atkinson et al., 2013; Augustin et al., 2013; Pruppacher and Klett, 1997; Pummer et al., 2012; Wex et al., 2015; Zolles et al., 2015). Comparison of our measurements with literature data show the important impact of droplet size, INP concentration and number of active sites on the T50 values. Here, the new set-up exhibits its strength in reproducibility and accuracy which is due to the defined and isolated droplets. Finally, it opens a temperature window down to -37˚ C for freezing experiments which was not accessible with former traditional approaches .Atkinson, J. D., Murray, B. J., Woodhouse, M. T., Whale, T. F., Baustian, K. J., Carslaw, K. S., Dobbie, S., O'Sullivan, D., and Malkin, T. L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds (vol 498, pg 355, 2013), Nature, 500, 491-491, 2013. Augustin, S., Wex, H., Niedermeier, D., Pummer, B., Grothe, H., Hartmann, S., Tomsche, L., Clauss, T., Voigtlander, J., Ignatius, K., and Stratmann, F.: Immersion freezing of birch pollen washing water, Atmos Chem Phys, 13, 10989-11003, 2013. Pruppacher, H. R. and Klett, J. D.: Microphysics of Clouds and Precipitation, Kluwer Academic Publishers, Dordrecht, 1997. 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. Wex, H., Augustin-Bauditz, S., Boose, Y., Budke, C., Curtius, J., Diehl, K., Dreyer, A., Frank, F., Hartmann, S., Hiranuma, N., Jantsch, E., Kanji, Z. A., Kiselev, A., Koop, T., Mohler, O., Niedermeier, D., Nillius, B., Rosch, M., Rose, D., Schmidt, C., Steinke, I., and Stratmann, F.: Intercomparing different devices for the investigation of ice nucleating particles using Snomax (R) as test substance, Atmos Chem Phys, 15, 1463-1485, 2015. Zolles, T., Burkart, J., Hausler, T., Pummer, B., Hitzenberger, R., and Grothe, H.: Identification of Ice Nucleation Active Sites on Feldspar Dust Particles, Journal of Physical Chemistry A, 119, 2692-2700, 2015.

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.

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.

Redistribution of ice nuclei between cloud and rain droplets: Parameterization and application to deep convective clouds: ICE NUCLEI IN RAIN DROPLETS

DOE PAGES

Paukert, M.; Hoose, C.; Simmel, M.

2017-02-21

In model studies of aerosol-dependent immersion freezing in clouds, a common assumption is that each ice nucleating aerosol particle corresponds to exactly one cloud droplet. Conversely, the immersion freezing of larger drops—“rain”—is usually represented by a liquid volume-dependent approach, making the parameterizations of rain freezing independent of specific aerosol types and concentrations. This may lead to inconsistencies when aerosol effects on clouds and precipitation shall be investigated, since raindrops consist of the cloud droplets—and corresponding aerosol particles—that have been involved in drop-drop-collisions. We introduce an extension to a two-moment microphysical scheme in order to account explicitly for particle accumulation inmore » raindrops by tracking the rates of selfcollection, autoconversion, and accretion. This also provides a direct link between ice nuclei and the primary formation of large precipitating ice particles. A new parameterization scheme of drop freezing is presented to consider multiple ice nuclei within one drop and effective drop cooling rates. In our test cases of deep convective clouds, we find that at altitudes which are most relevant for immersion freezing, the majority of potential ice nuclei have been converted from cloud droplets into raindrops. Compared to the standard treatment of freezing in our model, the less efficient mineral dust-based freezing results in higher rainwater contents in the convective core, affecting both rain and hail precipitation. The aerosol-dependent treatment of rain freezing can reverse the signs of simulated precipitation sensitivities to ice nuclei perturbations.« less

Redistribution of ice nuclei between cloud and rain droplets: Parameterization and application to deep convective clouds: ICE NUCLEI IN RAIN DROPLETS

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

Paukert, M.; Hoose, C.; Simmel, M.

In model studies of aerosol-dependent immersion freezing in clouds, a common assumption is that each ice nucleating aerosol particle corresponds to exactly one cloud droplet. Conversely, the immersion freezing of larger drops—“rain”—is usually represented by a liquid volume-dependent approach, making the parameterizations of rain freezing independent of specific aerosol types and concentrations. This may lead to inconsistencies when aerosol effects on clouds and precipitation shall be investigated, since raindrops consist of the cloud droplets—and corresponding aerosol particles—that have been involved in drop-drop-collisions. We introduce an extension to a two-moment microphysical scheme in order to account explicitly for particle accumulation inmore » raindrops by tracking the rates of selfcollection, autoconversion, and accretion. This also provides a direct link between ice nuclei and the primary formation of large precipitating ice particles. A new parameterization scheme of drop freezing is presented to consider multiple ice nuclei within one drop and effective drop cooling rates. In our test cases of deep convective clouds, we find that at altitudes which are most relevant for immersion freezing, the majority of potential ice nuclei have been converted from cloud droplets into raindrops. Compared to the standard treatment of freezing in our model, the less efficient mineral dust-based freezing results in higher rainwater contents in the convective core, affecting both rain and hail precipitation. The aerosol-dependent treatment of rain freezing can reverse the signs of simulated precipitation sensitivities to ice nuclei perturbations.« less

Aerosol processing in stratiform clouds in ECHAM6-HAM

NASA Astrophysics Data System (ADS)

Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

2013-04-01

Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the chemical components as well as 5 tracers for aerosol particles in ice crystals. This allows simulations of aerosol processing in warm, mixed-phase (e.g. through the Bergeron-Findeisen process) and ice clouds. The fixed scavenging ratios used for wet deposition in clouds in standard HAM are replaced by an explicit treatment of collision of cloud droplets/ice crystals with interstitial aerosol particles. Nucleation scavenging of aerosol particles by acting as cloud condensation nuclei or ice nuclei, freezing and evaporation of cloud droplets and melting and sublimation of ice crystals are treated explicitly. In extension to previous studies, aerosol particles from evaporating precipitation are released to modes which correspond to their size. Cloud processing of aerosol particles changes their size distribution and hence influences cloud droplet and ice crystal number concentrations as well as precipitation rate, which in turn affects aerosol concentrations. Results will be presented at the conference. Hoose et al., JGR, 2008a, doi: 10.1029/2007JD009251 Hoose et al., ACP, 2008b, doi: 10.5194/acp-8-6939-2008 Stevens et al., 2013, submitted Stier et al., ACP, 2005, doi: 10.5194/acp-5-1125-2005

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

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.

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.

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

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.

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

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

Immersion freezing of internally and externally mixed mineral dust species analyzed by stochastic and deterministic models

NASA Astrophysics Data System (ADS)

Wong, B.; Kilthau, W.; Knopf, D. A.

2017-12-01

Immersion freezing is recognized as the most important ice crystal formation process in mixed-phase cloud environments. It is well established that mineral dust species can act as efficient ice nucleating particles. Previous research has focused on determination of the ice nucleation propensity of individual mineral dust species. In this study, the focus is placed on how different mineral dust species such as illite, kaolinite and feldspar, initiate freezing of water droplets when present in internal and external mixtures. The frozen fraction data for single and multicomponent mineral dust droplet mixtures are recorded under identical cooling rates. Additionally, the time dependence of freezing is explored. Externally and internally mixed mineral dust droplet samples are exposed to constant temperatures (isothermal freezing experiments) and frozen fraction data is recorded based on time intervals. Analyses of single and multicomponent mineral dust droplet samples include different stochastic and deterministic models such as the derivation of the heterogeneous ice nucleation rate coefficient (J­­het), the single contact angle (α) description, the α-PDF model, active sites representation, and the deterministic model. Parameter sets derived from freezing data of single component mineral dust samples are evaluated for prediction of cooling rate dependent and isothermal freezing of multicomponent externally or internally mixed mineral dust samples. The atmospheric implications of our findings are discussed.

Redistribution of ice nuclei between cloud and rain droplets: Parameterization and application to deep convective clouds

NASA Astrophysics Data System (ADS)

Paukert, M.; Hoose, C.; Simmel, M.

2017-03-01

In model studies of aerosol-dependent immersion freezing in clouds, a common assumption is that each ice nucleating aerosol particle corresponds to exactly one cloud droplet. In contrast, the immersion freezing of larger drops—"rain"—is usually represented by a liquid volume-dependent approach, making the parameterizations of rain freezing independent of specific aerosol types and concentrations. This may lead to inconsistencies when aerosol effects on clouds and precipitation shall be investigated, since raindrops consist of the cloud droplets—and corresponding aerosol particles—that have been involved in drop-drop-collisions. Here we introduce an extension to a two-moment microphysical scheme in order to account explicitly for particle accumulation in raindrops by tracking the rates of selfcollection, autoconversion, and accretion. This provides a direct link between ice nuclei and the primary formation of large precipitating ice particles. A new parameterization scheme of drop freezing is presented to consider multiple ice nuclei within one drop and effective drop cooling rates. In our test cases of deep convective clouds, we find that at altitudes which are most relevant for immersion freezing, the majority of potential ice nuclei have been converted from cloud droplets into raindrops. Compared to the standard treatment of freezing in our model, the less efficient mineral dust-based freezing results in higher rainwater contents in the convective core, affecting both rain and hail precipitation. The aerosol-dependent treatment of rain freezing can reverse the signs of simulated precipitation sensitivities to ice nuclei perturbations.

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.

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

Investigating the heterogeneous freezing behavior of supercooled droplets containing different amounts of SNOMAX

NASA Astrophysics Data System (ADS)

Niedermeier, D.; Budke, C.; Koop, T.; Hartmann, S.; Augustin, S.; Stratmann, F.; Wex, H.

2013-12-01

Heterogeneous ice nucleation, a fundamental process for ice formation in the atmosphere, has been observed to occur in clouds at temperatures higher than -20 °C (Kanitz et al., 2011). However, laboratory studies showed that mineral dust particles, which are the most abundant atmospheric ice nuclei (IN), are ice active at lower temperature (Murray et al., 2012). Biological particles such as bacteria nucleate ice at higher temperatures similar to those observed in the atmosphere. But their atmospheric relevance is controversially discussed (Hartmann et al., 2013; Hoose et al., 2010). In order to achieve a better understanding, fundamental processes underlying ice nucleation on bacteria should be investigated. Within the Ice Nuclei research UnIT (INUIT), the ice nucleating ability of SNOMAX, which contains non-viable Pseudomonas syringae bacteria as well as their fragments, was quantified using different measurement devices featuring different measurement techniques. Here, results determined with the Bielefeld Ice Nucleation ARraY (BINARY, Budke et al., 2013) and the Leipzig Aerosol Cloud Interaction Simulator (LACIS, Hartmann et al., 2011) are presented exemplarily. Within these devices, droplets with different amounts of SNOMAX were exposed to supercooling temperatures until they froze (BINARY: cooling rate: 1K/min; LACIS: residence time of supercooled droplets at a certain temperature: ~0.2s). Frozen fractions were determined in a temperature range of ca. -4 to -20 °C. These fractions increase steeply and, in part, level off at values lower than 100% (i.e., they reach a plateau value indicating the number of SNOMAX IN per droplet) depending on the SNOMAX concentration. With increasing amount of SNOMAX per droplet, the frozen fraction curve is shifted to higher temperature and the plateau value increases, reaching 100% for the highest SNOMAX concentrations. It has been suggested that ice nucleation active (INA) macromolecules, i.e. protein complexes in the case of bacteria, initiate the freezing process (Wolber et al. 1986). The Soccer ball model (Niedermeier et al., 2011) was used to parameterize the ice nucleation behavior of these INA macromolecules. One parameter set (mean contact angle and its standard deviation) could be derived that matches the experimental results of both devices. This parameterization can be used to describe the ice nucleation behavior of the INA bacteria in atmospheric models for a given number concentration being present in the atmosphere. Acknowledgement This work is funded by the German Research Foundation (DFG projects WE 4722/1-1 and KO 2944/2-1, both part of the research unit INUIT). References Budke et al., Proc.19th ICNAA, Fort Collins, CO, USA, 949-951, 2013. Hartmann et al., Atmos. Chem. Phys., 11, 1753-1767, 2011. Hartmann et al., Atmos. Chem. Phys., 13, 5751-5766, 2013. Hoose et al., Environ. Res. Lett. 5, 024009, 2010. Kanitz et al., Geophys. Res. Lett., 38, L17802, 2011. Niedermeier et al., Atmos. Chem. Phys., 11, 8767-8775, 2011. Murray et al., Chem. Soc. Rev., 41, 6519-6554, 2012. Wolber et al., P. Natl. A. Sci., 83, 7256-7260, 1986.

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

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.;

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.

Further evidence for CCN aerosol concentrations determining the height of warm rain and ice initiation in convective clouds over the Amazon basin

NASA Astrophysics Data System (ADS)

Campos Braga, Ramon; Rosenfeld, Daniel; Weigel, Ralf; Jurkat, Tina; Andreae, Meinrat O.; Wendisch, Manfred; Pöschl, Ulrich; Voigt, Christiane; Mahnke, Christoph; Borrmann, Stephan; Albrecht, Rachel I.; Molleker, Sergej; Vila, Daniel A.; Machado, Luiz A. T.; Grulich, Lucas

2017-12-01

We have investigated how aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in situ data of hydrometeor size distributions measured with instruments mounted on HALO aircraft during the ACRIDICON-CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm-3) nucleated at cloud base (Dr ≈ 5 ṡ Nd). Additional cloud processes associated with Dr, such as GCCN, cloud, and mixing with ambient air and other processes, produce deviations of ˜ 21 % in the linear relationship, but it does not mask the clear relationship between Dr and Nd, which was also found at different regions around the globe (e.g., Israel and India). When Nd exceeded values of about 1000 cm-3, Dr became greater than 5000 m, and the first observed precipitation particles were ice hydrometeors. Therefore, no liquid water raindrops were observed within growing convective cumulus during polluted conditions. Furthermore, the formation of ice particles also took place at higher altitudes in the clouds in polluted conditions because the resulting smaller cloud droplets froze at colder temperatures compared to the larger drops in the unpolluted cases. The measured vertical profiles of droplet effective radius (re) were close to those estimated by assuming adiabatic conditions (rea), supporting the hypothesis that the entrainment and mixing of air into convective clouds is nearly inhomogeneous. Additional CCN activation on aerosol particles from biomass burning and air pollution reduced re below rea, which further inhibited the formation of raindrops and ice particles and resulted in even higher altitudes for rain and ice initiation.

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

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.

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

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.

Aerosol specification in single-column Community Atmosphere Model version 5

DOE PAGES

Lebassi-Habtezion, B.; Caldwell, P. M.

2015-03-27

Single-column model (SCM) capability is an important tool for general circulation model development. In this study, the SCM mode of version 5 of the Community Atmosphere Model (CAM5) is shown to handle aerosol initialization and advection improperly, resulting in aerosol, cloud-droplet, and ice crystal concentrations which are typically much lower than observed or simulated by CAM5 in global mode. This deficiency has a major impact on stratiform cloud simulations but has little impact on convective case studies because aerosol is currently not used by CAM5 convective schemes and convective cases are typically longer in duration (so initialization is less important).more » By imposing fixed aerosol or cloud-droplet and crystal number concentrations, the aerosol issues described above can be avoided. Sensitivity studies using these idealizations suggest that the Meyers et al. (1992) ice nucleation scheme prevents mixed-phase cloud from existing by producing too many ice crystals. Microphysics is shown to strongly deplete cloud water in stratiform cases, indicating problems with sequential splitting in CAM5 and the need for careful interpretation of output from sequentially split climate models. Droplet concentration in the general circulation model (GCM) version of CAM5 is also shown to be far too low (~ 25 cm −3) at the southern Great Plains (SGP) Atmospheric Radiation Measurement (ARM) site.« less

A Continuous Flow Diffusion Chamber Study of Sea Salt Particles Acting as Cloud Seeds: Deliquescence, Ice Nucleation and Sublimation

NASA Astrophysics Data System (ADS)

Kong, X.; Wolf, M. J.; Garimella, S.; Roesch, M.; Cziczo, D. J.

2016-12-01

Sea Salt Aerosols (SSA) are abundant in the atmosphere, and important to the Earth's chemistry and energy budget. However, the roles of sea salts in the context of cloud formation are still poorly understood, which is partially due to the complexity of the water-salt phase diagram. At ambient temperatures, even well below 0°C, SSA deliquesces at sub-water saturated conditions. Since the ratio of the partial pressure over ice versus super-cooled water continuously declines with decreasing temperatures, it is interesting to consider if SSA continues to deliquesce under a super-saturated condition of ice, or if particles act as depositional ice nuclei when a critical supersaturation is reached. Some recent studies suggest hydrated NaCl and simulated sea salt might deliquesce between -35°C to -44°C, and below that deposition freezing becomes possible. Deliquesced droplets can subsequently freeze via the immersion or homogenous freezing mode, depending on if the deliquescence processes is complete. After the droplets or ice particles are formed, it is also interesting to consider how the different processes influence physical properties after evaporation or sublimation. This data is important for climate modeling that includes bromine burst observed in Antarctica, which is hypothesized to be relevant to the sublimation of blowing snow particles. In this study we use a SPectrometer for Ice Nuclei (SPIN; DMT, Inc., Boulder, CO) to perform experiments over a wide range of temperature and RH conditions to quantify deliquescence, droplet formation and ice nucleation. The formation of droplets and ice particles is detected by an advanced Optical Particle Counter (OPC) and the liquid/solid phases are distinguished by a machine learning method based on laser scattering and polarization data. Using an atomizer, four different sea salt samples are generated: pure NaCl and MgCl2 solutions, synthetic seawater, and natural seawater. Downstream of the SPIN chamber, a Pumped Counterflow Virtual Impactor (PCVI) is connected to separate the activated ice particles/large droplets to allow them undergo complete evaporation and sublimation. The particle size distributions are measured and compared to those upstream of SPIN to determine the effects of the ice/droplet nucleation process on the aerosol physical parameters.

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.

Stochastic kinetics reveal imperative role of anisotropic interfacial tension to determine morphology and evolution of nucleated droplets in nematogenic films

NASA Astrophysics Data System (ADS)

Bhattacharjee, Amit Kumar

2017-01-01

For isotropic fluids, classical nucleation theory predicts the nucleation rate, barrier height and critical droplet size by ac- counting for the competition between bulk energy and interfacial tension. The nucleation process in liquid crystals is less understood. We numerically investigate nucleation in monolayered nematogenic films using a mesoscopic framework, in par- ticular, we study the morphology and kinetic pathway in spontaneous formation and growth of droplets of the stable phase in the metastable background. The parameter κ that quantifies the anisotropic elastic energy plays a central role in determining the geometric structure of the droplets. Noncircular nematic droplets with homogeneous director orientation are nucleated in a background of supercooled isotropic phase for small κ. For large κ, noncircular droplets with integer topological charge, accompanied by a biaxial ring at the outer surface, are nucleated. The isotropic droplet shape in a superheated nematic background is found to depend on κ in a similar way. Identical growth laws are found in the two cases, although an unusual two-stage mechanism is observed in the nucleation of isotropic droplets. Temporal distributions of successive events indi- cate the relevance of long-ranged elasticity-mediated interactions within the isotropic domains. Implications for a theoretical description of nucleation in anisotropic fluids are discussed.

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.

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.

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.

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.

How does increasing horizontal resolution in a global climate model improve the simulation of aerosol-cloud interactions?

DOE PAGES

Ma, Po-Lun; Rasch, Philip J.; Wang, Minghuai; ...

2015-06-23

We report the Community Atmosphere Model Version 5 is run at horizontal grid spacing of 2, 1, 0.5, and 0.25°, with the meteorology nudged toward the Year Of Tropical Convection analysis, and cloud simulators and the collocated A-Train satellite observations are used to explore the resolution dependence of aerosol-cloud interactions. The higher-resolution model produces results that agree better with observations, showing an increase of susceptibility of cloud droplet size, indicating a stronger first aerosol indirect forcing (AIF), and a decrease of susceptibility of precipitation probability, suggesting a weaker second AIF. The resolution sensitivities of AIF are attributed to those ofmore » droplet nucleation and precipitation parameterizations. Finally, the annual average AIF in the Northern Hemisphere midlatitudes (where most anthropogenic emissions occur) in the 0.25° model is reduced by about 1 W m -2 (-30%) compared to the 2° model, leading to a 0.26 W m -2 reduction (-15%) in the global annual average AIF.« less

Ion-induced nucleation in solution: promotion of solute nucleation in charged levitated droplets.

PubMed

Draper, Neil D; Bakhoum, Samuel F; Haddrell, Allen E; Agnes, George R

2007-09-19

We have investigated the nucleation and growth of sodium chloride in both single quiescent charged droplets and charged droplet populations that were levitated in an electrodynamic levitation trap (EDLT). In both cases, the magnitude of a droplet's net excess charge (ions(DNEC)) influenced NaCl nucleation and growth, albeit in different capacities. We have termed the phenomenon ion-induced nucleation in solution. For single quiescent levitated droplets, an increase in ions(DNEC) resulted in a significant promotion of NaCl nucleation, as determined by the number of crystals observed. For levitated droplet populations, a change in NaCl crystal habit, from regular cubic shapes to dome-shaped dendrites, was observed once a surface charge density threshold of -9 x 10(-4) e.nm(-2) was surpassed. Although promotion of NaCl nucleation was observed for droplet population experiments, this can be attributed in part to the increased rate of solvent evaporation observed for levitated droplet populations having a high net charge. Promotion of nucleation was also observed for two organic acids, 2,4,6-trihydroxyacetophenone monohydrate (THAP) and alpha-cyano-4-hydroxycinnamic acid (CHCA). These results are of direct relevance to processes that occur in both soft-ionization techniques for mass spectrometry and to a variety of industrial processes. To this end, we have demonstrated the use of ion-induced nucleation in solution to form ammonium nitrate particles from levitated droplets to be used in in vitro toxicology studies of ambient particle types.

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).

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.

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.

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.

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

A new optical ice particle counter at LACIS

NASA Astrophysics Data System (ADS)

Bieligk, Henner; Voelker, Georg Sebastian; Clauss, Tina; Grundmann, Marius; Stratmann, Frank

2014-05-01

Clouds play an important role within the climate system, especially for the radiative energy budget of the earth. The radiative properties of a cloud depend strongly on the fractions of ice crystals and water droplets, their size distributions, and the ice crystal shapes within the particular cloud. One option to gain this kind of information is using optical particle counters. A new optical particle counter is developed for laboratory work and is based on the concept of the Thermostabilized Optical Particle Spectrometer for the Detection of Ice Particles (TOPS-Ice, Clauss et al., 2013). TOPS-Ice uses linearly polarized green laser light and the depolarization of the scattered light at a scattering angle of 42.5° to discriminate between liquid water droplets and ice crystals in the lower μm range. However, the measurements are usually limited to ice fractions in the order of 1%. To improve the determination of the ice fraction, several modifications of the original setup are implemented including an additional detection system at another scattering angle. The new scattering angle is optimized for least interference between the droplet and ice signals. This is achieved by finding the angle with the maximum difference in scattered intensity of water droplets compared to ice crystals with the same volume equivalent diameter. The suitable scattering angle of 100° for linearly polarized light was chosen based on calculations using T-Matrix method, Lorenz-Mie theory, Müller matrices and distribution theory. The new optical setup is designed to run in combination with a laminar flow tube, the so-called Leipzig Aerosol Cloud Interaction Simulator (LACIS, Stratmann et al., 2004; Hartmann et al., 2011). Using LACIS and its precisely controlled thermodynamic conditions, we are able to form small water droplets and ice crystals which will then be detected, classified and sized by our new optical device. This setup is planned to be tested in ice measurements including Snomax® and several dusts (e.g. illite, kaolinite, ATD) as ice nuclei which all show different behaviors in ice formation. Furthermore, a detailed comparison of both instruments TOPS-Ice and the new setup is planned. This project is part of the Leipzig Graduate School on Clouds, Aerosols and Radiation and is partly supported by the German Research Foundation (DFG project WE 4722/1-1) within the DFG Research Unit FOR 1525 INUIT. Clauss, T., Kiselev, A., Hartmann, S., Augustin, S., Pfeifer, S., Niedermeier, D., Wex, H., and Stratmann, F, 2013, Application of linear polarized light for the discrimination of frozen and liquid droplets in ice nucleation experiments, Atmos. Meas. Tech., 6, 1041-1052. Hartmann, S., Niedermeier, D., Voigtländer, J., Clauss, T., Shaw, R. A., Kiselev, A., and Stratmann, F., 2011, Homogeneous and heterogeneous ice nucleation at LACIS: operating principle and theoretical studies, Atmos. Chem. Phys., 11, 1753-1767. Stratmann, F., Kiselev, A., Wurzler, S., Wendisch, M., Heintzenberg, J., Charlson, R. J., Diehl, K., Wex, H., and Schmidt, S., 2004, Laboratory Studies and Numerical Simulations of Cloud Droplet Formation under Realistic Supersaturation Conditions, J. Atmos. Oceanic. Technol., 21, 876-887.

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.

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.

Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine mediated particle formation in the marine boundary layer

NASA Astrophysics Data System (ADS)

Murray, B. J.; Haddrell, A. E.; Peppe, S.; Davies, J. F.; Reid, J. P.; O'Sullivan, D.; Price, H. C.; Kumar, R.; Saunders, R. W.; Plane, J. M. C.; Umo, N. S.; Wilson, T. W.

2012-09-01

Iodine oxide particles are known to nucleate in the marine boundary layer where gas phase molecular iodine and organoiodine species are produced by macroalgae. These ultra-fine particles may then grow through the condensation of other materials to sizes where they may serve as cloud condensation nuclei. There has been some debate over the chemical identity of the initially nucleated particles. In laboratory simulations, hygroscopic measurements have been used to infer that they are composed of insoluble I2O4, while elemental analysis of laboratory generated particles suggests soluble I2O5 or its hydrated form iodic acid, HIO3 (I2O5·H2O). In this paper we explore the response of super-micron sized aqueous iodic acid solution droplets to varying humidity using both Raman microscopy and single particle electrodynamic traps. These measurements reveal that the propensity of an iodic acid solution droplet to crystallise is negligible on drying to ~0% relative humidity (RH). On applying mechanical pressure to these droplets they shatter in a manner consistent with an ultra-viscous liquid or a brittle glass. Water retention in amorphous material at low RH is important for understanding the hygroscopic growth of aerosol particles and uptake of other condensable material. Subsequent water uptake between 10 and 20% RH causes their viscosity to reduce sufficiently that the cracked droplets flow and merge. The persistence of iodic acid solution in an amorphous state, rather than a crystalline state, suggests they will more readily accommodate other condensable material and are therefore more likely to grow to sizes where they may serve as cloud condensation nuclei. On increasing the humidity to ~90% the mass of the droplets only increases by ~20% with a corresponding increase in radius of only 6%, which is remarkably small for a highly soluble material. We suggest that the small growth factor of aqueous iodic acid solution droplets is consistent with the small aerosol growth factors observed in previous experiments.

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.

Crystallization of hard spheres revisited. II. Thermodynamic modeling, nucleation work, and the surface of tension.

PubMed

Richard, David; Speck, Thomas

2018-06-14

Combining three numerical methods (forward flux sampling, seeding of droplets, and finite-size droplets), we probe the crystallization of hard spheres over the full range from close to coexistence to the spinodal regime. We show that all three methods allow us to sample different regimes and agree perfectly in the ranges where they overlap. By combining the nucleation work calculated from forward flux sampling of small droplets and the nucleation theorem, we show how to compute the nucleation work spanning three orders of magnitude. Using a variation of the nucleation theorem, we show how to extract the pressure difference between the solid droplet and ambient liquid. Moreover, combining the nucleation work with the pressure difference allows us to calculate the interfacial tension of small droplets. Our results demonstrate that employing bulk quantities yields inaccurate results for the nucleation rate.

Engineering Surfaces for Enhanced Nucleation and Droplet Removal During Dropwise Condensation

NASA Astrophysics Data System (ADS)

Dutta, Sanmitra; Khan, Sameera; Anand, Sushant

2017-11-01

Condensation plays critical role in numerous industrial applications, such as condensers, HVAC,etc In the most applications, fast formation (i.e. high nucleation) and subsequent removal of water droplets is critical for enhancing the efficiencies of their associated systems. Significant focus has been placed on the aspect of droplet removal from surfaces. This has led to, development of superhydrophobic surfaces with special textures on which droplets are self-removed after coalescence. However,because of their inherent low surface energy, nucleation energy barriers are also high on such surfaces. In contrast to conventional superhydrophobic surfaces, here we show that surfaces can be engineered such that the simultaneous benefits of high nucleation rates and fast droplet removal can be obtained during the condensation process.These benefits are obtained by impregnating a superhydrophobic surface with an oil that despite its defect-free interface provides low nucleation energy barrier during condensation. At the same time, the oil facilitates high droplet shedding rates by providing a lubricating layer below the droplets due to which droplets have negligible contact angle hysteresis. We provide a guide to choose oils that lead to enhanced nucleation, and provide experimental evidence supporting the proposed guide. We discuss the importance of different oil properties in affecting the droplet growth and subsequent removal of water droplets.

Anthropogenic Sulfate, Clouds, and Climate Forcing

NASA Technical Reports Server (NTRS)

Ghan, Steven J.

1997-01-01

This research work is a joint effort between research groups at the Battelle Pacific Northwest Laboratory, Virginia Tech University, Georgia Institute of Technology, Brookhaven National Laboratory, and Texas A&M University. It has been jointly sponsored by the National Aeronautics and Space Administration, the U.S. Department of Energy, and the U.S. Environmental Protection Agency. In this research, a detailed tropospheric aerosol-chemistry model that predicts oxidant concentrations as well as concentrations of sulfur dioxide and sulfate aerosols has been coupled to a general circulation model that distinguishes between cloud water mass and cloud droplet number. The coupled model system has been first validated and then used to estimate the radiative impact of anthropogenic sulfur emissions. Both the direct radiative impact of the aerosols and their indirect impact through their influence on cloud droplet number are represented by distinguishing between sulfuric acid vapor and fresh and aged sulfate aerosols, and by parameterizing cloud droplet nucleation in terms of vertical velocity and the number concentration of aged sulfur aerosols. Natural sulfate aerosols, dust, and carbonaceous and nitrate aerosols and their influence on the radiative impact of anthropogenic sulfate aerosols, through competition as cloud condensation nuclei, will also be simulated. Parallel simulations with and without anthropogenic sulfur emissions are performed for a global domain. The objectives of the research are: To couple a state-of-the-art tropospheric aerosol-chemistry model with a global climate model. To use field and satellite measurements to evaluate the treatment of tropospheric chemistry and aerosol physics in the coupled model. To use the coupled model to simulate the radiative (and ultimately climatic) impacts of anthropogenic sulfur emissions.

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.

Modifications of steam condensation model implemented in commercial solver

NASA Astrophysics Data System (ADS)

Sova, Libor; Jun, Gukchol; ŠÅ¥astný, Miroslav

2017-09-01

Nucleation theory and droplet grow theory and methods how they are incorporated into numerical solvers are crucial factors for proper wet steam modelling. Unfortunately, they are still covered by cloud of uncertainty and therefore some calibration of these models according to reliable experimental results is important for practical analyses of steam turbines. This article demonstrates how is possible to calibrate wet steam model incorporated into commercial solver ANSYS CFX.

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.

Glory on Venus and selection among the unknown UV absorbers

NASA Astrophysics Data System (ADS)

Petrova, Elena V.

2018-05-01

The comparison of the phase profiles of glories observed on the cloud top of Venus by the Venus Monitoring Camera (Venus Express) and the light-scattering characteristics of sulfuric acid droplets, containing admixtures with a high refractive index, makes it easier to choose between some candidates for the so-called unknown UV absorber in the Venus clouds. Since among the candidates there are materials wetted and not wetted by sulfuric acid, we analyze whether small submicron particles adhered to or embedded into the 1-μm H2SO4 droplets may actually change the glory pattern normally produced by homogeneous spherical particles and what the conditions are, under which the composite particles formed in heterogeneous nucleation may still produce a glory feature. We have found that one of the most frequently considered candidates, sulfur, can hardly be responsible for the contrasts observed at 0.365 μm on the upper clouds, since it is not wetted by sulfuric acid and submicron sulfur particles, serving as condensation nuclei for sulfuric acid, can only adhere to the H2SO4 droplets rather than be enveloped by them. Such droplets decorated by sulfur blobs substantially distort the glory feature characteristic of the scattering by spherical particles or even smooth it at all, while a glory pattern is practically always seen in the images of Venus taken at small phase angles. At the same time, the grains of the other UV absorbers that can be embedded in H2SO4 droplets, e.g., the widely discussed ferric chloride, pose no problem in terms of interpretation of the observations of glory.

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.

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

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.

Cloud microphysics and aerosol indirect effects in the global climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Lohmann, U.; Stier, P.; Hoose, C.; Ferrachat, S.; Roeckner, E.; Zhang, J.

2007-03-01

The double-moment cloud microphysics scheme from ECHAM4 has been coupled to the size-resolved aerosol scheme ECHAM5-HAM. ECHAM5-HAM predicts the aerosol mass and number concentrations and the aerosol mixing state. This results in a much better agreement with observed vertical profiles of the black carbon and aerosol mass mixing ratios than with the previous version ECHAM4, where only the different aerosol mass mixing ratios were predicted. Also, the simulated liquid, ice and total water content and the cloud droplet and ice crystal number concentrations as a function of temperature in stratiform mixed-phase clouds between 0 and -35°C agree much better with aircraft observations in the ECHAM5 simulations. ECHAM5 performs better because more realistic aerosol concentrations are available for cloud droplet nucleation and because the Bergeron-Findeisen process is parameterized as being more efficient. The total anthropogenic aerosol effect includes the direct, semi-direct and indirect effects and is defined as the difference in the top-of-the-atmosphere net radiation between present-day and pre-industrial times. It amounts to -1.8 W m-2 in ECHAM5, when a relative humidity dependent cloud cover scheme and present-day aerosol emissions representative for the year 2000 are used. It is larger when either a statistical cloud cover scheme or a different aerosol emission inventory are employed.

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.

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.

Temperature-dependent formation of NaCl dihydrate in levitated NaCl and sea salt aerosol particles.

PubMed

Peckhaus, Andreas; Kiselev, Alexei; Wagner, Robert; Duft, Denis; Leisner, Thomas

2016-12-28

Recent laboratory studies indicate that the hydrated form of crystalline NaCl is potentially important for atmospheric processes involving depositional ice nucleation on NaCl dihydrate particles under cirrus cloud conditions. However, recent experimental studies reported a strong discrepancy between the temperature intervals where the efflorescence of NaCl dihydrate has been observed. Here we report the measurements of the volume specific nucleation rate of crystalline NaCl in the aqueous solution droplets of pure NaCl suspended in an electrodynamic balance at constant temperature and humidity in the range from 250 K to 241 K. Based on these measurements, we derive the interfacial energy of crystalline NaCl dihydrate in a supersaturated NaCl solution and determined its temperature dependence. Taking into account both temperature and concentration dependence of nucleation rate coefficients, we explain the difference in the observed fractions of NaCl dihydrate reported in the previous studies. Applying the heterogeneous classical nucleation theory model, we have been able to reproduce the 5 K shift of the NaCl dihydrate efflorescence curve observed for the sea salt aerosol particles, assuming the presence of super-micron solid inclusions (hypothetically gypsum or hemihydrate of CaSO 4 ). These results support the notion that the phase transitions in microscopic droplets of supersaturated solution should be interpreted by accounting for the stochastic nature of homogeneous and heterogeneous nucleation and cannot be understood on the ground of bulk phase diagrams alone.

Temperature-dependent formation of NaCl dihydrate in levitated NaCl and sea salt aerosol particles

NASA Astrophysics Data System (ADS)

Peckhaus, Andreas; Kiselev, Alexei; Wagner, Robert; Duft, Denis; Leisner, Thomas

2016-12-01

Recent laboratory studies indicate that the hydrated form of crystalline NaCl is potentially important for atmospheric processes involving depositional ice nucleation on NaCl dihydrate particles under cirrus cloud conditions. However, recent experimental studies reported a strong discrepancy between the temperature intervals where the efflorescence of NaCl dihydrate has been observed. Here we report the measurements of the volume specific nucleation rate of crystalline NaCl in the aqueous solution droplets of pure NaCl suspended in an electrodynamic balance at constant temperature and humidity in the range from 250 K to 241 K. Based on these measurements, we derive the interfacial energy of crystalline NaCl dihydrate in a supersaturated NaCl solution and determined its temperature dependence. Taking into account both temperature and concentration dependence of nucleation rate coefficients, we explain the difference in the observed fractions of NaCl dihydrate reported in the previous studies. Applying the heterogeneous classical nucleation theory model, we have been able to reproduce the 5 K shift of the NaCl dihydrate efflorescence curve observed for the sea salt aerosol particles, assuming the presence of super-micron solid inclusions (hypothetically gypsum or hemihydrate of CaSO4). These results support the notion that the phase transitions in microscopic droplets of supersaturated solution should be interpreted by accounting for the stochastic nature of homogeneous and heterogeneous nucleation and cannot be understood on the ground of bulk phase diagrams alone.

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.

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.

Initiation of the ice phase by marine biogenic surfaces in supersaturated gas and supercooled aqueous phases.

PubMed

Alpert, Peter A; Aller, Josephine Y; Knopf, Daniel A

2011-11-28

Biogenic particles have the potential to affect the formation of ice crystals in the atmosphere with subsequent consequences for the hydrological cycle and climate. We present laboratory observations of heterogeneous ice nucleation in immersion and deposition modes under atmospherically relevant conditions initiated by Nannochloris atomus and Emiliania huxleyi, marine phytoplankton with structurally and chemically distinct cell walls. Temperatures at which freezing, melting, and water uptake occur are observed using optical microscopy. The intact and fragmented unarmoured cells of N. atomus in aqueous NaCl droplets enhance ice nucleation by 10-20 K over the homogeneous freezing limit and can be described by a modified water activity based ice nucleation approach. E. huxleyi cells covered by calcite plates do not enhance droplet freezing temperatures. Both species nucleate ice in the deposition mode at an ice saturation ratio, S(ice), as low as ~1.2 and below 240 K, however, for each, different nucleation modes occur at warmer temperatures. These observations show that markedly different biogenic surfaces have both comparable and contrasting effects on ice nucleation behaviour depending on the presence of the aqueous phase and the extent of supercooling and water vapour supersaturation. We derive heterogeneous ice nucleation rate coefficients, J(het), and cumulative ice nuclei spectra, K, for quantification and analysis using time-dependent and time-independent approaches, respectively. Contact angles, α, derived from J(het)via immersion freezing depend on T, a(w), and S(ice). For deposition freezing, α can be described as a function of S(ice) only. The different approaches yield different predictions of atmospheric ice crystal numbers primarily due to the time evolution allowed for the time-dependent approach with implications for the evolution of mixed-phase and ice clouds.

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.

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.

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.

BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation

NASA Astrophysics Data System (ADS)

Budke, C.; Koop, T.

2015-02-01

A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY) ice nucleation can be studied simultaneously in 36 droplets at temperatures down to -40 °C (233 K) and at cooling rates between 0.1 and 10 K min-1. The droplets are separated from each other in individual compartments, thus preventing a Wegener-Bergeron-Findeisen type water vapor transfer between droplets as well as avoiding the seeding of neighboring droplets by formation and surface growth of frost halos. Analysis of freezing and melting occurs via an automated real-time image analysis of the optical brightness of each individual droplet. As an application ice nucleation in water droplets containing Snomax® at concentrations from 1 ng mL-1 to 1 mg mL-1 was investigated. Using different cooling rates, a small time dependence of ice nucleation induced by two different classes of ice nucleators (INs) contained in Snomax® was detected and the corresponding heterogeneous ice nucleation rate coefficient was quantified. The observed time dependence is smaller than those of other types of INs reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other INs of atmospheric interest, making it a useful tool for future investigations.

Designing magnetic droplet soliton nucleation employing spin polarizer

NASA Astrophysics Data System (ADS)

Mohseni, Morteza; Mohseni, Majid

2018-04-01

We show by means of micromagnetic simulations that spin polarizer in nano-contact (NC) spin torque oscillators as the representative of the fixed layer in an orthogonal pseudo-spin valve can be employed to design and to control magnetic droplet soliton nucleation and dynamics. We found that using a tilted spin polarizer layer decreases the droplet nucleation time which is more suitable for high speed applications. However, a tilted spin polarizer increases the nucleation current and decreases the frequency stability of the droplet. Additionally, by driving the magnetization inhomogenously at the NC region, it is found that a tilted spin polarizer reduces the precession angle of the droplet and through an interplay with the Oersted field of the DC current, it breaks the spatial symmetry of the droplet profile. Our findings explore fundamental insight into nano-scale magnetic droplet soliton dynamics with potential tunability parameters for future microwave electronics.

Parameterization of aerosol scavenging due to atmospheric ionization under varying relative humidity

NASA Astrophysics Data System (ADS)

Zhang, Liang; Tinsley, Brian A.

2017-05-01

Simulations and parameterizations of the modulation of aerosol scavenging by electric charges on particles and droplets for different relative humidities have been made for 3 μm radii droplets and a wide range of particle radii. For droplets and particles with opposite-sign charges, the attractive Coulomb force increases the collision rate coefficients above values due to other forces. With same-sign charges, the repulsive Coulomb force decreases the rate coefficients, and the short-range attractive image forces become important. The phoretic forces are attractive for relative humidity less than 100% and repulsive for relative humidity greater than 100% and have increasing overall effect for particle radii up to about 1 μm. There is an analytic solution for rate coefficients if only inverse square forces are present, but due to the presence of image forces, and for larger particles the intercept, weight, and the flow around the particle affecting the droplet trajectory, the simulated results usually depart far from the analytic solution. We give simple empirical parameterization formulas for some cases and more complex parameterizations for more exact fits to the simulated results. The results can be used in cloud models with growing droplets, as in updrafts, as well as with evaporating droplets in downdrafts. There is considered to be little scavenging of uncharged ice-forming nuclei in updrafts, but with charged ice-forming nuclei it is possible for scavenging in updrafts in cold clouds to produce contact ice nucleation. Scavenging in updrafts below the freezing level produces immersion nuclei that promote enhanced freezing as droplets rise above it.

The role of the cubic structure in freezing of a supercooled water droplet on an ice substrate

NASA Astrophysics Data System (ADS)

Takahashi, T.; Kobayashi, T.

1983-12-01

The possibility of the formation of a metastable cubic (diamond) structure and its role in freezing of a supercooled water droplet on an ice substrate are discussed in terms of two-dimensional nucleation. The mode of stacking sequence of new layers formed by two-dimensional nucleation is divided into single and multi-nucleation according to the degree of supercooling and to the size of the supercooled droplet. In the case of single nucleation a frozen droplet develops into a complete hexagonal single crystal or an optically single crystal (containing discontinuous stacking faults). In the case of multi-nucleation attention is paid to the size effect and the stacking direction of the nucleus to calculate the waiting time in the nucleation. Then the frozen droplets are crystallographically divided into three categories: completely single crystals, optically single crystals (containing a small cubic structure, i.e. stacking faults) and polycrystals with a misorientation of 70.53° between the c-axes.

Ice nucleation rates near ˜225 K

NASA Astrophysics Data System (ADS)

Amaya, Andrew J.; Wyslouzil, Barbara E.

2018-02-01

We have measured the ice nucleation rates, Jice, in supercooled nano-droplets with radii ranging from 6.6 nm to 10 nm and droplet temperatures, Td, ranging from 225 K to 204 K. The initial temperature of the 10 nm water droplets is ˜250 K, i.e., well above the homogeneous nucleation temperature for micron sized water droplets, TH ˜235 K. The nucleation rates increase systematically from ˜1021 cm-3 s-1 to ˜1022 cm-3 s-1 in this temperature range, overlap with the nucleation rates of Manka et al. [Phys. Chem. Chem. Phys. 14, 4505 (2012)], and suggest that experiments with larger droplets would extrapolate smoothly the rates of Hagen et al. [J. Atmos. Sci. 38, 1236 (1981)]. The sharp corner in the rate data as temperature drops is, however, difficult to match with available theory even if we correct classical nucleation theory and the physical properties of water for the high internal pressure of the nanodroplets.

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.

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.

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.

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.

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).

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.

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.

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.

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.

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.

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 rates of single protein complexes and single macromolecules

NASA Astrophysics Data System (ADS)

Stratmann, F.; Wex, H.; Niedermeier, D.; Hartmann, S.; Augustin, S.; Clauss, T.; Voigtlaender, J.; Pummer, B.; Grothe, H.

2012-12-01

With our flow-tube LACIS (Leipzig Aerosol cloud Interaction Simulator), we measured immersion freezing of droplets containing biological ice nucleating (IN) agents. From our measurements, we were able to deduce ice nucleation rates for single IN protein complexes (for Snomax) and for IN macromolecules (in the case of Birch pollen). For the measurements, aerosol particles were produced from solutions/suspensions of either Snomax (deadened and partly fractionalized pseudomonas syringae bacteria) or of Birch pollen washing water (BW in the following). All particles were dried and size selected before entering LACIS. In LACIS, particles were activated to droplets, and we measured the fraction of all droplets that froze (F(ice)) as function of temperature. For Snomax, a strong increase in F(ice) was observed around -7 to -10°C, for BW around -19 to -25°C, respectively. After this initial steep increase, F(ice) stayed constant for both examined substances down to -35°C. We found that the values of F(ice) in the plateau region depended on the dry particle size. The initial solution used to generate the particles contained parts of bacteria with ice active protein complexes on them in the case of Snomax, or IN macromolecules in the case of BW (Pummer et al., 2011). We show that the distribution of the IN proteins or IN molecules in the aerosol particles follows the Poisson distribution. With this knowledge, derivation of the ice nucleation rates for single IN protein complexes or for single IN macromolecules is possible. Combining the Poisson distribution with a stochastic model and using the derived nucleation rates, we can reproduce not only our measurements for both examined substances, but also past measurements done for Snomax and even pseudomonas syringae bacteria. As an additional peculiarity, we seem to observe two different macromolecules being ice active for Birch trees growing in Central Europe or Northern Europe, with the latter initiating freezing at slightly warmer temperatures. Pummer, B. G. et al. (2012), Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen, Aerosol Chem. Phys., 12, 2541-2550.

BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation

NASA Astrophysics Data System (ADS)

Budke, C.; Koop, T.

2014-09-01

A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY) ice nucleation can be studied simultaneously in 36 droplets at temperatures down to -40 °C (233 K) and at cooling rates between 0.1 K min-1 and 10 K min-1. The droplets are separated from each other in individual compartments, thus preventing a Wegener-Bergeron-Findeisen type water vapor transfer between droplets as well as avoiding the seeding of neighboring droplets by formation and surface growth of frost halos. Analysis of freezing and melting occurs via an automated real time image analysis of the optical brightness of each individual droplet. As an application ice nucleation in water droplets containing Snomax® at concentrations from 1 ng mL-1 to 1 mg mL-1 was investigated. Using different cooling rates a minute time dependence of ice nucleation induced by Class A and Class C ice nucleators contained in Snomax® was detected. For the Class A IN a very strong increase of the heterogeneous ice nucleation rate coefficient with decreasing temperature of λ ≡ -dln(jhet)/dT = 8.7 K-1 was observed emphasizing the capability of the BINARY device. This value is larger than those of other types of IN reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other IN of atmospheric interest, making it a useful tool for future investigations.

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.

Thermokinetics of heterogeneous droplet nucleation on conically textured substrates.

PubMed

Singha, Sanat K; Das, Prasanta K; Maiti, Biswajit

2015-11-28

Within the framework of the classical theory of heterogeneous nucleation, a thermokinetic model is developed for line-tension-associated droplet nucleation on conical textures considering growth or shrinkage of the formed cluster due to both interfacial and peripheral monomer exchange and by considering different geometric configurations. Along with the principle of free energy extremization, Katz kinetic approach has been employed to study the effect of substrate conicity and wettability on the thermokinetics of heterogeneous water droplet nucleation. Not only the peripheral tension is found to have a considerable effect on the free energy barrier but also the substrate hydrophobicity and hydrophilicity are observed to switch over their roles between conical crest and trough for different growth rates of the droplet. Besides, the rate of nucleation increases and further promotes nucleation for negative peripheral tension as it diminishes the free energy barrier appreciably. Moreover, nucleation inhibition can be achievable for positive peripheral tension due to the enhancement of the free energy barrier. Analyzing all possible geometric configurations, the hydrophilic narrower conical cavity is found to be the most preferred nucleation site. These findings suggest a physical insight into the context of surface engineering for the promotion or the suppression of nucleation on real or engineered substrates.

Laboratory and field studies of stratospheric aerosols: Phase changes under high supersaturation

NASA Technical Reports Server (NTRS)

Hallet, John

1991-01-01

It is well known that water in the form of isolated small droplets supercool as much as 40 C below their equilibrium melting point. Solutions similarly supercool (with respect to water) and supersaturate (with respect of the solute). Experiments are described in which bulk solutions typical of atmospheric aerosols (nitric acid, sulfuric acid, and hydrates; ammonium sulfate; ammonium bisulfate; sodium chloride) are supercooled and/or supersaturated and nucleated to initiate crystal growth. Supersaturation of 300 percent is readily attainable, with linear growth of crystals increasing roughly as (supercooling/supersaturation)sup 2. The implication of the experiments is that the situation of metastability in polar stratosphere clouds is very likely, with nucleation only occuring under a high degree of supercooling or supersaturation.

AirMSPI ORACLES Cloud Droplet Data V001

Atmospheric Science Data Center

2018-05-05

AirMSPI_ORACLES_Cloud_Droplet_Size_and_Cloud_Optical_Depth L2 Derived Geophysical Parameters ... Order: Earthdata Search Parameters:  Cloud Optical Depth Cloud Droplet Effective Radius Cloud Droplet ...

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.

Temperature uniformity in the CERN CLOUD chamber

NASA Astrophysics Data System (ADS)

Dias, António; Ehrhart, Sebastian; Vogel, Alexander; Williamson, Christina; Almeida, João; Kirkby, Jasper; Mathot, Serge; Mumford, Samuel; Onnela, Antti

2017-12-01

The CLOUD (Cosmics Leaving OUtdoor Droplets) experiment at CERN (European Council for Nuclear Research) investigates the nucleation and growth of aerosol particles under atmospheric conditions and their activation into cloud droplets. A key feature of the CLOUD experiment is precise control of the experimental parameters. Temperature uniformity and stability in the chamber are important since many of the processes under study are sensitive to temperature and also to contaminants that can be released from the stainless steel walls by upward temperature fluctuations. The air enclosed within the 26 m3 CLOUD chamber is equipped with several arrays (strings) of high precision, fast-response thermometers to measure its temperature. Here we present a study of the air temperature uniformity inside the CLOUD chamber under various experimental conditions. Measurements were performed under calibration conditions and run conditions, which are distinguished by the flow rate of fresh air and trace gases entering the chamber at 20 and up to 210 L min-1, respectively. During steady-state calibration runs between -70 and +20 °C, the air temperature uniformity is better than ±0.06 °C in the radial direction and ±0.1 °C in the vertical direction. Larger non-uniformities are present during experimental runs, depending on the temperature control of the make-up air and trace gases (since some trace gases require elevated temperatures until injection into the chamber). The temperature stability is ±0.04 °C over periods of several hours during either calibration or steady-state run conditions. During rapid adiabatic expansions to activate cloud droplets and ice particles, the chamber walls are up to 10 °C warmer than the enclosed air. This results in temperature differences of ±1.5 °C in the vertical direction and ±1 °C in the horizontal direction, while the air returns to its equilibrium temperature with a time constant of about 200 s.

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.

Experimental investigation on the phenomena around the onset nucleate boiling during the impacting of a droplet on the hot surface

NASA Astrophysics Data System (ADS)

Mitrakusuma, Windy H.; Deendarlianto, Kamal, Samsul; Indarto, Nuriyadi, M.

2016-06-01

Onset of nucleate boiling of a droplet when impacted onto hot surface was investigated. Three kinds of surfaces, normal stainless steel (NSS), stainless steel with TiO2 coating (UVN), and stainless steel with TiO2 coating and radiated by ultraviolet ray were employed to examine the effect of wettability. The droplet size was 2.4 mm diameter, and dropped under different We number. The image is generated by high speed camera with the frame speed of 1000 fps. The boiling conditions are identified as natural convection, nucleate boiling, critical heat flux, transition, and film boiling. In the present report, the discussion will be focused on the beginning of nucleate boiling on the droplet. Nucleate boiling occurs when bubbles are generated. These bubbles are probably caused by nucleation on the impurities within the liquid rather than at nucleation sites on the heated surface because the bubbles appear to be in the bulk of the liquid instead of at the liquid-solid interface. In addition, the smaller the contact angle, the fastest the boiling.

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.

Immersion freezing of birch pollen washing water

NASA Astrophysics Data System (ADS)

Augustin, S.; Wex, H.; Niedermeier, D.; Pummer, B.; Grothe, H.; Hartmann, S.; Tomsche, L.; Clauss, T.; Voigtländer, J.; Ignatius, K.; Stratmann, F.

2013-11-01

Birch pollen grains are known to be ice nucleating active biological particles. The ice nucleating activity has previously been tracked down to biological macromolecules that can be easily extracted from the pollen grains in water. In the present study, we investigated the immersion freezing behavior of these ice nucleating active (INA) macromolecules. Therefore we measured the frozen fractions of particles generated from birch pollen washing water as a function of temperature at the Leipzig Aerosol Cloud Interaction Simulator (LACIS). Two different birch pollen samples were considered, with one originating from Sweden and one from the Czech Republic. For the Czech and Swedish birch pollen samples, freezing was observed to start at -19 and -17 °C, respectively. The fraction of frozen droplets increased for both samples down to -24 °C. Further cooling did not increase the frozen fractions any more. Instead, a plateau formed at frozen fractions below 1. This fact could be used to determine the amount of INA macromolecules in the droplets examined here, which in turn allowed for the determination of nucleation rates for single INA macromolecules. The main differences between the Swedish birch pollen and the Czech birch pollen were obvious in the temperature range between -17 and -24 °C. In this range, a second plateau region could be seen for Swedish birch pollen. As we assume INA macromolecules to be the reason for the ice nucleation, we concluded that birch pollen is able to produce at least two different types of INA macromolecules. We were able to derive parameterizations for the heterogeneous nucleation rates for both INA macromolecule types, using two different methods: a simple exponential fit and the Soccer ball model. With these parameterization methods we were able to describe the ice nucleation behavior of single INA macromolecules from both the Czech and the Swedish birch pollen.

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.

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.

Experimental investigation on the phenomena around the onset nucleate boiling during the impacting of a droplet on the hot surface

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

Mitrakusuma, Windy H., E-mail: windyhm@polban.ac.id; Refrigeration and Airconditioning Department, Politeknik Negeri Bandung, Jl. Gegerkalong Hilir, Ds. Ciwaruga Kotak Pos 1234 Bandung; Deendarlianto,

2016-06-03

Onset of nucleate boiling of a droplet when impacted onto hot surface was investigated. Three kinds of surfaces, normal stainless steel (NSS), stainless steel with TiO{sub 2} coating (UVN), and stainless steel with TiO{sub 2} coating and radiated by ultraviolet ray were employed to examine the effect of wettability. The droplet size was 2.4 mm diameter, and dropped under different We number. The image is generated by high speed camera with the frame speed of 1000 fps. The boiling conditions are identified as natural convection, nucleate boiling, critical heat flux, transition, and film boiling. In the present report, the discussionmore » will be focused on the beginning of nucleate boiling on the droplet. Nucleate boiling occurs when bubbles are generated. These bubbles are probably caused by nucleation on the impurities within the liquid rather than at nucleation sites on the heated surface because the bubbles appear to be in the bulk of the liquid instead of at the liquid-solid interface. In addition, the smaller the contact angle, the fastest the boiling.« less

Heterogeneous nucleation on rough surfaces: Generalized Gibbs' approach.

PubMed

Abyzov, Alexander S; Schmelzer, Jürn W P; Davydov, Leonid N

2017-12-07

Heterogeneous nucleation (condensation) of liquid droplets from vapor (gas) on a defective solid surface is considered. The vapor is described by the van der Waals equation of state. The dependence of nucleating droplet parameters on droplet size is accounted for within the generalized Gibbs approach. As a surface defect, a conic void is taken. This choice allows us to simplify the analysis and at the same time to follow the main aspects of the influence of the surface roughness on the nucleation process. Similar to condensation on ideal planar surfaces, the contact angle and catalytic factor for heterogeneous nucleation on a rough surface depend on the degree of vapor overcooling. In the case of droplet formation on a hydrophilic surface of a conic void, the nucleation rate considerably increases in comparison with the condensation on a planar interface. In fact, the presence of a defect on the hydrophilic surface leads to a considerable shift of the spinodal towards lower supersaturation in comparison with heterogeneous nucleation on a planar interface. With the decrease in the void cone angle, the heterogeneous spinodal approaches the binodal, and the region of metastability is diminished at the expense of the instability region.

The WeIzmann Supercooled Droplets Observation on a Microarray (WISDOM) and application for ambient dust

NASA Astrophysics Data System (ADS)

Reicher, Naama; Segev, Lior; Rudich, Yinon

2018-01-01

The WeIzmann Supercooled Droplets Observation on Microarray (WISDOM) is a new setup for studying ice nucleation in an array of monodisperse droplets for atmospheric implications. WISDOM combines microfluidics techniques for droplets production and a cryo-optic stage for observation and characterization of freezing events of individual droplets. This setup is designed to explore heterogeneous ice nucleation in the immersion freezing mode, down to the homogeneous freezing of water (235 K) in various cooling rates (typically 0.1-10 K min-1). It can also be used for studying homogeneous freezing of aqueous solutions in colder temperatures. Frozen fraction, ice nucleation active surface site densities and freezing kinetics can be obtained from WISDOM measurements for hundreds of individual droplets in a single freezing experiment. Calibration experiments using eutectic solutions and previously studied materials are described. WISDOM also allows repeatable cycles of cooling and heating for the same array of droplets. This paper describes the WISDOM setup, its temperature calibration, validation experiments and measurement uncertainties. Finally, application of WISDOM to study the ice nucleating particle (INP) properties of size-selected ambient Saharan dust particles is presented.

Identification and quantification of ice nucleation active microorganisms by digital droplet PCR (ddPCR)

NASA Astrophysics Data System (ADS)

Linden, Martin; Pöschl, Ulrich; Fröhlich-Nowoisky, Janine

2015-04-01

Several bioaerosol types, including bacteria, fungi, pollen and lichen, have been identified as sources of biological ice nucleators (IN) which induce ice formation already at temperatures as high as -10 °C or above. Accordingly, they potentially contribute widely to environmental ice nucleation in the atmosphere and are of great interest in the study of natural heterogenous ice nucleation processes. Ice nucleation active microorganisms have been found and studied among bacteria (Proteobacteria) and fungi (phyla Basidiomycota and Ascomycota). The mechanisms enabling the microorganisms to ice nucleation are subject to ongoing research. While it has been demonstrated that whole cells can act as ice nucleators in the case of bacteria due to the presence of specific membrane proteins, cell-free ice nucleation active particles seem to be responsible for this phenomenon in fungi and lichen. The identification and quantification of these ice nucleation active microorganisms and their IN in atmospheric samples is crucial to understand their contribution to the pool of atmospheric IN. This is not a trivial task since the respective microorganisms are often prevalent in lowest concentrations and a variety of states, be it viable cells, spores or cell debris from dead cells. Molecular biology provides tools to identify and quantify ice nucleation active microorganisms independent of their state by detecting genetic markers specific for the organism of interest. Those methods are not without their drawbacks in terms of sample material concentration required or reliable standardization. Digital Droplet Polymerase Chain Reaction (ddPCR) was chosen for our demands as a more elegant, quick and specific method in the investigation of ice nucleation active microorganisms in atmospheric samples. The advantages of ddPCR lie in the simultaneous detection and quantification of genetic markers and their original copy numbers in a sample. This is facilitated by the fractionation of the PCR reaction volumes containing template DNA of ice nucleation active microorganisms from atmospheric samples in thousands of identical droplets. Each droplet encapsulates the reagents necessary for DNA amplification. With template DNA concentrations low enough, the droplets will statistically contain either no template molecules or one molecule. A molecule of template DNA corresponds to exactly one cell of an ice nucleation active microorganism in the original sample provided the genetic marker on the template is present in a single copy. Successful amplification in the presence of template DNA is coupled to a measurable fluorescence signal. The original template DNA concentration is automatically derived from the fraction of fluorescence positive droplets to total droplet number. This far, molecular probes against single-copy genetic markers for ice nucleation active fungi Mortierella alpina, Acremonium implicatum, Isaria farinosa and the ice nucleation active bacterium Pseudomonas syringae have been successfully designed and tested by our group.

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.

Simulation of the effects of aerosol on mixed-phase orographic clouds using the WRF model with a detailed bin microphysics scheme

NASA Astrophysics Data System (ADS)

Xiao, Hui; Yin, Yan; Jin, Lianji; Chen, Qian; Chen, Jinghua

2015-08-01

The Weather Research Forecast (WRF) mesoscale model coupled with a detailed bin microphysics scheme is used to investigate the impact of aerosol particles serving as cloud condensation nuclei and ice nuclei on orographic clouds and precipitation. A mixed-phase orographic cloud developed under two scenarios of aerosol (a typical continental background and a relatively polluted urban condition) and ice nuclei over an idealized mountain is simulated. The results show that, when the initial aerosol condition is changed from the relatively clean case to the polluted scenario, more droplets are activated, leading to a delay in precipitation, but the precipitation amount over the terrain is increased by about 10%. A detailed analysis of the microphysical processes indicates that ice-phase particles play an important role in cloud development, and their contribution to precipitation becomes more important with increasing aerosol particle concentrations. The growth of ice-phase particles through riming and Wegener-Bergeron-Findeisen regime is more effective under more polluted conditions, mainly due to the increased number of droplets with a diameter of 10-30 µm. Sensitivity tests also show that a tenfold increase in the concentration of ice crystals formed from ice nucleation leads to about 7% increase in precipitation, and the sensitivity of the precipitation to changes in the concentration and size distribution of aerosol particles is becoming less pronounced when the concentration of ice crystals is also increased.

Cloud droplet size distribution broadening during diffusional growth: ripening amplified by deactivation and reactivation

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

Yang, Fan; Kollias, Pavlos; Shaw, Raymond A.

Cloud droplet size distributions (CDSDs), which are related to cloud albedo and lifetime, are usually broader in warm clouds than predicted from adiabatic parcel calculations. We investigate a mechanism for the CDSD broadening using a Lagrangian bin-microphysics cloud parcel model that considers the condensational growth of cloud droplets formed on polydisperse, sub-micrometer aerosols in an adiabatic cloud parcel that undergoes vertical oscillations, such as those due to cloud circulations or turbulence. Results show that the CDSD can be broadened during condensational growth as a result of Ostwald ripening amplified by droplet deactivation and reactivation, which is consistent with Korolev (1995).more » The relative roles of the solute effect, curvature effect, deactivation and reactivation on CDSD broadening are investigated. Deactivation of smaller cloud droplets, which is due to the combination of curvature and solute effects in the downdraft region, enhances the growth of larger cloud droplets and thus contributes particles to the larger size end of the CDSD. Droplet reactivation, which occurs in the updraft region, contributes particles to the smaller size end of the CDSD. In addition, we find that growth of the largest cloud droplets strongly depends on the residence time of cloud droplet in the cloud rather than the magnitude of local variability in the supersaturation fluctuation. This is because the environmental saturation ratio is strongly buffered by smaller cloud droplets. Two necessary conditions for this CDSD broadening, which generally occur in the atmosphere, are: (1) droplets form on polydisperse aerosols of varying hygroscopicity and (2) the cloud parcel experiences upwards and downwards motions. Therefore we expect that this mechanism for CDSD broadening is possible in real clouds. Our results also suggest it is important to consider both curvature and solute effects before and after cloud droplet activation in a cloud model. The importance of this mechanism compared with other mechanisms on cloud properties should be investigated through in-situ measurements and 3-D dynamic models.« less

Cloud droplet size distribution broadening during diffusional growth: ripening amplified by deactivation and reactivation

DOE PAGES

Yang, Fan; Kollias, Pavlos; Shaw, Raymond A.; ...

2017-12-06

Cloud droplet size distributions (CDSDs), which are related to cloud albedo and lifetime, are usually broader in warm clouds than predicted from adiabatic parcel calculations. We investigate a mechanism for the CDSD broadening using a Lagrangian bin-microphysics cloud parcel model that considers the condensational growth of cloud droplets formed on polydisperse, sub-micrometer aerosols in an adiabatic cloud parcel that undergoes vertical oscillations, such as those due to cloud circulations or turbulence. Results show that the CDSD can be broadened during condensational growth as a result of Ostwald ripening amplified by droplet deactivation and reactivation, which is consistent with Korolev (1995).more » The relative roles of the solute effect, curvature effect, deactivation and reactivation on CDSD broadening are investigated. Deactivation of smaller cloud droplets, which is due to the combination of curvature and solute effects in the downdraft region, enhances the growth of larger cloud droplets and thus contributes particles to the larger size end of the CDSD. Droplet reactivation, which occurs in the updraft region, contributes particles to the smaller size end of the CDSD. In addition, we find that growth of the largest cloud droplets strongly depends on the residence time of cloud droplet in the cloud rather than the magnitude of local variability in the supersaturation fluctuation. This is because the environmental saturation ratio is strongly buffered by smaller cloud droplets. Two necessary conditions for this CDSD broadening, which generally occur in the atmosphere, are: (1) droplets form on polydisperse aerosols of varying hygroscopicity and (2) the cloud parcel experiences upwards and downwards motions. Therefore we expect that this mechanism for CDSD broadening is possible in real clouds. Our results also suggest it is important to consider both curvature and solute effects before and after cloud droplet activation in a cloud model. The importance of this mechanism compared with other mechanisms on cloud properties should be investigated through in-situ measurements and 3-D dynamic models.« less

Cloud droplet size distribution broadening during diffusional growth: ripening amplified by deactivation and reactivation

NASA Astrophysics Data System (ADS)

Yang, Fan; Kollias, Pavlos; Shaw, Raymond A.; Vogelmann, Andrew M.

2018-05-01

Cloud droplet size distributions (CDSDs), which are related to cloud albedo and rain formation, are usually broader in warm clouds than predicted from adiabatic parcel calculations. We investigate a mechanism for the CDSD broadening using a moving-size-grid cloud parcel model that considers the condensational growth of cloud droplets formed on polydisperse, submicrometer aerosols in an adiabatic cloud parcel that undergoes vertical oscillations, such as those due to cloud circulations or turbulence. Results show that the CDSD can be broadened during condensational growth as a result of Ostwald ripening amplified by droplet deactivation and reactivation, which is consistent with early work. The relative roles of the solute effect, curvature effect, deactivation and reactivation on CDSD broadening are investigated. Deactivation of smaller cloud droplets, which is due to the combination of curvature and solute effects in the downdraft region, enhances the growth of larger cloud droplets and thus contributes particles to the larger size end of the CDSD. Droplet reactivation, which occurs in the updraft region, contributes particles to the smaller size end of the CDSD. In addition, we find that growth of the largest cloud droplets strongly depends on the residence time of cloud droplet in the cloud rather than the magnitude of local variability in the supersaturation fluctuation. This is because the environmental saturation ratio is strongly buffered by numerous smaller cloud droplets. Two necessary conditions for this CDSD broadening, which generally occur in the atmosphere, are as follows: (1) droplets form on aerosols of different sizes, and (2) the cloud parcel experiences upwards and downwards motions. Therefore we expect that this mechanism for CDSD broadening is possible in real clouds. Our results also suggest it is important to consider both curvature and solute effects before and after cloud droplet activation in a cloud model. The importance of this mechanism compared with other mechanisms on cloud properties should be investigated through in situ measurements and 3-D dynamic models.

Acoustic droplet vaporization is initiated by superharmonic focusing.

PubMed

Shpak, Oleksandr; Verweij, Martin; Vos, Hendrik J; de Jong, Nico; Lohse, Detlef; Versluis, Michel

2014-02-04

Acoustically sensitive emulsion droplets composed of a liquid perfluorocarbon have the potential to be a highly efficient system for local drug delivery, embolotherapy, or for tumor imaging. The physical mechanisms underlying the acoustic activation of these phase-change emulsions into a bubbly dispersion, termed acoustic droplet vaporization, have not been well understood. The droplets have a very high activation threshold; its frequency dependence does not comply with homogeneous nucleation theory and localized nucleation spots have been observed. Here we show that acoustic droplet vaporization is initiated by a combination of two phenomena: highly nonlinear distortion of the acoustic wave before it hits the droplet and focusing of the distorted wave by the droplet itself. At high excitation pressures, nonlinear distortion causes significant superharmonics with wavelengths of the order of the droplet size. These superharmonics strongly contribute to the focusing effect; therefore, the proposed mechanism also explains the observed pressure thresholding effect. Our interpretation is validated with experimental data captured with an ultrahigh-speed camera on the positions of the nucleation spots, where we find excellent agreement with the theoretical prediction. Moreover, the presented mechanism explains the hitherto counterintuitive dependence of the nucleation threshold on the ultrasound frequency. The physical insight allows for the optimization of acoustic droplet vaporization for therapeutic applications, in particular with respect to the acoustic pressures required for activation, thereby minimizing the negative bioeffects associated with the use of high-intensity ultrasound.

Acoustic droplet vaporization is initiated by superharmonic focusing

PubMed Central

Shpak, Oleksandr; Verweij, Martin; Vos, Hendrik J.; de Jong, Nico; Lohse, Detlef; Versluis, Michel

2014-01-01

Acoustically sensitive emulsion droplets composed of a liquid perfluorocarbon have the potential to be a highly efficient system for local drug delivery, embolotherapy, or for tumor imaging. The physical mechanisms underlying the acoustic activation of these phase-change emulsions into a bubbly dispersion, termed acoustic droplet vaporization, have not been well understood. The droplets have a very high activation threshold; its frequency dependence does not comply with homogeneous nucleation theory and localized nucleation spots have been observed. Here we show that acoustic droplet vaporization is initiated by a combination of two phenomena: highly nonlinear distortion of the acoustic wave before it hits the droplet and focusing of the distorted wave by the droplet itself. At high excitation pressures, nonlinear distortion causes significant superharmonics with wavelengths of the order of the droplet size. These superharmonics strongly contribute to the focusing effect; therefore, the proposed mechanism also explains the observed pressure thresholding effect. Our interpretation is validated with experimental data captured with an ultrahigh-speed camera on the positions of the nucleation spots, where we find excellent agreement with the theoretical prediction. Moreover, the presented mechanism explains the hitherto counterintuitive dependence of the nucleation threshold on the ultrasound frequency. The physical insight allows for the optimization of acoustic droplet vaporization for therapeutic applications, in particular with respect to the acoustic pressures required for activation, thereby minimizing the negative bioeffects associated with the use of high-intensity ultrasound. PMID:24449879

Cloud Imagers Offer New Details on Earth's Health

NASA Technical Reports Server (NTRS)

2009-01-01

A stunning red sunset or purple sunrise is an aesthetic treat with a scientific explanation: The colors are a direct result of the absorption or reflectance of solar radiation by atmospheric aerosols, minute particles (either solid or liquid) in the Earth s atmosphere that occur both naturally and because of human activity. At the beginning or end of the day, the Sun s rays travel farther through the atmosphere to reach an observer s eyes and more green and yellow light is scattered, making the Sun appear red. Sunset and sunrise are especially colorful when the concentration of atmospheric particles is high. This ability of aerosols to absorb and reflect sunlight is not just pretty; it also determines the amount of radiation and heat that reaches the Earth s surface, and can profoundly affect climate. In the atmosphere, aerosols are also important as nuclei for the condensation of water droplets and ice crystals. Clouds with fewer aerosols cannot form as many water droplets (called cloud particles), and consequently, do not scatter light well. In this case, more sunlight reaches the Earth s surface. When aerosol levels in clouds are high, however, more nucleation points can form small liquid water droplets. These smaller cloud particles can reflect up to 90 percent of visible radiation to space, keeping the heat from ever reaching Earth s surface. The tendency for these particles to absorb or reflect the Sun s energy - called extinction by astronomers - depends on a number of factors, including chemical composition and the humidity and temperature in the surrounding air; because cloud particles are so small, they are affected quickly by minute changes in the atmosphere. Because of this sensitivity, atmospheric scientists study cloud particles to anticipate patterns and shifts in climate. Until recently, NASA s study of atmospheric aerosols and cloud particles has been focused primarily on satellite images, which, while granting large-scale atmospheric analysis, limited scientists ability to acquire detailed information about individual particles. Now, experiments with specialized equipment can be flown on standard jets, making it possible for researchers to monitor and more accurately anticipate changes in Earth s atmosphere and weather patterns.

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.

Partitioning of ice nucleating particles: Which modes matter?

NASA Astrophysics Data System (ADS)

Hande, Luke; Hoose, Corinna

2017-04-01

Ice particles in clouds have a large impact on cloud lifetime, precipitation amount, and cloud radiative properties through the indirect aerosol effect. Thus, correctly modelling ice formation processes is important for simulations preformed on all spatial and temporal scales. Ice forms on aerosol particles through several different mechanisms, namely deposition nucleation, immersion freezing, and contact freezing. However there is conflicting evidence as to which mode dominates, and the relative importance of the three heterogeneous ice nucleation mechanisms, as well as homogeneous nucleation, remains an open question. The environmental conditions, and hence the cloud type, have a large impact on determining which nucleation mode dominates. In order to understand this, simulations were performed with the COSMO-LES model, utilising state of the art parameterisations to describe the different nucleation mechanisms for several semi-idealised cloud types commonly occurring over central Europe. The cloud types investigated include a semi-idealised, and an idealised convective cloud, an orographic cloud, and a stratiform cloud. Results show that immersion and contact freezing dominate at warmer temperatures, and under most conditions, deposition nucleation plays only a minor role. In clouds where sufficiently high levels of water vapour are present at colder temperatures, deposition nucleation can play a role, however in general homogeneous nucleation dominates at colder temperatures. Since contact nucleation depends on the environmental relative humidity, enhancements in this nucleation mode can be seen in areas of dry air entrainment. The results indicate that ice microphysical processes are somewhat sensitve to the environmental conditions and therefore the cloud type.

Stable water isotopologue ratios in fog and cloud droplets of liquid clouds are not size-dependent

USGS Publications Warehouse

Spiegel, J.K.; Aemisegger, F.; Scholl, M.; Wienhold, F.G.; Collett, J.L.; Lee, T.; van Pinxteren, D.; Mertes, S.; Tilgner, A.; Herrmann, H.; Werner, Roland A.; Buchmann, N.; Eugster, W.

2012-01-01

In this work, we present the first observations of stable water isotopologue ratios in cloud droplets of different sizes collected simultaneously. We address the question whether the isotope ratio of droplets in a liquid cloud varies as a function of droplet size. Samples were collected from a ground intercepted cloud (= fog) during the Hill Cap Cloud Thuringia 2010 campaign (HCCT-2010) using a three-stage Caltech Active Strand Cloud water Collector (CASCC). An instrument test revealed that no artificial isotopic fractionation occurs during sample collection with the CASCC. Furthermore, we could experimentally confirm the hypothesis that the δ values of cloud droplets of the relevant droplet sizes (μm-range) were not significantly different and thus can be assumed to be in isotopic equilibrium immediately with the surrounding water vapor. However, during the dissolution period of the cloud, when the supersaturation inside the cloud decreased and the cloud began to clear, differences in isotope ratios of the different droplet sizes tended to be larger. This is likely to result from the cloud's heterogeneity, implying that larger and smaller cloud droplets have been collected at different moments in time, delivering isotope ratios from different collection times.

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)

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.

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.

Hierarchical Superhydrophobic Surfaces with Micropatterned Nanowire Arrays for High-Efficiency Jumping Droplet Condensation.

PubMed

Wen, Rongfu; Xu, Shanshan; Zhao, Dongliang; Lee, Yung-Cheng; Ma, Xuehu; Yang, Ronggui

2017-12-27

Self-propelled droplet jumping on nanostructured superhydrophobic surfaces is of interest for a variety of industrial applications including self-cleaning, water harvesting, power generation, and thermal management systems. However, the uncontrolled nucleation-induced Wenzel state of condensed droplets at large surface subcooling (high heat flux) leads to the formation of unwanted large pinned droplets, which results in the flooding phenomenon and greatly degrades the heat transfer performance. In this work, we present a novel strategy to manipulate droplet behaviors during the process from the droplet nucleation to growth and departure through a combination of spatially controlling initial nucleation for mobile droplets by closely spaced nanowires and promoting the spontaneous outward movement of droplets for rapid removal using micropatterned nanowire arrays. Through the optical visualization experiments and heat transfer tests, we demonstrate greatly improved condensation heat transfer characteristics on the hierarchical superhydrophobic surface including the higher density of microdroplets, smaller droplet departure radius, 133% wider range of surface subcooling for droplet jumping, and 37% enhancement in critical heat flux for jumping droplet condensation, compared to the-state-of-art jumping droplet condensation on nanostructured superhydrophobic surfaces. The excellent water repellency of such hierarchical superhydrophobic surfaces can be promising for many potential applications, such as anti-icing, antifogging, water desalination, and phase-change heat transfer.

Hierarchical Superhydrophobic Surfaces with Micropatterned Nanowire Arrays for High-Efficiency Jumping Droplet Condensation

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

Wen, Rongfu; Xu, Shanshan; Zhao, Dongliang

Self-propelled droplet jumping on nanostructured superhydrophobic surfaces is of interest for a variety of industrial applications including self-cleaning, water harvesting, power generation, and thermal management systems. However, the uncontrolled nucleation-induced Wenzel state of condensed droplets at large surface subcooling (high heat flux) leads to the formation of unwanted large pinned droplets, which results in the flooding phenomenon and greatly degrades the heat transfer performance. In this work, we present a novel strategy to manipulate droplet behaviors during the process from the droplet nucleation to growth and departure through a combination of spatially controlling initial nucleation for mobile droplets by closelymore » spaced nanowires and promoting the spontaneous outward movement of droplets for rapid removal using micropatterned nanowire arrays. Through the optical visualization experiments and heat transfer tests, we demonstrate greatly improved condensation heat transfer characteristics on the hierarchical superhydrophobic surface including the higher density of microdroplets, smaller droplet departure radius, 133% wider range of surface subcooling for droplet jumping, and 37% enhancement in critical heat flux for jumping droplet condensation, compared to the-state-of-art jumping droplet condensation on nanostructured superhydrophobic surfaces. The excellent water repellency of such hierarchical superhydrophobic surfaces can be promising for many potential applications, such as anti-icing, antifogging, water desalination, and phase-change heat transfer.« less

Hierarchical Superhydrophobic Surfaces with Micropatterned Nanowire Arrays for High-Efficiency Jumping Droplet Condensation

DOE PAGES

Wen, Rongfu; Xu, Shanshan; Zhao, Dongliang; ...

2017-12-07

Self-propelled droplet jumping on nanostructured superhydrophobic surfaces is of interest for a variety of industrial applications including self-cleaning, water harvesting, power generation, and thermal management systems. However, the uncontrolled nucleation-induced Wenzel state of condensed droplets at large surface subcooling (high heat flux) leads to the formation of unwanted large pinned droplets, which results in the flooding phenomenon and greatly degrades the heat transfer performance. In this work, we present a novel strategy to manipulate droplet behaviors during the process from the droplet nucleation to growth and departure through a combination of spatially controlling initial nucleation for mobile droplets by closelymore » spaced nanowires and promoting the spontaneous outward movement of droplets for rapid removal using micropatterned nanowire arrays. Through the optical visualization experiments and heat transfer tests, we demonstrate greatly improved condensation heat transfer characteristics on the hierarchical superhydrophobic surface including the higher density of microdroplets, smaller droplet departure radius, 133% wider range of surface subcooling for droplet jumping, and 37% enhancement in critical heat flux for jumping droplet condensation, compared to the-state-of-art jumping droplet condensation on nanostructured superhydrophobic surfaces. The excellent water repellency of such hierarchical superhydrophobic surfaces can be promising for many potential applications, such as anti-icing, antifogging, water desalination, and phase-change heat transfer.« less

Phase Transformation of Droplets into Particles and Nucleation in Atmospheric Pressure Discharges

NASA Astrophysics Data System (ADS)

Iqbal, M. M.; Stallard, C. P.; Dowling, D. P.; Turner, M. M.

2013-09-01

We investigate the mechanism of phase transformation of liquid precursor droplets into nano-particulates in an atmospheric pressure discharge (APD). This phase transformation is possible when the solid to a liquid mass ratio of slurry droplet reaches a threshold value. The behaviour of phase transformation of a single slurry droplet of HMDSO is described by developing a numerical model under the saturation condition of evaporation. It is observed from the temporal evolution of inner radius (Ri) of a single slurry droplet that its value approaches zero before the entire shifting of a liquid phase and which explains with an expansion in the crust thickness (Ro - Ri) . The solid traces of nano-particles are observed experimentally on the surface coating depositions because the time for transferring the slurry droplet of HMDSO into solid state is amplified with an increment in the radii of droplets and the entire phase transition occurs within residence time for the nano-sized liquid droplets. The GDE coupled with discharge plasma is numerically solved to describe the mechanism of nucleation of nano-sized particles in APD plasma under similar conditions of the experiment. The growth of nucleation in APD plasma depends on the type of liquid precursor, such as HMDSO, TEOS and water, which is verified with a sharp peak in the nucleation rate and saturation ratio. Science Foundation Ireland under Grant No. 08/SRC/I1411.

Preferential nucleation, guiding, and blocking of self-propelled droplets by dislocations

NASA Astrophysics Data System (ADS)

Kanjanachuchai, Songphol; Wongpinij, Thipusa; Kijamnajsuk, Suphakan; Himwas, Chalermchai; Panyakeow, Somsak; Photongkam, Pat

2018-04-01

Lattice-mismatched layers of GaAs/InGaAs are grown on GaAs(001) using molecular beam epitaxy and subsequently heated in vacuum while the surface is imaged in situ using low-energy electron microscopy, in order to study (i) the nucleation of group-III droplets formed as a result of noncongruent sublimation and (ii) the dynamics of these self-propelled droplets as they navigate the surface. It is found that the interfacial misfit dislocation network not only influences the nucleation sites of droplets, but also exerts unusual steering power over their subsequent motion. Atypical droplet flow patterns including 90° and 180° turns are found. The directions of these dislocations-guided droplets are qualitatively explained in terms of in-plane and out-of-plane stress fields associated with the buried dislocations and the driving forces due to chemical potential and stress gradients typical of Marangoni flow. The findings would benefit processes and devices that employ droplets as catalysts or active structures such as droplet epitaxy of quantum nanostructures, vapor-liquid-solid growth of nanowires, or the fabrication of self-integrated circuits.

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.

Characterization of individual ice residual particles by the single droplet freezing method: a case study in the Asian dust outflow region

NASA Astrophysics Data System (ADS)

Iwata, Ayumi; Matsuki, Atsushi

2018-02-01

In order to better characterize ice nucleating (IN) aerosol particles in the atmosphere, we investigated the chemical composition, mixing state, and morphology of atmospheric aerosols that nucleate ice under conditions relevant for mixed-phase clouds. Five standard mineral dust samples (quartz, K-feldspar, Na-feldspar, Arizona test dust, and Asian dust source particles) were compared with actual aerosol particles collected from the west coast of Japan (the city of Kanazawa) during Asian dust events in February and April 2016. Following droplet activation by particles deposited on a hydrophobic Si (silicon) wafer substrate under supersaturated air, individual IN particles were located using an optical microscope by gradually cooling the temperature to -30 °C. For the aerosol samples, both the IN active particles and non-active particles were analyzed individually by atomic force microscopy (AFM), micro-Raman spectroscopy, and scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDX). Heterogeneous ice nucleation in all standard mineral dust samples tested in this study was observed at consistently higher temperatures (e.g., -22.2 to -24.2 °C with K-feldspar) than the homogeneous freezing temperature (-36.5 °C). Meanwhile, most of the IN active atmospheric particles formed ice below -28 °C, i.e., at lower temperatures than the standard mineral dust samples of pure components. The most abundant IN active particles above -30 °C were predominantly irregular solid particles that showed clay mineral characteristics (or mixtures of several mineral components). Other than clay, Ca-rich particles internally mixed with other components, such as sulfate, were also regarded as IN active particle types. Moreover, sea salt particles were predominantly found in the non-active fraction, and internal mixing with sea salt clearly acted as a significant inhibiting agent for the ice nucleation activity of mineral dust particles. Also, relatively pure or fresh calcite, Ca(NO3)2, and (NH4)2SO4 particles were more often found in the non-active fraction. In this study, we demonstrated the capability of the combined single droplet freezing method and thorough individual particle analysis to characterize the ice nucleation activity of atmospheric aerosols. We also found that dramatic changes in the particle mixing states during long-range transport had a complex effect on the ice nucleation activity of the host aerosol particles. A case study in the Asian dust outflow region highlighted the need to consider particle mixing states, which can dramatically influence ice nucleation activity.

The relationships among cloud microphysics, chemistry, and precipitation rate in cold mountain clouds

NASA Astrophysics Data System (ADS)

Borys, Randolph D.; Lowenthal, Douglas H.; Mitchell, David L.

A study was conducted to examine the relationships among air pollutant loadings, cloud microphysics, and snowfall rates in cold mountain clouds. It was hypothesized that variations in pollutant loadings would be reflected in shifts in the cloud droplet size distribution. A field program was conducted at Storm Peak Laboratory (SPL) at an elevation of 3210 m MSL in northwestern Colorado. Cold precipitating clouds were sampled during January, 1995. Cloud water was collected and analyzed for major ion and trace element chemistry. Cloud droplet concentrations and size were measured continuously using a PMS FSSP-100. The results indicate a direct relationship between clear-air equivalent (CAE) sulfate concentrations in cloud water and cloud droplet concentrations, an indirect relationship between droplet number and droplet size, a direct relationship between droplet size and snowfall rate, and an indirect relationship between CAE sulfate concentration and snowfall rate.

Fractal Analyses of High-Resolution Cloud Droplet Measurements.

NASA Astrophysics Data System (ADS)

Malinowski, Szymon P.; Leclerc, Monique Y.; Baumgardner, Darrel G.

1994-02-01

Fractal analyses of individual cloud droplet distributions using aircraft measurements along one-dimensional horizontal cross sections through clouds are performed. Box counting and cluster analyses are used to determine spatial scales of inhomogeneity of cloud droplet spacing. These analyses reveal that droplet spatial distributions do not exhibit a fractal behavior. A high variability in local droplet concentration in cloud volumes undergoing mixing was found. In these regions, thin filaments of cloudy air with droplet concentration close to those observed in cloud cores were found. Results suggest that these filaments may be anisotropic. Additional box counting analyses performed for various classes of cloud droplet diameters indicate that large and small droplets are similarly distributed, except for the larger characteristic spacing of large droplets.A cloud-clear air interface defined by a certain threshold of total droplet count (TDC) was investigated. There are indications that this interface is a convoluted surface of a fractal nature, at least in actively developing cumuliform clouds. In contrast, TDC in the cloud interior does not have fractal or multifractal properties. Finally a random Cantor set (RCS) was introduced as a model of a fractal process with an ill-defined internal scale. A uniform measure associated with the RCS after several generations was introduced to simulate the TDC records. Comparison of the model with real TDC records indicates similar properties of both types of data series.

Charge Effects on the Efflorescence in Single Levitated Droplets.

PubMed

Hermann, Gunter; Zhang, Yan; Wassermann, Bernhard; Fischer, Henry; Quennet, Marcel; Rühl, Eckart

2017-09-14

The influence of electrical excess charges on the crystallization from supersaturated aqueous sodium chloride solutions is reported. This is accomplished by efflorescence studies on single levitated microdroplets using optical and electrodynamic levitation. Specifically, a strong increase in efflorescence humidity is observed as a function of the droplet's negative excess charge, ranging up to -2.1 pC, with a distinct threshold behavior, increasing the relative efflorescence humidity, at which spontaneous nucleation occurs, from 44% for the neutral microparticle to 60%. These findings are interpreted by using molecular dynamics simulations for determining plausible structural patterns located near the particle surface that could serve as suitable precursors for the formation of critical clusters overcoming the nucleation barrier. These results, facilitating heterogeneous nucleation in the case of negatively charged microparticles, are compared to recent work on charge-induced nucleation of neat supercooled water, where a distinctly different nucleation behavior as a function of droplet charge has been observed.

Hydrophilic directional slippery rough surfaces for water harvesting

PubMed Central

Sun, Nan; Nielsen, Steven O.; Wang, Jing

2018-01-01

Multifunctional surfaces that are favorable for both droplet nucleation and removal are highly desirable for water harvesting applications but are rare. Inspired by the unique functions of pitcher plants and rice leaves, we present a hydrophilic directional slippery rough surface (SRS) that is capable of rapidly nucleating and removing water droplets. Our surfaces consist of nanotextured directional microgrooves in which the nanotextures alone are infused with hydrophilic liquid lubricant. We have shown through molecular dynamics simulations that the physical origin of the efficient droplet nucleation is attributed to the hydrophilic surface functional groups, whereas the rapid droplet removal is due to the significantly reduced droplet pinning of the directional surface structures and slippery interface. We have further demonstrated that the SRS, owing to its large surface area, hydrophilic slippery interface, and directional liquid repellency, outperforms conventional liquid-repellent surfaces in water harvesting applications. PMID:29670942

Effect of supersaturation on L-glutamic acid polymorphs under droplet-based microchannels

NASA Astrophysics Data System (ADS)

Jiang, Nan; Wang, Zhanzhong; Dang, Leping; Wei, Hongyuan

2016-07-01

Supersaturation is an important controlling factor for crystallization process and polymorphism. Droplet-based microchannels and conventional crystallization were used to investigate polymorphs of L-gluatamic acid in this work. The results illustrate that it is easy to realize the accurate and rapid control of the crystallization temperature in the droplets, which is especially beneficial to heat and mass transfer during crystallization. It is also noted that higher degree of supersaturation favors the nucleation of α crystal form, while lower degree of supersaturation favors the nucleation of β crystal form under droplet-based microchannels for L-gluatamic acid. In addition, there is a different nucleation behavior to be found under droplet-based microchannels both for the β form and α form of L-glutamic acid. This new finding can provide important insight into the development and design of investigation meanings for drug polymorph.

Growth and melting of droplets in cold vapors.

PubMed

L'Hermite, Jean-Marc

2009-11-01

A model has been developed to investigate the growth of droplets in a supersaturated cold vapor taking into account their possible solid-liquid phase transition. It is shown that the solid-liquid phase transition is nontrivially coupled, through the energy released in attachment, to the nucleation process. The model is based on the one developed by J. Feder, K. C. Russell, J. Lothe, and G. M. Pound [Adv. Phys. 15, 111 (1966)], where the nucleation process is described as a thermal diffusion motion in a two-dimensional field of force given by the derivatives of a free-energy surface. The additional dimension accounts for droplets internal energy. The solid-liquid phase transition is introduced through a bimodal internal energy distribution in a Gaussian approximation derived from small clusters physics. The coupling between nucleation and melting results in specific nonequilibrium thermodynamical properties, exemplified in the case of water droplets. Analyzing the free-energy landscapes gives an insight into the nucleation dynamics. This landscape can be complex but generally exhibits two paths: the first one can generally be ascribed to the solid state, while the other to the liquid state. Especially at high supersaturation, the growth in the liquid state is often favored, which is not unexpected since in a supersaturated vapor the droplets can stand higher internal energy than at equilibrium. From a given critical temperature that is noticeably lower than the bulk melting temperature, nucleation may end in very large liquid droplets. These features can be qualitatively generalized to systems other than water.

Do Cloud Properties in a Puerto Rican Tropical Montane Cloud Forest Depend on Occurrence of Long-Range Transported African Dust?

NASA Astrophysics Data System (ADS)

Spiegel, Johanna K.; Buchmann, Nina; Mayol-Bracero, Olga L.; Cuadra-Rodriguez, Luis A.; Valle Díaz, Carlos J.; Prather, Kimberly A.; Mertes, Stephan; Eugster, Werner

2014-09-01

We investigated cloud properties of warm clouds in a tropical montane cloud forest at Pico del Este (1,051 m a.s.l.) in the northeastern part of Puerto Rico to address the question of whether cloud properties in the Caribbean could potentially be affected by African dust transported across the Atlantic Ocean. We analyzed data collected during 12 days in July 2011. Cloud droplet size spectra were measured using the FM-100 fog droplet spectrometer that measured droplet size distributions in the range from 2 to 49 µm, primarily during fog events. The droplet size spectra revealed a bimodal structure, with the first peak ( D < 6 µm) being more pronounced in terms of droplet number concentrations, whereas the second peak (10 µm < D < 20 µm) was found to be the one relevant for total liquid water content (LWC) of the cloud. We identified three major clusters of characteristic droplet size spectra by means of hierarchical clustering. All clusters differed significantly from each other in droplet number concentration (), effective diameter (ED), and median volume diameter (MVD). For the cluster comprising the largest droplets and the lowest droplet number concentrations, we found evidence of inhomogeneous mixing in the cloud. Contrastingly, the other two clusters revealed microphysical behavior, which could be expected under homogeneous mixing conditions. For those conditions, an increase in cloud condensation nuclei—e.g., from processed African dust transported to the site—is supposed to lead to an increased droplet concentration. In fact, one of these two clusters showed a clear shift of cloud droplet size spectra towards smaller droplet diameters. Since this cluster occurred during periods with strong evidence for the presence of long-range transported African dust, we hypothesize a link between the observed dust episodes and cloud characteristics in the Caribbean at our site, which is similar to the anthropogenic aerosol indirect effect.

Theory of droplet. Part 1: Renormalized laws of droplet vaporization in non-dilute sprays

NASA Technical Reports Server (NTRS)

Chiu, H. H.

1989-01-01

The vaporization of a droplet, interacting with its neighbors in a non-dilute spray environment is examined as well as a vaporization scaling law established on the basis of a recently developed theory of renormalized droplet. The interacting droplet consists of a centrally located droplet and its vapor bubble which is surrounded by a cloud of droplets. The distribution of the droplets and the size of the cloud are characterized by a pair-distribution function. The vaporization of a droplet is retarded by the collective thermal quenching, the vapor concentration accumulated in the outer sphere, and by the limited percolative passages for mass, momentum and energy fluxes. The retardation is scaled by the local collective interaction parameters (group combustion number of renormalized droplet, droplet spacing, renormalization number and local ambient conditions). The numerical results of a selected case study reveal that the vaporization correction factor falls from unity monotonically as the group combustion number increases, and saturation is likely to occur when the group combustion number reaches 35 to 40 with interdroplet spacing of 7.5 diameters and an environment temperature of 500 K. The scaling law suggests that dense sprays can be classified into: (1) a diffusively dense cloud characterized by uniform thermal quenching in the cloud; (2) a stratified dense cloud characterized by a radial stratification in temperature by the differential thermal quenching of the cloud; or (3) a sharply dense cloud marked by fine structure in the quasi-droplet cloud and the corresponding variation in the correction factor due to the variation in the topological structure of the cloud characterized by a pair-distribution function of quasi-droplets.

Dispersion of Droplet Clouds in Turbulence.

PubMed

Bocanegra Evans, Humberto; Dam, Nico; Bertens, Guus; van der Voort, Dennis; van de Water, Willem

2016-10-14

We measure the absolute dispersion of clouds of monodisperse, phosphorescent droplets in turbulent air by means of high-speed image-intensified video recordings. Laser excitation allows the initial preparation of well-defined, pencil-shaped luminous droplet clouds in a completely nonintrusive way. We find that the dispersion of the clouds is faster than the dispersion of fluid elements. We speculate that preferential concentration of inertial droplet clouds is responsible for the enhanced dispersion.

Global Survey of the Relationship Between Cloud Droplet Size and Albedo Using ISCCP

NASA Technical Reports Server (NTRS)

Han, Qingyuan; Rossow, William B.; Chou, Joyce; Welch, Ronald M.

1997-01-01

Aerosols affect climate through direct and indirect effects. The direct effect of aerosols (e.g., sulfates) includes reflection of sunlight back toward space and for some aerosols (e.g., smoke particles), absorption in the atmosphere; both effects cool the Earth's surface. The indirect effect of aerosols refers to the modification of cloud microphysical properties, thereby affecting the radiation balance. Higher concentrations of Cloud Condensation Nuclei (CCN) generally produce higher concentrations of cloud droplets, which are also usually assumed to lead to decreased cloud droplet sizes. The result is an increase in cloud albedo, producing a net radiative cooling, opposite to the warming caused by greenhouse gases (Charlson et al. 1992). The change in clouds that is directly induced by an increase of aerosol concentration is an increase of cloud droplet number density, N; but is is usually assumed that cloud droplet size decreases as if the water mass density Liquid Water Content (LWC) were constant. There is actually no reason why this should be the case. Shifting the cloud droplet size distribution to more numerous smaller droplets can change the relative rates of condensational and coalescence growth, leading to different LWC (e.g., Rossow 1978). Moreover, the resulting change in cloud albedo is usually ascribed to more efficient scattering by smaller droplets, when in fact it is the increase in droplet number density (assuming constant LWC) that produces the most important change in cloud albedo: e.g., holding N constant and decreasing the droplet size would actually decrease the scattering cross-section and, thus, the albedo much more than it is increased by the increased scattering efficiency.

Satellite Remote Sensing of the Liquid Water Sensitivity in Water Clouds

NASA Technical Reports Server (NTRS)

Han, Qing-Yuan; Rossow, William B.; Welch, Ronald; Zeng, Jane; Jansen, James E. (Technical Monitor)

2001-01-01

In estimation of the aerosol indirect effect, cloud liquid water path is considered either constant (Twomey effect) or increasing with enhanced droplet number concentrations (drizzle-suppression effect, or Albrecht effect) if cloud microphysics is the prevailing mechanism during the aerosol-cloud interactions. On the other hand, if cloud thermodynamics and dynamics are considered, the cloud liquid water path may be decreased with increasing droplet number concentration, which is predicted by model calculations and observed in ship-track and urban influence studies. This study is to examine the different responses of cloud liquid water path to changes of cloud droplet number concentration. Satellite data (January, April, July and October 1987) are used to retrieve the cloud liquid water sensitivity, defined as the changes of liquid water path versus changes of column droplet number concentrations. The results of a global survey reveal that 1) in at least one third of the cases the cloud liquid water sensitivity is negative, and the regional and seasonal variations of the negative liquid water sensitivity are consistent with other observations; 2) cloud droplet sizes are always inversely proportional to column droplet number concentrations. Our results suggest that an increase of cloud droplet number concentration leads to reduced cloud droplet size and enhanced evaporation, which weakens the coupling between water clouds and boundary layer in warm zones, decreases water supply from surface and desiccates cloud liquid water. Our results also suggest that the current evaluations of negative aerosol indirect forcing by global climate models (GCM), which are based on Twomey effect or Albrecht effect, may be overestimated.

Thermodynamics and kinetics of binary nucleation in ideal-gas mixtures.

PubMed

Alekseechkin, Nikolay V

2015-08-07

The nonisothermal single-component theory of droplet nucleation [N. V. Alekseechkin, Physica A 412, 186 (2014)] is extended to binary case; the droplet volume V, composition x, and temperature T are the variables of the theory. An approach based on macroscopic kinetics (in contrast to the standard microscopic model of nucleation operating with the probabilities of monomer attachment and detachment) is developed for the droplet evolution and results in the derived droplet motion equations in the space (V, x, T)—equations for V̇≡dV/dt, ẋ, and Ṫ. The work W(V, x, T) of the droplet formation is obtained in the vicinity of the saddle point as a quadratic form with diagonal matrix. Also, the problem of generalizing the single-component Kelvin equation for the equilibrium vapor pressure to binary case is solved; it is presented here as a problem of integrability of a Pfaffian equation. The equation for Ṫ is shown to be the first law of thermodynamics for the droplet, which is a consequence of Onsager's reciprocal relations and the linked-fluxes concept. As an example of ideal solution for demonstrative numerical calculations, the o-xylene-m-xylene system is employed. Both nonisothermal and enrichment effects are shown to exist; the mean steady-state overheat of droplets and their mean steady-state enrichment are calculated with the help of the 3D distribution function. Some qualitative peculiarities of the nucleation thermodynamics and kinetics in the water-sulfuric acid system are considered in the model of regular solution. It is shown that there is a small kinetic parameter in the theory due to the small amount of the acid in the vapor and, as a consequence, the nucleation process is isothermal.

Cloud Coverage Enhancement and Nocturnal Drizzle Suppression in Stratocumulus by Aerosols

NASA Technical Reports Server (NTRS)

Ackerman, Andrew S.; Toon, Owen B.; Stevens, David E.; Coakley, James A., Jr.; Gore, Warren J. (Technical Monitor)

2002-01-01

Recent satellite observations of ship tracks surprisingly indicate that cloud water decreases with increasing droplet concentrations. However, we find by analyzing detailed simulations of stratocumulus that the reported trend is likely an artifact of sampling, only overcast clouds. The simulations instead show cloud coverage increasing with droplet concentrations, accounting for 25% of cloud albedo increase at moderate droplet concentrations. Our simulations also show that increases in cloud water from drizzle suppression (by increasing droplet concentrations) are favored only at night or at extremely low droplet concentrations, suggesting that the indirect aerosol forcing is overestimated in climate change projections by many general circulation models.

Lagrangian condensation microphysics with Twomey CCN activation

NASA Astrophysics Data System (ADS)

Grabowski, Wojciech W.; Dziekan, Piotr; Pawlowska, Hanna

2018-01-01

We report the development of a novel Lagrangian microphysics methodology for simulations of warm ice-free clouds. The approach applies the traditional Eulerian method for the momentum and continuous thermodynamic fields such as the temperature and water vapor mixing ratio, and uses Lagrangian super-droplets to represent condensed phase such as cloud droplets and drizzle or rain drops. In other applications of the Lagrangian warm-rain microphysics, the super-droplets outside clouds represent unactivated cloud condensation nuclei (CCN) that become activated upon entering a cloud and can further grow through diffusional and collisional processes. The original methodology allows for the detailed study of not only effects of CCN on cloud microphysics and dynamics, but also CCN processing by a cloud. However, when cloud processing is not of interest, a simpler and computationally more efficient approach can be used with super-droplets forming only when CCN is activated and no super-droplet existing outside a cloud. This is possible by applying the Twomey activation scheme where the local supersaturation dictates the concentration of cloud droplets that need to be present inside a cloudy volume, as typically used in Eulerian bin microphysics schemes. Since a cloud volume is a small fraction of the computational domain volume, the Twomey super-droplets provide significant computational advantage when compared to the original super-droplet methodology. Additional advantage comes from significantly longer time steps that can be used when modeling of CCN deliquescence is avoided. Moreover, other formulation of the droplet activation can be applied in case of low vertical resolution of the host model, for instance, linking the concentration of activated cloud droplets to the local updraft speed. This paper discusses the development and testing of the Twomey super-droplet methodology, focusing on the activation and diffusional growth. Details of the activation implementation, transport of super-droplets in the physical space, and the coupling between super-droplets and the Eulerian temperature and water vapor field are discussed in detail. Some of these are relevant to the original super-droplet methodology as well and to the ice phase modeling using the Lagrangian approach. As a computational example, the scheme is applied to an idealized moist thermal rising in a stratified environment, with the original super-droplet methodology providing a benchmark to which the new scheme is compared.

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.

Sea spray aerosol as a unique source of ice nucleating particles

DOE PAGES

DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.; ...

2016-05-24

Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. In addition, data in the present study are also in accord with previously published INPmore » measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0°C, averaging an order of magnitude increase per 5°C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using “dry” geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. Lastly, these findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean.« less

Sea spray aerosol as a unique source of ice nucleating particles.

PubMed

DeMott, Paul J; Hill, Thomas C J; McCluskey, Christina S; Prather, Kimberly A; Collins, Douglas B; Sullivan, Ryan C; Ruppel, Matthew J; Mason, Ryan H; Irish, Victoria E; Lee, Taehyoung; Hwang, Chung Yeon; Rhee, Tae Siek; Snider, Jefferson R; McMeeking, Gavin R; Dhaniyala, Suresh; Lewis, Ernie R; Wentzell, Jeremy J B; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M; Ault, Andrew P; Axson, Jessica L; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M Dale; Deane, Grant B; Mayol-Bracero, Olga L; Grassian, Vicki H; Bertram, Timothy H; Bertram, Allan K; Moffett, Bruce F; Franc, Gary D

2016-05-24

Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using "dry" geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean.

Sea spray aerosol as a unique source of ice nucleating particles

PubMed Central

DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.; Prather, Kimberly A.; Ruppel, Matthew J.; Mason, Ryan H.; Irish, Victoria E.; Lee, Taehyoung; Hwang, Chung Yeon; Snider, Jefferson R.; McMeeking, Gavin R.; Dhaniyala, Suresh; Lewis, Ernie R.; Wentzell, Jeremy J. B.; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M.; Ault, Andrew P.; Axson, Jessica L.; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M. Dale; Deane, Grant B.; Mayol-Bracero, Olga L.; Grassian, Vicki H.; Bertram, Timothy H.; Bertram, Allan K.; Moffett, Bruce F.; Franc, Gary D.

2016-01-01

Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using “dry” geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean. PMID:26699469

Comparison of mineral dust and droplet residuals measured with two single particle aerosol mass spectrometers

NASA Astrophysics Data System (ADS)

Wonaschütz, Anna; Ludwig, Wolfgang; Zawadowicz, Maria; Hiranuma, Naruki; Hitzenberger, Regina; Cziczo, Daniel; DeMott, Paul; Möhler, Ottmar

2017-04-01

Single Particle mass spectrometers are used to gain information on the chemical composition of individual aerosol particles, aerosol mixing state, and other valuable aerosol characteristics. During the Mass Spectrometry Intercomparison at the Fifth Ice Nucleation (FIN-01) Workshop, the new LAAPTOF single particle aerosol mass spectrometer (AeroMegt GmbH) was conducting simultaneous measurements together with the PALMS (Particle Analysis by Laser Mass Spectrometry) instrument. The aerosol particles were sampled from the AIDA chamber during ice cloud expansion experiments. Samples of mineral dust and ice droplet residuals were measured simultaneously. In this work, three expansion experiments are chosen for a comparison between the two mass spectrometers. A fuzzy clustering routine is used to group the spectra. Cluster centers describing the ensemble of particles are compared. First results show that while differences in the peak heights are likely due to the use of an amplifier in PALMS, cluster centers are comparable.

Direct Observation of Zhang-Li Torque Expansion of Magnetic Droplet Solitons

NASA Astrophysics Data System (ADS)

Chung, Sunjae; Le, Q. Tuan; Ahlberg, Martina; Awad, Ahmad A.; Weigand, Markus; Bykova, Iuliia; Khymyn, Roman; Dvornik, Mykola; Mazraati, Hamid; Houshang, Afshin; Jiang, Sheng; Nguyen, T. N. Anh; Goering, Eberhard; Schütz, Gisela; Gräfe, Joachim; Åkerman, Johan

2018-05-01

Magnetic droplets are nontopological dynamical solitons that can be nucleated in nanocontact based spin torque nano-oscillators (STNOs) with perpendicular magnetic anisotropy free layers. While theory predicts that the droplet should be of the same size as the nanocontact, its inherent drift instability has thwarted attempts at observing it directly using microscopy techniques. Here, we demonstrate highly stable magnetic droplets in all-perpendicular STNOs and present the first detailed droplet images using scanning transmission X-ray microscopy. In contrast to theoretical predictions, we find that the droplet diameter is about twice as large as the nanocontact. By extending the original droplet theory to properly account for the lateral current spread underneath the nanocontact, we show that the large discrepancy primarily arises from current-in-plane Zhang-Li torque adding an outward pressure on the droplet perimeter. Electrical measurements on droplets nucleated using a reversed current in the antiparallel state corroborate this picture.

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.

The SPectrometer for Ice Nuclei (SPIN): An instrument to investigate ice nucleation

DOE PAGES

Garimella, Sarvesh; Kristensen, Thomas Bjerring; Ignatius, Karolina; ...

2016-07-06

The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nucleating particle (INP) counter manufactured by Droplet Measurement Technologies in Boulder, CO. The SPIN is a continuous flow diffusion chamber with parallel plate geometry based on the Zurich Ice Nucleation Chamber and the Portable Ice Nucleation Chamber. This study presents a standard description for using the SPIN instrument and also highlights methods to analyze measurements in more advanced ways. It characterizes and describes the behavior of the SPIN chamber, reports data from laboratory measurements, and quantifies uncertainties associated with the measurements. Experiments with ammonium sulfate are used to investigatemore » homogeneous freezing of deliquesced haze droplets and droplet breakthrough. Experiments with kaolinite, NX illite, and silver iodide are used to investigate heterogeneous ice nucleation. SPIN nucleation results are compared to those from the literature. A machine learning approach for analyzing depolarization data from the SPIN optical particle counter is also presented (as an advanced use). Altogether, we report that the SPIN is able to reproduce previous INP counter measurements.« less

Entrainment, Drizzle, and the Indirect Effect in Stratiform Clouds

NASA Technical Reports Server (NTRS)

Ackerman, Andrew

2005-01-01

Activation of some fraction of increased concentrations of sub-micron soluble aerosol particles lead to enhanced cloud droplet concentrations and hence smaller droplets, increasing their total cross sectional area and thus reflecting solar radiation more efficiently (the Twomey, or first indirect, effect). However, because of competition during condensational growth, droplet distributions tend to broaden as numbers increase, reducing the sensitivity of cloud albedo to droplet concentration on the order of 10%. Also, smaller droplets less effectively produce drizzle through collisions and coalescence, and it is widely expected (and found in large-scale models) that decreased precipitation leads to clouds with more cloud water on average (the so-called cloud lifetime, or second indirect, effect). Much of the uncertainty regarding the overall indirect aerosol effect stems from inadequate understanding of such changes in cloud water. Detailed simulations based on FIRE-I, ASTEX, and DYCOMS-II conditions show that suppression of precipitation from increased droplet concentrations leads to increased cloud water only when sufficient precipitation reaches the surface, a condition favored when the overlying air is-humid or droplet concentrations are very low. Otherwise, aerosol induced suppression of precipitation enhances entrainment of overlying dry air, thereby reducing cloud water and diminishing the indirect climate forcing.

Ice nucleation on nanotextured surfaces: the influence of surface fraction, pillar height and wetting states.

PubMed

Metya, Atanu K; Singh, Jayant K; Müller-Plathe, Florian

2016-09-29

In this work, we address the nucleation behavior of a supercooled monatomic cylindrical water droplet on nanoscale textured surfaces using molecular dynamics simulations. The ice nucleation rate at 203 K on graphite based textured surfaces with nanoscale roughness is evaluated using the mean fast-passage time method. The simulation results show that the nucleation rate depends on the surface fraction as well as the wetting states. The nucleation rate enhances with increasing surface fraction for water in the Cassie-Baxter state, while contrary behavior is observed for the case of Wenzel state. Based on the spatial histogram distribution of ice formation, we observed two pathways for ice nucleation. Heterogeneous nucleation is observed at a high surface fraction. However, the probability of homogeneous ice nucleation events increases with decreasing surface fraction. We further investigate the role of the nanopillar height in ice nucleation. The nucleation rate is enhanced with increasing nanopillar height. This is attributed to the enhanced contact area with increasing nanopillar height and the shift in nucleation events towards the three-phase contact line associated with the nanotextured surface. The ice-surface work of adhesion for the Wenzel state is found to be 1-2 times higher than that in the Cassie-Baxter state. Furthermore, the work of adhesion of ice in the Wenzel state is found to be linearly dependent on the contour length of the droplet, which is in line with that reported for liquid droplets.

Screening of plant resources with anti-ice nucleation activity for frost damage prevention.

PubMed

Suzuki, Shingo; Fukuda, Satoshi; Fukushi, Yukiharu; Arakawa, Keita

2017-11-01

Previous studies have shown that some polyphenols have anti-ice nucleation activity (anti-INA) against ice-nucleating bacteria that contribute to frost damage. In the present study, leaf disk freezing assay, a test of in vitro application to plant leaves, was performed for the screening of anti-INA, which inhibits the ice nucleation activity of an ice-nucleating bacterium Erwinia ananas in water droplets on the leaf surfaces. The application of polyphenols with anti-INA, kaempferol 7-O-β-glucoside and (-)-epigallocatechin gallate, to the leaf disk freezing assay by cooling at -4--6 °C for 3 h, revealed that both the compounds showed anti-INAs against E. ananas in water droplets on the leaf surfaces. Further, this assay also revealed that the extracts of five plant leaves showed high anti-INA against E. ananas in water droplets on leaf surfaces, indicating that they are the candidate resources to protect crops from frost damage.

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

Garimella, Sarvesh; Kristensen, Thomas Bjerring; Ignatius, Karolina

The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nucleating particle (INP) counter manufactured by Droplet Measurement Technologies in Boulder, CO. The SPIN is a continuous flow diffusion chamber with parallel plate geometry based on the Zurich Ice Nucleation Chamber and the Portable Ice Nucleation Chamber. This study presents a standard description for using the SPIN instrument and also highlights methods to analyze measurements in more advanced ways. It characterizes and describes the behavior of the SPIN chamber, reports data from laboratory measurements, and quantifies uncertainties associated with the measurements. Experiments with ammonium sulfate are used to investigatemore » homogeneous freezing of deliquesced haze droplets and droplet breakthrough. Experiments with kaolinite, NX illite, and silver iodide are used to investigate heterogeneous ice nucleation. SPIN nucleation results are compared to those from the literature. A machine learning approach for analyzing depolarization data from the SPIN optical particle counter is also presented (as an advanced use). Altogether, we report that the SPIN is able to reproduce previous INP counter measurements.« less

Meteorological and Aerosol effects on Marine Cloud Microphysical Properties

NASA Astrophysics Data System (ADS)

Sanchez, K. J.; Russell, L. M.; Modini, R. L.; Frossard, A. A.; Ahlm, L.; Roberts, G.; Hawkins, L. N.; Schroder, J. C.; Wang, Z.; Lee, A.; Abbatt, J.; Lin, J.; Nenes, A.; Wonaschuetz, A.; Sorooshian, A.; Noone, K.; Jonsson, H.; Albrecht, B. A.; Desiree, T. S.; Macdonald, A. M.; Seinfeld, J.; Zhao, R.

2015-12-01

Both meteorology and microphysics affect cloud formation and consequently their droplet distributions and shortwave reflectance. The Eastern Pacific Emitted Aerosol Cloud Experiment (EPEACE) and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) studies provide detailed measurements in 6 case studies of both cloud thermodynamic properties and initial particle number distribution and composition, as well as the resulting cloud drop distribution and composition. This study uses simulations of a detailed chemical and microphysical aerosol-cloud parcel (ACP) model with explicit kinetic drop activation to reproduce the observed cloud droplet distribution and composition. Four of the cases examined had a sub-adiabatic lapse rate, which was shown to have fewer droplets due to decreased maximum supersaturation, lower LWC and higher cloud base height, consistent with previous findings. These detailed case studies provided measured thermodynamics and microphysics that constrained the simulated droplet size distribution sufficiently to match the droplet number within 6% and the size within 19% for 4 of the 6 cases, demonstrating "closure" or consistency of the measured composition with the measured CCN spectra and the inferred and modeled supersaturation. The contribution of organic components to droplet formation shows small effects on the droplet number and size in the 4 marine cases that had background aerosol conditions with varying amounts of coastal, ship or other non-biogenic sources. In contrast, the organic fraction and hygroscopicity increased the droplet number and size in the cases with generated smoke and cargo ship plumes that were freshly emitted and not yet internally mixed with the background particles. The simulation results show organic hygroscopicity causes small effects on cloud reflectivity (<0.7%) with the exception of the cargo ship plume and smoke plume which increased absolute cloud reflectivity fraction by 0.02 and 0.20 respectively. In addition, the ACP model simulations are compared to those from a numerical parameterization of cloud droplet activation that is suitable for GCMs and show droplet concentrations are comparable between the two methods.

Aerosol effect on cloud droplet size as monitored from surface-based remote sensing over East China Sea region

NASA Astrophysics Data System (ADS)

Pandithurai, G.; Takamura, T.; Yamaguchi, J.; Miyagi, K.; Takano, T.; Ishizaka, Y.; Dipu, S.; Shimizu, A.

2009-07-01

The effect of increased aerosol concentrations on the low-level, non-precipitating, ice-free stratus clouds is examined using a suite of surface-based remote sensing systems. Cloud droplet effective radius and liquid water path are retrieved using cloud radar and microwave radiometer. Collocated measurements of aerosol scattering coefficient, size distribution and cloud condensation nuclei (CCN) concentrations were used to examine the response of cloud droplet size and optical thickness to increased CCN proxies. During the episodic events of increase in aerosol accumulation-mode volume distribution, the decrease in droplet size and increase in cloud optical thickness is observed. The indirect effect estimates are made for both droplet effective radius and cloud optical thickness for different liquid water path ranges and they range 0.02-0.18 and 0.005-0.154, respectively. Data are also categorized into thin and thick clouds based on cloud geometric thickness (Δz) and estimates show IE values are relatively higher for thicker clouds.

(NH4)2SO4 heterogeneous nucleation and glycerol evaporation of (NH4)2SO4-glycerol system in its dynamic efflorescence process

NASA Astrophysics Data System (ADS)

Cai, Chen; Luan, Ye-mei; Shi, Xiao-min; Zhang, Yun-hong

2017-02-01

Using the FTIR-ATR technique, we investigated the heterogeneous nucleation process of aqueous (NH4)2SO4 binary droplets and (NH4)2SO4/glycerol ternary droplets. From the red shift of δ-NH4+ with a linearly declining relative humidity (RH), the ERHs of pure (NH4)2SO4 droplets and mixed (NH4)2SO4/glycerol droplets with different organic-inorganic ratio (OIR) of 1:4, 1:2 and 1:1 ranges from ∼51.9 to ∼34.9%, ∼49.8 to ∼33.0%, ∼48.0 to ∼30.6% and ∼43.7 to ∼25.2%, respectively. From the changing absorbance of δ-NH4+ band, we determined the heterogeneous nucleation rates of crystalline (NH4)2SO4 in the pure and mixed droplets. The interfacial tension between an (NH4)2SO4 critical nucleus and surrounding (NH4)2SO4 solution was determined using classical nucleation theory and experimental data to be 0.031 ± 0.002 J m-2. Evaporation of glycerol in (NH4)2SO4/glycerol ternary droplets are also studied to be restrained by participation of (NH4)2SO4. Determined vapour pressure of glycerol is on the same magnitude with results from previous studies.

Water droplet excess free energy determined by cluster mitosis using guided molecular dynamics

NASA Astrophysics Data System (ADS)

Lau, Gabriel V.; Hunt, Patricia A.; Müller, Erich A.; Jackson, George; Ford, Ian J.

2015-12-01

Atmospheric aerosols play a vital role in affecting climate by influencing the properties and lifetimes of clouds and precipitation. Understanding the underlying microscopic mechanisms involved in the nucleation of aerosol droplets from the vapour phase is therefore of great interest. One key thermodynamic quantity in nucleation is the excess free energy of cluster formation relative to that of the saturated vapour. In our current study, the excess free energy is extracted for clusters of pure water modelled with the TIP4P/2005 intermolecular potential using a method based on nonequilibrium molecular dynamics and the Jarzynski relation. The change in free energy associated with the "mitosis" or division of a cluster of N water molecules into two N/2 sub-clusters is evaluated. This methodology is an extension of the disassembly procedure used recently to calculate the excess free energy of argon clusters [H. Y. Tang and I. J. Ford, Phys. Rev. E 91, 023308 (2015)]. Our findings are compared to the corresponding excess free energies obtained from classical nucleation theory (CNT) as well as internally consistent classical theory (ICCT). The values of the excess free energy that we obtain with the mitosis method are consistent with CNT for large cluster sizes but for the smallest clusters, the results tend towards ICCT; for intermediate sized clusters, we obtain values between the ICCT and CNT predictions. Furthermore, the curvature-dependent surface tension which can be obtained by regarding the clusters as spherical droplets of bulk density is found to be a monotonically increasing function of cluster size for the studied range. The data are compared to other values reported in the literature, agreeing qualitatively with some but disagreeing with the values determined by Joswiak et al. [J. Phys. Chem. Lett. 4, 4267 (2013)] using a biased mitosis approach; an assessment of the differences is the main motivation for our current study.

Water droplet excess free energy determined by cluster mitosis using guided molecular dynamics

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

Lau, Gabriel V.; Müller, Erich A.; Jackson, George

Atmospheric aerosols play a vital role in affecting climate by influencing the properties and lifetimes of clouds and precipitation. Understanding the underlying microscopic mechanisms involved in the nucleation of aerosol droplets from the vapour phase is therefore of great interest. One key thermodynamic quantity in nucleation is the excess free energy of cluster formation relative to that of the saturated vapour. In our current study, the excess free energy is extracted for clusters of pure water modelled with the TIP4P/2005 intermolecular potential using a method based on nonequilibrium molecular dynamics and the Jarzynski relation. The change in free energy associatedmore » with the “mitosis” or division of a cluster of N water molecules into two N/2 sub-clusters is evaluated. This methodology is an extension of the disassembly procedure used recently to calculate the excess free energy of argon clusters [H. Y. Tang and I. J. Ford, Phys. Rev. E 91, 023308 (2015)]. Our findings are compared to the corresponding excess free energies obtained from classical nucleation theory (CNT) as well as internally consistent classical theory (ICCT). The values of the excess free energy that we obtain with the mitosis method are consistent with CNT for large cluster sizes but for the smallest clusters, the results tend towards ICCT; for intermediate sized clusters, we obtain values between the ICCT and CNT predictions. Furthermore, the curvature-dependent surface tension which can be obtained by regarding the clusters as spherical droplets of bulk density is found to be a monotonically increasing function of cluster size for the studied range. The data are compared to other values reported in the literature, agreeing qualitatively with some but disagreeing with the values determined by Joswiak et al. [J. Phys. Chem. Lett. 4, 4267 (2013)] using a biased mitosis approach; an assessment of the differences is the main motivation for our current study.« less

RACORO aerosol data processing

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

Elisabeth Andrews

2011-10-31

The RACORO aerosol data (cloud condensation nuclei (CCN), condensation nuclei (CN) and aerosol size distributions) need further processing to be useful for model evaluation (e.g., GCM droplet nucleation parameterizations) and other investigations. These tasks include: (1) Identification and flagging of 'splash' contaminated Twin Otter aerosol data. (2) Calculation of actual supersaturation (SS) values in the two CCN columns flown on the Twin Otter. (3) Interpolation of CCN spectra from SGP and Twin Otter to 0.2% SS. (4) Process data for spatial variability studies. (5) Provide calculated light scattering from measured aerosol size distributions. Below we first briefly describe the measurementsmore » and then describe the results of several data processing tasks that which have been completed, paving the way for the scientific analyses for which the campaign was designed. The end result of this research will be several aerosol data sets which can be used to achieve some of the goals of the RACORO mission including the enhanced understanding of cloud-aerosol interactions and improved cloud simulations in climate models.« less

Modeling the relative contributions of secondary ice formation processes to ice crystal number concentrations within mixed-phase clouds

NASA Astrophysics Data System (ADS)

Sullivan, Sylvia; Hoose, Corinna; Nenes, Athanasios

2016-04-01

Measurements of in-cloud ice crystal number concentrations can be three or four orders of magnitude greater than the in-cloud ice nuclei number concentrations. This discrepancy can be explained by various secondary ice formation processes, which occur after initial ice nucleation, but the relative importance of these processes, and even the exact physics of each, is still unclear. A simple bin microphysics model (2IM) is constructed to investigate these knowledge gaps. 2IM extends the time-lag collision parameterization of Yano and Phillips, 2011 to include rime splintering, ice-ice aggregation, and droplet shattering and to incorporate the aspect ratio evolution as in Jensen and Harrington, 2015. The relative contribution of the secondary processes under various conditions are shown. In particular, temperature-dependent efficiencies are adjusted for ice-ice aggregation versus collision around -15°C, when rime splintering is no longer active, and the effect of aspect ratio on the process weighting is explored. The resulting simulations are intended to guide secondary ice formation parameterizations in larger-scale mixed-phase cloud schemes.

Determination of the chemical properties of residues retained in individual cloud droplets by XRF microprobe at SPring-8

NASA Astrophysics Data System (ADS)

Ma, C.-J.; Tohno, S.; Kasahara, M.; Hayakawa, S.

2004-06-01

To determine the chemical properties of residue retained in individual cloud droplets is primarily important for the understanding of rainout mechanism and aerosol modification in droplet. The sampling of individual cloud droplets were carried out on the summit of Mt. Taiko located in Tango peninsula, Kyoto prefecture, during Asian dust storm event in March of 2002. XRF microprobe system equipped at SPring-8, BL-37XU was applied to the subsequent quantification analysis of ultra trace elements in residues of individual cloud droplets. It was possible to form the replicas of separated individual cloud droplets on the thin collodion film. The two dimensional XRF maps for the residues in individual cloud droplets were clearly drawn by scanning of micro-beam. Also, XRF spectra of trace elements in residues were well resolved. From the XRF spectra for individual residues, the chemical mixed state of residues could be assumed. The chemical forms of Fe (Fe +++) and Zn (Zn +) could be clearly characterized by their K-edge micro-XANES spectra. By comparison of Z/Si mass ratios of residues in cloud droplets and those of the original sands collected in desert areas in China, the aging of ambient dust particles and their in cloud modification were indirectly assumed.

Immersion freezing of water and aqueous ammonium sulfate droplets initiated by humic-like substances as a function of water activity

DOE PAGES

Rigg, Y. J.; Alpert, P. A.; Knopf, Daniel A.

2013-07-12

Immersion freezing of water and aqueous (NH 4) 2SO 4 droplets containing leonardite (LEO) and Pahokee peat (PP) serving as surrogates for humic-like substances (HULIS) has been investigated. Organic aerosol containing HULIS are ubiquitous in the atmosphere; however, their potential for ice cloud formation is uncertain. Immersion freezing has been studied for temperatures as low as 215K and solution water activity, aw, from 0.85 to 1.0. The freezing temperatures of water and aqueous solution droplets containing LEO and PP are 5–15 K warmer than homogeneous ice nucleation temperatures. Heterogeneous freezing temperatures can be represented by a horizontal shift of themore » ice melting curve as a function of solution aw by Δ aw = 0.2703 and 0.2466, respectively. Corresponding heterogeneous ice nucleation rate coefficients, Jhet, are (9.6 ± 2.5) × 10 4 and (5.4 ± 1.4) × 10 4 cm -2 s -1 for LEO and PP containing droplets, respectively, and remain constant along freezing curves characterized by Δ aw. Consequently predictions of freezing temperatures and kinetics can be made without knowledge of the solute type when relative humidity and ice nuclei (IN) surface areas are known. The acquired ice nucleation data are applied to evaluate different approaches to fit and reproduce experimentally derived frozen fractions. In addition, we apply a basic formulation of classical nucleation theory (α( T)-model) to calculate contact angles and frozen fractions. Contact angles calculated for each ice nucleus as a function of temperature, α( T)-model, reproduce exactly experimentally derived frozen fractions without involving free-fit parameters. However, assigning the IN a single contact angle for the entire population (single-α model) is not suited to represent the frozen fractions. Application of α-PDF, active sites, and deterministic model approaches to measured frozen fractions yield similar good representations. Furthermore, when using a single parameterization of α-PDF or active sites distribution to fit all individual aw immersion freezing data simultaneously, frozen fraction curves are not reproduced. This implies that these fitting formulations cannot be applied to immersion freezing of aqueous solutions, and suggests that derived fit parameters do not represent independent particle properties. Thus, from fitting frozen fractions only, the underlying ice nucleation mechanism and nature of the ice nucleating sites cannot be inferred. In contrast to using fitted functions obtained to represent experimental conditions only, we suggest to use experimentally derived Jhet as a function of temperature and aw that can be applied to conditions outside of those probed in laboratory. Finally, this is because Jhet(T) is independent of time and IN surface areas in contrast to the fit parameters obtained by representation of experimentally derived frozen fractions.« less

Heterogeneous nucleation of a droplet pinned at a chemically inhomogeneous substrate: A simulation study of the two-dimensional Ising case

NASA Astrophysics Data System (ADS)

Trobo, Marta L.; Albano, Ezequiel V.; Binder, Kurt

2018-03-01

Heterogeneous nucleation is studied by Monte Carlo simulations and phenomenological theory, using the two-dimensional lattice gas model with suitable boundary fields. A chemical inhomogeneity of length b at one boundary favors the liquid phase, while elsewhere the vapor is favored. Switching on the bulk field Hb favoring the liquid, nucleation and growth of the liquid phase starting from the region of the chemical inhomogeneity are analyzed. Three regimes occur: for small fields, HbHb*), the droplets nucleated at the chemical inhomogeneity grow to the full system size. While the relaxation time for the growth scales as τG∝Hb-1, the nucleation time τN scales as ln τN∝Hb-1. However, the prefactor in the latter relation, as evaluated for our simulations results, is not in accord with an extension of the Volmer-Turnbull theory to two-dimensions, when the theoretical contact angle θc is used.

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.

Evaluation of long-term surface-retrieved cloud droplet number concentration with in situ aircraft observations: ARM Cloud Droplet Number Concentration

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

Lim, Kyo-Sun Sunny; Riihimaki, Laura; Comstock, Jennifer M.

A new cloud-droplet number concentration (NDROP) value added product (VAP) has been produced at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site for the 13 years from January 1998 to January 2011. The retrieval is based on surface radiometer measurements of cloud optical depth from the multi-filter rotating shadow-band radiometer (MFRSR) and liquid water path from the microwave radiometer (MWR). It is only applicable for single-layered warm clouds. Validation with in situ aircraft measurements during the extended-term aircraft field campaign, Routine ARM Aerial Facility (AAF) CLOWD Optical Radiative Observations (RACORO), shows that the NDROP VAP robustly reproduces themore » primary mode of the in situ measured probability density function (PDF), but produces a too wide distribution, primarily caused by frequent high cloud-droplet number concentration. Our analysis shows that the error in the MWR retrievals at low liquid water paths is one possible reason for this deficiency. Modification through the diagnosed liquid water path from the coordinate solution improves not only the PDF of the NDROP VAP but also the relationship between the cloud-droplet number concentration and cloud-droplet effective radius. Consideration of entrainment effects rather than assuming an adiabatic cloud improves the values of the NDROP retrieval by reducing the magnitude of cloud-droplet number concentration. Aircraft measurements and retrieval comparisons suggest that retrieving the vertical distribution of cloud-droplet number concentration and effective radius is feasible with an improvement of the parameter representing the mixing effects between environment and clouds and with a better understanding of the effect of mixing degree on cloud properties.« less

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.

Conditions for super-adiabatic droplet growth after entrainment mixing

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

Yang, Fan; Shaw, Raymond; Xue, Huiwen

Cloud droplet response to entrainment and mixing between a cloud and its environment is considered, accounting for subsequent droplet growth during adiabatic ascent following a mixing event. The vertical profile for liquid water mixing ratio after a mixing event is derived analytically, allowing the reduction to be predicted from the mixing fraction and from the temperature and humidity for both the cloud and environment. It is derived for the limit of homogeneous mixing. The expression leads to a critical height above the mixing level: at the critical height the cloud droplet radius is the same for both mixed and unmixedmore » parcels, and the critical height is independent of the updraft velocity and mixing fraction. Cloud droplets in a mixed parcel are larger than in an unmixed parcel above the critical height, which we refer to as the “super-adiabatic” growth region. Analytical results are confirmed with a bin microphysics cloud model. Using the model, we explore the effects of updraft velocity, aerosol source in the environmental air, and polydisperse cloud droplets. Results show that the mixed parcel is more likely to reach the super-adiabatic growth region when the environmental air is humid and clean. It is also confirmed that the analytical predictions are matched by the volume-mean cloud droplet radius for polydisperse size distributions. Lastly, these findings have implications for the origin of large cloud droplets that may contribute to onset of collision–coalescence in warm clouds.« less

Conditions for super-adiabatic droplet growth after entrainment mixing

DOE PAGES

Yang, Fan; Shaw, Raymond; Xue, Huiwen

2016-07-29

Cloud droplet response to entrainment and mixing between a cloud and its environment is considered, accounting for subsequent droplet growth during adiabatic ascent following a mixing event. The vertical profile for liquid water mixing ratio after a mixing event is derived analytically, allowing the reduction to be predicted from the mixing fraction and from the temperature and humidity for both the cloud and environment. It is derived for the limit of homogeneous mixing. The expression leads to a critical height above the mixing level: at the critical height the cloud droplet radius is the same for both mixed and unmixedmore » parcels, and the critical height is independent of the updraft velocity and mixing fraction. Cloud droplets in a mixed parcel are larger than in an unmixed parcel above the critical height, which we refer to as the “super-adiabatic” growth region. Analytical results are confirmed with a bin microphysics cloud model. Using the model, we explore the effects of updraft velocity, aerosol source in the environmental air, and polydisperse cloud droplets. Results show that the mixed parcel is more likely to reach the super-adiabatic growth region when the environmental air is humid and clean. It is also confirmed that the analytical predictions are matched by the volume-mean cloud droplet radius for polydisperse size distributions. Lastly, these findings have implications for the origin of large cloud droplets that may contribute to onset of collision–coalescence in warm clouds.« less

Broadening of cloud droplet spectra through turbulent entrainment and eddy hopping

NASA Astrophysics Data System (ADS)

Abade, Gustavo; Grabowski, Wojciech; Pawlowska, Hanna

2017-11-01

This work discusses the effect of cloud turbulence and turbulent entrainment on the evolution of the cloud droplet-size spectrum. We simulate an ensemble of idealized turbulent cloud parcels that are subject to entrainment events, modeled as a random Poisson process. Entrainment events, subsequent turbulent mixing inside the parcel, supersaturation fluctuations, and the resulting stochastic droplet growth by condensation are simulated using a Monte Carlo scheme. Quantities characterizing the turbulence intensity, entrainment rate and the mean fraction of environmental air entrained in an event are specified as external parameters. Cloud microphysics is described by applying Lagrangian particles, the so-called superdroplets. They are either unactivated cloud condensation nuclei (CCN) or cloud droplets that form from activated CCN. The model accounts for the transport of environmental CCN into the cloud by the entraining eddies at the cloud edge. Turbulent mixing of the entrained dry air with cloudy air is described using a linear model. We show that turbulence plays an important role in aiding entrained CCN to activate, providing a source of small cloud droplets and thus broadening the droplet size distribution. Further simulation results will be reported at the meeting.

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.

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.

A Model for Particle Microphysics,Turbulent Mixing, and Radiative Transfer in the Stratocumulus-Topped Marine Boundary Layer and Comparisons with Measurements

NASA Technical Reports Server (NTRS)

Ackerman, Andrew S.; Toon, Owen B.; Hobbs, Peter V.

1995-01-01

A detailed 1D model of the stratocumulus-topped marine boundary layer is described. The model has three coupled components: a microphysics module that resolves the size distributions of aerosols and cloud droplets, a turbulence module that treats vertical mixing between layers, and a multiple wavelength radiative transfer module that calculates radiative heating rates and cloud optical properties. The results of a 12-h model simulation reproduce reasonably well the bulk thermodynamics, microphysical properties, and radiative fluxes measured in an approx. 500-m thick, summertime marine stratocumulus cloud layer by Nicholls. However, in this case, the model predictions of turbulent fluxes between the cloud and subcloud layers exceed the measurements. Results of model simulations are also compared to measurements of a marine stratus layer made under gate conditions and with measurements of a high, thin marine stratocumulus layer. The variations in cloud properties are generally reproduced by the model, although it underpredicts the entrainment of overlying air at cloud top under gale conditions. Sensitivities of the model results are explored. The vertical profile of cloud droplet concentration is sensitive to the lower size cutoff of the droplet size distribution due to the presence of unactivated haze particles in the lower region of the modeled cloud. Increases in total droplet concentrations do not always produce less drizzle and more cloud water in the model. The radius of the mean droplet volume does not correlate consistently with drizzle, but the effective droplet radius does. The greatest impacts on cloud properties predicted by the model are produced by halving the width of the size distribution of input condensation nuclei and by omitting the effect of cloud-top radiative cooling on the condensational growth of cloud droplets. The omission of infrared scattering produces noticeable changes in cloud properties. The collection efficiencies for droplets less than 30-micron radius, and the value of the accommodation coefficient for condensational droplet growth, have noticeable effects on cloud properties. The divergence of the horizontal wind also has a significant effect on a 12-h model simulation of cloud structure. Conclusions drawn from the model are tentative because of the limitations of the 1D model framework. A principal simplification is that the model assumes horizontal homogeneity, and, therefore, does not resolve updrafts and downdrafts. Likely consequences of this simplification include overprediction of the growth of droplets by condensation in the upper region of the cloud, underprediction of droplet condensational growth in the lower region of the cloud, and under-prediction of peak supersaturations.

A Model for Particle Microphysics, Turbulent Mixing, and Radiative Transfer in the Stratocumulus-Topped Marine Boundary Layer and Comparisons with Measurements

NASA Technical Reports Server (NTRS)

Ackerman, Andrew S.; Toon, Owen B.; Hobbs, Peter V.

1995-01-01

A detailed 1D model of the stratocumulus-topped marine boundary layer is described. The model has three coupled components: a microphysics module that resolves the size distributions of aerosols and cloud droplets, a turbulence module that treats vertical mixing between layers, and a multiple wavelength radiative transfer module that calculates radiative heating rates and cloud optical properties. The results of a 12-h model simulation reproduce reasonably well the bulk thermodynamics, microphysical properties, and radiative fluxes measured in an approx. 500-m thick, summertime marine stratocumulus cloud layer by Nicholls. However, in this case, the model predictions of turbulent fluxes between the cloud and subcloud layers exceed the measurements. Results of model simulations are also compared to measurements of a marine stratus layer made under gale conditions and with measurements of a high, thin marine stratocumulus layer. The variations in cloud properties are generally reproduced by the model, although it underpredicts the entrainment of overlying air at cloud top under gale conditions. Sensitivities of the model results are explored. The vertical profile of cloud droplet concentration is sensitive to the lower size cutoff of the droplet size distribution due to the presence of unactivated haze particles in the lower region of the modeled cloud. Increases in total droplet concentrations do not always produce less drizzle and more cloud water in the model. The radius of the mean droplet volume does not correlate consistently with drizzle, but the effective droplet radius does. The greatest impacts on cloud properties predicted by the model are produced by halving the width of the size distribution of input condensation nuclei and by omitting the effect of cloud-top radiative cooling on the condensational growth of cloud droplets. The omission of infrared scattering produces noticeable changes in cloud properties. The collection efficiencies for droplets less than 30-micrometers radius, and the value of the accommodation coefficient for condensational droplet growth, have noticeable effects on cloud properties. The divergence of the horizontal wind also has a significant effect on a 12-h model simulation of cloud structure. Conclusions drawn from the model are tentative because of the limitations of the 1D model framework. A principal simplification is that the model assumes horizontal homogeneity, and, therefore, does not resolve updrafts and downdrafts. Likely consequences of this simplification include overprediction of the growth of droplets by condensation in the upper region of the cloud, underprediction of droplet condensational growth in the lower region of the cloud, and underprediction of peak supersaturations.

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.

Basic and applied research related to the technology of space energy conversion systems

NASA Technical Reports Server (NTRS)

Hertzberg, A.; Mattick, A. T.; Bruckner, A. P.

1988-01-01

The first six months' research effort on the Liquid Droplet Radiator (LDR) focussed on experimental and theoretical studies of radiation by an LDR droplet cloud. Improvements in the diagnostics for the radiation facility have been made which have permitted an accurate experimental test of theoretical predictions of LDR radiation over a wide range of optical depths, using a cloud of Dow silicone oil droplets. In conjunction with these measurements an analysis was made of the evolution of the cylindrical droplet cloud generated by a 2300-hole orifice plate. This analysis indicates that a considerable degree of agglomeration of droplets occurs over the first meter of travel. Theoretical studies have centered on developments of an efficient means of computing the angular scattering distribution from droplets in an LDR droplet cloud, so that a parameter study can be carried out for LDR radiative performance vs fluid optical properties and cloud geometry.

Rime and graupel: Description and characterization as revealed by low-temperature scanning electron microscopy

USGS Publications Warehouse

Rango, A.; Foster, J.; Josberger, E.G.; Erbe, E.F.; Pooley, C.; Wergin, W.P.

2003-01-01

Snow crystals, which form by vapor deposition, occasionally come in contact with supercooled cloud droplets during their formation and descent. When this occurs, the droplets adhere and freeze to the snow crystals in a process known as accretion. During the early stages of accretion, discrete snow crystals exhibiting frozen cloud droplets are referred to as rime. If this process continues, the snow crystal may become completely engulfed in frozen cloud droplets. The resulting particle is known as graupel. Light microscopic investigations have studied rime and graupel for nearly 100 years. However, the limiting resolution and depth of field associated with the light microscope have prevented detailed descriptions of the microscopic cloud droplets and the three-dimensional topography of the rime and graupel particles. This study uses low-temperature scanning electron microscopy to characterize the frozen precipitates that are commonly known as rime and graupel. Rime, consisting of frozen cloud droplets, is observed on all types of snow crystals including needles, columns, plates, and dendrites. The droplets, which vary in size from 10 to 100 μm, frequently accumulate along one face of a single snow crystal, but are found more randomly distributed on aggregations consisting of two or more snow crystals (snowflakes). The early stages of riming are characterized by the presence of frozen cloud droplets that appear as a layer of flattened hemispheres on the surface of the snow crystal. As this process continues, the cloud droplets appear more sinuous and elongate as they contact and freeze to the rimed crystals. The advanced stages of this process result in graupel, a particle 1 to 3 mm across, composed of hundreds of frozen cloud droplets interspersed with considerable air spaces; the original snow crystal is no longer discernible. This study increases our knowledge about the process and characteristics of riming and suggests that the initial appearance of the flattened hemispheres may result from impact of the leading face of the snow crystal with cloud droplets. The elongated and sinuous configurations of frozen cloud droplets that are encountered on the more advanced stages suggest that aerodynamic forces propel cloud droplets to the trailing face of the descending crystal where they make contact and freeze.

Nucleation of protein crystals under the influence of solution shear flow.

PubMed

Penkova, Anita; Pan, Weichun; Hodjaoglu, Feyzim; Vekilov, Peter G

2006-09-01

Several recent theories and simulations have predicted that shear flow could enhance, or, conversely, suppress the nucleation of crystals from solution. Such modulations would offer a pathway for nucleation control and provide a novel explanation for numerous mysteries in nucleation research. For experimental tests of the effects of shear flow on protein crystal nucleation, we found that if a protein solution droplet of approximately 5 microL (2-3 mm diameter at base) is held on a hydrophobic substrate in an enclosed environment and in a quasi-uniform constant electric field of 2 to 6 kV cm(-1), a rotational flow with a maximum rate at the droplet top of approximately 10 microm s(-1) is induced. The shear rate varies from 10(-3) to 10(-1) s(-1). The likely mechanism of the rotational flow involves adsorption of the protein and amphiphylic buffer molecules on the air-water interface and their redistribution in the electric field, leading to nonuniform surface tension of the droplet and surface tension-driven flow. Observations of the number of nucleated crystals in 24- and 72-h experiments with the proteins ferritin, apoferritin, and lysozyme revealed that the crystals are typically nucleated at a certain radius of the droplet, that is, at a preferred shear rate. Variations of the rotational flow velocity resulted in suppression or enhancement of the total number of nucleated crystals of ferritin and apoferritin, while all solution flow rates were found to enhance lysozyme crystal nucleation. These observations show that shear flow may strongly affect nucleation, and that for some systems, an optimal flow velocity, leading to fastest nucleation, exists. Comparison with the predictions of theories and simulations suggest that the formation of ordered nuclei in a "normal" protein solution cannot be affected by such low shear rates. We conclude that the flow acts by helping or suppressing the formation of ordered nuclei within mesoscopic metastable dense liquid clusters. Such clusters were recently shown to exist in protein solutions and to constitute the first step in the nucleation mechanism of many protein and nonproteinsystems.

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

Mishchenko, L; Khan, M; Aizenberg, J

Certain natural organisms use micro-patterned surface chemistry, or ice-nucleating species, to control water condensation and ice nucleation for survival under extreme conditions. As an analogy to these biological approaches, it is shown that functionalized, hydrophilic polymers and particles deposited on the tips of superhydrophobic posts induce precise topographical control over water condensation and freezing at the micrometer scale. A bottom-up deposition process is used to take advantage of the limited contact area of a non-wetting aqueous solution on a superhydrophobic surface. Hydrophilic polymer deposition on the tips of these geometrical structures allows spatial control over the nucleation, growth, and coalescencemore » of micrometer-scale water droplets. The hydrophilic tips nucleate water droplets with extremely uniform nucleation and growth rates, uniform sizes, an increased stability against coalescence, and asymmetric droplet morphologies. Control of freezing behavior is also demonstrated via deposition of ice-nucleating AgI nanoparticles on the tips of these structures. This combination of the hydrophilic polymer and AgI particles on the tips was used to achieve templating of ice nucleation at the micrometer scale. Preliminary results indicate that control over ice crystal size, spatial symmetry, and position might be possible with this method. This type of approach can serve as a platform for systematically analyzing micrometer-scale condensation and freezing phenomena, and as a model for natural systems.« less

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

Mishchenko, Lidiya; Khan, M.; Aizenberg, Joanna

Certain natural organisms use micro-patterned surface chemistry, or ice-nucleating species, to control water condensation and ice nucleation for survival under extreme conditions. As an analogy to these biological approaches, it is shown that functionalized, hydrophilic polymers and particles deposited on the tips of superhydrophobic posts induce precise topographical control over water condensation and freezing at the micrometer scale. A bottom-up deposition process is used to take advantage of the limited contact area of a non-wetting aqueous solution on a superhydrophobic surface. Hydrophilic polymer deposition on the tips of these geometrical structures allows spatial control over the nucleation, growth, and coalescencemore » of micrometer-scale water droplets. The hydrophilic tips nucleate water droplets with extremely uniform nucleation and growth rates, uniform sizes, an increased stability against coalescence, and asymmetric droplet morphologies. Furthermore, control of freezing behavior is also demonstrated via deposition of ice-nucleating AgI nanoparticles on the tips of these structures. The combination of the hydrophilic polymer and AgI particles on the tips was used to achieve templating of ice nucleation at the micrometer scale. Preliminary results indicate that control over ice crystal size, spatial symmetry, and position might be possible with this method. This type of approach can serve as a platform for systematically analyzing micrometer-scale condensation and freezing phenomena, and as a model for natural systems.« less

Heterogeneous Catalysis: On Bathroom Mirrors and Boiling Stones

ERIC Educational Resources Information Center

Philipse, Albert P.

2011-01-01

Though heterogeneous nucleation of liquid droplets on a smooth surface (such as a bathroom mirror) is a classical topic in nucleation theory, it is not well-known that this topic is actually a pedagogical example of heterogeneous catalysis: the one and only effect of the surface is to lower the activation Gibbs energy of droplet formation. In…

Self-propelled motion of Au-Si droplets on Si(111) mediated by monoatomic step dissolution

NASA Astrophysics Data System (ADS)

Curiotto, S.; Leroy, F.; Cheynis, F.; Müller, P.

2015-02-01

By Low Energy Electron Microscopy, we show that the spontaneous motion of gold droplets on silicon (111) is chemically driven: the droplets tend to dissolve silicon monoatomic steps to reach the temperature-dependent Au-Si equilibrium stoichiometry. According to the droplet size, the motion details are different. In the first stages of Au deposition small droplets nucleate at steps and move continuously on single terraces. The droplets temporarily pin at each step they meet during their motion. During pinning, the growing droplets become supersaturated in Au. They depin from the steps when a notch nucleate on the upper step. Then the droplets climb up and locally dissolve the Si steps, leaving behind them deep tracks formed by notched steps. Measurements of the dissolution rate and the displacement lengths enable us to describe quantitatively the motion mechanism, also in terms of anisotropy of Si dissolution kinetics. Scaling laws for the droplet position as a function of time are proposed: x ∝ tn with 1/3 < n < 2/3.

From Initial Nucleation to Cassie-Baxter State of Condensed Droplets on Nanotextured Superhydrophobic Surfaces.

PubMed

Lv, Cunjing; Zhang, Xiwen; Niu, Fenglei; He, Feng; Hao, Pengfei

2017-02-16

Understanding how droplet condensation happens plays an essential role for our fundamental insights of wetting behaviors in nature and numerous applications. Since there is a lack of study of the initial formation and growing processes of condensed droplets down to nano-/submicroscale, relevant underlying mechanisms remain to be explored. We report an in situ observation of vapor condensation on nano-/microtextured superhydrophobic surfaces using optical microscopy. An interesting picture of the vapor condensation, from the initial appearance of individual small droplets (≤1 μm) to a Cassie-Baxter wetting state (>30 μm), are exhibited. It is found that individual droplets preferentially nucleate at the top and the edge of single micropillars with very high apparent contact angles on the nanotextures. Scenarios of two distinguished growing modes are reported statistically and the underlying mechanisms are discussed in the view of thermodynamics. We particularly reveal that the formation of the Cassie-Baxter wetting state is a result of a continuous coalescence of individual small droplets, in which the nanotexture-enhanced superhydrophobicity plays a crucial role. We envision that these fundamental findings can deepen our understanding of the nucleation and development of condensed droplets in nanoscale, so as to optimize design strategies of superhydrophobic materials for a broad range of water-harvesting and heat-transfer systems.

From Initial Nucleation to Cassie-Baxter State of Condensed Droplets on Nanotextured Superhydrophobic Surfaces

NASA Astrophysics Data System (ADS)

Lv, Cunjing; Zhang, Xiwen; Niu, Fenglei; He, Feng; Hao, Pengfei

2017-02-01

Understanding how droplet condensation happens plays an essential role for our fundamental insights of wetting behaviors in nature and numerous applications. Since there is a lack of study of the initial formation and growing processes of condensed droplets down to nano-/submicroscale, relevant underlying mechanisms remain to be explored. We report an in situ observation of vapor condensation on nano-/microtextured superhydrophobic surfaces using optical microscopy. An interesting picture of the vapor condensation, from the initial appearance of individual small droplets (≤1 μm) to a Cassie-Baxter wetting state (>30 μm), are exhibited. It is found that individual droplets preferentially nucleate at the top and the edge of single micropillars with very high apparent contact angles on the nanotextures. Scenarios of two distinguished growing modes are reported statistically and the underlying mechanisms are discussed in the view of thermodynamics. We particularly reveal that the formation of the Cassie-Baxter wetting state is a result of a continuous coalescence of individual small droplets, in which the nanotexture-enhanced superhydrophobicity plays a crucial role. We envision that these fundamental findings can deepen our understanding of the nucleation and development of condensed droplets in nanoscale, so as to optimize design strategies of superhydrophobic materials for a broad range of water-harvesting and heat-transfer systems.

Effect of ageing of K-feldspar on its ice nucleating efficiency in immersion, deposition and contact freezing modes

NASA Astrophysics Data System (ADS)

Peckhaus, Andreas; Bachmann, Felix; Hoffmann, Nadine; Koch, Michael; Kiselev, Alexei; Leisner, Thomas

2015-04-01

Recently K-feldspar was identified as one of the most active atmospheric ice nucleating particles (INP) of mineral origin [1]. Seeking the explanation to this phenomena we have conducted extensive experimental investigation of the ice nucleating efficiency of K-feldspar in three heterogeneous freezing modes. The immersion freezing of K-feldspar was investigated with the cold stage using arrays of nanoliter-size droplets containing aqueous suspension of polydisperse feldspar particles. For contact freezing, the charged droplets of supercooled water were suspended in the laminar flow of the DMA-selected feldspar-containing particles, allowing for determination of freezing probability on a single particle-droplet contact [2]. The nucleation and growth of ice via vapor deposition on the crystalline surfaces of macroscopic feldspar particles have been investigated in the Environmental Scanning Electron Microscope (ESEM) under humidified nitrogen atmosphere. The ice nucleation experiments were supplemented with measurements of effective surface area of feldspar particles and ion chromatography (IC) analysis of the leached framework cations (K+, Na+, Ca2+, Mg2+). In this contribution we focus on the role of surface chemistry influencing the IN efficiency of K-feldspar, in particular the connection between the degree of surface hydroxylation and its ability to induce local structural ordering in the interfacial layer in water molecules (as suggested by recent modeling efforts). We mimic the natural process of feldspar ageing by suspending it in water or weak aqueous solution of carbonic acid for different time periods, from minutes to months, and present its freezing efficiency as a function of time. Our immersion freezing experiments show that ageing have a nonlinear effect on the freezing behavior of feldspar within the investigated temperature range (-40°C to -10°C). On the other hand, deposition nucleation of ice observed in the ESEM reveals clear different pattern between freshly cleaved and aged mineral surfaces. This effect is especially pronounced for surfaces having different crystallographic orientations (001 and 010), with 001 being clearly preferential for ice nucleation. The factor two change of the BET effective area of the naturally aged feldspar particles is also indicative for the change in the surface morphology. Based on the IC analysis of framework cations removal from the surface of feldspar, we discuss the possible implications of this process for the interpretation of observed freezing behavior of feldspars. [1] Atkinson, J.D., Murray, B.J., Woodhouse, M.T., Whale, T.F., Baustian, K.J., Carslaw, K.S., Dobbie, S., O'Sullivan, D., and Malkin, T.L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds. Nature, 498, 355-358, 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., 6, 2373-2382, 2013.

Homogeneous ice nucleation and supercooled liquid water in orographic wave clouds

NASA Technical Reports Server (NTRS)

Heymsfield, Andrew J.; Miloshevich, Larry M.

1993-01-01

This study investigates ice nucleation mechanisms in cold lenticular wave clouds, a cloud type characterized by quasi-steady-state air motions and microphysical properties. It is concluded that homogeneous ice nucleation is responsible for the ice production in these clouds at temperatures below about -33 C. The lack of ice nucleation observed above -33 C indicates a dearth of ice-forming nuclei, and hence heterogeneous ice nucleation, in these clouds. Aircraft measurements in the temperature range -31 to -41 C show the following complement of simultaneous and abrupt changes in cloud properties that indicate a transition from the liquid phase to ice: disappearance of liquid water; decrease in relative humidity from near water saturation to ice saturation; increase in mean particle size; change in particle concentration; and change in temperature due to the release of latent heat. A numerical model of cloud particle growth and homogeneous ice nucleation is used to aid in interpretation of our in situ measurements. The abrupt changes in observed cloud properties compare favorably, both qualitatively and quantitatively, with results from the homogeneous ice nucleation model. It is shown that the homogeneous ice nucleation rates from the measurements are consistent with the temperature-dependent rates employed by the model (within a factor of 100, corresponding to about 1 C in temperature) in the temperature range -35 deg to -38 C. Given the theoretical basis of the modeled rates, it may be reasonable to apply them throughout the -30 to -50 C temperature range considered by the theory.

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

Biomass Burning Organic Aerosol as a Modulator of Droplet Number in the Southern Atlantic

NASA Astrophysics Data System (ADS)

Kacarab, M.; Howell, S. G.; Small Griswold, J. D.; Thornhill, K. L., II; Wood, R.; Redemann, J.; Nenes, A.

2017-12-01

Aerosols play a significant yet highly variable role in local and global air quality and climate. They act as cloud condensation nuclei (CCN) and both scatter and absorb radiation, lending a large source of uncertainty to climate predictions. Biomass burning organic aerosol (BBOA) can drastically elevate CCN concentrations, but the response in cloud droplet number may be suppressed or even reversed due to low supersaturations that develop from strong competition for water vapor. Constraining droplet response to BBOA is a key factor to understanding aerosol-cloud interactions. The southeastern Atlantic (SEA) cloud deck off the west coast of central Africa is a prime opportunity to study these cloud-BBOA interactions for marine stratocumulus as during winter in the southern hemisphere the SEA cloud deck is overlain by a large, optically thick BBOA plume. The NASA ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES) study focuses on increasing the understanding of how these BBOA affect the SEA cloud deck. Measurements of CCN concentration, aerosol size distribution and composition, updraft velocities, and cloud droplet number in and around the SEA cloud deck and associated BBOA plume were taken aboard the NASA P-3 aircraft during the first two years of the ORACLES campaign in September 2016 and August 2017. Here we evaluate the predicted and observed droplet number sensitivity to the aerosol fluctuations and quantify, using the data, the drivers of droplet number variability (vertical velocity or aerosol properties) as a function of biomass burning plume characteristics. Over the course of the campaign, different levels of BBOA influence in the marine boundary layer (MBL) were observed, allowing for comparison of cloud droplet number, hygroscopicity parameter (κ), and maximum in-cloud supersaturation over a range of "clean" and "dirty" conditions. Droplet number sensitivity to aerosol concentration, κ, and vertical updraft velocities are also evaluated. Generally, an increase in BBOA led to increased droplet number along with decreased κ and maximum in-cloud supersaturation (leading to an increase in competition for water vapor). This work seeks to contribute to an increased understanding of how CCN and aerosol properties affect the radiative and hydrological properties and impact of the cloud.

Spatial distribution of cloud droplets in a turbulent cloud-chamber flow

NASA Astrophysics Data System (ADS)

Jaczewski, A.; Malinowski, S. P.

2005-07-01

We present the results of a laboratory study of the spatial distribution of cloud droplets in a turbulent environment. An artificial, weakly turbulent cloud, consisting of droplets of diameter around 14 m, is observed in a laboratory chamber. Droplets on a vertical cross-section through the cloud interior are imaged using laser sheet photography. Images are digitized and numerically processed in order to retrieve droplet positions in a vertical plane. The spatial distribution of droplets in the range of scales, l, from 4 to 80 mm is characterized by: the clustering index CI(l), the volume averaged pair correlation function eta;(l) and a local density defined on a basis of correlation analysis. The results indicate that, even in weak turbulence in the chamber that is less intense and less intermittent than turbulence observed in clouds, droplets are not spread according to the Poisson distribution. The importance of this deviation from the Poisson distribution is unclear when looking at CI(l) and (l). The local density indicates that in small scales each droplet has, on average, more neighbours than expected from the average droplet concentration and gives a qualitative and intuitive measure of clustering.

Turbulent Mixing at the Edge of a Cloud

NASA Astrophysics Data System (ADS)

Shaw, Raymond; Beals, Matthew; Fugal, Jacob; Kumar, Bipin; Lu, Jiang; Schumacher, Joerg; Stith, Jeffrey

2013-11-01

Numerical and field experiments have been brought to bear on the question of how atmospheric clouds respond when they experience turbulent mixing with their environment. Simply put, we ask when a cloud is diluted, do all droplets evaporate uniformly (homogeneous mixing) or does a subset of droplets evaporate completely, leaving the remaining droplets unaffected (inhomogeneous mixing)? First, the entrainment of clear air and its subsequent mixing with a filament of cloudy air is studied in DNS that combine the Eulerian description of the turbulent velocity, temperature and vapor fields with a Lagrangian cloud droplet ensemble. The simulations provide guidance on the proper definition of the thermodynamic response time for the Damkoehler number, and demonstrate the transition from inhomogeneous to homogeneous mixing as mixing progresses within the inertial subrange. Second, an airborne digital holographic instrument (Holodec) shows that cloud edges are inhomogeneous at the centimeter scales. In local cloud volumes the droplet size distribution fluctuates strongly in number density but with a nearly unchanging mean droplet diameter, until the fluctuations finally cascade to the centimeter scale, when the droplet diameter begins to respond.

A Condensation-coalescence Cloud Model for Exoplanetary Atmospheres: Formulation and Test Applications to Terrestrial and Jovian Clouds

NASA Astrophysics Data System (ADS)

Ohno, Kazumasa; Okuzumi, Satoshi

2017-02-01

A number of transiting exoplanets have featureless transmission spectra that might suggest the presence of clouds at high altitudes. A realistic cloud model is necessary to understand the atmospheric conditions under which such high-altitude clouds can form. In this study, we present a new cloud model that takes into account the microphysics of both condensation and coalescence. Our model provides the vertical profiles of the size and density of cloud and rain particles in an updraft for a given set of physical parameters, including the updraft velocity and the number density of cloud condensation nuclei (CCNs). We test our model by comparing with observations of trade-wind cumuli on Earth and ammonia ice clouds in Jupiter. For trade-wind cumuli, the model including both condensation and coalescence gives predictions that are consistent with observations, while the model including only condensation overestimates the mass density of cloud droplets by up to an order of magnitude. For Jovian ammonia clouds, the condensation-coalescence model simultaneously reproduces the effective particle radius, cloud optical thickness, and cloud geometric thickness inferred from Voyager observations if the updraft velocity and CCN number density are taken to be consistent with the results of moist convection simulations and Galileo probe measurements, respectively. These results suggest that the coalescence of condensate particles is important not only in terrestrial water clouds but also in Jovian ice clouds. Our model will be useful to understand how the dynamics, compositions, and nucleation processes in exoplanetary atmospheres affect the vertical extent and optical thickness of exoplanetary clouds via cloud microphysics.

What does Reflection from Cloud Sides tell us about Vertical Distribution of Cloud Droplet Sizes?

NASA Technical Reports Server (NTRS)

Marshak, A.; Martins, J. V.; Zubko, V.; Kaufman, Y. J.

2006-01-01

Cloud development, the onset of precipitation and the effect of aerosol on clouds depend on the structure of the cloud profiles of droplet size and phase. Aircraft measurements of cloud profiles are limited in their temporal and spatial extent. Satellites were used to observe cloud tops not cloud profiles with vertical profiles of precipitation-sized droplets anticipated from CloudSat. The recently proposed CLAIM-3D satellite mission (cloud aerosol interaction mission in 3-D) suggests to measure profiles of cloud microphysical properties by retrieving them from the solar and infrared radiation reflected or emitted from cloud sides. Inversion of measurements from the cloud sides requires rigorous understanding of the 3-dimentional(3-D) properties of clouds. Here we discuss the reflected sunlight from the cloud sides and top at two wavelengths: one nonabsorbing to solar radiation (0.67 microns) and one with liquid water efficient absorption of solar radiation (2.1 microns). In contrast to the plane-parallel approximation, a conventional approach to all current operational retrievals, 3-D radiative transfer is used for interpreting the observed reflectances. General properties of the radiation reflected from the sides of an isolated cloud are discussed. As a proof of concept, the paper shows a few examples of radiation reflected from cloud fields generated by a simple stochastic cloud model with the prescribed vertically resolved microphysics. To retrieve the information about droplet sizes, we propose to use the probability density function of the droplet size distribution and its first two moments instead of the assumption about fixed values of the droplet effective radius. The retrieval algorithm is based on the Bayesian theorem that combines prior information about cloud structure and microphysics with radiative transfer calculations.

ARM Evaluation Product : Droplet Number Concentration Value-Added Product

DOE Data Explorer

Riihimaki, Laura

2014-05-15

Cloud droplet number concentration is an important factor in understanding aerosol-cloud interactions. As aerosol concentration increases, it is expected that droplet number concentration, Nd, will increase and droplet size decrease, for a given liquid water path (Twomey 1977), which will greatly affect cloud albedo as smaller droplets reflect more shortwave radiation. However, the magnitude and variability of these processes under different environmental conditions is still uncertain. McComiskey et al. (2009) have implemented a method, based on Boers and Mitchell (1994), for calculating Nd from ground-based remote sensing measurements of optical depth and liquid water path. They show that the magnitude of the aerosol-cloud interactions (ACI) varies with a range of factors, including the relative value of the cloud liquid water path (LWP), the aerosol size distribution, and the cloud updraft velocity. Estimates of Nd under a range of cloud types and conditions and at a variety of sites are needed to further quantify the impacts of aerosol cloud interactions.

Combustion Organic Aerosol as Cloud Condensation Nuclei in Ship Tracks.

NASA Astrophysics Data System (ADS)

Russell, Lynn M.; Noone, Kevin J.; Ferek, Ronald J.; Pockalny, Robert A.; Flagan, Richard C.; Seinfeld, John H.

2000-08-01

Polycyclic aromatic hydrocarbons (PAHs) have been sampled in marine stratiform clouds to identify the contribution of anthropogenic combustion emissions in activation of aerosol to cloud droplets. The Monterey Area Ship Track experiment provided an opportunity to acquire data on the role of organic compounds in ambient clouds and in ship tracks identified in satellite images. Identification of PAHs in cloud droplet residual samples indicates that several PAHs are present in cloud condensation nuclei in anthropogenically influenced air and do result in activated droplets in cloud. These results establish the presence of combustion products, such as PAHs, in submicrometer aerosols in anthropogenically influenced marine air, with enhanced concentrations in air polluted by ship effluent. The presence of PAHs in droplet residuals in anthropogenically influenced air masses indicates that some fraction of those combustion products is present in the cloud condensation nuclei that activate in cloud. Although a sufficient mass of droplet residuals was not collected to establish a similar role for organics from measurements in satellite-identified ship tracks, the available evidence from the fraction of organics present in the interstitial aerosol is consistent with part of the organic fraction partitioning to the droplet population. In addition, the probability that a compound will be found in cloud droplets rather than in the unactivated aerosol and the compound's water solubility are compared. The PAHs studied are only weakly soluble in water, but most of the sparse data collected support more soluble compounds having a higher probability of activation.

Crystallization of aqueous ammonium sulfate particles internally mixed with soot and kaolinite: crystallization relative humidities and nucleation rates.

PubMed

Pant, Atul; Parsons, Matthew T; Bertram, Allan K

2006-07-20

Using optical microscopy, we investigated the crystallization of aqueous ammonium sulfate droplets containing soot and kaolinite, as well as the crystallization of aqueous ammonium sulfate droplets free of solid material. Our results show that soot did not influence the crystallization RH of aqueous ammonium sulfate particles under our experimental conditions. In contrast, kaolinite increased the crystallization RH of the aqueous ammonium sulfate droplets by approximately 10%. In addition, our results show that the crystallization RH of aqueous ammonium sulfate droplets free of solid material does not depend strongly on particle size. This is consistent with conclusions made previously in the literature, based on comparisons of results from different laboratories. From the crystallization results we determined the homogeneous nucleation rates of crystalline ammonium sulfate in aqueous ammonium sulfate droplets and the heterogeneous nucleation rates of crystalline ammonium sulfate in aqueous ammonium sulfate particles containing kaolinite. Using classical nucleation theory and our experimental data, we determined that the interfacial tension between an ammonium sulfate critical nucleus and an aqueous ammonium sulfate solution is 0.064 +/- 0.003 J m(-2) (in agreement with our previous measurements), and the contact angle between an ammonium sulfate critical nucleus and a kaolinite surface is 59 +/- 2 degrees. On the basis of our results, we argue that soot will not influence the crystallization RH of aqueous ammonium sulfate droplets in the atmosphere, but kaolinite can significantly modify the crystallization RH of atmospheric ammonium sulfate droplets. As an example, the CRH50 (the relative humidity at which 50% of the droplets crystallize) ranges from about 41 to 51% RH when the diameter of the kaolinite inclusion ranges from 0.1 to 5 microm. For comparison, the CRH50 of aqueous ammonium sulfate droplets (0.5 microm diameter) free of solid material is approximately 34.3% RH under atmospheric conditions.

Effects of turbulence on the collision rate of cloud droplets

NASA Astrophysics Data System (ADS)

Ayala, Orlando

This dissertation concerns effects of air turbulence on the collision rate of atmospheric cloud droplets. This research was motivated by the speculation that air turbulence could enhance the collision rate thereby help transform cloud droplets to rain droplets in a short time as observed in nature. The air turbulence within clouds is assumed to be homogeneous and isotropic, and its small-scale motion (1 mm to 10 cm scales) is computationally generated by direct numerical integration of the full Navier-Stokes equations. Typical droplet and turbulence parameters of convective warm clouds are used to determine the Stokes numbers (St) and the nondimensional terminal velocities (Sv) which characterize droplet relative inertia and gravitational settling, respectively. A novel and efficient methodology for conducting direct numerical simulations (DNS) of hydrodynamically-interacting droplets in the context of cloud microphysics has been developed. This numerical approach solves the turbulent flow by the pseudo-spectral method with a large-scale forcing, and utilizes an improved superposition method to embed analytically the local, small-scale (10 mum to 1 mm) disturbance flows induced by the droplets. This hybrid representation of background turbulent air motion and the induced disturbance flows is then used to study the combined effects of hydrodynamic interactions and airflow turbulence on the motion and collisions of cloud droplets. Hybrid DNS results show that turbulence can increase the geometric collision kernel relative to the gravitational geometric kernel by as much as 42% due to enhanced radial relative motion and preferential concentration of droplets. The exact level of enhancements depends on the Taylor-microscale Reynolds number, turbulent dissipation rate, and droplet pair size ratio. One important finding is that turbulence has a relatively dominant effect on the collision process between droplets close in size as the gravitational collision mechanism diminishes. A theory was developed to predict the radial relative velocity between droplets at contact. The theory agrees with our DNS results to within 5% for cloud droplets with strong settling. In addition, an empirical model is developed to quantify the radial distribution function. (Abstract shortened by UMI.)

Parameterizations of Cloud Microphysics and Indirect Aerosol Effects

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

Tao, Wei-Kuo

1. OVERVIEW Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds [NRC, 2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e.,more » Twomey)" effect on the cloud droplet sizes for a constant liquid water path [Twomey, 1977] and the "semi-direct" effect on cloud coverage [e.g., Ackerman et al., 2000]. Enhanced aerosol concentrations can also suppress warm rain processes by producing a narrow droplet spectrum that inhibits collision and coalescence processes [e.g., Squires and Twomey, 1961; Warner and Twomey, 1967; Warner, 1968; Rosenfeld, 1999]. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect [Albrecht, 1989], is even more complex, especially for mixed-phase convective clouds. Table 1 summarizes the key observational studies identifying the microphysical properties, cloud characteristics, thermodynamics and dynamics associated with cloud systems from high-aerosol continental environments. For example, atmospheric aerosol concentrations can influence cloud droplet size distributions, warm-rain process, cold-rain process, cloud-top height, the depth of the mixed phase region, and occurrence of lightning. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing an enhanced source of cloud condensation nuclei (CCN). Hypotheses have been developed to explain the effect of urban regions on convection and precipitation [van den Heever and Cotton, 2007 and Shepherd, 2005]. Recently, a detailed spectral-bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and summertime convection over a mid-latitude continent with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. The impact of atmospheric aerosol concentration on cloud and precipitation will be investigated. 2. MODEL DESCRIPTION AND CASE STUDIES 2.1 GCE MODEL The model used in this study is the 2D version of the GCE model. Modeled flow is anelastic. Second- or higher-order advection schemes can produce negative values in the solution. Thus, a Multi-dimensional Positive Definite Advection Transport Algorithm (MPDATA) has been implemented into the model. All scalar variables (potential temperature, water vapor, turbulent coefficient and all five hydrometeor classes) use forward time differencing and the MPDATA for advection. Dynamic variables, u, v and w, use a second-order accurate advection scheme and a leapfrog time integration (kinetic energy semi-conserving method). Short-wave (solar) and long-wave radiation as well as a subgrid-scale TKE turbulence scheme are also included in the model. Details of the model can be found in Tao and Simpson (1993) and Tao et al. (2003). 2.2 Microphysics (Bin Model) The formulation of the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (cloud droplets and raindrops), and six types of ice particles: pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail. Each type is described by a special size distribution function containing 33 categories (bins). Atmospheric aerosols are also described using number density size-distribution functions (containing 33 bins). Droplet nucleation (activation) is derived from the analytical calculation of super-saturation, which is used to determine the sizes of aerosol particles to be activated and the corresponding sizes of nucleated droplets. Primary nucleation of each type of ice crystal takes place within certain temperature ranges. A detailed description of these explicitly parameterized processes can be found in Khain and Sednev (1996) and Khain et al. (1999, 2001). 2.3 Case Studies Three cases, a tropical oceanic squall system observed during TOGA COARE (Tropical Ocean and Global Atmosphere Coupled Ocean-Atmosphere Response Experiment, which occurred over the Pacific Ocean warm pool from November 1992 to February 1993), a midlatitude continental squall system observed during PRESTORM (Preliminary Regional Experiment for STORM-Central, which occurred in Kansas and Oklahoma during May-June 1985), and mid-afternoon convection observed during CRYSTAL-FACE (Cirrus Regional Study of Tropical Anvils and Cirrus Layers – Florida Area Cumulus Experiment, which occurred in Florida during July 2002), will be used to examine the impact of aerosols on deep, precipitating systems. 3. SUMMARY of RESULTS • For all three cases, higher CCN produces smaller cloud droplets and a narrower spectrum. Dirty conditions delay rain formation, increase latent heat release above the freezing level, and enhance vertical velocities at higher altitude for all cases. Stronger updrafts, deeper mixed-phase regions, and more ice particles are simulated with higher CCN in good agreement with observations. • In all cases, rain reaches the ground early with lower CCN. Rain suppression is also evident in all three cases with high CCN in good agreement with observations (Rosenfeld, 1999, 2000 and others). Rain suppression, however, only occurs during the first hour of simulation. This result suggests that microphysical processes dominate the impact of aerosols on precipitation in the early stage of precipitation development. • During the mature stage of the simulations, the effect of increasing aerosol concentration ranges from rain suppression in the PRESTORM case to little effect on surface rainfall in the CRYSTAL-FACE case to rain enhancement in the TOGA COARE case. • The model results suggest that evaporative cooling is a key process in determining whether higher CCN reduces or enhances precipitation. Cold pool strength can be enhanced by stronger evaporation. When cold pool interacts with the near surface wind shear, the low-level convergence can be stronger, facilitating secondary cloud formation and more vigorous precipitation processes. Evaporative cooling is more than two times stronger at low levels with higher CCN for the TOGA COARE case during the early stages of precipitation development. However, evaporative cooling is slightly stronger at lower levels with lower CCN for the PRESTORM case. The early formation of rain in the clean environment could allow for the formation of an earlier and stronger cold pool compared to a dirty environment. PRESTORM has a very dry environment and both large and small rain droplets can evaporate. Consequently, the cold pool is relatively weaker, and the system is relatively less intense with higher CCN. • Sensitivity tests are conducted to determine the impact of ice processes on aerosol-precipitation interaction. The results suggested that ice processes are crucial for suppressing precipitation due to high CCN for the PRESTORM case. More and smaller ice particles are generated in the dirty case and transported to the trailing stratiform region. This reduces the heavy convective rain and contributes to the weakening of the cold pool. Warm rain processes dominate the TOGA COARE case. Therefore, ice processes only play a secondary role in terms of aerosol-precipitation interaction. • Two of the three cloud systems presented in this paper formed a line structure (squall system). A 2D simulation, therefore, gives a good approximation to such a line of convective clouds. Since the real atmosphere is 3D, further 3D cloud-resolving simulations are needed to address aerosol-precipitation interactions. 4. REFERENCES Tao, W.-K., X. Li, A. Khain, T. Matsui, S. Lang, and J. Simpson, 2007: The role of atmospheric aerosol concentration on deep convective precipitation: Cloud-resolving model simulations. J. Geophy. Res., 112, D24S18, doi:10.1029/2007JD008728. All other references can be found in above paper. 5. Acknowledgements The GCE model is mainly supported by the NASA Headquarters Atmospheric Dynamics and Thermodynamics Program and the NASA Tropical Rainfall Measuring Mission (TRMM). The research was also supported by the Office of Science (BER), U. S. Department of Energy/Atmospheric Radiation Measurement (DOE/ARM) Interagency. The authors acknowledge NASA Goddard Space Flight Center for computer time used in this research.« less

What Does Reflection from Cloud Sides Tell Us About Vertical Distribution of Cloud Droplet Sizes?

NASA Technical Reports Server (NTRS)

Marshak, Alexander; Martins, J. Vanderlei; Zubko, Victor; Kaufman, Yoram, J.

2005-01-01

Cloud development, the onset of precipitation and the effect of aerosol on clouds depend on the structure of the cloud profiles of droplet size and phase. Aircraft measurements of cloud profiles are limited in their temporal and spatial extent. Satellites were used to observe cloud tops not cloud profiles with vertical profiles of precipitation-sized droplets anticipated from Cloudsat. The recently proposed CLAIM-3D satellite mission (cloud aerosol interaction mission in 3D) suggests to measure profiles of cloud microphysical properties by retrieving them from the solar and infrared radiation reflected or emitted from cloud sides. Inversion of measurements from the cloud sides requires rigorous understanding of the 3-dimensional (3D) properties of clouds. Here we discuss the reflected sunlight from the cloud sides and top at two wavelengths: one nonabsorbing to solar radiation (0.67 micrometers) and one with liquid water efficient absorption of solar radiation (2.1 micrometers). In contrast to the plane-parallel approximation, a conventional approach to all current operational retrievals, 3D radiative transfer is used for interpreting the observed reflectances. General properties of the radiation reflected from the sides of an isolated cloud are discussed. As a proof of concept, the paper shows a few examples of radiation reflected from cloud fields generated by a simple stochastic cloud model with the prescribed vertically resolved microphysics. To retrieve the information about droplet sizes, we propose to use the probability density function of the droplet size distribution and its first two moments instead of the assumption about fixed values of the droplet effective radius. The retrieval algorithm is based on the Bayesian theorem that combines prior information about cloud structure and microphysics with radiative transfer calculations.

Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures

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

Kürten, Andreas; Bianchi, Federico; Almeida, Joao

Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF ratesmore » spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 10 5 and 1 × 10 9cm -3, and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximumof ~1400 parts per trillion by volume (pptv).We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm -3 s -1 to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH 3 levels. In conclusion, we compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.« less

Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures

DOE PAGES

Kürten, Andreas; Bianchi, Federico; Almeida, Joao; ...

2016-10-27

Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF ratesmore » spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 10 5 and 1 × 10 9cm -3, and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximumof ~1400 parts per trillion by volume (pptv).We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm -3 s -1 to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH 3 levels. In conclusion, we compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.« less

Contrasting Cloud Composition Between Coupled and Decoupled Marine Boundary Layer Clouds

NASA Astrophysics Data System (ADS)

WANG, Z.; Mora, M.; Dadashazar, H.; MacDonald, A.; Crosbie, E.; Bates, K. H.; Coggon, M. M.; Craven, J. S.; Xian, P.; Campbell, J. R.; AzadiAghdam, M.; Woods, R. K.; Jonsson, H.; Flagan, R. C.; Seinfeld, J.; Sorooshian, A.

2016-12-01

Marine stratocumulus clouds often become decoupled from the vertical layer immediately above the ocean surface. This study contrasts cloud chemical composition between coupled and decoupled marine stratocumulus clouds. Cloud water and droplet residual particle composition were measured in clouds off the California coast during three airborne experiments in July-August of separate years (E-PEACE 2011, NiCE 2013, BOAS 2015). Decoupled clouds exhibited significantly lower overall mass concentrations in both cloud water and droplet residual particles, consistent with reduced cloud droplet number concentration and sub-cloud aerosol (Dp > 100 nm) number concentration, owing to detachment from surface sources. Non-refractory sub-micrometer aerosol measurements show that coupled clouds exhibit higher sulfate mass fractions in droplet residual particles, owing to more abundant precursor emissions from the ocean and ships. Consequently, decoupled clouds exhibited higher mass fractions of organics, nitrate, and ammonium in droplet residual particles, owing to effects of long-range transport from more distant sources. Total cloud water mass concentration in coupled clouds was dominated by sodium and chloride, and their mass fractions and concentrations exceeded those in decoupled clouds. Conversely, with the exception of sea salt constituents (e.g., Cl, Na, Mg, K), cloud water mass fractions of all species examined were higher in decoupled clouds relative to coupled clouds. These results suggest that an important variable is the extent to which clouds are coupled to the surface layer when interpreting microphysical data relevant to clouds and aerosol particles.

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.

Limits to the Indirect Aerosol Forcing in Stratocumulus

NASA Technical Reports Server (NTRS)

Ackerman, Andrew; Toon, O.; Stevens, D.; Coakley, J., Jr.

2003-01-01

The indirect radiative forcing of aerosols is poorly constrained by the observational data underlying the simple cloud parameterizations in GCMs. signal of cloud response to increased aerosol concentrations from meteorological noise. Recent satellite observations indicate a significant decrease of cloud water in ship tracks, in contrast to an ensemble of in situ measurements showing no average change in cloud water relative to the surrounding clouds. Both results contradict the expectation of cloud water increasing in polluted clouds. We find through large-eddy simulations of stratocumulus that the trend in the satellite data is likely an artifact of sampling only overcast clouds. The simulations instead show cloud cover increasing with droplet concentrations. The simulations also show that increases in cloud water from suppressing drizzle by increased droplet concentrations are favored at night or at extremely low droplet concentrations. At typical droplet concentrations we find that the Twomey effect on cloud albedo is amplified very little by the secondary indirect effect of drizzle suppression, largely because the absorption of solar radiation by cloud water reduces boundary-layer mixing in the daytime and thereby restricts any possible increase in cloud water from drizzle suppression. The cloud and boundary layer respond to radiative heating variations on a time scale of hours, and on longer time scales respond to imbalances between large-scale horizontal advection and the entrainment of inversion air. We analyze the co-varying response of cloud water, cloud thickness, width of droplet size distributions, and dispersion of the optical depth, as well as the overall response of cloud albedo, to changes in droplet concentrations. We also dissect the underlying physical mechanisms through sensitivity studies. Ship tracks represent an ideal natural laboratory to extricate the

What does reflection from cloud sides tell us about vertical distribution of cloud droplets?

NASA Technical Reports Server (NTRS)

Marshak, A.; Kaufman, Yoram; Martins, V.; Zubko, Victor

2006-01-01

In order to accurately measure the interaction of clouds with aerosols, we have to resolve the vertical distribution of cloud droplet sizes and determine the temperature of glaciation for clean and polluted clouds. Knowledge of the droplet vertical profile is also essential for understanding precipitation. So far, all existing satellites either measure cloud microphysics only at cloud top (e.g., MODIS) or give a vertical profile of precipitation sized droplets (e.g., Cloudsat). What if one measures cloud microphysical properties in the vertical by retrieving them from the solar and infrared radiation reflected or emitted from cloud sides? This was the idea behind CLAIM-3D (A 3D - cloud aerosol interaction mission) recently proposed by NASA GSFC. This presentation will focus on the interpretation of the radiation reflected from cloud sides. In contrast to plane-parallel approximation, a conventional approach to all current operational retrievals, 3D radiative transfer will be used for interpreting the observed reflectances. As a proof of concept, we will show a few examples of radiation reflected from cloud fields generated by a simple stochastic cloud model with prescribed microphysics. Instead of fixed values of the retrieved effective radii, the probability density functions of droplet size distributions will serve as possible retrievals.

Nucleation and growth mechanism of self-catalyzed InAs nanowires on silicon

NASA Astrophysics Data System (ADS)

Gomes, U. P.; Ercolani, D.; Zannier, V.; David, J.; Gemmi, M.; Beltram, F.; Sorba, L.

2016-06-01

We report on the nucleation and growth mechanism of self-catalyzed InAs nanowires (NWs) grown on Si (111) substrates by chemical beam epitaxy. Careful choices of the growth parameters lead to In-rich conditions such that the InAs NWs nucleate from an In droplet and grow by the vapor-liquid-solid mechanism while sustaining an In droplet at the tip. As the growth progresses, new NWs continue to nucleate on the Si (111) surface causing a spread in the NW size distribution. The observed behavior in NW nucleation and growth is described within a suitable existing theoretical model allowing us to extract relevant growth parameters. We argue that these results provide useful guidelines to rationally control the growth of self-catalyzed InAs NWs for various applications.

Thermodynamic wetness loss calculation in nozzle and turbine cascade: nucleating steam flow

NASA Astrophysics Data System (ADS)

Joseph, Joby; Subramanian, Sathyanarayanan; Vigney, K.; Prasad, B. V. S. S. S.; Biswas, D.

2017-11-01

Rapid expansion of steam in turbines and nozzles cause condensation. The formation of liquid droplets due to condensation results in wetness losses, which include aerodynamic losses (due to friction between liquid droplets and the vapour), thermodynamic losses (due to irreversible latent heat addition), and braking losses (due to the impact of liquid droplets on the turbine blade). In this study, a numerical investigation of the thermodynamic loss in a nucleating steam flow is performed. The thermodynamic loss is calculated using the change in entropy due to condensation. The effect of different operating conditions on the thermodynamic loss is estimated for a nozzle and turbine cascade in a nucleating flow. The non-equilibrium condensation in high-speed steam flows is modelled using Eulerian-Eulerian approach.

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.

An Oil-Stream Photomicrographic Aeroscope for Obtaining Cloud Liquid-Water Content and Droplet Size Distributions in Flight

NASA Technical Reports Server (NTRS)

Hacker, Paul T.

1956-01-01

An airborne cloud aeroscope by which droplet size, size distribution, and liquid-water content of clouds can be determined has been developed and tested in flight and in wind tunnels with water sprays. In this aeroscope the cloud droplets are continuously captured in a stream of oil, which Is then photographed by a photomicrographic camera. The droplet size and size distribution can be determined directly from the photographs. With the droplet size distribution known, the liquid-water content of the cloud can be computed from the geometry of the aeroscope, the airspeed, and the oil-flow rate. The aeroscope has the following features: Data are obtained semi-automatically, and permanent data are taken in the form of photographs. A single picture usually contains a sufficient number of droplets to establish the droplet size distribution. Cloud droplets are continuously captured in the stream of oil, but pictures are taken at Intervals. The aeroscope can be operated in icing and non-icing conditions. Because of mixing of oil in the instrument, the droplet-distribution patterns and liquid-water content values from a single picture are exponentially weighted average values over a path length of about 3/4 mile at 150 miles per hour. The liquid-water contents, volume-median diameters, and distribution patterns obtained on test flights and in the Lewis icing tunnel are similar to previously published data.

Kinetic Model of the Initial Stage of the Nanowire Growth

NASA Astrophysics Data System (ADS)

Filimonov, S. N.; Hervieu, Yu. Yu.

2018-03-01

A kinetic model of the formation of pyramid-like bulges (pedestals) at the bases of vertical nanowires is proposed. The formation of the pedestals at the early stage of the nanowire growth is assumed to be induced by a higher nucleation rate of two-dimensional islands under the catalyst droplet, as compared to the nucleation rate at the non-activated surface areas. Kinetics of the nucleation and propagation of the steps in the pyramid is described with a model of the multilayer growth, taking into account that the catalyst droplet at the nanowire top is a strong sink for adatoms. It is shown that the transition from the growth of the pyramid to the axial growth of the nanowire is possible if the appearance of a nucleus of the new layer under the catalyst droplet results in a partial dissolution of the underlying layer. In this case a segment of the nanowire sidewall is formed, preventing the lateral growth of the layers generated by the droplet.

Interface-Resolving Simulation of Collision Efficiency of Cloud Droplets

NASA Astrophysics Data System (ADS)

Wang, Lian-Ping; Peng, Cheng; Rosa, Bodgan; Onishi, Ryo

2017-11-01

Small-scale air turbulence could enhance the geometric collision rate of cloud droplets while large-scale air turbulence could augment the diffusional growth of cloud droplets. Air turbulence could also enhance the collision efficiency of cloud droplets. Accurate simulation of collision efficiency, however, requires capture of the multi-scale droplet-turbulence and droplet-droplet interactions, which has only been partially achieved in the recent past using the hybrid direct numerical simulation (HDNS) approach. % where Stokes disturbance flow is assumed. The HDNS approach has two major drawbacks: (1) the short-range droplet-droplet interaction is not treated rigorously; (2) the finite-Reynolds number correction to the collision efficiency is not included. In this talk, using two independent numerical methods, we will develop an interface-resolved simulation approach in which the disturbance flows are directly resolved numerically, combined with a rigorous lubrication correction model for near-field droplet-droplet interaction. This multi-scale approach is first used to study the effect of finite flow Reynolds numbers on the droplet collision efficiency in still air. Our simulation results show a significant finite-Re effect on collision efficiency when the droplets are of similar sizes. Preliminary results on integrating this approach in a turbulent flow laden with droplets will also be presented. This work is partially supported by the National Science Foundation.

Aerosol partitioning between the interstitial and the condensed phase in mixed-phase clouds

NASA Astrophysics Data System (ADS)

Verheggen, Bart; Cozic, Julie; Weingartner, Ernest; Bower, Keith; Mertes, Stephan; Connolly, Paul; Gallagher, Martin; Flynn, Michael; Choularton, Tom; Baltensperger, Urs

2007-12-01

The partitioning of aerosol particles between the cloud and the interstitial phase (i.e., unactivated aerosol) has been investigated during several Cloud and Aerosol Characterization Experiments (CLACE-3, CLACE-3? and CLACE-4) conducted in winter and summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m altitude, Switzerland). Ambient air was sampled using different inlets in order to determine the activated fraction of aerosol particles, FN, defined as the fraction of the total aerosol number concentration (with particle diameter dp > 100 nm) that has been incorporated into cloud particles. The liquid and ice water content of mixed-phase clouds were characterized by analyzing multiple cloud probes. The dependence of the activated fraction on several environmental factors is discussed on the basis of more than 900 h of in-cloud observations and parameterizations for key variables are given. FN is found to increase with increasing liquid water content and to decrease with increasing particle number concentration in liquid clouds. FN also decreases with increasing cloud ice mass fraction and with decreasing temperature from 0 to -25°C. The Wegener-Bergeron-Findeisen process probably contributed to this trend, since the presence of ice crystals causes liquid droplets to evaporate, thus releasing the formerly activated particles back into the interstitial phase. Ice nucleation could also have prevented additional cloud condensation nuclei from activating. The observed activation behavior has significant implications for our understanding of the indirect effect of aerosols on climate.

Regiospecific Nucleation and Growth of Silane Coupling Agent Droplets onto Colloidal Particles

PubMed Central

2017-01-01

Nucleation-and-growth processes are used extensively in the synthesis of spherical colloids, and more recently regiospecific nucleation-and-growth processes have been exploited to prepare more complex colloids such as patchy particles. We demonstrate that surface geometry alone can be made to play the dominant role in determining the final particle geometry in such syntheses, meaning that intricate chemical surface patternings are not required. We present a synthesis method for “lollipop”-shaped colloidal heterodimers (patchy particles), combining a recently published nucleation-and-growth technique with our recent findings that particle geometry influences the locus of droplet adsorption onto anisotropic template particles. Specifically, 3-methacryloxypropyl trimethoxysilane (MPTMS) is nucleated and grown onto bullet-shaped and nail-shaped colloids. The shape of the template particle can be chosen such that the MPTMS adsorbs regiospecifically onto the flat ends. In particular, we find that particles with a wider base increase the range of droplet volumes for which the minimum in the free energy of adsorption is located at the flat end of the particle compared with bullet-shaped particles of the same aspect ratio. We put forward an extensive analysis of the synthesis mechanism and experimentally determine the physical properties of the heterodimers, supported by theoretical simulations. Here we numerically optimize, for the first time, the shape of finite-sized droplets as a function of their position on the rod-like silica particle surface. We expect that our findings will give an impulse to complex particle creation by regiospecific nucleation and growth. PMID:29057028

Entrainment, Drizzle, and Stratocumulus Cloud Albedo

NASA Technical Reports Server (NTRS)

Ackerman, A. S.; Kirkpatrick, M. P.; Stevens, D. E.; Toon, O. B.

2004-01-01

Globally averaged cloud changes from GCMs on average show a doubling of the Twomey effect, which is the change in cloud albedo with respect to changes in droplet concentrations for fixed cloud water and droplet dispersion. In contrast, ship-track measurements show a much more modest amplification of the Twomey effect, suggesting that the GCMs are exaggerating the indirect aerosol effect. We have run large-eddy simulations with bin microphysics of marine stratocumulus from multiple field campaigns, and find that the large-eddy simulations are in much better agreement with the ship-track measurements. The inversion strength over N. Pacific stratocumulus (as measured during DYCOMS-II) is generally much stronger than over N. Atlantic stratocumulus (as measured during ASTEX), and we have found that the response of cloud water to increasing droplet concentration changes sign as the inversion strengthens. For the different environmental conditions, we will show the overall response of cloud albedo to droplet concentrations, and decompose the response into its contributing factors of changes in cloud water, droplet dispersion, and horizontal inhomogeneity.

The local environment of ice particles in arctic mixed-phase clouds

NASA Astrophysics Data System (ADS)

Schlenczek, Oliver; Fugal, Jacob P.; Schledewitz, Waldemar; Borrmann, Stephan

2015-04-01

During the RACEPAC field campaign in April and May 2014, research flights were made with the Polar 5 and Polar 6 aircraft from the Alfred Wegener Institute in Arctic clouds near Inuvik, Northwest Territories, Canada. One flight with the Polar 6 aircraft, done on May 16, 2014, flew under precipitating, stratiform, mid-level clouds with several penetrations through cloud base. Measurements with HALOHolo, an airborne digital in-line holographic instrument for cloud particles, show ice particles in a field of other cloud particles in a local three-dimensional sample volume (~14x19x130 mm3 or ~35 cm^3). Each holographic sample volume is a snapshot of a 3-dimensional piece of cloud at the cm-scale with typically thousands of cloud droplets per sample volume, so each sample volume yields a statistically significant droplet size distribution. Holograms are recorded at a rate of six times per second, which provides one volume sample approx. every 12 meters along the flight path. The size resolution limit for cloud droplets is better than 1 µm due to advanced sizing algorithms. Shown are preliminary results of, (1) the ice/liquid water partitioning at the cloud base and the distribution of water droplets around each ice particle, and (2) spatial and temporal variability of the cloud droplet size distributions at cloud base.

Controlling condensation and frost growth with chemical micropatterns.

PubMed

Boreyko, Jonathan B; Hansen, Ryan R; Murphy, Kevin R; Nath, Saurabh; Retterer, Scott T; Collier, C Patrick

2016-01-22

In-plane frost growth on chilled hydrophobic surfaces is an inter-droplet phenomenon, where frozen droplets harvest water from neighboring supercooled liquid droplets to grow ice bridges that propagate across the surface in a chain reaction. To date, no surface has been able to passively prevent the in-plane growth of ice bridges across the population of supercooled condensate. Here, we demonstrate that when the separation between adjacent nucleation sites for supercooled condensate is properly controlled with chemical micropatterns prior to freezing, inter-droplet ice bridging can be slowed and even halted entirely. Since the edge-to-edge separation between adjacent supercooled droplets decreases with growth time, deliberately triggering an early freezing event to minimize the size of nascent condensation was also necessary. These findings reveal that inter-droplet frost growth can be passively suppressed by designing surfaces to spatially control nucleation sites and by temporally controlling the onset of freezing events.

Controlling condensation and frost growth with chemical micropatterns

PubMed Central

Boreyko, Jonathan B.; Hansen, Ryan R.; Murphy, Kevin R.; Nath, Saurabh; Retterer, Scott T.; Collier, C. Patrick

2016-01-01

In-plane frost growth on chilled hydrophobic surfaces is an inter-droplet phenomenon, where frozen droplets harvest water from neighboring supercooled liquid droplets to grow ice bridges that propagate across the surface in a chain reaction. To date, no surface has been able to passively prevent the in-plane growth of ice bridges across the population of supercooled condensate. Here, we demonstrate that when the separation between adjacent nucleation sites for supercooled condensate is properly controlled with chemical micropatterns prior to freezing, inter-droplet ice bridging can be slowed and even halted entirely. Since the edge-to-edge separation between adjacent supercooled droplets decreases with growth time, deliberately triggering an early freezing event to minimize the size of nascent condensation was also necessary. These findings reveal that inter-droplet frost growth can be passively suppressed by designing surfaces to spatially control nucleation sites and by temporally controlling the onset of freezing events. PMID:26796663

The effect of different spectral shape parameterizations of cloud droplet size distribution on first and second aerosol indirect effects in NACR CAM5 and evaluation with satellite data

NASA Astrophysics Data System (ADS)

Wang, M.; Peng, Y.; Xie, X.; Liu, Y.

2017-12-01

Aerosol cloud interaction continues to constitute one of the most significant uncertainties for anthropogenic climate perturbations. The parameterization of cloud droplet size distribution and autoconversion process from large scale cloud to rain can influence the estimation of first and second aerosol indirect effects in global climate models. We design a series of experiments focusing on the microphysical cloud scheme of NCAR CAM5 (Community Atmospheric Model Version 5) in transient historical run with realistic sea surface temperature and sea ice. We investigate the effect of three empirical, two semi-empirical and one analytical expressions for droplet size distribution on cloud properties and explore the statistical relationships between aerosol optical thickness (AOT) and simulated cloud variables, including cloud top droplet effective radius (CDER), cloud optical depth (COD), cloud water path (CWP). We also introduce the droplet spectral shape parameter into the autoconversion process to incorporate the effect of droplet size distribution on second aerosol indirect effect. Three satellite datasets (MODIS Terra/ MODIS Aqua/ AVHRR) are used to evaluate the simulated aerosol indirect effect from the model. Evident CDER decreasing with significant AOT increasing is found in the east coast of China to the North Pacific Ocean and the east coast of USA to the North Atlantic Ocean. Analytical and semi-empirical expressions for spectral shape parameterization show stronger first aerosol indirect effect but weaker second aerosol indirect effect than empirical expressions because of the narrower droplet size distribution.

From Initial Nucleation to Cassie-Baxter State of Condensed Droplets on Nanotextured Superhydrophobic Surfaces

PubMed Central

Lv, Cunjing; Zhang, Xiwen; Niu, Fenglei; He, Feng; Hao, Pengfei

2017-01-01

Understanding how droplet condensation happens plays an essential role for our fundamental insights of wetting behaviors in nature and numerous applications. Since there is a lack of study of the initial formation and growing processes of condensed droplets down to nano-/submicroscale, relevant underlying mechanisms remain to be explored. We report an in situ observation of vapor condensation on nano-/microtextured superhydrophobic surfaces using optical microscopy. An interesting picture of the vapor condensation, from the initial appearance of individual small droplets (≤1 μm) to a Cassie-Baxter wetting state (>30 μm), are exhibited. It is found that individual droplets preferentially nucleate at the top and the edge of single micropillars with very high apparent contact angles on the nanotextures. Scenarios of two distinguished growing modes are reported statistically and the underlying mechanisms are discussed in the view of thermodynamics. We particularly reveal that the formation of the Cassie-Baxter wetting state is a result of a continuous coalescence of individual small droplets, in which the nanotexture-enhanced superhydrophobicity plays a crucial role. We envision that these fundamental findings can deepen our understanding of the nucleation and development of condensed droplets in nanoscale, so as to optimize design strategies of superhydrophobic materials for a broad range of water-harvesting and heat-transfer systems. PMID:28202939

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.

Enhancement of Cloud Cover and Suppression of Nocturnal Drizzle in Stratocumulus Polluted by Haze

NASA Technical Reports Server (NTRS)

Ackerman, Andrew S.; Toon, O. B.; Stevens, D. E.; Coakley, J. A., Jr.; Gore, Warren J. (Technical Monitor)

2002-01-01

Recent satellite observations indicate a significant decrease of cloud water in ship tracks, in contrast to an ensemble of in situ ship-track measurements that show no average change in cloud water relative to the surrounding clouds. We find through large-eddy simulations of stratocumulus that the trend in the satellite data is likely an artifact of sampling only overcast clouds. The simulations instead show cloud cover increasing with droplet concentrations. Our simulations also show that increases in cloud water from drizzle suppression (by increasing droplet concentrations) are favored at night or at extremely low droplet concentrations.

Stochastic growth of cloud droplets by collisions during settling

NASA Astrophysics Data System (ADS)

Madival, Deepak G.

2018-04-01

In the last stage of droplet growth in clouds which leads to drizzle formation, larger droplets begin to settle under gravity and collide and coalesce with smaller droplets in their path. In this article, we shall deal with the simplified problem of a large drop settling amidst a population of identical smaller droplets. We present an expression for the probability that a given large drop suffers a given number of collisions, for a general statistically homogeneous distribution of droplets. We hope that our approach will serve as a valuable tool in dealing with droplet distribution in real clouds, which has been found to deviate from the idealized Poisson distribution due to mechanisms such as inertial clustering.

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

Chitra Sivaraman, PNNL

Cloud droplet number concentration is an important factor in understanding aerosol-cloud interactions. As aerosol concentration increases, it is expected that droplet number concentration (Nd) will increase and droplet size will decrease, for a given liquid water path. This will greatly affect cloud albedo as smaller droplets reflect more shortwave radiation; however, the magnitude and variability of these processes under different environmental conditions is still uncertain.McComiskey et al. (2009) have implemented a method, based onBoers and Mitchell (1994), for calculating Nd from ground-based remote sensing measurements of optical depth and liquid water path. They show that the magnitude of the aerosol-cloudmore » interactions (ACI) varies with a range of factors, including the relative value of the cloud liquid water path (LWP), the aerosol size distribution, and the cloud updraft velocity. Estimates of Nd under a range of cloud types and conditions and at a variety of sites are needed to further quantify the impacts of aerosol cloud interactions. In order to provide data sets for studying aerosol-cloud interactions, the McComiskey et al. (2009) method was implemented as the Droplet Number Concentration (NDROP) value-added product (VAP).« less

Homogeneous crystal nucleation in Ni droplets

NASA Astrophysics Data System (ADS)

Kožíšek, Zdeněk; Demo, Pavel

2017-10-01

Crystal nucleation kinetics is often represented by induction times or metastable zone widths (Kulkarni et al., 2013; Bokeloh et al., 2011). Repeating measurements of supercooling or time delay, at which phase transition is detected, are statistically processed to determine the so-called survivorship function, from which nucleation rate is computed. The size distribution of nuclei is difficult to measure near the critical size directly, and it is not clear which amount of nuclei is formed at the moment when the phase transition is detected. In the present paper, kinetic nucleation equations are solved for the crystal nucleation in Ni liquid droplet to determine the number of nuclei formed within a considered system. Analysis of supercooling experimental data, based on the classical nucleation theory CNT), computes appropriate values of the nucleation rate. However, CNT underestimates the number of nuclei F (F ≪ 1 for supercritical sizes). Taking into account the dependence of the surface energy on nucleus size to data analysis overcomes this discrepancy and leads to reasonable values of the size distribution of nuclei.

Effect of ship-stack effluents on cloud reflectivity

NASA Technical Reports Server (NTRS)

Coakley, James A., Jr.; Bernstein, Robert L.; Durkee, Philip A.

1987-01-01

Under stable meteorological conditions the effect of ship-stack exhaust on overlying clouds was detected in daytime satellite images as an enhancement in cloud reflectivity at 3.7 micrometers. The exhaust is a source of cloud-condensation nuclei that increases the number of cloud droplets while reducing droplet size. This reduction in droplet size causes the reflectivity at 3.7 micrometers to be greater than the levels for nearby noncontaminated clouds of similar physical characteristics. The increase in droplet number causes the reflectivity at 0.63 micrometer to be significantly higher for the contaminated clouds despite the likelihood that the exhaust is a source of particles that absorb at visible wavelengths. The effect of aerosols on cloud reflectivity is expected to have a larger influence on the earth's albedo than that due to the direct scattering and absorption of sunlight by the aerosols alone.

Dimethylamine as a major alkyl amine species in particles and cloud water: Observations in semi-arid and coastal regions.

PubMed

Youn, J-S; Crosbie, E; Maudlin, L C; Wang, Z; Sorooshian, A

2015-12-01

Aerosol and cloud water measurements of dimethylamine (DMA), the most abundant amine in this study, were conducted in semi-arid (Tucson, Arizona) and marine (Nucleation in California Experiment, NiCE; central coast of California) areas. In both regions, DMA exhibits a unimodal aerosol mass size distribution with a dominant peak between 0.18 and 0.56 μm. Particulate DMA concentrations increase as a function of marine biogenic emissions, sulfate, BVOC emissions, and aerosol-phase water. Such data supports biogenic sources of DMA, aminium salt formation, and partitioning of DMA to condensed phases. DMA concentrations exhibit positive correlations with various trace elements and most especially vanadium, which warrants additional investigation. Cloud water DMA levels are enhanced significantly during wildfire periods unlike particulate DMA levels, including in droplet residual particles, due to effective dissolution of DMA into cloud water and probably DMA volatilization after drop evaporation. DMA:NH + 4 molar ratios peak between 0.18 and 1.0 μm depending on the site and time of year, suggesting that DMA competes better with NH 3 in those sizes in terms of reactive uptake by particles.

Integrated approach towards understanding interactions of mineral dust aerosol with warm clouds

NASA Astrophysics Data System (ADS)

Kumar, Prashant

2011-12-01

Mineral dust is ubiquitous in the atmosphere and represents a dominant type of particulate matter by mass. Dust particles can serve as cloud condensation nuclei (CCN), giant CCN (GCCN), or ice nuclei (IN), thereby, affecting cloud microphysics, albedo, and lifetime. Despite its well-recognized importance, assessments of dust impacts on clouds and climate remain highly uncertain. This thesis addresses the role of dust as CCN and GCCN with the goal of improving our understanding of dust-warm cloud interactions and their representation in climate models. Most studies to date focus on the soluble fraction of aerosol particles when describing cloud droplet nucleation, and overlook the interactions of the hydrophilic insoluble fraction with water vapor. A new approach to include such interactions (expressed by the process of water vapor adsorption) is explored, by combining multilayer Frenkel-Halsey-Hill (FHH) physical adsorption isotherm and curvature (Kelvin) effects. The importance of adsorption activation theory (FHH-AT) is corroborated by measurements of CCN activity of mineral aerosols generated from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. A new aerosol generation setup for CCN measurements was developed based on a dry generation technique capable of reproducing natural dust aerosol emission. Based on the dependence of critical supersaturation with particle dry diameter, it is found that the FHH-AT is a better framework for describing fresh (and unprocessed) dust CCN activity than the classical Kohler theory (KT). Ion Chromatography (IC) measurements performed on fresh regional dust samples indicate negligible soluble fraction, and support that water vapor adsorption is the prime source of CCN activity in the dust. CCN measurements with the commonly used wet generated mineral aerosol (from atomization of a dust aqueous suspension) are also carried out. Results indicate that the method is subject to biases as it generates a bimodal size distribution with a broad range of hygroscopicity. It is found that smaller particles generated in the more hygroscopic peak follow CCN activation by KT, while the larger peak is less hydrophilic with activation similar to dry generated dust that follow FHH-AT. Droplet activation kinetics measurements demonstrate that dry generated mineral aerosol display retarded activation kinetics with an equivalent water vapor uptake coefficient that is 30 - 80% lower relative to ammonium sulfate aerosol. Wet generated mineral aerosols, however, display similar activation kinetics to ammonium sulfate. These results suggest that at least a monolayer of water vapor (the rate-limiting step for adsorption) persists during the timescale of aerosol generation in the experiment, and questions the atmospheric relevance of studies on mineral aerosol generated from wet atomization method. A new parameterization of cloud droplet formation from insoluble dust CCN for regional and global climate models is also developed. The parameterization framework considers cloud droplet formation from dust CCN activating via FHH-AT, and soluble aerosol with activation described through KT. The parameterization is validated against a numerical parcel model, agreeing with predictions to within 10% (R2 ˜ 0.98). The potential role of dust GCCN activating by FHH-AT within warm stratocumulus and convective clouds is also evaluated. It is found that under pristine aerosol conditions, dust GCCN can act as collector drops with implications to dust-cloud-precipitation linkages. Biases introduced from describing dust GCCN activation by KT are also addressed. The results demonstrate that dust particles do not require deliquescent material to act as CCN in the atmosphere. Furthermore, the impact of dust particles as giant CCN on warm cloud and precipitation must be considered. Finally, the new parameterization of cloud droplet formation can be implemented in regional and global models providing an improved treatment of mineral aerosol on clouds and precipitation. The new framework is uniquely placed to address dust aerosol indirect effects on climate.

In situ observations of Arctic cloud properties across the Beaufort Sea marginal ice zone

NASA Astrophysics Data System (ADS)

Corr, C.; Moore, R.; Winstead, E.; Thornhill, K. L., II; Crosbie, E.; Ziemba, L. D.; Beyersdorf, A. J.; Chen, G.; Martin, R.; Shook, M.; Corbett, J.; Smith, W. L., Jr.; Anderson, B. E.

2016-12-01

Clouds play an important role in Arctic climate. This is particularly true over the Arctic Ocean where feedbacks between clouds and sea-ice impact the surface radiation budget through modifications of sea-ice extent, ice thickness, cloud base height, and cloud cover. This work summarizes measurements of Arctic cloud properties made aboard the NASA C-130 aircraft over the Beaufort Sea during ARISE (Arctic Radiation - IceBridge Sea&Ice Experiment) in September 2014. The influence of surface-type on cloud properties is also investigated. Specifically, liquid water content (LWC), droplet concentrations, and droplet size distributions are compared for clouds sampled over three distinct regimes in the Beaufort Sea: 1) open water, 2) the marginal ice zone, and 3) sea-ice. Regardless of surface type, nearly all clouds intercepted during ARISE were liquid-phase clouds. However, differences in droplet size distributions and concentrations were evident for the surface types; clouds over the MIZ and sea-ice generally had fewer and larger droplets compared to those over open water. The potential implication these results have for understanding cloud-surface albedo climate feedbacks in Arctic are discussed.

Flame Spread and Group-Combustion Excitation in Randomly Distributed Droplet Clouds with Low-Volatility Fuel near the Excitation Limit: a Percolation Approach Based on Flame-Spread Characteristics in Microgravity

NASA Astrophysics Data System (ADS)

Mikami, Masato; Saputro, Herman; Seo, Takehiko; Oyagi, Hiroshi

2018-03-01

Stable operation of liquid-fueled combustors requires the group combustion of fuel spray. Our study employs a percolation approach to describe unsteady group-combustion excitation based on findings obtained from microgravity experiments on the flame spread of fuel droplets. We focus on droplet clouds distributed randomly in three-dimensional square lattices with a low-volatility fuel, such as n-decane in room-temperature air, where the pre-vaporization effect is negligible. We also focus on the flame spread in dilute droplet clouds near the group-combustion-excitation limit, where the droplet interactive effect is assumed negligible. The results show that the occurrence probability of group combustion sharply decreases with the increase in mean droplet spacing around a specific value, which is termed the critical mean droplet spacing. If the lattice size is at smallest about ten times as large as the flame-spread limit distance, the flame-spread characteristics are similar to those over an infinitely large cluster. The number density of unburned droplets remaining after completion of burning attained maximum around the critical mean droplet spacing. Therefore, the critical mean droplet spacing is a good index for stable combustion and unburned hydrocarbon. In the critical condition, the flame spreads through complicated paths, and thus the characteristic time scale of flame spread over droplet clouds has a very large value. The overall flame-spread rate of randomly distributed droplet clouds is almost the same as the flame-spread rate of a linear droplet array except over the flame-spread limit.

The effects of van der Waals attractions on cloud droplet growth by coalescence

NASA Technical Reports Server (NTRS)

Rogers, Jan R.; Davis, Robert H.

1990-01-01

The inclusion of van der Waals attractions in the interaction between cloud droplets has been recently shown to significantly increase the collision efficiencies of the smaller droplets. In the current work, these larger values for the collision efficiencies are used in a population dynamics model of the droplet size distribution evolution with time, in hopes of at least partially resolving the long-standing paradox in cloud microphysics that predicted rates of the onset of precipitation are generally much lower than those which are observed. Evolutions of several initial cloud droplet spectra have been tracked in time. Size evolutions are compared as predicted from the use of collision efficiencies computed using two different models to allow for droplet-droplet contact: one which considers slip flow effects only, and one which considers the combined effects of van der Waals forces and slip flow. The rate at which the droplet mass density function shifts to larger droplet sizes is increased by typically 20-25 percent, when collision efficiencies which include van der Waals forces are used.

Magnetic control of heterogeneous ice nucleation with nanophase magnetite: Biophysical and agricultural implications.

PubMed

Kobayashi, Atsuko; Horikawa, Masamoto; Kirschvink, Joseph L; Golash, Harry N

2018-05-22

In supercooled water, ice nucleation is a stochastic process that requires ∼250-300 molecules to transiently achieve structural ordering before an embryonic seed crystal can nucleate. This happens most easily on crystalline surfaces, in a process termed heterogeneous nucleation; without such surfaces, water droplets will supercool to below -30 °C before eventually freezing homogeneously. A variety of fundamental processes depends on heterogeneous ice nucleation, ranging from desert-blown dust inducing precipitation in clouds to frost resistance in plants. Recent experiments have shown that crystals of nanophase magnetite (Fe 3 O 4 ) are powerful nucleation sites for this heterogeneous crystallization of ice, comparable to other materials like silver iodide and some cryobacterial peptides. In natural materials containing magnetite, its ferromagnetism offers the possibility that magneto-mechanical motion induced by external oscillating magnetic fields could act to disrupt the water-crystal interface, inhibiting the heterogeneous nucleation process in subfreezing water and promoting supercooling. For this to act, the magneto-mechanical rotation of the particles should be higher than the magnitude of Brownian motions. We report here that 10-Hz precessing magnetic fields, at strengths of 1 mT and above, on ∼50-nm magnetite crystals dispersed in ultrapure water, meet these criteria and do indeed produce highly significant supercooling. Using these rotating magnetic fields, we were able to elicit supercooling in two representative plant and animal tissues (celery and bovine muscle), both of which have detectable, natural levels of ferromagnetic material. Tailoring magnetic oscillations for the magnetite particle size distribution in different tissues could maximize this supercooling effect. Copyright © 2018 the Author(s). Published by PNAS.

An interfacial mechanism for cloud droplet formation on organic aerosols

DOE PAGES

Ruehl, C. R.; Davies, J. F.; Wilson, K. R.

2016-03-25

Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depressionmore » by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation.« less

An interfacial mechanism for cloud droplet formation on organic aerosols

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

Ruehl, C. R.; Davies, J. F.; Wilson, K. R.

Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depressionmore » by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation.« less

An interfacial mechanism for cloud droplet formation on organic aerosols.

PubMed

Ruehl, Christopher R; Davies, James F; Wilson, Kevin R

2016-03-25

Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depression by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation. Copyright © 2016, American Association for the Advancement of Science.

Aerosol indirect effect from turbulence-induced broadening of cloud-droplet size distributions.

PubMed

Chandrakar, Kamal Kant; Cantrell, Will; Chang, Kelken; Ciochetto, David; Niedermeier, Dennis; Ovchinnikov, Mikhail; Shaw, Raymond A; Yang, Fan

2016-12-13

The influence of aerosol concentration on the cloud-droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud-droplet growth and fallout. As aerosol concentration is increased, the cloud-droplet mean diameter decreases, as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics ([Formula: see text]) for high aerosol concentration, and slow microphysics ([Formula: see text]) for low aerosol concentration; here, [Formula: see text] is the phase-relaxation time and [Formula: see text] is the turbulence-correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as [Formula: see text], and the measurements are in excellent agreement with this finding. The result underscores the importance of droplet size dispersion for aerosol indirect effects: increasing aerosol concentration changes the albedo and suppresses precipitation formation not only through reduction of the mean droplet diameter but also by narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol/slow microphysics limit are likely of leading importance for precipitation formation.

An improved model of homogeneous nucleation for high supersaturation conditions: aluminum vapor.

PubMed

Savel'ev, A M; Starik, A M

2016-12-21

A novel model of stationary nucleation, treating the thermodynamic functions of small clusters, has been built. The model is validated against the experimental data on the nucleation rate of water vapor obtained in a broad range of supersaturation values (S = 10-120), and, at high supersaturation values, it reproduces the experimental data much better than the traditional classical nucleation model. A comprehensive analysis of the nucleation of aluminum vapor with the usage of developed stationary and non-stationary nucleation models has been performed. It has been shown that, at some value of supersaturation, there exists a double potential nucleation barrier. It has been revealed that the existence of this barrier notably delayed the establishment of a stationary distribution of subcritical clusters. It has also been demonstrated that the non-stationary model of the present work and the model of liquid-droplet approximation predict different values of nucleation delay time, τ s . In doing so, the liquid-droplet model can underestimate notably (by more than an order of magnitude) the value of τ s .

Nucleation and initial radius of self-catalyzed III-V nanowires

NASA Astrophysics Data System (ADS)

Dubrovskii, V. G.; Borie, S.; Dagnet, T.; Reynes, L.; André, Y.; Gil, E.

2017-02-01

We treat theoretically the initial nucleation step of self-catalyzed III-V nanowires under simultaneously deposited group III and V vapor fluxes and with surface diffusion of a group III element. Our model is capable of describing the droplet size at which the very first nanowire monolayer nucleates depending on the element fluxes and surface temperature. This size determines the initial nanowire radius in growth techniques without pre-deposition of gallium. We show that useful self-catalyzed III-V nanowires can form only under the appropriately balanced V/III flux ratios and temperatures. Such balance is required to obtain nucleation from reasonably sized droplets that are neither too small under excessive arsenic flux nor too large in the arsenic-poor conditions.

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.

Evaporation-triggered microdroplet nucleation and the four life phases of an evaporating Ouzo drop

NASA Astrophysics Data System (ADS)

Tan, Huanshu; Diddens, Christian; Lv, Pengyu; Kuerten, J. G. M.; Zhang, Xuehua; Lohse, Detlef

2016-11-01

Evaporating liquid droplets are omnipresent in nature and technology, such as in inkjet printing, coating, deposition of materials, medical diagnostics, agriculture, the food industry, cosmetics, or spills of liquids. Here we show that the evaporation of such ternary mixtures can trigger a phase transition and the nucleation of microdroplets of one of the components of the mixture. As a model system, we pick a sessile Ouzo droplet (as known from daily life) and reveal and theoretically explain its four life phases: In phase I, the spherical cap-shaped droplet remains transparent while the more volatile ethanol is evaporating, preferentially at the rim of the drop because of the singularity there. This leads to a local ethanol concentration reduction and correspondingly to oil droplet nucleation there. This is the beginning of phase II, in which oil microdroplets quickly nucleate in the whole drop, leading to its milky color that typifies the so-called "Ouzo effect." Once all ethanol has evaporated, the drop, which now has a characteristic nonspherical cap shape, has become clear again, with a water drop sitting on an oil ring (phase III), finalizing the phase inversion. Finally, in phase IV, all water has evaporated, leaving behind a tiny spherical cap-shaped oil drop.

A Condensation–coalescence Cloud Model for Exoplanetary Atmospheres: Formulation and Test Applications to Terrestrial and Jovian Clouds

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

Ohno, Kazumasa; Okuzumi, Satoshi

A number of transiting exoplanets have featureless transmission spectra that might suggest the presence of clouds at high altitudes. A realistic cloud model is necessary to understand the atmospheric conditions under which such high-altitude clouds can form. In this study, we present a new cloud model that takes into account the microphysics of both condensation and coalescence. Our model provides the vertical profiles of the size and density of cloud and rain particles in an updraft for a given set of physical parameters, including the updraft velocity and the number density of cloud condensation nuclei (CCNs). We test our modelmore » by comparing with observations of trade-wind cumuli on Earth and ammonia ice clouds in Jupiter. For trade-wind cumuli, the model including both condensation and coalescence gives predictions that are consistent with observations, while the model including only condensation overestimates the mass density of cloud droplets by up to an order of magnitude. For Jovian ammonia clouds, the condensation–coalescence model simultaneously reproduces the effective particle radius, cloud optical thickness, and cloud geometric thickness inferred from Voyager observations if the updraft velocity and CCN number density are taken to be consistent with the results of moist convection simulations and Galileo probe measurements, respectively. These results suggest that the coalescence of condensate particles is important not only in terrestrial water clouds but also in Jovian ice clouds. Our model will be useful to understand how the dynamics, compositions, and nucleation processes in exoplanetary atmospheres affect the vertical extent and optical thickness of exoplanetary clouds via cloud microphysics.« less

Cloud Microphysics Parameterization in a Shallow Cumulus Cloud Simulated by a Largrangian Cloud Model

NASA Astrophysics Data System (ADS)

Oh, D.; Noh, Y.; Hoffmann, F.; Raasch, S.

2017-12-01

Lagrangian cloud model (LCM) is a fundamentally new approach of cloud simulation, in which the flow field is simulated by large eddy simulation and droplets are treated as Lagrangian particles undergoing cloud microphysics. LCM enables us to investigate raindrop formation and examine the parameterization of cloud microphysics directly by tracking the history of individual Lagrangian droplets simulated by LCM. Analysis of the magnitude of raindrop formation and the background physical conditions at the moment at which every Lagrangian droplet grows from cloud droplets to raindrops in a shallow cumulus cloud reveals how and under which condition raindrops are formed. It also provides information how autoconversion and accretion appear and evolve within a cloud, and how they are affected by various factors such as cloud water mixing ratio, rain water mixing ratio, aerosol concentration, drop size distribution, and dissipation rate. Based on these results, the parameterizations of autoconversion and accretion, such as Kessler (1969), Tripoli and Cotton (1980), Beheng (1994), and Kharioutdonov and Kogan (2000), are examined, and the modifications to improve the parameterizations are proposed.

A~comprehensive parameterization of heterogeneous ice nucleation of dust surrogate: laboratory study with hematite particles and its application to atmospheric models

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Paukert, M.; Steinke, I.; Zhang, K.; Kulkarni, G.; Hoose, C.; Schnaiter, M.; Saathoff, H.; Möhler, O.

2014-06-01

A new heterogeneous ice nucleation parameterization that covers a~wide temperature range (-36 to -78 °C) is presented. Developing and testing such an ice nucleation parameterization, which is constrained through identical experimental conditions, is critical in order to accurately simulate the ice nucleation processes in cirrus clouds. The surface-scaled ice nucleation efficiencies of hematite particles, inferred by ns, were derived from AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber measurements under water subsaturated conditions that were realized by continuously changing temperature (T) and relative humidity with respect to ice (RHice) in the chamber. Our measurements showed several different pathways to nucleate ice depending on T and RHice conditions. For instance, almost T-independent freezing was observed at -60 °C < T < -50 °C, where RHice explicitly controlled ice nucleation efficiency, while both T and RHice played roles in other two T regimes: -78 °C < T < -60 °C and -50 °C < T < -36 °C. More specifically, observations at T colder than -60 °C revealed that higher RHice was necessary to maintain constant ns, whereas T may have played a significant role in ice nucleation at T warmer than -50 °C. We implemented new ns parameterizations into two cloud models to investigate its sensitivity and compare with the existing ice nucleation schemes towards simulating cirrus cloud properties. Our results show that the new AIDA-based parameterizations lead to an order of magnitude higher ice crystal concentrations and inhibition of homogeneous nucleation in colder temperature regions. Our cloud simulation results suggest that atmospheric dust particles that form ice nuclei at lower temperatures, below -36 °C, can potentially have stronger influence on cloud properties such as cloud longevity and initiation when compared to previous parameterizations.

A comprehensive parameterization of heterogeneous ice nucleation of dust surrogate: laboratory study with hematite particles and its application to atmospheric models

NASA Astrophysics Data System (ADS)

Hiranuma, N.; Paukert, M.; Steinke, I.; Zhang, K.; Kulkarni, G.; Hoose, C.; Schnaiter, M.; Saathoff, H.; Möhler, O.

2014-12-01

A new heterogeneous ice nucleation parameterization that covers a wide temperature range (-36 to -78 °C) is presented. Developing and testing such an ice nucleation parameterization, which is constrained through identical experimental conditions, is important to accurately simulate the ice nucleation processes in cirrus clouds. The ice nucleation active surface-site density (ns) of hematite particles, used as a proxy for atmospheric dust particles, were derived from AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber measurements under water subsaturated conditions. These conditions were achieved by continuously changing the temperature (T) and relative humidity with respect to ice (RHice) in the chamber. Our measurements showed several different pathways to nucleate ice depending on T and RHice conditions. For instance, almost T-independent freezing was observed at -60 °C < T < -50 °C, where RHice explicitly controlled ice nucleation efficiency, while both T and RHice played roles in other two T regimes: -78 °C < T < -60 °C and -50 °C < T < -36 °C. More specifically, observations at T lower than -60 °C revealed that higher RHice was necessary to maintain a constant ns, whereas T may have played a significant role in ice nucleation at T higher than -50 °C. We implemented the new hematite-derived ns parameterization, which agrees well with previous AIDA measurements of desert dust, into two conceptual cloud models to investigate their sensitivity to the new parameterization in comparison to existing ice nucleation schemes for simulating cirrus cloud properties. Our results show that the new AIDA-based parameterization leads to an order of magnitude higher ice crystal concentrations and to an inhibition of homogeneous nucleation in lower-temperature regions. Our cloud simulation results suggest that atmospheric dust particles that form ice nuclei at lower temperatures, below -36 °C, can potentially have a stronger influence on cloud properties, such as cloud longevity and initiation, compared to previous parameterizations.

A Comprehensive Parameterization of Heterogeneous Ice Nucleation of Dust Surrogate: Laboratory Study with Hematite Particles and Its Application to Atmospheric Models

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

Hiranuma, Naruki; Paukert, Marco; Steinke, Isabelle

2014-12-10

A new heterogeneous ice nucleation parameterization that covers a wide temperature range (-36 °C to -78 °C) is presented. Developing and testing such an ice nucleation parameterization, which is constrained through identical experimental conditions, is critical in order to accurately simulate the ice nucleation processes in cirrus clouds. The surface-scaled ice nucleation efficiencies of hematite particles, inferred by n s, were derived from AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber measurements under water subsaturated conditions that were realized by continuously changing temperature (T) and relative humidity with respect to ice (RH ice) in the chamber. Our measurementsmore » showed several different pathways to nucleate ice depending on T and RH ice conditions. For instance, almost independent freezing was observed at -60 °C < T < -50 °C, where RH ice explicitly controlled ice nucleation efficiency, while both T and RH ice played roles in other two T regimes: -78 °C < T < -60 °C and -50 °C < T < -36 °C. More specifically, observations at T colder than -60 °C revealed that higher RHice was necessary to maintain constant n s, whereas T may have played a significant role in ice nucleation at T warmer than -50 °C. We implemented new n s parameterizations into two cloud models to investigate its sensitivity and compare with the existing ice nucleation schemes towards simulating cirrus cloud properties. Our results show that the new AIDA-based parameterizations lead to an order of magnitude higher ice crystal concentrations and inhibition of homogeneous nucleation in colder temperature regions. Our cloud simulation results suggest that atmospheric dust particles that form ice nuclei at lower temperatures, below -36 °C, can potentially have stronger influence on cloud properties such as cloud longevity and initiation when compared to previous parameterizations.« less

Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine oxide particles in the coastal marine boundary layer

NASA Astrophysics Data System (ADS)

Murray, B. J.; Haddrell, A. E.; Peppe, S.; Davies, J. F.; Reid, J. P.; O'Sullivan, D.; Price, H. C.; Kumar, R.; Saunders, R. W.; Plane, J. M. C.; Umo, N. S.; Wilson, T. W.

2012-03-01

Iodine oxide particles are known to nucleate in the marine boundary layer where gas phase molecular iodine and organoiodine species are produced by macroalgae. There has been some debate over the chemical identity of these particles. Hygroscopic measurements have been used to infer that they are composed of insoluble I2O4, while elemental analysis of laboratory generated particles suggests soluble I2O5 or its hydrated form iodic acid, HIO3 (I2O5 · H2O). In this paper we explore the response of super-micron sized aqueous iodic acid solution droplets to varying humidity using both Raman microscopy and single particle electrodynamic traps. These measurements reveal that the propensity of an iodic acid solution droplet to crystallise is negligible on drying to ~0% relative humidity (RH). On applying mechanical pressure to these droplets they shatter in a manner consistent with an ultra-viscous liquid or a brittle glass, but subsequent water uptake between 10 and 20% RH causes their viscosity to reduce sufficiently that the cracked droplets flow and merge. The persistence of iodic acid solution in an amorphous state, rather than a crystalline state, suggests they will more readily accommodate other condensable material and are therefore more likely to grow to sizes where they may serve as cloud condensation nuclei. On increasing the humidity to ~90% the mass of the droplets only increases by ~20% with a corresponding increase in radius of only ~6 %, which is remarkably small for a highly soluble material. We suggest that the small growth factor of aqueous iodic acid solution droplets is consistent with the small aerosol growth factors observed in field experiments.

Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability.

PubMed

Ghan, Steven; Wang, Minghuai; Zhang, Shipeng; Ferrachat, Sylvaine; Gettelman, Andrew; Griesfeller, Jan; Kipling, Zak; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Zhang, Kai

2016-05-24

A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing.

Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability

PubMed Central

Ghan, Steven; Wang, Minghuai; Zhang, Shipeng; Ferrachat, Sylvaine; Gettelman, Andrew; Griesfeller, Jan; Kipling, Zak; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G.; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Zhang, Kai

2016-01-01

A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing. PMID:26921324

Ice nucleation active particles in continental air samples over Mainz, Germany

NASA Astrophysics Data System (ADS)

Pummer, Bernhard G.; Pöschl, Ulrich; Fröhlich-Nowoisky, Janine

2016-04-01

Aerosol particles are of central importance for atmospheric chemistry and physics, climate and public health. Some of these particles possess ice nucleation activity (INA), which is highly relevant for cloud formation and precipitation. In 2010, air filter samples were collected with a high-volume filter sampler separating fine and coarse particles (aerodynamic cut-off diameter 3 μm) in Mainz, Germany. In this study, the INA of the atmospheric particles deposited on these filters was determined. Therefore,they were extracted with ultrapure water, which was then measured in a droplet freezing assay, as described in Fröhlich-Nowoisky et al. (2015). The determined concentration of ice nucleators (INs) was between 0.3 and 2per m³ at 266 K, and between5 and 75 per m³ at 260 K. The INs were further characterized by different treatments, like heating (308 K, 371 K), filtration (0.1 μm, 300 kDa), and digestion with papain (10 mg/ml). We further investigated, which atmospheric conditions (e.g. weather) and distinguished events (e.g. dust storms, volcanic eruptions, and pollen peaks) influenced the number and nature of these INs. Fröhlich-Nowoisky, J., Hill, T. C. J., Pummer, B. G., Yordanova, P., Franc, G. D., and Pöschl, U.: Ice nucleation activity in the widespread soil fungus Mortierella alpina, Biogeosci., 12, 1057-1071, doi:10.5194/bg-12-1057-2015, 2015.

An improved ice cloud formation parameterization in the EMAC model

NASA Astrophysics Data System (ADS)

Bacer, Sara; Pozzer, Andrea; Karydis, Vlassis; Tsimpidi, Alexandra; Tost, Holger; Sullivan, Sylvia; Nenes, Athanasios; Barahona, Donifan; Lelieveld, Jos

2017-04-01

Cirrus clouds cover about 30% of the Earth's surface and are an important modulator of the radiative energy budget of the atmosphere. Despite their importance in the global climate system, there are still large uncertainties in understanding the microphysical properties and interactions with aerosols. Ice crystal formation is quite complex and a variety of mechanisms exists for ice nucleation, depending on aerosol characteristics and environmental conditions. Ice crystals can be formed via homogeneous nucleation or heterogeneous nucleation of ice-nucleating particles in different ways (contact, immersion, condensation, deposition). We have implemented the computationally efficient cirrus cloud formation parameterization by Barahona and Nenes (2009) into the EMAC (ECHAM5/MESSy Atmospheric Chemistry) model in order to improve the representation of ice clouds and aerosol-cloud interactions. The parameterization computes the ice crystal number concentration from precursor aerosols and ice-nucleating particles accounting for the competition between homogeneous and heterogeneous nucleation and among different freezing modes. Our work shows the differences and the improvements obtained after the implementation with respect to the previous version of EMAC.

The role of updraft velocity in temporal variability of cloud hydrometeor number

NASA Astrophysics Data System (ADS)

Sullivan, Sylvia; Nenes, Athanasios; Lee, Dong Min; Oreopoulos, Lazaros

2016-04-01

Significant effort has been dedicated to incorporating direct aerosol-cloud links, through parameterization of liquid droplet activation and ice crystal nucleation, within climate models. This significant accomplishment has generated the need for understanding which parameters affecting hydrometer formation drives its variability in coupled climate simulations, as it provides the basis for optimal parameter estimation as well as robust comparison with data, and other models. Sensitivity analysis alone does not address this issue, given that the importance of each parameter for hydrometer formation depends on its variance and sensitivity. To address the above issue, we develop and use a series of attribution metrics defined with adjoint sensitivities to attribute the temporal variability in droplet and crystal number to important aerosol and dynamical parameters. This attribution analysis is done both for the NASA Global Modeling and Assimilation Office Goddard Earth Observing System Model, Version 5 and the National Center for Atmospheric Research Community Atmosphere Model Version 5.1. Within the GEOS simulation, up to 48% of temporal variability in output ice crystal number and 61% in droplet number can be attributed to input updraft velocity fluctuations, while for the CAM simulation, they explain as much as 89% of the ice crystal number variability. This above results suggest that vertical velocity in both model frameworks is seen to be a very important (or dominant) driver of hydrometer variability. Yet, observations of vertical velocity are seldomly available (or used) to evaluate the vertical velocities in simulations; this strikingly contrasts the amount and quality of data available for aerosol-related parameters. Consequentially, there is a strong need for retrievals or measurements of vertical velocity for addressing this important knowledge gap that requires a significant investment and effort by the atmospheric community. The attribution metrics as a tool of understanding for hydrometer variability can be instrumental for understanding the source of differences between models used for aerosol-cloud-climate interaction studies.

A novel optical freezing array for the examination of cooling rate dependence in heterogeneous ice nucleation

NASA Astrophysics Data System (ADS)

Budke, Carsten; Dreischmeier, Katharina; Koop, Thomas

2014-05-01

Homogeneous ice nucleation is a stochastic process, implying that it is not only temperature but also time dependent. For heterogeneous ice nucleation it is still under debate whether there is a significant time dependence or not. In case of minor time dependence it is probably sufficient to use a singular or slightly modified singular approach, which mainly supposes temperature dependence and just small stochastic variations. We contribute to this discussion using a novel optical freezing array termed BINARY (Bielefeld Ice Nucleation ARraY). The setup consists of an array of microliter-sized droplets on a Peltier cooling stage. The droplets are separated from each other with a polydimethylsiloxane (PDMS) spacer to prevent a Bergeron-Findeisen process, in which the first freezing droplets grow at the expense of the remaining liquid ones due to their vapor pressure differences. An automatic detection of nucleation events is realized optically by the change in brightness during freezing. Different types of ice nucleating agents were tested with the presented setup, e. g. pollen and clay mineral dust. Exemplarily, cooling rate dependent measurements are shown for the heterogeneous ice nucleation induced by Snomax®. The authors gratefully acknowledge funding by the German Research Foundation (DFG) through the project BIOCLOUDS (KO 2944/1-1) and through the research unit INUIT (FOR 1525) under KO 2944/2-1. We particularly thank our INUIT partners for fruitful collaboration and sharing of ideas and IN samples.

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

On the Representation of Ice Nucleation in Global Climate Models, and its Importance for Simulations of Climate Forcings and Feedbacks

NASA Astrophysics Data System (ADS)

Storelvmo, T.

2015-12-01

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. Despite the growing effort in improving the cloud microphysical schemes in GCMs, most of this effort has not focused on improving the ability of GCMs to accurately simulate phase partitioning in mixed-phase clouds. Getting the relative proportion of liquid droplets and ice crystals in clouds right in GCMs is critical for the representation of cloud radiative forcings and cloud-climate feedbacks. Here, we first present satellite observations of cloud phase obtained by NASA's CALIOP instrument, and report on robust statistical relationships between cloud phase and several aerosols species that have been demonstrated to act as ice nuclei (IN) in laboratory studies. We then report on results from model intercomparison projects that reveal that GCMs generally underestimate the amount of supercooled liquid in clouds. For a selected GCM (NCAR 's CAM5), we thereafter show that the underestimate can be attributed to two main factors: i) the presence of IN in the mixed-phase temperature range, and ii) the Wegener-Bergeron-Findeisen process, which converts liquid to ice once ice crystals have formed. Finally, we show that adjusting these two processes such that the GCM's cloud phase is in agreement with the observed has a substantial impact on the simulated radiative forcing due to IN perturbations, as well as on the cloud-climate feedbacks and ultimately climate sensitivity simulated by the GCM.

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.

Negative Aerosol-Cloud re Relationship From Aircraft Observations Over Hebei, China

NASA Astrophysics Data System (ADS)

Zhao, Chuanfeng; Qiu, Yanmei; Dong, Xiaobo; Wang, Zhien; Peng, Yiran; Li, Baodong; Wu, Zhihui; Wang, Yang

2018-01-01

Using six flights observations in September 2015 over Hebei, China, this study shows a robust negative aerosol-cloud droplet effective radius (re) relationship for liquid clouds, which is different from previous studies that found positive aerosol-cloud re relationship over East China using satellite observations. A total of 27 cloud samples was analyzed with the classification of clean and polluted conditions using lower and upper 1/3 aerosol concentration at 200 m below the cloud bases. By normalizing the profiles of cloud droplet re, we found significant smaller values under polluted than under clean condition at most heights. Moreover, the averaged profiles of cloud liquid water content (LWC) show larger values under polluted than clean conditions, indicating even stronger negative aerosol-cloud re relationship if LWC is kept constant. The droplet size distributions further demonstrate that more droplets concentrate within smaller size ranges under polluted conditions. Quantitatively, the aerosol-cloud interaction is found around 0.10-0.19 for the study region.

An Instrument Employing a Coronal Discharge for the Determination of Droplet-Size Distribution in Clouds

NASA Technical Reports Server (NTRS)

Brun, Rinaldo J.; Levine, Joseph; Kleinknecht, Kenneth S.

1951-01-01

A flight instrument that uses electric means for measuring the droplet-size distribution in above-freezing clouds has been devised and given preliminary evaluation in flight. An electric charge is placed on the droplets and they are separated aerodynamically according to their mass. Because the charge placed on the droplets is a. function of the droplet size, the size spectrum can 'be determined by measurement of the charge deposited on cylinders of several different sizes placed to intercept the charged droplets. An expression for the rate of charge acquisition by a water droplet in a field of coronal discharge is derived. The results obtained in flight with an instrument based on the method described indicate that continuous records of droplet-size spectrum variations in clouds can be obtained. The experimental instrument was used to evaluate the method and was not refined to the extent necessary for obtaining conclusive meteorological data. The desirable features of an instrument based on the method described are (i) The instrument can be used in clouds with temperatures above freezing; (2) the size and the shape of the cylinders do not change during the exposure time; (3) the readings are instantaneous and continuous; (4) the available sensitivity permits the study of variations in cloud structures of less than 200 feet in extent.

New particle formation in the sulfuric acid-dimethylamine-water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

NASA Astrophysics Data System (ADS)

Kürten, Andreas; Li, Chenxi; Bianchi, Federico; Curtius, Joachim; Dias, António; Donahue, Neil M.; Duplissy, Jonathan; Flagan, Richard C.; Hakala, Jani; Jokinen, Tuija; Kirkby, Jasper; Kulmala, Markku; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Onnela, Antti; Rissanen, Matti P.; Simon, Mario; Sipilä, Mikko; Stozhkov, Yuri; Tröstl, Jasmin; Ye, Penglin; McMurry, Peter H.

2018-01-01

A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (˜ 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 106 and 3 × 107 cm-3, and dimethylamine mixing ratio of ˜ 40 pptv, i.e., 1 × 109 cm-3).

Remote Sensing the Vertical Profile of Cloud Droplet Effective Radius, Thermodynamic Phase, and Temperature

NASA Technical Reports Server (NTRS)

Martins, J. V.; Marshak, A.; Remer, L. A.; Rosenfeld, D.; Kaufman, Y. J.; Fernandez-Borda, R.; Koren, I.; Correia, A. L.; Zubko, V.; Artaxo, P.

2011-01-01

Cloud-aerosol interaction is a key issue in the climate system, affecting the water cycle, the weather, and the total energy balance including the spatial and temporal distribution of latent heat release. Information on the vertical distribution of cloud droplet microphysics and thermodynamic phase as a function of temperature or height, can be correlated with details of the aerosol field to provide insight on how these particles are affecting cloud properties and their consequences to cloud lifetime, precipitation, water cycle, and general energy balance. Unfortunately, today's experimental methods still lack the observational tools that can characterize the true evolution of the cloud microphysical, spatial and temporal structure in the cloud droplet scale, and then link these characteristics to environmental factors and properties of the cloud condensation nuclei. Here we propose and demonstrate a new experimental approach (the cloud scanner instrument) that provides the microphysical information missed in current experiments and remote sensing options. Cloud scanner measurements can be performed from aircraft, ground, or satellite by scanning the side of the clouds from the base to the top, providing us with the unique opportunity of obtaining snapshots of the cloud droplet microphysical and thermodynamic states as a function of height and brightness temperature in clouds at several development stages. The brightness temperature profile of the cloud side can be directly associated with the thermodynamic phase of the droplets to provide information on the glaciation temperature as a function of different ambient conditions, aerosol concentration, and type. An aircraft prototype of the cloud scanner was built and flew in a field campaign in Brazil.

A better understanding of POLDER's cloud droplet size retrieval: impact of cloud horizontal inhomogeneity and directional sampling

NASA Astrophysics Data System (ADS)

Shang, H.; Chen, L.; Bréon, F.-M.; Letu, H.; Li, S.; Wang, Z.; Su, L.

2015-07-01

The principles of the Polarization and Directionality of the Earth's Reflectance (POLDER) cloud droplet size retrieval requires that clouds are horizontally homogeneous. Nevertheless, the retrieval is applied by combining all measurements from an area of 150 km × 150 km to compensate for POLDER's insufficient directional sampling. Using the POLDER-like data simulated with the RT3 model, we investigate the impact of cloud horizontal inhomogeneity and directional sampling on the retrieval, and then analyze which spatial resolution is potentially accessible from the measurements. Case studies show that the sub-scale variability in droplet effective radius (CDR) can mislead both the CDR and effective variance (EV) retrievals. Nevertheless, the sub-scale variations in EV and cloud optical thickness (COT) only influence the EV retrievals and not the CDR estimate. In the directional sampling cases studied, the retrieval is accurate using limited observations and is largely independent of random noise. Several improvements have been made to the original POLDER droplet size retrieval. For example, the measurements in the primary rainbow region (137-145°) are used to ensure accurate large droplet (> 15 μm) retrievals and reduce the uncertainties caused by cloud heterogeneity. We apply the improved method using the POLDER global L1B data for June 2008, the new CDR results are compared with the operational CDRs. The comparison show that the operational CDRs tend to be underestimated for large droplets. The reason is that the cloudbow oscillations in the scattering angle region of 145-165° are weak for cloud fields with CDR > 15 μm. Lastly, a sub-scale retrieval case is analyzed, illustrating that a higher resolution, e.g., 42 km × 42 km, can be used when inverting cloud droplet size parameters from POLDER measurements.

Impact of Aerosol Processing on Orographic Clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, Sara; Zubler, Elias M.; Lohmann, Ulrike

2010-05-01

Aerosol particles undergo significant modifications during their residence time in the atmosphere. Physical processes like coagulation, coating and water uptake, and aqueous surface chemistry alter the aerosol size distribution and composition. At this, clouds play a primary role as physical and chemical processing inside cloud droplets contributes considerably to the changes in aerosol particles. A previous study estimates that on global average atmospheric particles are cycled three times through a cloud before being removed from the atmosphere [1]. An explicit and detailed treatment of cloud-borne particles has been implemented in the regional weather forecast and climate model COSMO-CLM. The employed model version includes a two-moment cloud microphysical scheme [2] that has been coupled to the aerosol microphysical scheme M7 [3] as described by Muhlbauer and Lohmann, 2008 [4]. So far, the formation, transfer and removal of cloud-borne aerosol number and mass were not considered in the model. Following the parameterization for cloud-borne particles developed by Hoose et al., 2008 [5], distinction between in-droplet and in-crystal particles is made to more physically account for processes in mixed-phase clouds, such as the Wegener-Bergeron-Findeisen process and contact and immersion freezing. In our model, this approach has been extended to allow for aerosol particles in five different hydrometeors: cloud droplets, rain drops, ice crystals, snow flakes and graupel. We account for nucleation scavenging, freezing and melting processes, autoconversion, accretion, aggregation, riming and selfcollection, collisions between interstitial aerosol particles and hydrometeors, ice multiplication, sedimentation, evaporation and sublimation. The new scheme allows an evaluation of the cloud cycling of aerosol particles by tracking the particles even when scavenged into hydrometeors. Global simulations of aerosol processing in clouds have recently been conducted by Hoose et al. [6]. Our investigation regarding the influence of aerosol processing will focus on the regional scale using a cloud-system resolving model with a much higher resolution. Emphasis will be placed on orographic mixed-phase precipitation. Different two-dimensional simulations of idealized orographic clouds will be conducted to estimate the effect of aerosol processing on orographic cloud formation and precipitation. Here, cloud lifetime, location and extent as well as the cloud type will be of particular interest. In a supplementary study, the new parameterization will be compared to observations of total and interstitial aerosol concentrations and size distribution at the remote high alpine research station Jungfraujoch in Switzerland. In addition, our simulations will be compared to recent simulations of aerosol processing in warm, mixed-phase and cold clouds, which have been carried out at the location of Jungfraujoch station [5]. References: [1] Pruppacher & Jaenicke (1995), The processing of water vapor and aerosols by atmospheric clouds, a global estimate, Atmos. Res., 38, 283295. [2] Seifert & Beheng (2006), A two-moment microphysics parameterization for mixed-phase clouds. Part 1: Model description, Meteorol. Atmos. Phys., 92, 4566. [3] Vignati et al. (2004), An efficient size-resolved aerosol microphysics module for large-scale transport models, J. Geophys. Res., 109, D22202 [4] Muhlbauer & Lohmann (2008), Sensitivity studies of the role of aerosols in warm-phase orographic precipitation in different flow regimes, J. Atmos. Sci., 65, 25222542. [5] Hoose et al. (2008), Aerosol processing in mixed-phase clouds in ECHAM5HAM: Model description and comparison to observations, J. Geophys. Res., 113, D071210. [6] Hoose et al. (2008), Global simulations of aerosol processing in clouds, Atmos. Chem. Phys., 8, 69396963.

Homogeneous nucleation and droplet growth in nitrogen. M.S. Thesis

NASA Technical Reports Server (NTRS)

Dotson, E. H.

1983-01-01

A one dimensional computer model of the homogeneous nucleation process and growth of condensate for nitrogen flows over airfoils is developed to predict the onset of condensation and thus to be able to take advantage of as much of Reynolds capability of cryogenic tunnels as possible. Homogeneous nucleation data were taken using a DFVLR CAST-10 airfoil in the 0.3-Meter Transonic Cryogenic Tunnel and are used to evaluate the classical liquid droplet theory and several proposed corrections to it. For predicting liquid nitrogen condensation effects, use of the arbitrary Tolman constant of 0.25 x 250 billionth m or the Reiss or Kikuchi correction agrees with the CAST-10 data. Because no solid nitrogen condensation were found experimentally during the CAST-10 experiments, earlier nozzle data are used to evaluate corrections to the classical liquid droplet theory in the lower temperature regime. A theoretical expression for the surface tension of solid nitrogen is developed.

Mechanism of supercooled droplet freezing on surfaces.

PubMed

Jung, Stefan; Tiwari, Manish K; Doan, N Vuong; Poulikakos, Dimos

2012-01-10

Understanding ice formation from supercooled water on surfaces is a problem of fundamental importance and general utility. Superhydrophobic surfaces promise to have remarkable 'icephobicity' and low ice adhesion. Here we show that their icephobicity can be rendered ineffective by simple changes in environmental conditions. Through experiments, nucleation theory and heat transfer physics, we establish that humidity and/or the flow of a surrounding gas can fundamentally switch the ice crystallization mechanism, drastically affecting surface icephobicity. Evaporative cooling of the supercooled liquid can engender ice crystallization by homogeneous nucleation at the droplet-free surface as opposed to the expected heterogeneous nucleation at the substrate. The related interplay between droplet roll-off and rapid crystallization is also studied. Overall, we bring a novel perspective to icing and icephobicity, unveiling the strong influence of environmental conditions in addition to the accepted effects of the surface conditions and hydrophobicity.

Aerosol indirect effect from turbulence-induced broadening of cloud-droplet size distributions

PubMed Central

Chandrakar, Kamal Kant; Cantrell, Will; Chang, Kelken; Ciochetto, David; Niedermeier, Dennis; Ovchinnikov, Mikhail; Shaw, Raymond A.; Yang, Fan

2016-01-01

The influence of aerosol concentration on the cloud-droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud-droplet growth and fallout. As aerosol concentration is increased, the cloud-droplet mean diameter decreases, as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τc<τt) for high aerosol concentration, and slow microphysics (τc>τt) for low aerosol concentration; here, τc is the phase-relaxation time and τt is the turbulence-correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τs−1=τc−1+τt−1, and the measurements are in excellent agreement with this finding. The result underscores the importance of droplet size dispersion for aerosol indirect effects: increasing aerosol concentration changes the albedo and suppresses precipitation formation not only through reduction of the mean droplet diameter but also by narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol/slow microphysics limit are likely of leading importance for precipitation formation. PMID:27911802

Aerosol indirect effect from turbulence-induced broadening of cloud-droplet size distributions

DOE PAGES

Chandrakar, Kamal Kant; Cantrell, Will; Chang, Kelken; ...

2016-11-28

Here, the influence of aerosol concentration on cloud droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud droplet growth and fallout. As aerosol concentration is increased the cloud droplet mean diameter decreases as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τ c < τ t) for high aerosol concentration, and slow microphysics (τ c > τ t) for low aerosolmore » concentration; here, τ c is the phase relaxation time and τ t is the turbulence correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τ s -1 =τ c -1 + τ t -1, and the measurements are in excellent agreement with this finding. This finding underscores the importance of droplet size dispersion for the aerosol indirect effect: increasing aerosol concentration not only suppresses precipitation formation through reduction of the mean droplet diameter, but perhaps more importantly, through narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol / slow microphysics limit are likely of leading importance for precipitation formation.« less

Aerosol indirect effect from turbulence-induced broadening of cloud-droplet size distributions

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

Chandrakar, Kamal Kant; Cantrell, Will; Chang, Kelken

Here, the influence of aerosol concentration on cloud droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud droplet growth and fallout. As aerosol concentration is increased the cloud droplet mean diameter decreases as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τ c < τ t) for high aerosol concentration, and slow microphysics (τ c > τ t) for low aerosolmore » concentration; here, τ c is the phase relaxation time and τ t is the turbulence correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τ s -1 =τ c -1 + τ t -1, and the measurements are in excellent agreement with this finding. This finding underscores the importance of droplet size dispersion for the aerosol indirect effect: increasing aerosol concentration not only suppresses precipitation formation through reduction of the mean droplet diameter, but perhaps more importantly, through narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol / slow microphysics limit are likely of leading importance for precipitation formation.« less

Aerosol indirect effect from turbulence-induced broadening of cloud-droplet size distributions

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

Chandrakar, Kamal Kant; Cantrell, Will; Chang, Kelken

2016-11-28

The influence of aerosol concentration on cloud droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud droplet growth and fallout. As aerosol concentration is increased the cloud droplet mean diameter decreases as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τ c < τ t) for high aerosol concentration, and slow microphysics (τ c > τ t) for low aerosol concentration;more » here, τ c is the phase relaxation time and τ t is the turbulence correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τ s -1 =τ c -1 + τ t -1, and the measurements are in excellent agreement with this finding. This finding underscores the importance of droplet size dispersion for the aerosol indirect effect: increasing aerosol concentration not only suppresses precipitation formation through reduction of the mean droplet diameter, but perhaps more importantly, through narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol / slow microphysics limit are likely of leading importance for precipitation formation.« less

The first observed cloud echoes and microphysical parameter retrievals by China's 94-GHz cloud radar

NASA Astrophysics Data System (ADS)

Wu, Juxiu; Wei, Ming; Hang, Xin; Zhou, Jie; Zhang, Peichang; Li, Nan

2014-06-01

By using the cloud echoes first successfully observed by China's indigenous 94-GHz SKY cloud radar, the macrostructure and microphysical properties of drizzling stratocumulus clouds in Anhui Province on 8 June 2013 are analyzed, and the detection capability of this cloud radar is discussed. The results are as follows. (1) The cloud radar is able to observe the time-varying macroscopic and microphysical parameters of clouds, and it can reveal the microscopic structure and small-scale changes of clouds. (2) The velocity spectral width of cloud droplets is small, but the spectral width of the cloud containing both cloud droplets and drizzle is large. When the spectral width is more than 0.4 m s-1, the radar reflectivity factor is larger (over -10 dBZ). (3) The radar's sensitivity is comparatively higher because the minimum radar reflectivity factor is about -35 dBZ in this experiment, which exceeds the threshold for detecting the linear depolarized ratio (LDR) of stratocumulus (commonly -11 to -14 dBZ; decreases with increasing turbulence). (4) After distinguishing of cloud droplets from drizzle, cloud liquid water content and particle effective radius are retrieved. The liquid water content of drizzle is lower than that of cloud droplets at the same radar reflectivity factor.

New Particle Formation in an Urban Atmosphere: The Role of Various Ingredients Investigated in the CLOUD Chamber

NASA Astrophysics Data System (ADS)

Baltensperger, U.; Xiao, M.; Hoyle, C.; Dada, L.; Garmash, O.; Stolzenburg, D.; Molteni, U.; Lehtipalo, K.; El-Haddad, I.; Dommen, J.

2017-12-01

Atmospheric aerosols play an important role on climate via aerosol-radiation interaction and aerosol-cloud interaction. The latter is strongly influenced by new particle formation (NPF). The physical and chemical mechanisms behind the NPF process are still under investigation. Great advancements were made in resolving chemical and physical mechanisms of NPF with a series of experiments conducted at the CLOUD (Cosmics Leaving Outdoor Droplets) chamber facility at CERN (Geneva, Switzerland), including binary nucleation of sulfuric acid - water, ternary nucleation of sulfuric acid - water with ammonia or dimethylamine as well as oxidation products (highly oxygenated molecules, HOMs) from biogenic precursors with and without the presence of sulfuric acid. Here, we investigate possible NPF mechanisms in urban atmospheres, where large populations are exposed to high aerosol concentrations; these mechanisms are still missing and are urgently needed. Urban atmospheres are highly polluted with high concentrations of SO2, ammonia, NOx and volatile organic vapors from anthropogenic activity as well as with high particle concentrations, which provide a high condensation sink for condensable gases. Aromatic hydrocarbons from industrial activities, traffic and residential combustion are present at high concentrations and contribute significantly to photochemical smog in the urban environment.The experiments were conducted at the CLOUD chamber facility during the CLOUD11 campaign in fall 2016. Three aromatic hydrocarbons were selected: toluene, 1,2,4-trimethylbenzene (1,2,4-TMB) and naphthalene (NPT). Experiments were also conducted with mixtures of the three aromatic hydrocarbons to better represent the urban atmosphere. All the experiments were conducted in the presence of sulfuric acid concentrations with or without the addition of ammonia and NOx. New particle formation rates and early growth rates derived for each precursor and their mixture, together with sulfuric acid and with or without the addition of ammonia and NOx will be reported.

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.

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

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-01-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented in the regional weather forecast and climate model COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snow flakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snow flakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. However, the processes not only impact the total aerosol number and mass, but also the shape of the aerosol size distributions by enhancing the internally mixed/soluble accumulation mode and generating coarse mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number concentration.

Examination of the potential impacts of dust and pollution aerosol acting as cloud nucleating aerosol on water resources in the Colorado River Basin

NASA Astrophysics Data System (ADS)

Jha, Vandana

In this study we examine the cumulative effect of dust acting as cloud nucleating aerosol (cloud condensation nuclei (CCN), giant cloud condensation nuclei (GCCN), and ice nuclei (IN)) along with anthropogenic aerosol pollution acting primarily as CCN, over the entire Colorado Rocky Mountains from the months of October to April in the year 2004-2005; the snow year. This ˜6.5 months analysis provides a range of snowfall totals and variability in dust and anthropogenic aerosol pollution. The specific objectives of this research is to quantify the impacts of both dust and pollution aerosols on wintertime precipitation in the Colorado Mountains using the Regional Atmospheric Modeling System (RAMS). In general, dust enhances precipitation primarily by acting as IN, while aerosol pollution reduces water resources in the CRB via the so-called "spill-over" effect, by enhancing cloud droplet concentrations and reducing riming rates. Dust is more episodic and aerosol pollution is more pervasive throughout the winter season. Combined response to dust and aerosol pollution is a net reduction of water resources in the CRB. The question is by how much are those water resources affected? Our best estimate is that total winter-season precipitation loss for for the CRB the 2004-2005 winter season due to the combined influence of aerosol pollution and dust is 5,380,00 acre-feet of water. Sensitivity studies for different cases have also been run for the specific cases in 2004-2005 winter season to analyze the impact of changing dust and aerosol ratios on precipitation in the Colorado River Basin. The dust is varied from 3 to 10 times in the experiments and the response is found to be non monotonic and depends on various environmental factors. The sensitivity studies show that adding dust in a wet system increases precipitation when IN affects are dominant. For a relatively dry system high concentrations of dust can result in over-seeding the clouds and reductions in precipitation. However, when adding dust to a system with warmer cloud bases, the response is non-monotonical, and when CCN affects are dominant, reductions in precipitation are found.

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 representation of aerosol activation and its influence on model-derived estimates of the aerosol indirect effect

NASA Astrophysics Data System (ADS)

Rothenberg, Daniel; Avramov, Alexander; Wang, Chien

2018-06-01

Interactions between aerosol particles and clouds contribute a great deal of uncertainty to the scientific community's understanding of anthropogenic climate forcing. Aerosol particles serve as the nucleation sites for cloud droplets, establishing a direct linkage between anthropogenic particulate emissions and clouds in the climate system. To resolve this linkage, the community has developed parameterizations of aerosol activation which can be used in global climate models to interactively predict cloud droplet number concentrations (CDNCs). However, different activation schemes can exhibit different sensitivities to aerosol perturbations in different meteorological or pollution regimes. To assess the impact these different sensitivities have on climate forcing, we have coupled three different core activation schemes and variants with the CESM-MARC (two-Moment, Multi-Modal, Mixing-state-resolving Aerosol model for Research of Climate (MARC) coupled with the National Center for Atmospheric Research's (NCAR) Community Earth System Model (CESM; version 1.2)). Although the model produces a reasonable present-day CDNC climatology when compared with observations regardless of the scheme used, ΔCDNCs between the present and preindustrial era regionally increase by over 100 % in zonal mean when using the most sensitive parameterization. These differences in activation sensitivity may lead to a different evolution of the model meteorology, and ultimately to a spread of over 0.8 W m-2 in global average shortwave indirect effect (AIE) diagnosed from the model, a range which is as large as the inter-model spread from the AeroCom intercomparison. Model-derived AIE strongly scales with the simulated preindustrial CDNC burden, and those models with the greatest preindustrial CDNC tend to have the smallest AIE, regardless of their ΔCDNC. This suggests that present-day evaluations of aerosol-climate models may not provide useful constraints on the magnitude of the AIE, which will arise from differences in model estimates of the preindustrial aerosol and cloud climatology.

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.

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.

Refreeze experiments with water droplets containing different types of ice nuclei interpreted by classical nucleation theory

NASA Astrophysics Data System (ADS)

Kaufmann, Lukas; Marcolli, Claudia; Luo, Beiping; Peter, Thomas

2017-03-01

Homogeneous nucleation of ice in supercooled water droplets is a stochastic process. In its classical description, the growth of the ice phase requires the emergence of a critical embryo from random fluctuations of water molecules between the water bulk and ice-like clusters, which is associated with overcoming an energy barrier. For heterogeneous ice nucleation on ice-nucleating surfaces both stochastic and deterministic descriptions are in use. Deterministic (singular) descriptions are often favored because the temperature dependence of ice nucleation on a substrate usually dominates the stochastic time dependence, and the ease of representation facilitates the incorporation in climate models. Conversely, classical nucleation theory (CNT) describes heterogeneous ice nucleation as a stochastic process with a reduced energy barrier for the formation of a critical embryo in the presence of an ice-nucleating surface. The energy reduction is conveniently parameterized in terms of a contact angle α between the ice phase immersed in liquid water and the heterogeneous surface. This study investigates various ice-nucleating agents in immersion mode by subjecting them to repeated freezing cycles to elucidate and discriminate the time and temperature dependences of heterogeneous ice nucleation. Freezing rates determined from such refreeze experiments are presented for Hoggar Mountain dust, birch pollen washing water, Arizona test dust (ATD), and also nonadecanol coatings. For the analysis of the experimental data with CNT, we assumed the same active site to be always responsible for freezing. Three different CNT-based parameterizations were used to describe rate coefficients for heterogeneous ice nucleation as a function of temperature, all leading to very similar results: for Hoggar Mountain dust, ATD, and larger nonadecanol-coated water droplets, the experimentally determined increase in freezing rate with decreasing temperature is too shallow to be described properly by CNT using the contact angle α as the only fit parameter. Conversely, birch pollen washing water and small nonadecanol-coated water droplets show temperature dependencies of freezing rates steeper than predicted by all three CNT parameterizations. Good agreement of observations and calculations can be obtained when a pre-factor β is introduced to the rate coefficient as a second fit parameter. Thus, the following microphysical picture emerges: heterogeneous freezing occurs at ice-nucleating sites that need a minimum (critical) surface area to host embryos of critical size to grow into a crystal. Fits based on CNT suggest that the critical active site area is in the range of 10-50 nm2, with the exact value depending on sample, temperature, and CNT-based parameterization. Two fitting parameters are needed to characterize individual active sites. The contact angle α lowers the energy barrier that has to be overcome to form the critical embryo at the site compared to the homogeneous case where the critical embryo develops in the volume of water. The pre-factor β is needed to adjust the calculated slope of freezing rate increase with temperature decrease. When this slope is steep, this can be interpreted as a high frequency of nucleation attempts, so that nucleation occurs immediately when the temperature is low enough for the active site to accommodate a critical embryo. This is the case for active sites of birch pollen washing water and for small droplets coated with nonadecanol. If the pre-factor is low, the frequency of nucleation attempts is low and the increase in freezing rate with decreasing temperature is shallow. This is the case for Hoggar Mountain dust, the large droplets coated with nonadecanol, and ATD. Various hypotheses why the value of the pre-factor depends on the nature of the active sites are discussed.

Performance of some nucleation theories with a nonsharp droplet-vapor interface.

PubMed

Napari, Ismo; Julin, Jan; Vehkamäki, Hanna

2010-10-21

Nucleation theories involving the concept of nonsharp boundary between the droplet and vapor are compared to recent molecular dynamics (MD) simulation data of Lennard-Jones vapors at temperatures above the triple point. The theories are diffuse interface theory (DIT), extended modified liquid drop-dynamical nucleation theory (EMLD-DNT), square gradient theory (SGT), and density functional theory (DFT). Particular attention is paid to thermodynamic consistency in the comparison: the applied theories either use or, with a proper parameter adjustment, result in the same values of equilibrium vapor pressure, bulk liquid density, and surface tension as the MD simulations. Realistic pressure-density correlations are also used. The best agreement between the simulated nucleation rates and calculations is obtained from DFT, SGT, and EMLD-DNT, all of which, in the studied temperature range, show deviations of less than one order of magnitude in the nucleation rate. DIT underestimates the nucleation rate by up to two orders of magnitude. DFT and SGT give the best estimate of the molecular content of the critical nuclei. Overall, at the vapor conditions of this study, all the investigated theories perform better than classical nucleation theory in predicting nucleation rates.

Uncertainty in aerosol hygroscopicity resulting from semi-volatile organic compounds

NASA Astrophysics Data System (ADS)

Goulden, Olivia; Crooks, Matthew; Connolly, Paul

2018-01-01

We present a novel method of exploring the effect of uncertainties in aerosol properties on cloud droplet number using existing cloud droplet activation parameterisations. Aerosol properties of a single involatile particle mode are randomly sampled within an uncertainty range and resulting maximum supersaturations and critical diameters calculated using the cloud droplet activation scheme. Hygroscopicity parameters are subsequently derived and the values of the mean and uncertainty are found to be comparable to experimental observations. A recently proposed cloud droplet activation scheme that includes the effects of co-condensation of semi-volatile organic compounds (SVOCs) onto a single lognormal mode of involatile particles is also considered. In addition to the uncertainties associated with the involatile particles, concentrations, volatility distributions and chemical composition of the SVOCs are randomly sampled and hygroscopicity parameters are derived using the cloud droplet activation scheme. The inclusion of SVOCs is found to have a significant effect on the hygroscopicity and contributes a large uncertainty. For non-volatile particles that are effective cloud condensation nuclei, the co-condensation of SVOCs reduces their actual hygroscopicity by approximately 25 %. A new concept of an effective hygroscopicity parameter is introduced that can computationally efficiently simulate the effect of SVOCs on cloud droplet number concentration without direct modelling of the organic compounds. These effective hygroscopicities can be as much as a factor of 2 higher than those of the non-volatile particles onto which the volatile organic compounds condense.

Chemical consequences of the initial diffusional growth of cloud droplets - A clean marine case

NASA Technical Reports Server (NTRS)

Twohy, C. H.; Charlson, R. J.; Austin, P. H.

1989-01-01

A simple microphysical cloud parcel model and a simple representation of the background marine aerosol are used to predict the concentrations and compositions of droplets of various sizes near cloud base. The aerosol consists of an externally-mixed ammonium bisulfate accumulation mode and a sea-salt coarse particle mode. The difference in diffusional growth rates between the small and large droplets as well as the differences in composition between the two aerosol modes result in substantial differences in solute concentration and composition with size of droplets in the parcel. The chemistry of individual droplets is not, in general, representative of the bulk (volume-weighted mean) cloud water sample. These differences, calculated to occur early in the parcel's lifetime, should have important consequences for chemical reactions such as aqueous phase sulfate production.

Quantifying the radiative and microphysical impacts of fire aerosols on cloud dynamics in the tropics using temporally offset satellite observations

NASA Astrophysics Data System (ADS)

Tosca, M. G.; Diner, D. J.; Garay, M. J.; Kalashnikova, O.

2013-12-01

Anthropogenic fires in Southeast Asia and Central America emit smoke that affects cloud dynamics, meteorology, and climate. We measured the cloud response to direct and indirect forcing from biomass burning aerosols using aerosol retrievals from the Multi-angle Imaging SpectroRadiometer (MISR) and non-synchronous cloud retrievals from the MODerate resolution Imaging Spectroradiometer (MODIS) from collocated morning and afternoon overpasses. Level 2 data from thirty-one individual scenes acquired between 2006 and 2010 were used to quantify changes in cloud fraction, cloud droplet size, cloud optical depth and cloud top temperature from morning (10:30am local time) to afternoon (1:30pm local time) in the presence of varying aerosol burdens. We accounted for large-scale meteorological differences between scenes by normalizing observed changes to the mean difference per individual scene. Elevated AODs reduced cloud fraction and cloud droplet size and increased cloud optical depths in both Southeast Asia and Central America. In mostly cloudy regions, aerosols significantly reduced cloud fraction and cloud droplet sizes, but in clear skies, cloud fraction, cloud optical thickness and cloud droplet sizes increased. In clouds with vertical development, aerosols reduced cloud fraction via semi-direct effects but spurred cloud growth via indirect effects. These results imply a positive feedback loop between anthropogenic burning and cloudiness in both Central America and Southeast Asia, and are consistent with previous studies linking smoke aerosols to both cloud reduction and convective invigoration.

Retrievals of Cloud Droplet Size from the RSP Data: Validation Using in Situ Measurements

NASA Technical Reports Server (NTRS)

Alexandrov, Mikhail D.; Cairns, Brian; Sinclair, Kenneth; Wasilewski, Andrzej P.; Ziemba, Luke; Crosbie, Ewan; Hair, John; Hu, Yongxiang; Hostetler, Chris; Stamnes, Snorre

2016-01-01

We present comparisons of cloud droplet size distributions retrieved from the Research Scanning Polarimeter (RSP) data with correlative in situ measurements made during the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES). This field experiment was based at St. Johns airport, Newfoundland, Canada with the latest deployment in May - June 2016. RSP was onboard the NASA C-130 aircraft together with an array of in situ and other remote sensing instrumentation. The RSP is an along-track scanner measuring polarized and total reflectances in9 spectral channels. Its unique high angular resolution allows for characterization of liquid water droplet size using the rainbow structure observed in the polarized reflectances in the scattering angle range between 135 and 165 degrees. A parametric fitting algorithm applied to the polarized reflectances provides retrievals of the droplet effective radius and variance assuming a prescribed size distribution shape (gamma distribution). In addition to this, we use a non-parametric method, Rainbow Fourier Transform (RFT), which allows us to retrieve the droplet size distribution (DSD) itself. The latter is important in the case of clouds with complex structure, which results in multi-modal DSDs. During NAAMES the aircraft performed a number of flight patterns specifically designed for comparison of remote sensing retrievals and in situ measurements. These patterns consisted of two flight segments above the same straight ground track. One of these segments was flown above clouds allowing for remote sensing measurements, while the other was at the cloud top where cloud droplets were sampled. We compare the DSDs retrieved from the RSP data with in situ measurements made by the Cloud Droplet Probe (CDP). The comparisons show generally good agreement with deviations explainable by the position of the aircraft within cloud and by presence of additional cloud layers in RSP view that do not contribute to the in situ DSDs. In the latter case the distributions retrieved from the RSP data were consistent with the multi-layer cloud structures observed in the correlative High Spectral Resolution Lidar (HSRL) profiles. The comparison results provide a rare validation of polarimetric droplet size retrieval techniques, which can be used for analysis of satellite data on global scale.

Surface tension prevails over solute effect in organic-influenced cloud droplet activation.

PubMed

Ovadnevaite, Jurgita; Zuend, Andreas; Laaksonen, Ari; Sanchez, Kevin J; Roberts, Greg; Ceburnis, Darius; Decesari, Stefano; Rinaldi, Matteo; Hodas, Natasha; Facchini, Maria Cristina; Seinfeld, John H; O' Dowd, Colin

2017-06-29

The spontaneous growth of cloud condensation nuclei (CCN) into cloud droplets under supersaturated water vapour conditions is described by classic Köhler theory. This spontaneous activation of CCN depends on the interplay between the Raoult effect, whereby activation potential increases with decreasing water activity or increasing solute concentration, and the Kelvin effect, whereby activation potential decreases with decreasing droplet size or increases with decreasing surface tension, which is sensitive to surfactants. Surface tension lowering caused by organic surfactants, which diminishes the Kelvin effect, is expected to be negated by a concomitant reduction in the Raoult effect, driven by the displacement of surfactant molecules from the droplet bulk to the droplet-vapour interface. Here we present observational and theoretical evidence illustrating that, in ambient air, surface tension lowering can prevail over the reduction in the Raoult effect, leading to substantial increases in cloud droplet concentrations. We suggest that consideration of liquid-liquid phase separation, leading to complete or partial engulfing of a hygroscopic particle core by a hydrophobic organic-rich phase, can explain the lack of concomitant reduction of the Raoult effect, while maintaining substantial lowering of surface tension, even for partial surface coverage. Apart from the importance of particle size and composition in droplet activation, we show by observation and modelling that incorporation of phase-separation effects into activation thermodynamics can lead to a CCN number concentration that is up to ten times what is predicted by climate models, changing the properties of clouds. An adequate representation of the CCN activation process is essential to the prediction of clouds in climate models, and given the effect of clouds on the Earth's energy balance, improved prediction of aerosol-cloud-climate interactions is likely to result in improved assessments of future climate change.

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

Improvements for retrieval of cloud droplet size by the POLDER instrument

NASA Astrophysics Data System (ADS)

Shang, H.; Husi, L.; Bréon, F. M.; Ma, R.; Chen, L.; Wang, Z.

2017-12-01

The principles of cloud droplet size retrieval via Polarization and Directionality of the Earth's Reflectance (POLDER) requires that clouds be horizontally homogeneous. The retrieval is performed by combining all measurements from an area of 150 km × 150 km to compensate for POLDER's insufficient directional sampling. Using POLDER-like data simulated with the RT3 model, we investigate the impact of cloud horizontal inhomogeneity and directional sampling on the retrieval and analyze which spatial resolution is potentially accessible from the measurements. Case studies show that the sub-grid-scale variability in droplet effective radius (CDR) can significantly reduce valid retrievals and introduce small biases to the CDR ( 1.5µm) and effective variance (EV) estimates. Nevertheless, the sub-grid-scale variations in EV and cloud optical thickness (COT) only influence the EV retrievals and not the CDR estimate. In the directional sampling cases studied, the retrieval using limited observations is accurate and is largely free of random noise. Several improvements have been made to the original POLDER droplet size retrieval. For example, measurements in the primary rainbow region (137-145°) are used to ensure retrievals of large droplet (>15 µm) and to reduce the uncertainties caused by cloud heterogeneity. A premium resoltion of 0.8° is determined by considering successful retrievals and cloud horizontal homogeneity. The improved algorithm is applied to measurements of POLDER in 2008, and we further compared our retrievals with cloud effective radii estimations of Moderate Resolution Imaging Spectroradiometer (MODIS). The results indicate that in global scale, the cloud effective radii and effective variance is larger in the central ocean than inland and coast areas. Over heavy polluted regions, the cloud droplets has small effective radii and narraw distribution due to the influence of aerosol particles.

Direct Observations of Isoprene Secondary Organic Aerosol Formation in Ambient Cloud Droplets

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Bell, D.; Thornton, J. A.; Fast, J. D.; Shrivastava, M. B.; Berg, L. K.; Imre, D. G.; Mei, F.; Shilling, J.; Suski, K. J.; Liu, J.; Tomlinson, J. M.; Wang, J.

2017-12-01

Multiphase chemistry of isoprene photooxidation products has been shown to be one of the major sources of secondary organic aerosol (SOA) in the atmosphere. A number of recent studies indicate that aqueous aerosol phase provides a medium for reactive uptake of isoprene photooxidation products, and in particular, isomeric isoprene epoxydiols (IEPOX), with reaction rates and yields being dependent on aerosol acidity, water content, sulfate concentration, and organic coatings. However, very few studies focused on chemistry occurring within actual cloud droplets. We will present data acquired during recent Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) Campaign, which provide direct evidence for IEPOX-SOA formation in cloud droplets. Single particle mass spectrometer, miniSPLAT, and a high-resolution, time-of-flight aerosol mass spectrometer were used to characterize the composition of aerosol particles and cloud droplet residuals, while a high-resolution, time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) was used to characterize gas-phase compounds. We find that the composition of cloud droplet residuals was markedly different than that of aerosol particles sampled outside the cloud. Cloud droplet residuals were comprised of individual particles with high relative fractions of sulfate and nitrate and significant fraction of particles with mass spectra that are nearly identical to those of laboratory-generated IEPOX-SOA particles. The observed cloud-induced formation of IEPOX-SOA was accompanied by simultaneous decrease in measured concentrations of IEPOX and other gas-phase isoprene photooxidation products. Ultimately, the combined cloud, aerosol, and gas-phase measurements conducted during HI-SCALE will be used to develop and evaluate model treatments of aqueous-phase isoprene SOA formation.

A comparative study of K-rich and Na/Ca-rich feldspar ice-nucleating particles in a nanoliter droplet freezing assay

NASA Astrophysics Data System (ADS)

Peckhaus, Andreas; Kiselev, Alexei; Hiron, Thibault; Ebert, Martin; Leisner, Thomas

2016-09-01

A recently designed droplet freezing assay was used to study the freezing of up to 1500 identical 0.2 nL water droplets containing suspensions of one Na/Ca-rich feldspar and three K-rich and one Na/Ca-rich feldspar particles. Three types of experiments have been conducted: cooling ramp, isothermal freezing at a constant temperature, and freeze-thaw cycles. The observed freezing behavior has been interpreted with the help of a model based on the classical nucleation theory (soccer ball model (SBM); Niedermeier et al., 2015). By applying the model to the different freezing experiments conducted with the same ice-nucleating material, the unique sets of model parameters for specific feldspar suspensions could be derived. The SBM was shown to adequately describe the observed cooling rate dependence, the ice-nucleating active sites (INAS) surface density ns(T) in a wide temperature range, and the shift of the freezing curves towards lower temperature with dilution. Moreover, the SBM was capable of reproducing the variation of INAS surface density ns(T) with concentration of ice-nucleating particles in the suspension droplets and correctly predicting the leveling-off of ns(T) at low temperature. The freeze-thaw experiments have clearly shown that the heterogeneous freezing induced even by very active ice-nucleating species still possesses a stochastic nature, with the degree of randomness increasing towards homogeneous nucleation. A population of the high-temperature INAS has been identified in one of the K-rich feldspar samples. The freezing of 0.8 wt % suspension droplets of this particular feldspar was observed already at -5 °C. These high-temperature active sites could be deactivated by treating the sample with hydrogen peroxide but survived heating up to 90 °C. Given a high mass concentration of these high-temperature active sites (2.9 × 108 g-1) and a very low value of contact angle (0.56 rad) the possibility of biological contamination of the sample was concluded to be unlikely but could not be completely ruled out. The freezing efficacy of all feldspar samples has been shown to reduce only slightly after suspension in water for over 5 months.

Influence of Microphysical Variability on Stochastic Condensation in Turbulent Clouds

NASA Astrophysics Data System (ADS)

Desai, N.; Chandrakar, K. K.; Chang, K.; Glienke, S.; Cantrell, W. H.; Fugal, J. P.; Shaw, R. A.

2017-12-01

We investigate the influence of variability in droplet number concentration and radius on the evolution of cloud droplet size distributions. Measurements are made on the centimeter scale using digitial inline holography, both in a controlled laboratory setting and in the field using HOLODEC measurements from CSET. We created steady state cloud conditions in the laboratory Pi Chamber, in which a turbulent cloud can be sustained for long periods of time. Using holographic imaging, we directly observe the variations in local number concentration and droplet size distribution and, thereby, the integral radius. We interpret the measurements in the context of stochastic condensation theory to determine how fluctuations in integral radius contribute to droplet growth. We find that the variability in integral radius is primarily driven by variations in the droplet number concentration and not the droplet radius. This variability does not contribute significantly to the mean droplet growth rate, but contributes significantly to the rate of increase of the size distribution width. We compare these results with in-situ measurements and find evidence for microphysical signatures of stochastic condensation. The results suggest that supersaturation fluctuations lead to broader size distributions and allow droplets to reach the collision-coalescence stage.

Atmospheric Ice-Nucleating Particles in the Dusty Tropical Atlantic

NASA Astrophysics Data System (ADS)

Price, H. C.; Baustian, K. J.; McQuaid, J. B.; Blyth, A.; Bower, K. N.; Choularton, T.; Cotton, R. J.; Cui, Z.; Field, P. R.; Gallagher, M.; Hawker, R.; Merrington, A.; Miltenberger, A.; Neely, R. R., III; Parker, S. T.; Rosenberg, P. D.; Taylor, J. W.; Trembath, J.; Vergara-Temprado, J.; Whale, T. F.; Wilson, T. W.; Young, G.; Murray, B. J.

2018-02-01

Desert dust is one of the most important atmospheric ice-nucleating aerosol species around the globe. However, there have been very few measurements of ice-nucleating particle (INP) concentrations in dusty air close to desert sources. In this study we report the concentration of INPs in dust laden air over the tropical Atlantic within a few days' transport of one of the world's most important atmospheric sources of desert dust, the Sahara. These measurements were performed as part of the Ice in Clouds Experiment-Dust campaign based in Cape Verde, during August 2015. INP concentrations active in the immersion mode, determined using a droplet-on-filter technique, ranged from around 102 m-3 at -12°C to around 105 m-3 at -23°C. There is about 2 orders of magnitude variability in INP concentration for a particular temperature, which is determined largely by the variability in atmospheric dust loading. These measurements were made at altitudes from 30 to 3,500 m in air containing a range of dust loadings. The ice active site density (ns) for desert dust dominated aerosol derived from our measurements agrees with several laboratory-based parameterizations for ice nucleation by desert dust within 1 to 2 orders of magnitude. The small variability in ns values determined from our measurements (within about 1 order of magnitude) is striking given that the back trajectory analysis suggests that the sources of dust were geographically diverse. This is consistent with previous work, which indicates that desert dust's ice-nucleating activity is only weakly dependent on source.

Study of the Fine-Scale Structure of Cumulus Clouds.

NASA Astrophysics Data System (ADS)

Rodi, Alfred R.

Small cumulus clouds are studied using data from an instrumented aircraft. Two aspects of the role of turbulence and mixing in these couds are examined: (1) the effect of mixing on the droplet size distribution, and (2) the effect of turbulence on the spread of ice crystal plumes artificially generated with cloud seeding agents. The data were collected in the course of the Bureau of Reclamation's High Plains Cooperative Experiment (HIPLEX) in Montana in the summers of 1978-80 by the University of Wyoming King Air aircraft. The shape of the cloud droplet spectrum as measured by the Particle Measuring Systems (PMS) Forward Scattering Spectrometer Probe (FSSP) is found to be very sensitive to entrainment of dry environmental air into the cloud. The narrowest cloud droplet spectra, the highest droplet concentrations, and the largest sized droplets are found in the cloud parcels which are least affected by entrainment. The most dilute regions of cloud exhibit the broadest spectra which are frequently bimodal. A procedure for measuring cloud inhomogeneity from FSSP is developed. The data shows that the clouds are extremely inhomogeneous in structure. Current models of inhomogeneous mixing are shown to be inadequate in explaining droplet spectrum effects. However, the inhomogeneous models characterize the data far better than classical models of droplet spectrum evolution. High resolution measurements of ice crystals from the PMS two dimensional imaging probe are used to characterize the spread of the ice crystal plume in seeded clouds. Plume spread is found to be a very complicated process which is in some cases dominated by organized motions in the cloud. As a result, classical diffusion theory is often inadequate to predict plume growth. The turbulent diffusion that occurs is shown to be best modeled using the relative diffusion concept of Richardson. Procedures for adapting aircraft data to the relative diffusion model are developed, including techniques for converting the aircraft Eulerian data into estimates of Lagrangian correlations. Predictions of the model are compared with observations of plume growth. A detailed analysis of errors in the air motion sensing system on the aircraft is presented. A procedure is developed to estimate the errors due to aircraft gyroscope sensitivity to horizontal accelerations.

Individual aerosol particles in ambient and updraft conditions below convective cloud bases in the Oman mountain region

NASA Astrophysics Data System (ADS)

Semeniuk, T. A.; Bruintjes, R. T.; Salazar, V.; Breed, D. W.; Jensen, T. L.; Buseck, P. R.

2014-03-01

An airborne study of cloud microphysics provided an opportunity to collect aerosol particles in ambient and updraft conditions of natural convection systems for transmission electron microscopy (TEM). Particles were collected simultaneously on lacey carbon and calcium-coated carbon (Ca-C) TEM grids, providing information on particle morphology and chemistry and a unique record of the particle's physical state on impact. In total, 22 particle categories were identified, including single, coated, aggregate, and droplet types. The fine fraction comprised up to 90% mixed cation sulfate (MCS) droplets, while the coarse fraction comprised up to 80% mineral-containing aggregates. Insoluble (dry), partially soluble (wet), and fully soluble particles (droplets) were recorded on Ca-C grids. Dry particles were typically silicate grains; wet particles were mineral aggregates with chloride, nitrate, or sulfate components; and droplets were mainly aqueous NaCl and MCS. Higher numbers of droplets were present in updrafts (80% relative humidity (RH)) compared with ambient conditions (60% RH), and almost all particles activated at cloud base (100% RH). Greatest changes in size and shape were observed in NaCl-containing aggregates (>0.3 µm diameter) along updraft trajectories. Their abundance was associated with high numbers of cloud condensation nuclei (CCN) and cloud droplets, as well as large droplet sizes in updrafts. Thus, compositional dependence was observed in activation behavior recorded for coarse and fine fractions. Soluble salts from local pollution and natural sources clearly affected aerosol-cloud interactions, enhancing the spectrum of particles forming CCN and by forming giant CCN from aggregates, thus, making cloud seeding with hygroscopic flares ineffective in this region.

An Algorithm for the Retrieval of Droplet Number Concentration and Geometrical Thickness of Stratiform Marine Boundary Layer Clouds Applied to MODIS Radiometric Observations.

NASA Astrophysics Data System (ADS)

Schüller, Lothar; Bennartz, Ralf; Fischer, Jürgen; Brenguier, Jean-Louis

2005-01-01

Algorithms are now currently used for the retrieval of cloud optical thickness and droplet effective radius from multispectral radiance measurements. This paper extends their application to the retrieval of cloud droplet number concentration, cloud geometrical thickness, and liquid water path in shallow convective clouds, using an algorithm that was previously tested with airborne measurements of cloud radiances and validated against in situ measurements of the same clouds. The retrieval is based on a stratified cloud model of liquid water content and droplet spectrum. Radiance measurements in visible and near-infrared channels of the Moderate Resolution Imaging Spectroradiometer (MODIS), which is operated from the NASA platforms Terra and Aqua, are analyzed. Because of uncertainties in the simulation of the continental surface reflectance, the algorithm is presently limited to the monitoring of the microphysical structure of boundary layer clouds over the ocean. Two MODIS scenes of extended cloud fields over the North Atlantic Ocean trade wind region are processed. A transport and dispersion model (the Hybrid Single-Particle Lagrangian Integrated Trajectory Model, HYSPLIT4) is also used to characterize the origin of the air masses and hence their aerosol regimes. One cloud field formed in an air mass that was advected from southern Europe and North Africa. It shows high values of the droplet concentration when compared with the second cloud system, which developed in a more pristine environment. The more pristine case also exhibits a higher geometrical thickness and, thus, liquid water path, which counterbalances the expected cloud albedo increase of the polluted case. Estimates of cloud liquid water path are then compared with retrievals from the Special Sensor Microwave Imager (SSM/I). SSM/I-derived liquid water paths are in good agreement with the MODIS-derived values.

Worldwide data sets constrain the water vapor uptake coefficient in cloud formation

PubMed Central

Raatikainen, Tomi; Nenes, Athanasios; Seinfeld, John H.; Morales, Ricardo; Moore, Richard H.; Lathem, Terry L.; Lance, Sara; Padró, Luz T.; Lin, Jack J.; Cerully, Kate M.; Bougiatioti, Aikaterini; Cozic, Julie; Ruehl, Christopher R.; Chuang, Patrick Y.; Anderson, Bruce E.; Flagan, Richard C.; Jonsson, Haflidi; Mihalopoulos, Nikos; Smith, James N.

2013-01-01

Cloud droplet formation depends on the condensation of water vapor on ambient aerosols, the rate of which is strongly affected by the kinetics of water uptake as expressed by the condensation (or mass accommodation) coefficient, αc. Estimates of αc for droplet growth from activation of ambient particles vary considerably and represent a critical source of uncertainty in estimates of global cloud droplet distributions and the aerosol indirect forcing of climate. We present an analysis of 10 globally relevant data sets of cloud condensation nuclei to constrain the value of αc for ambient aerosol. We find that rapid activation kinetics (αc > 0.1) is uniformly prevalent. This finding resolves a long-standing issue in cloud physics, as the uncertainty in water vapor accommodation on droplets is considerably less than previously thought. PMID:23431189

Worldwide data sets constrain the water vapor uptake coefficient in cloud formation.

PubMed

Raatikainen, Tomi; Nenes, Athanasios; Seinfeld, John H; Morales, Ricardo; Moore, Richard H; Lathem, Terry L; Lance, Sara; Padró, Luz T; Lin, Jack J; Cerully, Kate M; Bougiatioti, Aikaterini; Cozic, Julie; Ruehl, Christopher R; Chuang, Patrick Y; Anderson, Bruce E; Flagan, Richard C; Jonsson, Haflidi; Mihalopoulos, Nikos; Smith, James N

2013-03-05

Cloud droplet formation depends on the condensation of water vapor on ambient aerosols, the rate of which is strongly affected by the kinetics of water uptake as expressed by the condensation (or mass accommodation) coefficient, αc. Estimates of αc for droplet growth from activation of ambient particles vary considerably and represent a critical source of uncertainty in estimates of global cloud droplet distributions and the aerosol indirect forcing of climate. We present an analysis of 10 globally relevant data sets of cloud condensation nuclei to constrain the value of αc for ambient aerosol. We find that rapid activation kinetics (αc > 0.1) is uniformly prevalent. This finding resolves a long-standing issue in cloud physics, as the uncertainty in water vapor accommodation on droplets is considerably less than previously thought.

Microphysical response of cloud droplets in a fluctuating updraft. Ph.D. Thesis

NASA Technical Reports Server (NTRS)

Harding, D. D.

1977-01-01

The effect of a fluctuating updraft upon a distribution of cloud droplets is examined. Computations are performed for fourteen vertical velocity patterns; each allows a closed parcel of cloud air to undergo downward as well as upward motion. Droplet solution and curvature effects are included. The classical equations for the growth rate of an individual droplet by vapor condensation relies on simplifying assumptions. Those assumptions are isolated and examined. A unique approach is presented in which all energy sources and sinks of a droplet may be considered and is termed the explicit model. It is speculated that the explicit model may enhance the growth of large droplets at greater heights. Such a model is beneficial to the studies of pollution scavenging and acid rain.

From hygroscopic aerosols to cloud droplets: The HygrA-CD campaign in the Athens basin - An overview.

PubMed

Papayannis, A; Argyrouli, A; Bougiatioti, A; Remoundaki, E; Vratolis, S; Nenes, A; Solomos, S; Komppula, M; Giannakaki, E; Kalogiros, J; Banks, R; Eleftheriadis, K; Mantas, E; Diapouli, E; Tzanis, C G; Kazadzis, S; Binietoglou, I; Labzovskii, L; Vande Hey, J; Zerefos, C S

2017-01-01

The international experimental campaign Hygroscopic Aerosols to Cloud Droplets (HygrA-CD), organized in the Greater Athens Area (GAA), Greece from 15 May to 22 June 2014, aimed to study the physico-chemical properties of aerosols and their impact on the formation of clouds in the convective Planetary Boundary Layer (PBL). We found that under continental (W-NW-N) and Etesian (NE) synoptic wind flow and with a deep moist PBL (~2-2.5km height), mixed hygroscopic (anthropogenic, biomass burning and marine) particles arrive over the GAA, and contribute to the formation of convective non-precipitating PBL clouds (of ~16-20μm mean diameter) with vertical extent up to 500m. Under these conditions, high updraft velocities (1-2ms -1 ) and cloud condensation nuclei (CCN) concentrations (~2000cm -3 at 1% supersaturation), generated clouds with an estimated cloud droplet number of ~600cm -3 . Under Saharan wind flow conditions (S-SW) a shallow PBL (<1-1.2km height) develops, leading to much higher CCN concentrations (~3500-5000cm -3 at 1% supersaturation) near the ground; updraft velocities, however, were significantly lower, with an estimated maximum cloud droplet number of ~200cm -3 and without observed significant PBL cloud formation. The largest contribution to cloud droplet number variance is attributed to the updraft velocity variability, followed by variances in aerosol number concentration. Copyright © 2016 Elsevier B.V. All rights reserved.

Applying super-droplets as a compact representation of warm-rain microphysics for aerosol-cloud-aerosol interactions

NASA Astrophysics Data System (ADS)

Arabas, S.; Jaruga, A.; Pawlowska, H.; Grabowski, W. W.

2012-12-01

Clouds may influence aerosol characteristics of their environment. The relevant processes include wet deposition (rainout or washout) and cloud condensation nuclei (CCN) recycling through evaporation of cloud droplets and drizzle drops. Recycled CCN physicochemical properties may be altered if the evaporated droplets go through collisional growth or irreversible chemical reactions (e.g. SO2 oxidation). The key challenge of representing these processes in a numerical cloud model stems from the need to track properties of activated CCN throughout the cloud lifecycle. Lack of such "memory" characterises the so-called bulk, multi-moment as well as bin representations of cloud microphysics. In this study we apply the particle-based scheme of Shima et al. 2009. Each modelled particle (aka super-droplet) is a numerical proxy for a multiplicity of real-world CCN, cloud, drizzle or rain particles of the same size, nucleus type,and position. Tracking cloud nucleus properties is an inherent feature of the particle-based frameworks, making them suitable for studying aerosol-cloud-aerosol interactions. The super-droplet scheme is furthermore characterized by linear scalability in the number of computational particles, and no numerical diffusion in the condensational and in the Monte-Carlo type collisional growth schemes. The presentation will focus on processing of aerosol by a drizzling stratocumulus deck. The simulations are carried out using a 2D kinematic framework and a VOCALS experiment inspired set-up (see http://www.rap.ucar.edu/~gthompsn/workshop2012/case1/).

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.

Heat transfer studies on the liquid droplet radiator

NASA Technical Reports Server (NTRS)

Mattick, A. T.; Nelson, M.

1987-01-01

This paper examines radiation transfer in the droplet sheet of a liquid droplet radiator including non-isotropic scattering by the droplets. Non-isotropic scattering becomes significant for small droplets (diameter less than 0.1 mm) and for low emissivity liquids. For droplets with an emittance of 0.1 and for a droplet sheet optical depth or 5, the radiated power varies by about 12 percent, depending on whether scattering is predominantly forward or backward. An experimental measurement of the power emitted by a cylindrical cloud of heated droplets of silicone fluid is also reported. The measured cloud emissivity correlates, within experimental error, with the analytical model.

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.

An economical model for simulating droplet spectrum evolution in turbulent cloud chambers and wind tunnels

NASA Astrophysics Data System (ADS)

Krueger, Steven; Cantrell, W.; Niedermeier, D.; Shaw, R.; Stratmann, F.

2017-11-01

Although airborne instruments provide detailed information about the microphysical structure of clouds, the measurements provide only a few snapshots of each cloud. Deducing the droplet spectrum evolution from such measurements is next to impossible. We are using two alternative approaches: laboratory studies and numerical simulations. The former relies on a new turbulent cloud chamber (the Pi Chamber) at Michigan Technical University, as well as the first humid turbulent wind tunnel (LACIS-T) at the Leibniz Institute for Tropospheric Research. Both produce conditions for droplet growth (i.e., supersaturation) by mixing saturated vapor at different temperatures. The Pi Chamber produces turbulence by inducing Rayleigh-Bénard convection, while the wind tunnel generates turbulence with a grid. We are using the Explicit Mixing Parcel Model (EMPM) to numerically simulate droplet spectrum evolution in these flows. The EMPM explicitly links turbulent mixing and droplet spectrum evolution by representing a turbulent flow in a 1D domain with the linear eddy model. The EMPM can economically span scales from those of the smallest turbulent eddies to those of the largest. The EMPM grows or evaporates thousands of individual cloud droplets according to their local environments.

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

Cecchini, Micael A.; Machado, Luiz A. T.; Comstock, Jennifer M.

The remote atmosphere over the Amazon can be similar to oceanic regions in terms of aerosol conditions and cloud type formations. This is especially true during the wet season. The main aerosol-related disturbances over the Amazon have both natural sources, such as dust transport from Africa, and anthropogenic sources, such as biomass burning or urban pollution. The present work considers the impacts of the latter on the microphysical properties of warm-phase clouds by analysing observations of the interactions between the Manaus pollution plume and its surroundings, as part of the GoAmazon2014/5 Experiment. The analysed period corresponds to the wet seasonmore » (specifically from February to March 2014 and corresponding to the first Intensive Operating Period (IOP1) of GoAmazon2014/5). The droplet size distributions reported are in the range 1 µm ≤ D≤50 µm in order to capture the processes leading up to the precipitation formation. The wet season largely presents a clean background atmosphere characterized by frequent rain showers. As such, the contrast between background clouds and those affected by the Manaus pollution can be observed and detailed. The focus is on the characteristics of the initial microphysical properties in cumulus clouds predominantly at their early stages. The pollution-affected clouds are found to have smaller effective diameters and higher droplet number concentrations. The differences range from 10 to 40% for the effective diameter and are as high as 1000% for droplet concentration for the same vertical levels. The growth rates of droplets with altitude are slower for pollution-affected clouds (2.90 compared to 5.59 µm km ₋1), as explained by the absence of bigger droplets at the onset of cloud development. Clouds under background conditions have higher concentrations of larger droplets (>20 µm) near the cloud base, which would contribute significantly to the growth rates through the collision–coalescence process. The overall shape of the droplet size distribution (DSD) does not appear to be predominantly determined by updraught strength, especially beyond the 20 µm range. The aerosol conditions play a major role in that case. However, the updraughts modulate the DSD concentrations and are responsible for the vertical transport of water in the cloud. The larger droplets found in background clouds are associated with weak water vapour competition and a bimodal distribution of droplet sizes in the lower levels of the cloud, which enables an earlier initiation of the collision–coalescence process. This study shows that the pollution produced by Manaus significantly affects warm-phase microphysical properties of the surrounding clouds by changing the initial DSD formation. The corresponding effects on ice-phase processes and precipitation formation will be the focus of future endeavours.« less

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.

Impact of cloud horizontal inhomogeneity and directional sampling on the retrieval of cloud droplet size by the POLDER instrument

NASA Astrophysics Data System (ADS)

Shang, H.; Chen, L.; Bréon, F. M.; Letu, H.; Li, S.; Wang, Z.; Su, L.

2015-11-01

The principles of cloud droplet size retrieval via Polarization and Directionality of the Earth's Reflectance (POLDER) requires that clouds be horizontally homogeneous. The retrieval is performed by combining all measurements from an area of 150 km × 150 km to compensate for POLDER's insufficient directional sampling. Using POLDER-like data simulated with the RT3 model, we investigate the impact of cloud horizontal inhomogeneity and directional sampling on the retrieval and analyze which spatial resolution is potentially accessible from the measurements. Case studies show that the sub-grid-scale variability in droplet effective radius (CDR) can significantly reduce valid retrievals and introduce small biases to the CDR (~ 1.5 μm) and effective variance (EV) estimates. Nevertheless, the sub-grid-scale variations in EV and cloud optical thickness (COT) only influence the EV retrievals and not the CDR estimate. In the directional sampling cases studied, the retrieval using limited observations is accurate and is largely free of random noise. Several improvements have been made to the original POLDER droplet size retrieval. For example, measurements in the primary rainbow region (137-145°) are used to ensure retrievals of large droplet (> 15 μm) and to reduce the uncertainties caused by cloud heterogeneity. We apply the improved method using the POLDER global L1B data from June 2008, and the new CDR results are compared with the operational CDRs. The comparison shows that the operational CDRs tend to be underestimated for large droplets because the cloudbow oscillations in the scattering angle region of 145-165° are weak for cloud fields with CDR > 15 μm. Finally, a sub-grid-scale retrieval case demonstrates that a higher resolution, e.g., 42 km × 42 km, can be used when inverting cloud droplet size distribution parameters from POLDER measurements.

Saltwater icephobicity: Influence of surface chemistry on saltwater icing

PubMed Central

Carpenter, Katherine; Bahadur, Vaibhav

2015-01-01

Most studies on icephobicity focus on ice formation with pure water. This manuscript presents studies to understand the influence of surfaces on saltwater ice nucleation and propagation. Experiments are conducted to quantify the influence of surface chemistry on saltwater ice nucleation and to understand the utility of superhydrophobic surfaces for saltwater icephobicity. These experiments are conducted with pure water and two sodium chloride solutions, which represent the salinity of seawater and briny produced water. It is seen that the presence of salt slows down the ice front propagation velocity significantly. Saltwater droplet impact dynamics on superhydrophobic surfaces are also different from pure water. Saltwater droplets retract more and a greater fraction of impacting liquid is repelled from the superhydrophobic surface. It is seen that the greater bounciness of saltwater droplets is a result of slower ice nucleation propagation kinetics. These experiments indicate that superhydrophobic surfaces will have better resistance to impact icing with saltwater than pure water and can remain useful at temperatures as low as −40 °C. Overall, this work is a starting point for further studies on heterogeneous nucleation in saltwater and serves as a bridge between the widely studied freshwater icephobic surfaces and saltwater-related applications. PMID:26626958

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

Fan, Jiwen; Rosenfeld, Daniel; Zhang, Yuwei

Aerosol-cloud interactions remain the largest uncertainty in climate projections. Ultrafine aerosol particles smaller than 50 nanometers (UAP <50) can be abundant in the troposphere, but are conventionally considered too small to affect cloud formation. However, observational evidence and numerical simulations of deep convective clouds (DCCs) over the Amazon show that DCCs forming in a low aerosol environment can develop very large vapor supersaturation because fast droplet coalescence reduces integrated droplet surface area and subsequent condensation. UAP <50 from pollution plumes that are ingested into such clouds can be activated to form additional cloud droplets on which excess supersaturation condenses andmore » forms additional cloud water and latent heating, thus intensifying convective strength. This mechanism suggests a strong anthropogenic invigoration of DCCs in previously pristine regions of the world.« less

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-08-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number concentration.

Two space scatterer formalism calculation of bulk parameters of thunderclouds

NASA Technical Reports Server (NTRS)

Phanord, Dieudonne D.

1994-01-01

In a previous study, we used a modified two-space scatterer formalism of Twersky to establish for a cloud modeled as a statistically homogeneous distribution of spherical water droplets, the dispersion relations that determine its bulk propagation numbers and bulk indexes of refraction in terms of the vector equivalent scattering amplitude and the dyadic scattering amplitude of the single water droplet in isolation. The results were specialized to the forward direction of scattering while demanding that the scatterers preserve the incident polarization. We apply this approach to obtain specific numerical values for the macroscopic parameters of the cloud. We work with a cloud of density rho = 100 cm(exp -3), a wavelength lambda = 0.7774 microns, and with spherical water droplets of common radius alpha = 10 microns. In addition, the scattering medium is divided into three parts, the medium outside the cloud, moist air (the medium inside the cloud but outside the droplets), and the medium inside the spherical water droplets. The results of this report are applicable to a cloud of any geometry since the boundary does not interfere with the calculations. Also, it is important to notice the plane wave nature of the incidence wave in the moist atmosphere.

Crystallization kinetics from mixture Na2SO4/glycerol droplets of Na2SO4 by FTIR-ATR

NASA Astrophysics Data System (ADS)

Tan, Dan-Ting; Cai, Chen; Zhang, Yun; Wang, Na; Pang, Shu-Feng; Zhang, Yun-Hong

2016-08-01

The efflorescence of mixed Na2SO4/glycerol aerosols on the ZnSe substrate with various mole ratios (Na2SO4/glycerol = 1:1, 1:2, 1:4) has been studied in the relative humidity (RH) linearly decline process, using a situ Fourier transform infrared attenuated total reflection (FTIR-ATR) technique. The crystal ratio at a given RH can be gained by the absorbance of the band at 1132 cm-1, which shows the incomplete nucleation for mixed Na2SO4/glycerol aerosols and the decreased amount of the droplets crystallized at the lowest RH with the glycerol increase. Using the volume fraction of droplets that have yet to crystallize, the heterogeneous nucleation kinetics has been gained. By the Extended Aerosol Inorganics Model (E-AIM), the nucleation rate as the function of solute saturation degree has been gained for various mixed Na2SO4/glycerol aerosols.

SO 2 oxidation in an entraining cloud model with explicit microphysics

NASA Astrophysics Data System (ADS)

Bower, K. N.; Hill, T. A.; Coe, H.; Choularton, T. W.

A model of the chemical evolution of the droplets in a hill-cap cloud is presented. The chemistry of individual droplets forming on cloud condensation nuclei of differing size and chemical composition is considered, and the take-up of species from the gas phase by the droplets is treated explicity for the droplet population. Oxidation of S(IV) dissolved in cloud droplets is assumed to be dominated by hydrogen peroxide and ozone. Hydrogen peroxide is normally found to be the dominant oxidant for the oxidation of sulphur dioxide (except in the presence of substantial concentrations of ammonia gas, which increases droplet pH and the contribution made by the oxidant ozone). The entrainment of hydrogen peroxide from above the cloud top increases the amount of sulphate produced in conditions where the reaction is otherwise oxidant limited by the availability hydrogen peroxide. These conditions occur when there are high concentrations of sulphur dioxide accompanied by low cloudwater pH values. Within droplets formed on sodium chloride aerosol, reduced levels of acidity lead to an increase in sulphate production as a result of an enhanced reaction between SO 2 and the oxidant ozone. This results in an overall higher increase in cloudwater sulphate than would be expected assuming an even distribution of all reactants amongst the droplets. In addition, concentrations of the hydrogen sulphite ion predicted to occur in the cloudwater can be substantially in excess of those predicted from the bulk cloudwater pH. This is consistent with recent observations.

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.

A new airborne sampler for interstitial particles in ice and liquid clouds

NASA Astrophysics Data System (ADS)

Moharreri, A.; Craig, L.; Rogers, D. C.; Brown, M.; Dhaniyala, S.

2011-12-01

In-situ measurements of cloud droplets and aerosols using aircraft platforms are required for understanding aerosol-cloud processes and aiding development of improved aerosol-cloud models. A variety of clouds with different temperature ranges and cloud particle sizes/phases must be studied for comprehensive knowledge about the role of aerosols in the formation and evolution of cloud systems under different atmospheric conditions. While representative aerosol measurements are regularly made from aircrafts under clear air conditions, aerosol measurements in clouds are often contaminated by the generation of secondary particles from the high speed impaction of ice particles and liquid droplets on the surfaces of the aircraft probes/inlets. A new interstitial particle sampler, called the blunt-body aerosol sampler (BASE) has been designed and used for aerosol sampling during two recent airborne campaigns using NCAR/NSF C-130 aircraft: PLOWS (2009-2010) and ICE-T (2011). Central to the design of the new interstitial inlet is an upstream blunt body housing that acts to shield/deflect large cloud droplets and ice particles from an aft sampling region. The blunt-body design also ensures that small shatter particles created from the impaction of cloud-droplets on the blunt-body are not present in the aft region where the interstitial inlet is located. Computational fluid dynamics (CFD) simulations along with particle transport modeling and wind tunnel studies have been utilized in different stages of design and development of this inlet. The initial flights tests during the PLOWS campaign showed that the inlet had satisfactory performance only in warm clouds and when large precipitation droplets were absent. In the presence of large droplets and ice, the inlet samples were contaminated with significant shatter artifacts. These initial results were reanalyzed in conjunction with a computational droplet shatter model and the numerical results were used to arrive at an improved sampler design. Analysis of the data from the recent ICE-T campaign with the improved sampler design shows that the modified version of BASE can provide shatter-artifact free sampling of aerosol particles in the presence of ice particles and significantly reduced shatter artifacts in warm clouds. Detailed design and modeling aspects of the sampler will be discussed and the sampler performance in warm and cold clouds will be presented and compared with measurements made using other aerosol inlets flown on the NCAR/NSF C-130 aircraft.

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

A Novel Tool for Simulating Aerosol-cloud Interactions with a Sectional Model Implemented to a Large-Eddy Simulator

NASA Astrophysics Data System (ADS)

Tonttila, J.; Romakkaniemi, S.; Kokkola, H.; Maalick, Z.; Korhonen, H.; Liqing, H.

2015-12-01

A new cloud-resolving model setup for studying aerosol-cloud interactions, with a special emphasis on partitioning and wet deposition of semi-volatile aerosol species, is presented. The model is based on modified versions of two well-established model components: the Large-Eddy Simulator (LES) UCLALES, and the sectional aerosol model SALSA, previously employed in the ECHAM climate model family. Implementation of the UCLALES-SALSA is described in detail. As the basis for this work, SALSA has been extended to include a sectional representation of the size distributions of cloud droplets and precipitation. Microphysical processes operating on clouds and precipitation have also been added. Given our main motivation, the cloud droplet size bins are defined according to the dry particle diameter. The droplet wet diameter is solved dynamically through condensation equations, but represents an average droplet diameter inside each size bin. This approach allows for accurate tracking of the aerosol properties inside clouds, but minimizes the computational cost. Since the actual cloud droplet diameter is not fully resolved inside the size bins, processes such as precipitation formation rely on parameterizations. For realistic growth of drizzle drops to rain, which is critical for the aerosol wet deposition, the precipitation size bins are defined according to the actual drop size. With these additions, the implementation of the SALSA model replaces most of the microphysical and thermodynamical components within the LES. The cloud properties and aerosol-cloud interactions simulated by the model are analysed and evaluated against detailed cloud microphysical boxmodel results and in-situ aerosol-cloud interaction observations from the Puijo measurement station in Kuopio, Finland. The ability of the model to reproduce the impacts of wet deposition on the aerosol population is demonstrated.

Impacts of the Manaus pollution plume on the microphysical properties of Amazonian warm-phase clouds in the wet season

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

Cecchini, Micael A.; Machado, Luiz A. T.; Comstock, Jennifer M.

The remote atmosphere over the Amazon can be similar to oceanic regions in terms of aerosol conditions and cloud type formations. This is especially true during the wet season. The main aerosol-related disturbances over the Amazon have both natural sources, such as dust transport from Africa, and anthropogenic sources, such as biomass burning or urban pollution. The present work considers the impacts of the latter on the microphysical properties of warm-phase clouds by analyzing observations of the interactions between the Manaus pollution plume and its surroundings, as part of the GoAmazon2014/5 Experiment. The analyzed period corresponds to the wet seasonmore » (specifically from February to March 2014 and corresponding to the first Intensive Operating Period (IOP1) of GoAmazon2014/5). The droplet size distributions reported are in the range 1 µm ≤ D ≤ 50 µm in order to capture the processes leading up to the precipitation formation. The wet season largely presents a clean background atmosphere characterized by frequent rain showers. As such, the contrast between background clouds and those affected by the Manaus pollution can be observed and detailed. The focus is on the characteristics of the initial microphysical properties in cumulus clouds predominantly at their early stages. The pollution-affected clouds are found to have smaller effective diameters and higher droplet number concentrations. The differences range from 10 to 40 % for the effective diameter and are as high as 1000% for droplet concentration for the same vertical levels. The growth rates of droplets with altitude are slower for pollution-affected clouds (2.90 compared to 5.59 µm km –1), as explained by the absence of bigger droplets at the onset of cloud development. Clouds under background conditions have higher concentrations of larger droplets (> 20 µm) near the cloud base, which would contribute significantly to the growth rates through the collision–coalescence process. The overall shape of the droplet size distribution (DSD) does not appear to be predominantly determined by updraught strength, especially beyond the 20 µm range. The aerosol conditions play a major role in that case. However, the updraughts modulate the DSD concentrations and are responsible for the vertical transport of water in the cloud. The larger droplets found in background clouds are associated with weak water vapour competition and a bimodal distribution of droplet sizes in the lower levels of the cloud, which enables an earlier initiation of the collision–coalescence process. This paper shows that the pollution produced by Manaus significantly affects warm-phase microphysical properties of the surrounding clouds by changing the initial DSD formation. The corresponding effects on ice-phase processes and precipitation formation will be the focus of future endeavors.« less

Impacts of the Manaus pollution plume on the microphysical properties of Amazonian warm-phase clouds in the wet season

DOE PAGES

Cecchini, Micael A.; Machado, Luiz A. T.; Comstock, Jennifer M.; ...

2016-06-09

The remote atmosphere over the Amazon can be similar to oceanic regions in terms of aerosol conditions and cloud type formations. This is especially true during the wet season. The main aerosol-related disturbances over the Amazon have both natural sources, such as dust transport from Africa, and anthropogenic sources, such as biomass burning or urban pollution. The present work considers the impacts of the latter on the microphysical properties of warm-phase clouds by analyzing observations of the interactions between the Manaus pollution plume and its surroundings, as part of the GoAmazon2014/5 Experiment. The analyzed period corresponds to the wet seasonmore » (specifically from February to March 2014 and corresponding to the first Intensive Operating Period (IOP1) of GoAmazon2014/5). The droplet size distributions reported are in the range 1 µm ≤ D ≤ 50 µm in order to capture the processes leading up to the precipitation formation. The wet season largely presents a clean background atmosphere characterized by frequent rain showers. As such, the contrast between background clouds and those affected by the Manaus pollution can be observed and detailed. The focus is on the characteristics of the initial microphysical properties in cumulus clouds predominantly at their early stages. The pollution-affected clouds are found to have smaller effective diameters and higher droplet number concentrations. The differences range from 10 to 40 % for the effective diameter and are as high as 1000% for droplet concentration for the same vertical levels. The growth rates of droplets with altitude are slower for pollution-affected clouds (2.90 compared to 5.59 µm km –1), as explained by the absence of bigger droplets at the onset of cloud development. Clouds under background conditions have higher concentrations of larger droplets (> 20 µm) near the cloud base, which would contribute significantly to the growth rates through the collision–coalescence process. The overall shape of the droplet size distribution (DSD) does not appear to be predominantly determined by updraught strength, especially beyond the 20 µm range. The aerosol conditions play a major role in that case. However, the updraughts modulate the DSD concentrations and are responsible for the vertical transport of water in the cloud. The larger droplets found in background clouds are associated with weak water vapour competition and a bimodal distribution of droplet sizes in the lower levels of the cloud, which enables an earlier initiation of the collision–coalescence process. This paper shows that the pollution produced by Manaus significantly affects warm-phase microphysical properties of the surrounding clouds by changing the initial DSD formation. The corresponding effects on ice-phase processes and precipitation formation will be the focus of future endeavors.« less

Simulating glories and cloudbows in color.

PubMed

Gedzelman, Stanley D

2003-01-20

Glories and cloudbows are simulated in color by use of the Mie scattering theory of light upwelling from small-droplet clouds of finite optical thickness embedded in a Rayleigh scattering atmosphere. Glories are generally more distinct for clouds of droplets of as much as approximately 10 microm in radius. As droplet radius increases, the glory shrinks and becomes less prominent, whereas the cloudbow becomes more distinct and eventually colorful. Cloudbows typically consist of a broad, almost white band with a slightly orange outer edge and a dark inner band. Multiple light and dark bands that are related to supernumerary rainbows first appear inside the cloudbow as droplet radius increases above approximately 10 microm and gradually become more prominent when all droplets are the same size. Bright glories with multiple rings and high color purity are simulated when all droplets are the same size and every light beam is scattered just once. Color purity decreases and outer rings fade as the range of droplet sizes widens and when skylight, reflected light from the ground or background, and multiply scattered light from the cloud are included. Consequently, the brightest and most colorful glories and bows are seen when the observer is near a cloud or a rain swath with optical thickness of approximately 0.25 that consists of uniform-sized drops and when a dark or shaded background lies a short distance behind the cloud.

On the relevance of droplet sedimentation in stratocumulus-top mixing

NASA Astrophysics Data System (ADS)

Mellado, Juan Pedro; de Lozar, Alberto

2017-11-01

The interaction between droplet sedimentation, turbulent mixing, evaporative cooling, and radiative cooling at the top of stratocumulus clouds has been studied using direct numerical simulations. This interaction is important to determine the mixing rate of the cloud and dry air above it, which eventually determines the cloud lifetime. By investigating the entrainment-rate equation, which is an analytical relationship between the contributions to cloud-top entrainment from the phenomena indicated above, we have found that the reduction of entrainment velocity by droplet sedimentation can be 2 to 3 times larger than previously conjectured. The reason is twofold. First, the reduction of evaporative cooling as droplets fall out of the inversion is stronger than previously observed in large-eddy simulations, where excessive mixing by turbulence models and numerical artifacts may have partially masked this effect of sedimentation on entrainment. Second, there is a non-negligible direct contribution from mass loading, as falling droplets leave behind more buoyant air in the inversion. This contribution is proportional to the fifth moment of the droplet-size distribution, which provides further evidence for the need to better understand the evolution of the droplet-size distribution.

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…

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).

In situ observation on the dynamic process of evaporation and crystallization of sodium nitrate droplets on a ZnSe substrate by FTIR-ATR.

PubMed

Zhang, Qing-Nuan; Zhang, Yun; Cai, Chen; Guo, Yu-Cong; Reid, Jonathan P; Zhang, Yun-Hong

2014-04-17

Sodium nitrate is a main component of aging sea salt aerosol, and its phase behavior has been studied repeatedly with wide ranges observed in the efflorescence relative humidity (RH) in particular. Studies of the efflorescence dynamics of NaNO3 droplets deposited on a ZnSe substrate are reported, using an in situ Fourier transform infrared attenuated total reflection (FTIR-ATR) technique. The time-dependence of the infrared spectra of NaNO3 aerosols accompanying step changes in RH have been measured with high signal-to-noise ratio. From the IR difference spectra recorded, changes of the time-dependent absorption peak area of the O-H stretching band (ν-OH, ∼3400 cm(-1)) and the nitrate out-of-plane bending band (ν2-NO3(-), ∼836 cm(-1)) are obtained. From these measurements, changes in the IR signatures can be attributed to crystalline and solution phase nitrate ions, allowing the volume fraction of the solution droplets that have crystallized to be determined. Then, using these clear signatures of the volume fraction of droplets that have yet to crystallize, the homogeneous and heterogeneous nucleation kinetics can be studied from conventional measurements using a steady decline in RH. The nucleation rate measurements confirm that the rate of crystallization in sodium nitrate droplets is considerably less than in ammonium sulfate droplets at any particular degree of solute supersaturation, explaining the wide range of efflorescence RHs observed for sodium nitrate in previous studies. We demonstrate that studying nucleation kinetics using the FTIR-ATR approach has many advantages over brightfield imaging studies on smaller numbers of larger droplets or measurements made on single levitated particles.

Au-Assisted Substrate-Faceting for Inclined Nanowire Growth.

PubMed

Kang, Jung-Hyun; Krizek, Filip; Zaluska-Kotur, Magdalena; Krogstrup, Peter; Kacman, Perla; Beidenkopf, Haim; Shtrikman, Hadas

2018-06-12

We study the role of gold droplets in the initial stage of nanowire growth via the vapor-liquid-solid method. Apart from serving as a collections center for growth species, the gold droplets carry an additional crucial role that necessarily precedes the nanowire emergence, that is, they assist the nucleation of nanocraters with strongly faceted {111}B side walls. Only once these facets become sufficiently large and regular, the gold droplets start nucleating and guiding the growth of nanowires. We show that this dual role of the gold droplets can be detected and monitored by high-energy electron diffraction during growth. Moreover, gold-induced formation of craters and the onset of nanowires growth on the {111}B facets inside the craters are confirmed by the results of Monte Carlo simulations. The detailed insight into the growth mechanism of inclined nanowires will help to engineer new and complex nanowire-based device architectures.

Thermodynamic and kinetic theory of nucleation, deliquescence and efflorescence transitions in the ensemble of droplets on soluble particles.

PubMed

Shchekin, Alexander K; Shabaev, Ilya V; Hellmuth, Olaf

2013-02-07

Thermodynamic and kinetic peculiarities of nucleation, deliquescence and efflorescence transitions in the ensemble of droplets formed on soluble condensation nuclei from a solvent vapor have been considered. The interplay of the effects of solubility and the size of condensation nuclei has been analyzed. Activation barriers for the deliquescence and phase transitions and for the reverse efflorescence transition have been determined as functions of the relative humidity of the vapor-gas atmosphere, initial size, and solubility of condensation nuclei. It has been demonstrated that, upon variations in the relative humidity of the atmosphere, the crossover in thermodynamically stable and unstable variables of the droplet state takes place. The physical meaning of stable and unstable variables has been clarified. The kinetic equations for establishing equilibrium and steady distributions of binary droplets have been solved. The specific times for relaxation, deliquescence and efflorescence transitions have been calculated.

An Examination of the Impact of Drizzle Drops on Satellite-Retrieved Effective Particle Sizes

NASA Technical Reports Server (NTRS)

Minnis, Patrick; Arduini, Robert F.; Young, David F.; Ayers, J, Kirk; Albrecht, Bruce A.; Sharon, Tarah; Stevens, Bjorn

2004-01-01

In general, cloud effective droplet radii are remotely sensed in the near-infrared using the assumption of a monomodal droplet size distribution. It has been observed in many instances, especially in relatively pristine marine environments, that cloud effective droplet radii derived from satellite data often exceed 15 m or more. Comparisons of remotely sensed and in situ retrievals indicate that the former often overestimates the latter in clouds with drizzle-size droplets. To gain a better understanding of this discrepancy, this paper performs a theoretical and empirical evaluation of the impact of drizzle drops on the derived effective radius.

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.

Substantial convection and precipitation enhancements by ultrafine aerosol particles

DOE PAGES

Fan, Jiwen; Rosenfeld, Daniel; Zhang, Yuwei; ...

2018-01-26

Aerosol-cloud interactions remain the largest uncertainty in climate projections. Ultrafine aerosol particles smaller than 50 nanometers (UAP <50) can be abundant in the troposphere, but are conventionally considered too small to affect cloud formation. However, observational evidence and numerical simulations of deep convective clouds (DCCs) over the Amazon show that DCCs forming in a low aerosol environment can develop very large vapor supersaturation because fast droplet coalescence reduces integrated droplet surface area and subsequent condensation. UAP <50 from pollution plumes that are ingested into such clouds can be activated to form additional cloud droplets on which excess supersaturation condenses andmore » forms additional cloud water and latent heating, thus intensifying convective strength. This mechanism suggests a strong anthropogenic invigoration of DCCs in previously pristine regions of the world.« less

Evidence for Natural Variability in Marine Stratocumulus Cloud Properties Due to Cloud-Aerosol

NASA Technical Reports Server (NTRS)

Albrecht, Bruce; Sharon, Tarah; Jonsson, Haf; Minnis, Patrick; Minnis, Patrick; Ayers, J. Kirk; Khaiyer, Mandana M.

2004-01-01

In this study, aircraft observations from the Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter are used to characterize the variability in drizzle, cloud, and aerosol properties associated with cloud rifts and the surrounding solid clouds observed off the coast of California. A flight made on 16 July 1999 provided measurements directly across an interface between solid and rift cloud conditions. Aircraft instrumentation allowed for measurements of aerosol, cloud droplet, and drizzle spectra. CCN concentrations were measured in addition to standard thermodynamic variables and the winds. A Forward Scatter Spectrometer Probe (FSSP) measured size distribution of cloud-sized droplets. A Cloud Imaging Probe (CIP) was used to measure distributions of drizzle-sized droplets. Aerosol distributions were obtained from a Cloud Aerosol Scatterprobe (CAS). The CAS probe measured aerosols, cloud droplets and drizzle-sized drops; for this study. The CAS probe was used to measure aerosols in the size range of 0.5 micron - 1 micron. Smaller aerosols were characterized using an Ultrafine Condensation Particle Counter (CPC) sensor. The CPC was used to measure particles with diameters greater than 0.003 micron. By subtracting different count concentrations measured with the CPC, this probe was capable of identifying ultrafine particles those falling in the size range of 3 nanometers - 7 nanometers that are believed to be associated with new particle production.

Alterations of Cloud Microphysics Due to Cloud Processed CCN

NASA Astrophysics Data System (ADS)

Hudson, J. G.; Tabor, S. S.; Noble, S. R., Jr.

2015-12-01

High-resolution CCN spectra have revealed bimodality (Hudson et al. 2015) similar to aerosol size spectra (e.g., Hoppel et al. 1985). Bimodality is caused by chemical and physical cloud processes that increase mass or hygroscopicity of only CCN that produced activated cloud droplets. Bimodality is categorized by relative CCN concentrations (NCCN) within the two modes, Nu-Np; i.e., NCCN within the higher critical supersaturation, Sc, mode that did not undergo cloud processing minus NCCN within the lower Sc mode that was cloud processed. Lower, especially negative, Nu-Np designates greater processing. The table shows regressions between Nu-Np and characteristics of clouds nearest the CCN measurements. ICE-T MASE parameter R SL R SL Nc 0.17 93.24 -0.26 98.65 MD -0.31 99.69 0.33 99.78 σ -0.27 99.04 0.48 100.00 Ld -0.31 99.61 0.38 99.96 Table. Correlation coefficients, R, and one-tailed significance levels in percent, SL, for Nu-Np with microphysics of the clouds closest to each CCN measurement, 75 ICE-T and 74 MASE cases. Nc is cloud droplet concentration, MD is cloud droplet mean diameter, σ is standard deviation of cloud droplet spectra, Ldis drizzle drop LWC. Two aircraft field campaigns, Ice in Clouds Experiment-Tropical (ICE-T) and Marine Stratus/Stratocumulus Experiment (MASE) show opposite R signs because coalescence dominated cloud processing in low altitude ICE-T cumuli whereas chemical transformations predominated in MASE low altitude polluted stratus. Coalescence reduces Nc and NCCN, which thus increases MD, and σ, which promote Ld. Chemical transformations, e.g., SO2 to SO4, increase CCN hygroscopicity, thus reducing Sc, but not affecting Nc or NCCN. Lower Sc CCN are capable of producing greater Nc in subsequent cloud cycles, which leads to lower MD and σ which reduce Ld (figure). These observations are consistent with cloud droplet growth models for the higher vertical wind (W) of cumuli and lower W of stratus. Coalescence thus reduces the indirect aerosol effect (IAE) with a positive feedback that further enhances coalescence and drizzle. Chemical cloud processing enhances both components of IAE; 1st IAE by greater droplet surface area, 2ndIAE by suppressing drizzle and thus increasing cloudiness. Hoppel, Fitzgerald and Larson: JGR 90, 2365-79 Hudson, Noble and Tabor: JGRA 120, 3436-52

Interpretation of multi-wavelength-retrieved cloud droplet effective radii in terms of cloud vertical inhomogeneity based on water cloud simulations using a spectral-bin microphysics cloud model

NASA Astrophysics Data System (ADS)

Matsui, T. N.; Suzuki, K.; Nakajima, T. Y.; Matsumae, Y.

2011-12-01

Clouds play an import role in energy balance and climate changes of the Earth. IPCC AR4, however, pointed out that cloud feedback is still the large source of uncertainty in climate estimates. In the recent decade, the new satellites with the active instruments (e.g. Cloudsat) represented a new epoch in earth observations. The active remote sensing is powerful for illustrating the vertical structures of clouds, but the passive remote sensing from satellite images also contribute to better understating of cloud system. For instance, Nakajima et al. (2010a) and Suzuki et al. (2010) illustrated transition of cloud growth, from cloud droplet to drizzle to rain, using the combine analysis of the cloud droplet size retrieved from passive images (MODIS) and the reflectivity profiles from Cloudsat. Furthermore, EarthCARE that is a new satellite launched years later is composed of not only the active but also passive instruments for the combined analysis. On the other hands, the methods to retrieve the advanced information of cloud properties are also required because many imagers have been operated and are now planned (e.g. GCOM-C/SGLI), and have the advantages such as wide observation width and more observation channels. Cloud droplet effective radius (CDR) and cloud optical thickness (COT) can be retrieved using a non-water-absorbing band (e.g. 0.86μm) and a water-absorbing band (1.6, 2.1, 3.7μm) of imagers under the assumptions such as the log-normal droplet size distribution and the plane-parallel cloud structure. However, the differences between three retrieved CDRs using 1.6, 2.1 or 3.7μm (R16, R21 and R37) are found in the satellite observations. Several studies pointed out that vertical/horizontal inhomogeneity of cloud structure, difference of penetration depth of water-absorbing bands, multi-modal droplet distribution and/or 3-D radiative transfer effect cause the CDR differences. In other words, the advanced information of clouds may lie hidden in the differences. Nakajima et al. (2010b) investigated the impact of the differences sensitivities to particle size and the penetration depth in an attempt to explain the CDR differences found in by using a simple two-layer cloud model with the bi-modal size distribution functions. Their results showed the sensitivity differences between 1.6, 2.1 and 3.7μm bands to droplet sizes and their vertical stratification. In this study, we further investigate the impact of the vertical inhomogeneity structure including the drizzle by using a spectral-bin microphysics cloud model. We apply the 1-D radiative transfer computation to the numerical cloud fields generated by the cloud model, and retrieve the CDRs from the reflectances thus simulated at each band. We then compare the statistics of these retrieved CDRs with the CDRs obtained from MODIS observations and derive the sensitivity functions of the retrieved CDRs to the particle size and the optical depth from the sets of the droplet distribution functions predicted by the model and the retrieved CDRs. This study is an attempt to interpret the CDR differences in terms of the cloud vertical structure and the cloud particle growth processes.

Cloud microstructure studies

NASA Technical Reports Server (NTRS)

Blau, H. H., Jr.; Fowler, M. G.; Chang, D. T.; Ryan, R. T.

1972-01-01

Over two thousand individual cloud droplet size distributions were measured with an optical cloud particle spectrometer flown on the NASA Convair 990 aircraft. Representative droplet spectra and liquid water content, L (gm/cu m) were obtained for oceanic stratiform and cumuliform clouds. For non-precipitating clouds, values of L range from 0.1 gm/cu m to 0.5 gm/cu m; with precipitation, L is often greater than 1 gm/cu m. Measurements were also made in a newly formed contrail and in cirrus clouds.

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 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.

Backscatter laser depolarization studies of simulated stratospheric aerosols - Crystallized sulfuric acid droplets

NASA Technical Reports Server (NTRS)

Sassen, Kenneth; Zhao, Hongjie; Yu, Bing-Kun

1989-01-01

The optical depolarizing properties of simulated stratospheric aerosols were studied in laboratory laser (0.633 micrometer) backscattering experiments for application to polarization lidar observations. Clouds composed of sulfuric acid solution droplets, some treated with ammonia gas, were observed during evaporation. The results indicate that the formation of minute ammonium sulfate particles from the evaporation of acid droplets produces linear depolarization ratios of beta equivalent to 0.02, but beta equivalent to 0.10 to 0.15 are generated from aged acid cloud aerosols and acid droplet crystalization effects following the introduction of ammonia gas into the chamber. It is concluded that partially crystallized sulfuric acid droplets are a likely candidate for explaining the lidar beta equivalent to 0.10 values that have been observed in the lower stratosphere in the absence of the relatively strong backscattering from homogeneous sulfuric acid droplet (beta equivalent to 0) or ice crystal (beta equivalent to 0.5) clouds.

Backscatter laser depolarization studies of simulated stratospheric aerosols: Crystallized sulfuric acid droplets

NASA Technical Reports Server (NTRS)

Sassen, Kenneth; Zhao, Hongjie; Yu, Bing-Kun

1988-01-01

The optical depolarizing properties of simulated stratospheric aerosols were studied in laboratory laser (0.633 micrometer) backscattering experiments for application to polarization lidar observations. Clouds composed of sulfuric acid solution droplets, some treated with ammonia gas, were observed during evaporation. The results indicate that the formation of minute ammonium sulfate particles from the evaporation of acid droplets produces linear depolarization ratios of beta equivalent to 0.02, but beta equivalent to 0.10 to 0.15 are generated from aged acid cloud aerosols and acid droplet crystallization effects following the introduction of ammonia gas into the chamber. It is concluded that partially crystallized sulfuric acid droplets are a likely candidate for explaining the lidar beta equivalent to 0.10 values that have been observed in the lower stratosphere in the absence of the relatively strong backscattering from homogeneous sulfuric acid droplet (beta equivalent to 0) or ice crystal (beta equivalent to 0.5) clouds.

Optical cloud detection from a disposable airborne sensor

NASA Astrophysics Data System (ADS)

Nicoll, Keri; Harrison, R. Giles; Brus, David

2016-04-01

In-situ measurement of cloud droplet microphysical properties is most commonly made from manned aircraft platforms due to the size and weight of the instrumentation, which is both costly and typically limited to sampling only a few clouds. This work describes the development of a small, lightweight (<200g), disposable, optical cloud sensor which is designed for use on routine radiosonde balloon flights and also small unmanned aerial vehicle (UAV) platforms. The sensor employs the backscatter principle, using an ultra-bright LED as the illumination source, with a photodiode detector. Scattering of the LED light by cloud droplets generates a small optical signal which is separated from background light fluctuations using a lock-in technique. The signal to noise obtained permits cloud detection using the scattered LED light, even in daytime. During recent field tests in Pallas, Finland, the retrieved optical sensor signal has been compared with the DMT Cloud and Aerosol Spectrometer (CAS) which measures cloud droplets in the size range from 0.5 to 50 microns. Both sensors were installed at the hill top observatory of Sammaltunturi during a field campaign in October and November 2015, which experienced long periods of immersion inside cloud. Preliminary analysis shows very good agreement between the CAPS and the disposable cloud sensor for cloud droplets >5micron effective diameter. Such data and calibration of the sensor will be discussed here, as will simultaneous balloon launches of the optical cloud sensor through the same cloud layers.

Modeling the Impact of Drizzle and 3D Cloud Structure on Remote Sensing of Effective Radius

NASA Technical Reports Server (NTRS)

Platnick, Steven; Zinner, Tobias; Ackerman, S.

2008-01-01

Remote sensing of cloud particle size with passive sensors like MODIS is an important tool for cloud microphysical studies. As a measure of the radiatively relevant droplet size, effective radius can be retrieved with different combinations of visible through shortwave infrared channels. MODIS observations sometimes show significantly larger effective radii in marine boundary layer cloud fields derived from the 1.6 and 2.1 pm channel observations than for 3.7 pm retrievals. Possible explanations range from 3D radiative transport effects and sub-pixel cloud inhomogeneity to the impact of drizzle formation on the droplet distribution. To investigate the potential influence of these factors, we use LES boundary layer cloud simulations in combination with 3D Monte Carlo simulations of MODIS observations. LES simulations of warm cloud spectral microphysics for cases of marine stratus and broken stratocumulus, each for two different values of cloud condensation nuclei density, produce cloud structures comprising droplet size distributions with and without drizzle size drops. In this study, synthetic MODIS observations generated from 3D radiative transport simulations that consider the full droplet size distribution will be generated for each scene. The operational MODIS effective radius retrievals will then be applied to the simulated reflectances and the results compared with the LES microphysics.

Aerosol-cloud feedbacks in a turbulent environment: Laboratory measurements representative of conditions in boundary layer clouds

NASA Astrophysics Data System (ADS)

Cantrell, W. H.; Chandrakar, K. K.; Karki, S.; Kinney, G.; Shaw, R.

2017-12-01

Many of the climate impacts of boundary layer clouds are modulated by aerosol particles. As two examples, their interactions with incoming solar and upwelling terrestrial radiation and their propensity for precipitation are both governed by the population of aerosol particles upon which the cloud droplets formed. In turn, clouds are the primary removal mechanism for aerosol particles smaller than a few micrometers and larger than a few nanometers. Aspects of these interconnected phenomena are known in exquisite detail (e.g. Köhler theory), but other parts have not been as amenable to study in the laboratory (e.g. scavenging of aerosol particles by cloud droplets). As a complicating factor, boundary layer clouds are ubiquitously turbulent, which introduces fluctuations in the water vapor concentration and temperature, which govern the saturation ratio which mediates aerosol-cloud interactions. We have performed laboratory measurements of aerosol-cloud coupling and feedbacks, using Michigan Tech's Pi Chamber (Chang et al., 2016). In conditions representative of boundary layer clouds, our data suggest that the lifetime of most interstitial particles in the accumulation mode is governed by cloud activation - particles are removed from the Pi Chamber when they activate and settle out of the chamber as cloud droplets. As cloud droplets are removed, these interstitial particles activate until the initially polluted cloud cleans itself and all particulates are removed from the chamber. At that point, the cloud collapses. Our data also indicate that smaller particles, Dp < ˜ 20 nm are not activated, but are instead removed through diffusion, enhanced by the fact that droplets are moving relative to the suspended aerosol. I will discuss results from both warm (i.e. liquid water only) and mixed phase clouds, showing that cloud and aerosol properties are coupled through fluctuations in the supersaturation, and that threshold behaviors can be defined through the use of the Dämkohler number, the ratio of the characteristic turbulence timescale to the cloud's microphysical response time. Chang, K., et al., 2016. A laboratory facility to study gas-aerosol-cloud interactions in a turbulent environment: The Π Chamber. Bull. Amer. Meteor. Soc., doi:10.1175/BAMS-D-15-00203.1

An aerosol activation metamodel of v1.2.0 of the pyrcel cloud parcel model: development and offline assessment for use in an aerosol–climate model

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

Rothenberg, Daniel; Wang, Chien

We describe an emulator of a detailed cloud parcel model which has been trained to assess droplet nucleation from a complex, multimodal aerosol size distribution simulated by a global aerosol–climate model. The emulator is constructed using a sensitivity analysis approach (polynomial chaos expansion) which reproduces the behavior of the targeted parcel model across the full range of aerosol properties and meteorology simulated by the parent climate model. An iterative technique using aerosol fields sampled from a global model is used to identify the critical aerosol size distribution parameters necessary for accurately predicting activation. Across the large parameter space used tomore » train them, the emulators estimate cloud droplet number concentration (CDNC) with a mean relative error of 9.2% for aerosol populations without giant cloud condensation nuclei (CCN) and 6.9% when including them. Versus a parcel model driven by those same aerosol fields, the best-performing emulator has a mean relative error of 4.6%, which is comparable with two commonly used activation schemes also evaluated here (which have mean relative errors of 2.9 and 6.7%, respectively). We identify the potential for regional biases in modeled CDNC, particularly in oceanic regimes, where our best-performing emulator tends to overpredict by 7%, whereas the reference activation schemes range in mean relative error from -3 to 7%. The emulators which include the effects of giant CCN are more accurate in continental regimes (mean relative error of 0.3%) but strongly overestimate CDNC in oceanic regimes by up to 22%, particularly in the Southern Ocean. Finally, the biases in CDNC resulting from the subjective choice of activation scheme could potentially influence the magnitude of the indirect effect diagnosed from the model incorporating it.« less

An aerosol activation metamodel of v1.2.0 of the pyrcel cloud parcel model: development and offline assessment for use in an aerosol–climate model

DOE PAGES

Rothenberg, Daniel; Wang, Chien

2017-04-27

We describe an emulator of a detailed cloud parcel model which has been trained to assess droplet nucleation from a complex, multimodal aerosol size distribution simulated by a global aerosol–climate model. The emulator is constructed using a sensitivity analysis approach (polynomial chaos expansion) which reproduces the behavior of the targeted parcel model across the full range of aerosol properties and meteorology simulated by the parent climate model. An iterative technique using aerosol fields sampled from a global model is used to identify the critical aerosol size distribution parameters necessary for accurately predicting activation. Across the large parameter space used tomore » train them, the emulators estimate cloud droplet number concentration (CDNC) with a mean relative error of 9.2% for aerosol populations without giant cloud condensation nuclei (CCN) and 6.9% when including them. Versus a parcel model driven by those same aerosol fields, the best-performing emulator has a mean relative error of 4.6%, which is comparable with two commonly used activation schemes also evaluated here (which have mean relative errors of 2.9 and 6.7%, respectively). We identify the potential for regional biases in modeled CDNC, particularly in oceanic regimes, where our best-performing emulator tends to overpredict by 7%, whereas the reference activation schemes range in mean relative error from -3 to 7%. The emulators which include the effects of giant CCN are more accurate in continental regimes (mean relative error of 0.3%) but strongly overestimate CDNC in oceanic regimes by up to 22%, particularly in the Southern Ocean. Finally, the biases in CDNC resulting from the subjective choice of activation scheme could potentially influence the magnitude of the indirect effect diagnosed from the model incorporating it.« less

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

Penner, Joyce E.; Zhou, Cheng

Observation-based studies have shown that the aerosol cloud lifetime effect or the increase of cloud liquid water path (LWP) with increased aerosol loading may have been overestimated in climate models. Here, we simulate shallow warm clouds on 05/27/2011 at the Southern Great Plains (SGP) measurement site established by Department of Energy's Atmospheric Radiation Measurement (ARM) Program using a single column version of a global climate model (Community Atmosphere Model or CAM) and a cloud resolving model (CRM). The LWP simulated by CAM increases substantially with aerosol loading while that in the CRM does not. The increase of LWP in CAMmore » is caused by a large decrease of the autoconversion rate when cloud droplet number increases. In the CRM, the autoconversion rate is also reduced, but this is offset or even outweighed by the increased evaporation of cloud droplets near cloud top, resulting in an overall decrease in LWP. Our results suggest that climate models need to include the dependence of cloud top growth and the evaporation/condensation process on cloud droplet number concentrations.« less

The Route to Raindrop Formation in a Shallow Cumulus Cloud Simulated by a Lagrangian Cloud Model

NASA Astrophysics Data System (ADS)

Noh, Yign; Hoffmann, Fabian; Raasch, Siegfried

2017-11-01

The mechanism of raindrop formation in a shallow cumulus cloud is investigated using a Lagrangian cloud model (LCM). The analysis is focused on how and under which conditions a cloud droplet grows to a raindrop by tracking the history of individual Lagrangian droplets. It is found that the rapid collisional growth, leading to raindrop formation, is triggered when single droplets with a radius of 20 μm appear in the region near the cloud top, characterized by a large liquid water content, strong turbulence, large mean droplet size, a broad drop size distribution (DSD), and high supersaturations. Raindrop formation easily occurs when turbulence-induced collision enhancement(TICE) is considered, with or without any extra broadening of the DSD by another mechanism (such as entrainment and mixing). In contrast, when TICE is not considered, raindrop formation is severely delayed if no other broadening mechanism is active. The reason leading to the difference is clarified by the additional analysis of idealized box-simulations of the collisional growth process for different DSDs in varied turbulent environments. It is found that TICE does not accelerate the timing of the raindrop formation for individual droplets, but it enhances the collisional growth rate significantly afterward. KMA R & D Program (Korea), DFG (Germany).

Entrainment, Drizzle, and Cloud Albedo

NASA Technical Reports Server (NTRS)

Ackerman, A. S.; Kirkpatrick, J. P.; Stevens, D. E.; Toon, O. B.

2004-01-01

Increased aerosol and hence droplet concentrations in polluted clouds are expected to inhibit precipitation and thereby increase cloud water, leading to more reflective clouds that partially offset global warming. Yet polluted clouds are not generally observed to hold more water. Much of the uncertainty regarding the indirect aerosol effect stems from inadequate understanding of such changes in cloud water. Detailed simulations show that the relative humidity of air overlying stratocumulus is a leading factor determining whether cloud water increases or decreases when precipitation is suppressed. When the overlying air is dry, cloud water can decrease as droplet concentrations increase.

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.

Effects of Chemical Aging on the Heterogeneous Freezing of Organic Aerosols

NASA Astrophysics Data System (ADS)

Collier, K.; Brooks, S. D.

2014-12-01

Organic aerosols are emitted into the atmosphere from a variety of sources and display a wide range of effectiveness in promoting the nucleation of ice in clouds. Soot and polycyclic aromatic hydrocarbons (PAHS) arise from incomplete combustion and other pollutant sources. Hydrocarbon compounds in diesel motor oil and other fuel blends include compounds such as octacosane (a straight saturated alkane), squalane (a branched saturated alkane) and squalene (an unsaturated branched alkene). At temperatures above -36°C, the formation of ice crystals in the atmosphere is facilitated by heterogeneous freezing processes in which atmospheric aerosols act as ice nuclei (IN). The variability in ability of organic particles to facilitate heterogeneous ice nucleation causes major uncertainties in predictions of aerosol effects on climate. Further, atmospheric aerosol composition and ice nucleation ability can be altered via chemical aging and reactions with atmospheric oxidants such as ozone. In this study, we take a closer look at the role of chemical oxidation on the efficiency of specific IN during contact freezing laboratory experiments. The freezing temperatures of droplets in contact with representative organic aerosols are determined through the use of an optical microscope apparatus equipped with a cooling stage and a digital camera. Chemical changes at the surface of aerosols due to ozone exposure are characterized using Raman Microspectroscopy and Fourier Transform Infrared Spectroscopy with Horizontal Attenuated Total Reflectance. Our results indicate that oxidation of certain atmospheric organics (soot and PAHS) enhances their ice nucleation ability. In this presentation, results of heterogeneous nucleation on various types of organic aerosols will be presented, and the role of structure in promoting freezing will be discussed.

Time dependent charging of layer clouds in the global electric circuit

NASA Astrophysics Data System (ADS)

Zhou, Limin; Tinsley, Brian A.

2012-09-01

There is much observational data consistent with the hypothesis that the ionosphere-earth current density (Jz) in the global electric circuit, which is modulated by both solar activity and thunderstorm activity, affects atmospheric dynamics and cloud cover. One candidate mechanism involves Jz causing the accumulation of space charge on droplets and aerosol particles, that affects the rate of scavenging of the latter, notably those of Cloud Condensation Nuclei (CCN) and Ice Forming Nuclei (IFN) (Tinsley, 2008, 2010). Space charge is the difference, per unit volume, between total positive and total negative electrical charge that is on droplets, aerosol particles (including the CCN and IFN) and air ions. The cumulative effects of the scavenging in stratiform clouds and aerosol layers in an air mass over the lifetime of the aerosol particles of 1-10 days affects the concentration and size distribution of the CCN, so that in subsequent episodes of cloud formation (including deep convective clouds) there can be effects on droplet size distribution, coagulation, precipitation processes, and even storm dynamics.Because the time scales for charging for some clouds can be long compared to cloud lifetimes, the amount of charge at a given time, and its effect on scavenging, depend more on the charging rate than on the equilibrium charge that would eventually be attained. To evaluate this, a new time-dependent charging model has been developed. The results show that for typical altostratus clouds with typical droplet radii 10 μm and aerosol particles of radius of 0.04 μm, the time constant for charging in response to a change in Jz is about 800 s, which is comparable to cloud formation and dissipation timescales for some cloud situations. The charging timescale is found to be strong functions of altitude and aerosol concentration, with the time constant for droplet charging at 2 km in air with a high concentration of aerosols being about an hour, and for clouds at 10 km in clean air being about a minute. The charging timescale is also a strong function of droplet size, with the rate for 15 μm radii droplets being about 70% longer than that for 10 μm droplets, and the rate for 5 μm radii droplets being about 50% smaller. The equilibrium charges accumulated on droplets ranged from tens to hundreds of elementary charges, which is comparable to observed values, and to vary approximately directly with Jz and inversely with the ion production rate q, which is due to the Galactic Cosmic Ray (GCR) flux and depends strongly on altitude.For the case of Jz varying directly with q, which to some extent is the case during Forbush decreases of the GCR flux, the effects on the equilibrium charge tend to cancel. In one run with the model, both q and Jz were decreased by 30%. There was little change in equilibrium charge, but the timescale for charging increased by about 40%, or equivalently, the rate of charging decreased by about 40%. Thus, for exploring the hypothesis that space charge provides a link between GCR (and other inputs that modulate Jz) and changes in clouds and atmospheric dynamics, it is necessary to consider variations in the rate of charging. The present work is intended to provide illustrative examples of time dependent charging for several different types of layer clouds.

Turbulence and cloud droplets in cumulus clouds

NASA Astrophysics Data System (ADS)

Saito, Izumi; Gotoh, Toshiyuki

2018-02-01

In this paper, we report on the successful and seamless simulation of turbulence and the evolution of cloud droplets to raindrops over 10 minutes from microscopic viewpoints by using direct numerical simulation. Included processes are condensation-evaporation, collision-coalescence of droplets with hydrodynamic interaction, Reynolds number dependent drag, and turbulent flow within a parcel that is ascending within a self-consistently determined updraft inside a cumulus cloud. We found that the altitude and the updraft velocity of the parcel, the mean supersaturation, and the liquid water content are insensitive to the turbulence intensity, and that when the turbulence intensity increases, the droplet number density swiftly decreases while the spectral width of droplets rapidly increases. This study marks the first time the evolution of the mass density distribution function has been successfully calculated from microscopic computations. The turbulence accelerated to form a second peak in the mass density distribution function, leading to the raindrop formation, and the radius of the largest drop was over 300 μm at the end of the simulation. We also found that cloud droplets modify the turbulence in a way that is unlike the Kolmogorov-Obukhov-Corrsin theory. For example, the temperature and water vapor spectra at low wavenumbers become shallower than {k}-5/3 in the inertial-convective range, and decrease slower than exponentially in the diffusive range. This spectra modification is explained by nonlinear interactions between turbulent mixing and the evaporation-condensation process associated with large numbers of droplets.

Height Dependency of Aerosol-Cloud Interaction Regimes: Height Dependency of ACI Regime

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

Chen, Jingyi; Liu, Yangang; Zhang, Minghua

This study investigates the height dependency of aerosol-cloud interaction regimes in terms of the joint dependence of the key cloud microphysical properties (e.g. cloud droplet number concentration, cloud droplet relative dispersion, etc.) on aerosol number concentration (N a) and vertical velocity (w). The three distinct regimes with different microphysical features are the aerosol-limited regime, the updraft-limited regime, and the transitional regime. The results reveal two new phenomena in updraft-limited regime: 1) The “condensational broadening” of cloud droplet size distribution in contrast to the well-known “condensational narrowing” in the aerosol-limited regime; 2) Above the level of maximum supersaturation, some cloud dropletsmore » are deactivated into interstitial aerosols in the updraft-limited regime whereas all droplets remain activated in the aerosol-limited regime. Further analysis shows that the particle equilibrium supersaturation plays important role in understanding these unique features. Also examined is the height of warm rain initiation and its dependence on N a and w. The rain initiation height is found to depend primarily on either N a or w or both in different N a-w regimes, thus suggesting a strong regime dependence of the second aerosol indirect effect.« less

Height Dependency of Aerosol-Cloud Interaction Regimes: Height Dependency of ACI Regime

DOE PAGES

Chen, Jingyi; Liu, Yangang; Zhang, Minghua; ...

2018-01-10

This study investigates the height dependency of aerosol-cloud interaction regimes in terms of the joint dependence of the key cloud microphysical properties (e.g. cloud droplet number concentration, cloud droplet relative dispersion, etc.) on aerosol number concentration (N a) and vertical velocity (w). The three distinct regimes with different microphysical features are the aerosol-limited regime, the updraft-limited regime, and the transitional regime. The results reveal two new phenomena in updraft-limited regime: 1) The “condensational broadening” of cloud droplet size distribution in contrast to the well-known “condensational narrowing” in the aerosol-limited regime; 2) Above the level of maximum supersaturation, some cloud dropletsmore » are deactivated into interstitial aerosols in the updraft-limited regime whereas all droplets remain activated in the aerosol-limited regime. Further analysis shows that the particle equilibrium supersaturation plays important role in understanding these unique features. Also examined is the height of warm rain initiation and its dependence on N a and w. The rain initiation height is found to depend primarily on either N a or w or both in different N a-w regimes, thus suggesting a strong regime dependence of the second aerosol indirect effect.« less

The free radical chemistry of cloud droplets and its impact upon the composition of rain

NASA Technical Reports Server (NTRS)

Chameides, W. L.; Davis, D. D.

1982-01-01

Calculations are presented that simulate the free radical chemistries of the gas phase and aqueous phase within a warm cloud during midday. It is demonstrated that in the presence of midday solar fluxes, the heterogeneous scavenging of OH and HO2 from the gas phase by cloud droplets can represent a major source of free radicals to cloud water, provided the accommodation or sticking coefficient for these species impinging upon water droplets is not less than 0.0001. The aqueous-phase of HO2 radicals are found to be converted to H2O2 by aqueous-phase chemical reactions at a rate that suggests that this mechanism could produce a significant fraction of the H2O2 found in cloud droplets. The rapid oxidation of sulfur species dissolved in cloudwater by this free-radical-produced H2O2 as well as by aqueous-phase OH radicals could conceivably have a significant impact upon the chemical composition of rain.

Droplet Growth Kinetics in Various Environments

NASA Astrophysics Data System (ADS)

Raatikainen, T. E.; Lathem, T. L.; Moore, R.; Lin, J. J.; Cerully, K. M.; Padro, L.; Lance, S.; Cozic, J.; Anderson, B. E.; Nenes, A.

2012-12-01

The largest uncertainties in the effects of atmospherics aerosols on the global radiation budget are related to their indirect effects on cloud properties (IPCC, the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, 2007). Cloud formation is a kinetic process where the resulting cloud properties depend on aerosol properties and meteorological parameters such as updraft velocity (e.g. McFiggans et al., Atmos. Chem. Phys., 6, 2593-2649, 2006). Droplet growth rates are limited by the water vapor diffusion, but additional kinetic limitations, e.g., due to organic surface films, slow solute dissociation or highly viscous or glassy aerosol states have been hypothesized. Significant additional kinetic limitations can lead to increased cloud droplet number concentration, thus the effect is similar to those of increased aerosol number concentration or changes in vertical velocity (e.g. Nenes et al., Geophys. Res. Lett., 29, 1848, 2002). There are a few studies where slow droplet growth has been observed (e.g. Ruehl et al., Geophys. Res. Lett., 36, L15814, 2009), however, little is currently known about their global occurrence and magnitude. Cloud micro-physics models often describe kinetic limitations by an effective water vapor uptake coefficient or similar parameter. Typically, determining aerosol water vapor uptake coefficients requires experimental observations of droplet growth which are interpreted by a numerical droplet growth model where the uptake coefficient is an adjustable parameter (e.g. Kolb et al., Atmos. Chem. Phys., 10, 10561-10605, 2010). Such methods have not been practical for high time-resolution or long term field measurements, until a model was recently developed for analyzing Droplet Measurement Technologies (DMT) cloud condensation nuclei (CCN) counter data (Raatikainen et al., Atmos. Chem. Phys., 12, 4227-4243, 2012). Model verification experiments showed that the calibration aerosol droplet size can be predicted accurately for various instrument settings and also in the case of high CCN concentrations when water vapor depletion decreases supersaturation and droplet size (Lathem and Nenes, Aerosol Sci. Tech., 45, 604-615, 2011). The model also accounts for aerosol hygroscopicity and size distribution variations, which can have significant effects on the droplet size. We have examined cloud droplet activation and growth kinetics by analyzing several DMT CCN counter data sets collected from various environments including boreal forests, arctic areas, fresh and aged biomass burning plumes, and polluted and biogenically influenced urban areas (Raatikainen et al., In preparation, 2012). Model simulations show that the variations in observed droplet size are caused by water vapor depletion effects, changes in dry particle size distributions and hygroscopicity, and changes in instrument supersaturation profiles. This means that fast droplet growth kinetics with water uptake coefficient close to 0.2 is prevalent at least for the studied environments.

Correlations for Vapor Nucleating Critical Embryo Parameters

NASA Astrophysics Data System (ADS)

Magnusson, Lars-Erik; Koropchak, John A.; Anisimov, Michael P.; Poznjakovskiy, Valeriy M.; de la Mora, Juan Fernandez

2003-12-01

Condensation nucleation light scattering detection in principle works by converting the effluent of the chromatographic separation into an aerosol and then selectively evaporating the mobile phase, leaving less volatile analytes and nonvolatile impurities as dry aerosol particles. The dry particles produced are then exposed to an environment that is saturated with the vapors of an organic solvent (commonly n-butanol). The blend of aerosol particles and organic vapor is then cooled so that conditions of vapor supersaturation are achieved. In principle, the vapor then condenses onto the dry particles, growing each particle (ideally) from as small as a few nanometers in diameter into a droplet with a diameter up to about 10 μm. The grown droplets are then passed through a beam of light, and the light scattered by the droplets is detected and used as the detector response. This growth and detection step is generally carried out using commercial continuous-flow condensation nucleus counters. In the present research, the possibility of using other fluids than the commonly used n-butanol is investigated. The Kelvin equation and the Nucleation theorem [Anisimov et al. (1978)] are used to evaluate a range of fluids for efficacy of growing small particles by condensation nucleation. Using the available experimental data on vapor nucleation, the correlations of Kelvin diameters (the critical embryo sizes) and the bulk surface tension with dielectric constants of working liquids are found. A simple method for choosing the most efficient fluid, within a class of fluids, for growth of small particles is suggested.

Using amphiphilic nanostructures to enable long-range ensemble coalescence and surface rejuvenation in dropwise condensation.

PubMed

Anderson, David M; Gupta, Maneesh K; Voevodin, Andrey A; Hunter, Chad N; Putnam, Shawn A; Tsukruk, Vladimir V; Fedorov, Andrei G

2012-04-24

Controlling coalescence events in a heterogeneous ensemble of condensing droplets on a surface is an outstanding fundamental challenge in surface and interfacial sciences, with a broad practical importance in applications ranging from thermal management of high-performance electronic devices to moisture management in high-humidity environments. Nature-inspired superhydrophobic surfaces have been actively explored to enhance heat and mass transfer rates by achieving favorable dynamics during dropwise condensation; however, the effectiveness of such chemically homogeneous surfaces has been limited because condensing droplets tend to form as pinned Wenzel drops rather than mobile Cassie ones. Here, we introduce an amphiphilic nanostructured surface, consisting of a hydrophilic base with hydrophobic tips, which promotes the periodic regeneration of nucleation sites for small droplets, thus rendering the surface self-rejuvenating. This unique amphiphilic nanointerface generates an arrangement of condensed Wenzel droplets that are fluidically linked by a wetted sublayer, promoting previously unobserved coalescence events where numerous droplets simultaneously merge, without direct contact. Such ensemble coalescences rapidly create fresh nucleation sites, thereby shifting the overall population toward smaller droplets and enhancing the rates of mass and heat transfer during condensation.

Investigations of cloud microphysical response to mixing using digital holography

NASA Astrophysics Data System (ADS)

Beals, Matthew Jacob

Cloud edge mixing plays an important role in the life cycle and development of clouds. Entrainment of subsaturated air affects the cloud at the microscale, altering the number density and size distribution of its droplets. The resulting effect is determined by two timescales: the time required for the mixing event to complete, and the time required for the droplets to adjust to their new environment. If mixing is rapid, evaporation of droplets is uniform and said to be homogeneous in nature. In contrast, slow mixing (compared to the adjustment timescale) results in the droplets adjusting to the transient state of the mixture, producing an inhomogeneous result. Studying this process in real clouds involves the use of airborne optical instruments capable of measuring clouds at the 'single particle' level. Single particle resolution allows for direct measurement of the droplet size distribution. This is in contrast to other 'bulk' methods (i.e. hot-wire probes, lidar, radar) which measure a higher order moment of the distribution and require assumptions about the distribution shape to compute a size distribution. The sampling strategy of current optical instruments requires them to integrate over a path tens to hundreds of meters to form a single size distribution. This is much larger than typical mixing scales (which can extend down to the order of centimeters), resulting in difficulties resolving mixing signatures. The Holodec is an optical particle instrument that uses digital holography to record discrete, local volumes of droplets. This method allows for statistically significant size distributions to be calculated for centimeter scale volumes, allowing for full resolution at the scales important to the mixing process. The hologram also records the three dimensional position of all particles within the volume, allowing for the spatial structure of the cloud volume to be studied. Both of these features represent a new and unique view into the mixing problem. In this dissertation, holographic data recorded during two different field projects is analyzed to study the mixing structure of cumulus clouds. Using Holodec data, it is shown that mixing at cloud top can produce regions of clear but humid air that can subside down along the edge of the cloud as a narrow shell, or advect down shear as a 'humid halo'. This air is then entrained into the cloud at lower levels, producing mixing that appears to be very inhomogeneous. This inhomogeneous-like mixing is shown to be well correlated with regions containing elevated concentrations of large droplets. This is used to argue in favor of the hypothesis that dilution can lead to enhanced droplet growth rates. I also make observations on the microscale spatial structure of observed cloud volumes recorded by the Holodec.

Evaporation-triggered microdroplet nucleation and the four life phases of an evaporating Ouzo drop.

PubMed

Tan, Huanshu; Diddens, Christian; Lv, Pengyu; Kuerten, J G M; Zhang, Xuehua; Lohse, Detlef

2016-08-02

Evaporating liquid droplets are omnipresent in nature and technology, such as in inkjet printing, coating, deposition of materials, medical diagnostics, agriculture, the food industry, cosmetics, or spills of liquids. Whereas the evaporation of pure liquids, liquids with dispersed particles, or even liquid mixtures has intensively been studied over the past two decades, the evaporation of ternary mixtures of liquids with different volatilities and mutual solubilities has not yet been explored. Here we show that the evaporation of such ternary mixtures can trigger a phase transition and the nucleation of microdroplets of one of the components of the mixture. As a model system, we pick a sessile Ouzo droplet (as known from daily life-a transparent mixture of water, ethanol, and anise oil) and reveal and theoretically explain its four life phases: In phase I, the spherical cap-shaped droplet remains transparent while the more volatile ethanol is evaporating, preferentially at the rim of the drop because of the singularity there. This leads to a local ethanol concentration reduction and correspondingly to oil droplet nucleation there. This is the beginning of phase II, in which oil microdroplets quickly nucleate in the whole drop, leading to its milky color that typifies the so-called "Ouzo effect." Once all ethanol has evaporated, the drop, which now has a characteristic nonspherical cap shape, has become clear again, with a water drop sitting on an oil ring (phase III), finalizing the phase inversion. Finally, in phase IV, all water has evaporated, leaving behind a tiny spherical cap-shaped oil drop.

Evaporation-triggered microdroplet nucleation and the four life phases of an evaporating Ouzo drop

NASA Astrophysics Data System (ADS)

Tan, Huanshu; Diddens, Christian; Lv, Pengyu; Kuerten, J. G. M.; Zhang, Xuehua; Lohse, Detlef

2016-08-01

Evaporating liquid droplets are omnipresent in nature and technology, such as in inkjet printing, coating, deposition of materials, medical diagnostics, agriculture, the food industry, cosmetics, or spills of liquids. Whereas the evaporation of pure liquids, liquids with dispersed particles, or even liquid mixtures has intensively been studied over the past two decades, the evaporation of ternary mixtures of liquids with different volatilities and mutual solubilities has not yet been explored. Here we show that the evaporation of such ternary mixtures can trigger a phase transition and the nucleation of microdroplets of one of the components of the mixture. As a model system, we pick a sessile Ouzo droplet (as known from daily life—a transparent mixture of water, ethanol, and anise oil) and reveal and theoretically explain its four life phases: In phase I, the spherical cap-shaped droplet remains transparent while the more volatile ethanol is evaporating, preferentially at the rim of the drop because of the singularity there. This leads to a local ethanol concentration reduction and correspondingly to oil droplet nucleation there. This is the beginning of phase II, in which oil microdroplets quickly nucleate in the whole drop, leading to its milky color that typifies the so-called “Ouzo effect.” Once all ethanol has evaporated, the drop, which now has a characteristic nonspherical cap shape, has become clear again, with a water drop sitting on an oil ring (phase III), finalizing the phase inversion. Finally, in phase IV, all water has evaporated, leaving behind a tiny spherical cap-shaped oil drop.

Evaporation-triggered microdroplet nucleation and the four life phases of an evaporating Ouzo drop

PubMed Central

Tan, Huanshu; Diddens, Christian; Lv, Pengyu; Kuerten, J. G. M.; Zhang, Xuehua; Lohse, Detlef

2016-01-01

Evaporating liquid droplets are omnipresent in nature and technology, such as in inkjet printing, coating, deposition of materials, medical diagnostics, agriculture, the food industry, cosmetics, or spills of liquids. Whereas the evaporation of pure liquids, liquids with dispersed particles, or even liquid mixtures has intensively been studied over the past two decades, the evaporation of ternary mixtures of liquids with different volatilities and mutual solubilities has not yet been explored. Here we show that the evaporation of such ternary mixtures can trigger a phase transition and the nucleation of microdroplets of one of the components of the mixture. As a model system, we pick a sessile Ouzo droplet (as known from daily life—a transparent mixture of water, ethanol, and anise oil) and reveal and theoretically explain its four life phases: In phase I, the spherical cap-shaped droplet remains transparent while the more volatile ethanol is evaporating, preferentially at the rim of the drop because of the singularity there. This leads to a local ethanol concentration reduction and correspondingly to oil droplet nucleation there. This is the beginning of phase II, in which oil microdroplets quickly nucleate in the whole drop, leading to its milky color that typifies the so-called “Ouzo effect.” Once all ethanol has evaporated, the drop, which now has a characteristic nonspherical cap shape, has become clear again, with a water drop sitting on an oil ring (phase III), finalizing the phase inversion. Finally, in phase IV, all water has evaporated, leaving behind a tiny spherical cap-shaped oil drop. PMID:27418601

Development and characterization of an ice-selecting pumped counterflow virtual impactor (IS-PCVI) to study ice crystal residuals

NASA Astrophysics Data System (ADS)

Hiranuma, Naruki; Möhler, Ottmar; Kulkarni, Gourihar; Schnaiter, Martin; Vogt, Steffen; Vochezer, Paul; Järvinen, Emma; Wagner, Robert; Bell, David M.; Wilson, Jacqueline; Zelenyuk, Alla; Cziczo, Daniel J.

2016-08-01

Separation of particles that play a role in cloud activation and ice nucleation from interstitial aerosols has become necessary to further understand aerosol-cloud interactions. The pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to accelerate the particles and increase their momentum, provides an accessible option for dynamic and inertial separation of cloud elements. However, the use of a traditional PCVI to extract large cloud hydrometeors is difficult mainly due to its small cut-size diameters (< 5 µm). Here, for the first time we describe a development of an ice-selecting PCVI (IS-PCVI) to separate ice in controlled mixed-phase cloud system based on the particle inertia with the cut-off diameter ≥ 10 µm. We also present its laboratory application demonstrating the use of the impactor under a wide range of temperature and humidity conditions. The computational fluid dynamics simulations were initially carried out to guide the design of the IS-PCVI. After fabrication, a series of validation laboratory experiments were performed coupled with the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) expansion cloud simulation chamber. In the AIDA chamber, test aerosol particles were exposed to the ice supersaturation conditions (i.e., RHice > 100 %), where a mixture of droplets and ice crystals was formed during the expansion experiment. In parallel, the flow conditions of the IS-PCVI were actively controlled, such that it separated ice crystals from a mixture of ice crystals and cloud droplets, which were of diameter ≥ 10 µm. These large ice crystals were passed through the heated evaporation section to remove the water content. Afterwards, the residuals were characterized with a suite of online and offline instruments downstream of the IS-PCVI. These results were used to assess the optimized operating parameters of the device in terms of (1) the critical cut-size diameter, (2) the transmission efficiency and (3) the counterflow-to-input flow ratio. Particle losses were characterized by comparing the residual number concentration to the rejected interstitial particle number concentration. Overall results suggest that the IS-PCVI enables inertial separation of particles with a volume-equivalent particle size in the range of ~ 10-30 µm in diameter with small inadvertent intrusion (~  5 %) of unwanted particles.

Why do general circulation models overestimate the aerosol cloud lifetime effect? A case study comparing CAM5 and a CRM

NASA Astrophysics Data System (ADS)

Zhou, Cheng; Penner, Joyce E.

2017-01-01

Observation-based studies have shown that the aerosol cloud lifetime effect or the increase of cloud liquid water path (LWP) with increased aerosol loading may have been overestimated in climate models. Here, we simulate shallow warm clouds on 27 May 2011 at the southern Great Plains (SGP) measurement site established by the Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) program using a single-column version of a global climate model (Community Atmosphere Model or CAM) and a cloud resolving model (CRM). The LWP simulated by CAM increases substantially with aerosol loading while that in the CRM does not. The increase of LWP in CAM is caused by a large decrease of the autoconversion rate when cloud droplet number increases. In the CRM, the autoconversion rate is also reduced, but this is offset or even outweighed by the increased evaporation of cloud droplets near the cloud top, resulting in an overall decrease in LWP. Our results suggest that climate models need to include the dependence of cloud top growth and the evaporation/condensation process on cloud droplet number concentrations.

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.

Radiative Susceptibility of Cloudy Atmospheres to Droplet Number Perturbations: 1. Theoretical Analysis and Examples from MODIS

NASA Technical Reports Server (NTRS)

Platnick, Steven; Oreopoulos, Lazaros

2008-01-01

Theoretical and satellite-based assessments of the sensitivity of broadband shortwave radiative fluxes in cloudy atmospheres to small perturbations in the cloud droplet number concentration (N) of liquid water clouds under constant water conditions are performed. Two approaches to study this sensitivity are adopted: absolute increases in N, for which the radiative response is referred to as absolute cloud susceptibility, and relative increases in N or relative cloud susceptibility. Estimating the former is more challenging as it requires an assumed value for either cloud liquid water content or geometrical thickness; both susceptibilities require an assumed relationship between the droplet volume and effective radius. Expanding upon previous susceptibility studies, present radiative calculations include the effect of AN perturbations on droplet asymmetry parameter and single-scattering albedo, in addition to extinction. Absolute cloud susceptibility has a strong nonlinear dependence on the droplet effective radius as expected, while relative cloud susceptibility is primarily dependent on optical thickness. Molecular absorption and reflecting surfaces both reduce the relative contribution of the cloud to the top-of-atmosphere (TOA) flux and therefore also reduce the TOA albedo susceptibility. Transmittance susceptibilities are negative with absolute values similar to albedo susceptibility, while atmospheric absorptance susceptibilities are about an order of magnitude smaller than albedo susceptibilities and can be either positive or negative. Observation-based susceptibility calculations are derived from MODIS pixel-level retrievals of liquid water cloud optical thickness, effective radius, and cloud top temperature; two data granule examples are shown. Susceptibility quantifies the aerosol indirect effect sensitivity in a way that can be easily computed from model fields. As such, susceptibilities derived from MODIS observations provide a higher-order test of model cloud properties used for indirect effect studies. MODIS-derived global distributions of cloud susceptibility and radiative forcing calculations are presented in a companion paper.

Coupled Retrieval of Liquid Water Cloud and Above-Cloud Aerosol Properties Using the Airborne Multiangle SpectroPolarimetric Imager (AirMSPI)

NASA Astrophysics Data System (ADS)

Xu, Feng; van Harten, Gerard; Diner, David J.; Davis, Anthony B.; Seidel, Felix C.; Rheingans, Brian; Tosca, Mika; Alexandrov, Mikhail D.; Cairns, Brian; Ferrare, Richard A.; Burton, Sharon P.; Fenn, Marta A.; Hostetler, Chris A.; Wood, Robert; Redemann, Jens

2018-03-01

An optimization algorithm is developed to retrieve liquid water cloud properties including cloud optical depth (COD), droplet size distribution and cloud top height (CTH), and above-cloud aerosol properties including aerosol optical depth (AOD), single-scattering albedo, and microphysical properties from sweep-mode observations by Jet Propulsion Laboratory's Airborne Multiangle SpectroPolarimetric Imager (AirMSPI) instrument. The retrieval is composed of three major steps: (1) initial estimate of the mean droplet size distribution across the entire image of 80-100 km along track by 10-25 km across track from polarimetric cloudbow observations, (2) coupled retrieval of image-scale cloud and above-cloud aerosol properties by fitting the polarimetric data at all observation angles, and (3) iterative retrieval of 1-D radiative transfer-based COD and droplet size distribution at pixel scale (25 m) by establishing relationships between COD and droplet size and fitting the total radiance measurements. Our retrieval is tested using 134 AirMSPI data sets acquired during the National Aeronautics and Space Administration (NASA) field campaign ObseRvations of Aerosols above CLouds and their intEractionS. The retrieved above-cloud AOD and CTH are compared to coincident HSRL-2 (HSRL-2, NASA Langley Research Center) data, and COD and droplet size distribution parameters (effective radius reff and effective variance veff) are compared to coincident Research Scanning Polarimeter (RSP) (NASA Goddard Institute for Space Studies) data. Mean absolute differences between AirMSPI and HSRL-2 retrievals of above-cloud AOD at 532 nm and CTH are 0.03 and <0.5 km, respectively. At RSP's footprint scale ( 323 m), mean absolute differences between RSP and AirMSPI retrievals of COD, reff, and veff in the cloudbow area are 2.33, 0.69 μm, and 0.020, respectively. Neglect of smoke aerosols above cloud leads to an underestimate of image-averaged COD by 15%.

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

Kulkarni, Gourihar R.; Zhang, Kai; Zhao, Chun

Changes in the ice nucleation characteristics of atmospherically relevant mineral dust particles due to nitric acid coating are not well understood. Further, the atmospheric implications of dust coating on ice-cloud properties under different assumptions of primary ice nucleation mechanisms are unknown. We investigated ice nucleation ability of Arizona test dust, illite, K-feldspar and quartz as a function of temperature (-25 to -30°C) and relative humidity with respect to water (75 to 110%). Particles were size selected at 250 nm and transported (bare or coated) to the ice nucleation chamber to determine the fraction of particles nucleating ice at various temperaturemore » and water saturation conditions. All dust nucleated ice at water-subsaturated conditions, but the coated particles showed a reduction in their ice nucleation ability compared to bare particles. However, at water-supersaturated conditions, we observed that bare and coated particles had nearly similar ice nucleation characteristics. X-ray diffraction patterns indicated that structural properties of bare dust particles modified after acid treatment. We found that lattice parameters were slightly different, but crystallite sizes of the coated particles were reduced compared to bare particles. Next, single-column model results show that simulated ice crystal number concentrations mostly depends upon fraction of particles that are coated, primary ice nucleation mechanisms, and the competition between ice nucleation mechanisms to nucleate ice. In general, we observed that coating modify the ice-cloud properties and the picture of ice and mixed-phase cloud evolution is complex when different primary ice nucleation mechanisms are competing for fixed water vapor mass.« less

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.

Sensitivity of Cirrus Properties to Ice Nuclei Abundance

NASA Technical Reports Server (NTRS)

Jensen, Eric

2014-01-01

The relative importance of heterogeneous and homogeneous ice nucleation for cirrus formation remains an active area of debate in the cloud physics community. From a theoretical perspective, a number of modeling studies have investigated the sensitivity of ice number concentration to the nucleation mechanism and the abundance of ice nuclei. However, these studies typically only addressed ice concentration immediately after ice nucleation. Recent modeling work has shown that the high ice concentrations produced by homogeneous freezing may not persist very long, which is consistent with the low frequency of occurrence of high ice concentrations indicated by cirrus measurements. Here, I use idealized simulations to investigate the impact of ice nucleation mechanism and ice nuclei abundance on the full lifecycle of cirrus clouds. The primary modeling framework used includes different modes of ice nucleation, deposition growth/sublimation, aggregation, sedimentation, and radiation. A limited number of cloud-resolving simulations that treat radiation/dynamics interactions will also been presented. I will show that for typical synoptic situations with mesoscale waves present, the time-averaged cirrus ice crystal size distributions and bulk cloud properties are less sensitive to ice nucleation processes than might be expected from the earlier simple ice nucleation calculations. I will evaluate the magnitude of the ice nuclei impact on cirrus for a range of temperatures and mesoscale wave specifications, and I will discuss the implications for cirrus aerosol indirect effects in general.

Evaporation of a sessile water drop and a drop of aqueous salt solution.

PubMed

Misyura, S Y

2017-11-07

The influence of various factors on the evaporation of drops of water and aqueous salt solution has been experimentally studied. Typically, in the studies of drop evaporation, only the diffusive vapor transfer, radiation and the molecular heat conduction are taken into account. However, vapor-gas convection plays an important role at droplet evaporation. In the absence of droplet boiling, the influence of gas convection turns out to be the prevailing factor. At nucleate boiling, a prevailing role is played by bubbles generation and vapor jet discharge at a bubble collapse. The gas convection behavior for water and aqueous salt solution is substantially different. With a growth of salt concentration over time, the influence of the convective component first increases, reaches an extremum and then significantly decreases. At nucleate boiling in a salt solution it is incorrect to simulate the droplet evaporation and the heat transfer in quasi-stationary approximation. The evaporation at nucleate boiling in a liquid drop is divided into several characteristic time intervals. Each of these intervals is characterized by a noticeable change in both the evaporation rate and the convection role.

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.

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.

Icing Cloud Calibration of the NASA Glenn Icing Research Tunnel

NASA Technical Reports Server (NTRS)

Ide, Robert F.; Oldenburg, John R.

2001-01-01

The icing research tunnel at the NASA Glenn Research Center underwent a major rehabilitation in 1999, necessitating recalibration of the icing clouds. This report describes the methods used in the recalibration, including the procedure used to establish a uniform icing cloud and the use of a standard icing blade technique for measurement of liquid water content. The instruments and methods used to perform the droplet size calibration are also described. The liquid water content/droplet size operating envelopes of the icing tunnel are shown for a range of airspeeds and compared to the FAA icing certification criteria. The capabilities of the IRT to produce large droplet icing clouds is also detailed.

Twomey Effect in Subtropical Stratocumulus Clouds from UV Depolarization LIDAR

NASA Astrophysics Data System (ADS)

de Graaf, Martin; Brown, Jessica; Donovan, David

2018-04-01

Marine stratocumulus clouds are important climate regulators, reflecting sunlight over a dark ocean background. A UV-depolarization lidar on Ascension, a small remote island in the south Atlantic, measured cloud droplet sizes and number concentration using an inversion method based on Monte Carlo (MC) modelling of multiple scattering in idealised semiadiabatic clouds. The droplet size and number concentration weremodulated due to smoke from the African continent, measured by the same instrument.

Iridescent clouds and distorted coronas.

PubMed

Laven, Philip

2017-07-01

Near-forward scattering of sunlight generates coronas and iridescence on clouds. Coronas are caused by diffraction, whereas iridescence is less easily explained. Iridescence often appears as bands of color aligned with the edges of clouds or as apparently random patches of color on clouds. This paper suggests that iridescence is due to interference between light that has been diffracted by a spherical droplet of water and light that has been transmitted through the same droplet.

A microphysical parameterization of aqSOA and sulfate formation in clouds

NASA Astrophysics Data System (ADS)

McVay, Renee; Ervens, Barbara

2017-07-01

Sulfate and secondary organic aerosol (cloud aqSOA) can be chemically formed in cloud water. Model implementation of these processes represents a computational burden due to the large number of microphysical and chemical parameters. Chemical mechanisms have been condensed by reducing the number of chemical parameters. Here an alternative is presented to reduce the number of microphysical parameters (number of cloud droplet size classes). In-cloud mass formation is surface and volume dependent due to surface-limited oxidant uptake and/or size-dependent pH. Box and parcel model simulations show that using the effective cloud droplet diameter (proportional to total volume-to-surface ratio) reproduces sulfate and aqSOA formation rates within ≤30% as compared to full droplet distributions; other single diameters lead to much greater deviations. This single-class approach reduces computing time significantly and can be included in models when total liquid water content and effective diameter are available.

Biogenic influence on cloud microphysics in the 'clean' oceanic atmosphere

NASA Astrophysics Data System (ADS)

Lana, A.; Simó, R.; Vallina, S. M.; Jurado, E.; Dachs, J.

2009-12-01

A 20 years old hypothesis postulates a feedback relationship between marine biota and climate through the emission of dimethylsulfide (DMS) as the principal natural source of Sulfate Secondary Aerosols (S-DMS) that are very efficient as cloud condensation nuclei (CCN). In recent years, the biological influence on cloud microphysics have been expanded to other potential biogenic cloud precursors: (i) volatile organic compounds produced by plankton and emitted to the atmosphere to form Secondary Organic Aerosols (SOA); (ii) biological particles and biogenic polymers, lifted with the seaspray by wind friction and bubble-bursting processes, that act as Primary Organic Aerosols (POA). Besides these biogenic aerosols, also seaspray-associated Sea Salt (SS) emissions, which are the dominant contribution to aerosol mass in the remote mixed boundary layer, also contribute to cloud condensation. All these aerosols affect cloud microphysics by providing new CCN, reducing the size of cloud droplets, and increasing cloud albedo. We have compared the seasonalities of the parameterized source functions of these natural cloud precursors with that of the satellite-derived cloud droplet effective radius (CLEFRA) over large regions of the ocean. Regions where big loads of continental aerosols (including anthropogenic -industrial, urban, and biomass burning) dominate during a significant part of the year were identified by use of remote sensing aerosol optical properties and excluded from our analysis. Our results show that the seasonality of cloud droplet effective radius matches those of S-DMS and SOA in the clean marine atmosphere, whereas SS and chlorophyll-associated POA on their own do not seem to play a major role in driving cloud droplet size.

A Method for Determining Cloud-Droplet Impingement on Swept Wings

NASA Technical Reports Server (NTRS)

Dorsch, Robert G.; Brun, Rinaldo J.

1953-01-01

The general effect of wing sweep on cloud-droplet trajectories about swept wings of high aspect ratio moving at subsonic speeds is discussed. A method of computing droplet trajectories about yawed cylinders and swept wings is presented, and illustrative droplet trajectories are computed. A method of extending two-dimensional calculations of droplet impingement on nonswept wings to swept wings is presented. It is shown that the extent of impingement of cloud droplets on an airfoil surface, the total rate of collection of water, and the local rate of impingement per unit area of airfoil surface can be found for a swept wing from two-dimensional data for a nonswept wing. The impingement on a swept wing is obtained from impingement data for a nonswept airfoil section which is the same as the section in the normal plane of the swept wing by calculating all dimensionless parameters with respect to flow conditions in the normal plane of the swept wing.

Modeling cumulus clouds in a two-phase wind tunnel

NASA Astrophysics Data System (ADS)

Bordás, R.; Thévenin, D.

2009-04-01

Experiments in wind-tunnels concerning meteorological flows are not very frequent in the literature. However, they are indispensable for a well-controlled and accurate investigation of turbulence-droplet interactions at the micro-scale. Of course it is impossible to reproduce perfectly the turbulent properties of clouds in a comparatively small wind-tunnel. The enormous length scales that are predominant in nature (integral length scale of typically 100 meters) lead to very high Reynolds numbers, roughly 107 calculated with the cloud dimensions or 104 as Taylor Reynolds number Reλ. Nevertheless, it is not necessary to reproduce exactly the whole turbulence spectrum to investigate the issue of rain formation in cumulus clouds. Only those scales and turbulence properties should be reproduced in the wind tunnel, which are physically important for the droplet population. In this work the key properties of cumulus clouds will be identified and implemented in a two-phase wind tunnel, allowing reproducible and accurate measurements. These properties are in particular the droplet number density, the turbulent kinetic energy and its dissipation rate. It is demonstrated by means of non-intrusive optical measurement techniques that the flow velocity, droplet number density, and key turbulence properties have been matched and are in the right order of magnitude. In this manner wind-tunnel investigations become possible and deliver realistic information concerning the interaction between droplets and turbulence in cumulus clouds.

Investigation of heterogeneous ice nucleation in pollen suspensions and washing water

NASA Astrophysics Data System (ADS)

Dreischmeier, Katharina; Budke, Carsten; Koop, Thomas

2014-05-01

Biological particles such as pollen often show ice nucleation activity at temperatures higher than -20 °C. Immersion freezing experiments of pollen washing water demonstrate comparable ice nucleation behaviour as water containing the whole pollen bodies (Pummer et al., 2012). It was suggested that polysaccharide molecules leached from the grains are responsible for the ice nucleation. Here, heterogeneous ice nucleation in birch pollen suspensions and their washing water was investigated by two different experimental methods. The optical freezing array BINARY (Bielefeld Ice Nucleation ARraY) allows the direct observation of freezing of microliter-sized droplets. The IN spectra obtained from such experiments with birch pollen suspensions over a large concentration range indicate several different ice nucleation active species, two of which are present also in the washing water. The latter was probed also in differential scanning calorimeter (DSC) experiments of emulsified sub-picoliter droplets. Due to the small droplet size in the emulsion samples and at small concentration of IN in the washing water, such DSC experiments can exhibit the ice nucleation behaviour of a single nucleus. The two heterogeneous freezing signals observed in the DSC thermograms can be assigned to two different kinds of ice nuclei, confirming the observation from the BINARY measurements, and also previous studies on Swedish birch pollen washing water (Augustin et al., 2012). The authors gratefully acknowledge funding by the German Research Foundation (DFG) through the project BIOCLOUDS (KO 2944/1-1) and through the research unit INUIT (FOR 1525) under KO 2944/2-1. We particularly thank our INUIT partners for fruitful collaboration and sharing of ideas and IN samples. S. Augustin, H. Wex, D. Niedermeier, B. Pummer, H. Grothe, S. Hartmann, L. Tomsche, T. Clauss, J. Voigtländer, K. Ignatius, and F. Stratmann, Immersion freezing of birch pollen washing water, Atmos. Chem. Phys., 13, 10989-11003, 2013. B. Pummer, H Bauer, J. Bernardi, S. Bleicher, H. Grothe, Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen, Atmos. Chem. Phys., 12, 2541-2550, 2012.

Investigating the significance of zero-point motion in small molecular clusters of sulphuric acid and water

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

Stinson, Jake L.; Kathmann, Shawn M.; Ford, Ian J.

2014-01-14

The nucleation of particles from trace gases in the atmosphere is an important source of cloud condensation nuclei (CCN), and these are vital for the formation of clouds in view of the high supersaturations required for homogeneous water droplet nucleation. The methods of quantum chemistry have increasingly been employed to model nucleation due to their high accuracy and efficiency in calculating configurational energies; and nucleation rates can be obtained from the associated free energies of particle formation. However, even in such advanced approaches, it is typically assumed that the nuclei have a classical nature, which is questionable for some systems.more » The importance of zero-point motion (also known as quantum nuclear dynamics) in modelling small clusters of sulphuric acid and water is tested here using the path integral molecular dynamics (PIMD) method at the density functional theory (DFT) level of theory. We observe a small zero-point effect on the the equilibrium structures of certain clusters. One configuration is found to display a bimodal behaviour at 300 K in contrast to the stable ionised state suggested from a zero temperature classical geometry optimisation. The general effect of zero-point motion is to promote the extent of proton transfer with respect to classical behaviour. We thank Prof. Angelos Michaelides and his group in University College London (UCL) for practical advice and helpful discussions. This work benefited from interactions with the Thomas Young Centre through seminar and discussions involving the PIMD method. SMK was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. JLS and IJF were supported by the IMPACT scheme at UCL and by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. We are grateful for use of the UCL Legion High Performance Computing Facility and the resources of the National Energy Research Scientific Computing Center (NERSC), which is supported by the U.S. Department of Energy, Office of Science of the under Contract No. DE-AC02-05CH11231.« less

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.

Particle size distributions in Arctic polar stratospheric clouds, growth and freezing of sulfuric acid droplets, and implications for cloud formation

NASA Technical Reports Server (NTRS)

Dye, James E.; Baumgardner, D.; Gandrud, B. W.; Kawa, S. R.; Kelly, K. K.; Loewenstein, M.; Ferry, G. V.; Chan, K. R.; Gary, B. L.

1992-01-01

The paper uses particle size and volume measurements obtained with the forward scattering spectrometer probe model 300 during January and February 1989 in the Airborne Arctic Stratospheric Experiment to investigate processes important in the formation and growth of polar stratospheric cloud (PSC) particles. It is suggested on the basis of comparisons of the observations with expected sulfuric acid droplet deliquescence that in the Arctic a major fraction of the sulfuric acid droplets remain liquid until temperatures at least as low as 193 K. It is proposed that homogeneous freezing of the sulfuric acid droplets might occur near 190 K and might play a role in the formation of PSCs.

The global impact of mineral dust on cloud droplet number concentration

NASA Astrophysics Data System (ADS)

Karydis, V.; Tsimpidi, A.; Bacer, S.; Pozzer, A.; Nenes, A.; Lelieveld, J.

2016-12-01

This study assesses the importance of mineral dust for cloud droplet formation by taking into account i) the adsorption of water on the surface of insoluble dust particles, ii) the coating of soluble material on the surface of mineral particles which augments their cloud condensation nuclei activity, and iii) the effect of dust on the inorganic aerosol concentrations through thermodynamic interactions with mineral cations. Simulations are carried out with the EMAC chemistry climate model that calculates the global atmospheric aerosol composition using the ISORROPIA-II thermodynamic equilibrium model and considers the gas phase interactions with K+-Ca2+-Mg2+-NH4+-Na+-SO42-NO3-Cl-H2O particle components. Emissions of the inert mineral dust and the reactive dust aerosol components are calculated online by taking into account the soil particle size distribution and chemical composition of different deserts worldwide (Karydis et al., 2016). We have implemented the "unified dust activation parameterization" (Kumar et al., 2011; Karydis et al., 2011) to calculate the droplet number concentration by taking into account the inherent hydrophilicity from adsorption and the acquired hygroscopicity from soluble salts by dust particles. Our simulations suggest that mineral dust significantly increases the cloud droplet number concentration (CDNC) over the main deserts and the adjacent oceans. However, over polluted areas the CDNC decreases significantly in the presence of dust. Furthermore, we investigate the role of adsorption activation of insoluble aerosols and the mineral dust thermodynamic interactions with inorganic anions on the cloud droplet formation. The CDNC sensitivity to the emission load, chemical composition, and inherent hydrophilicity of mineral dust is also tested. ReferencesKarydis, et al. (2011). "On the effect of dust particles on global cloud condensation nuclei and cloud droplet number." J. Geophys. Res. Atmos. 116. Karydis, et al. (2016). "Effects of mineral dust on global atmospheric nitrate concentrations." Atmos. Chem. Phys. 16(3): 1491-1509. Kumar, et al. (2011). "Measurements of cloud condensation nuclei activity and droplet activation kinetics of wet processed regional dust samples and minerals." Atmos. Chem. Phys. Discuss. 11(4): 12561-12605.

Experimental investigation on the effect of liquid injection by multiple orifices in the formation of droplets in a Venturi scrubber.

PubMed

Guerra, V G; Gonçalves, J A S; Coury, J R

2009-01-15

Venturi scrubbers are widely utilized in gas cleaning. The cleansing elements in these scrubbers are droplets formed from the atomization of a liquid into a dust-laden gas. In industrial scrubbers, this liquid is injected through several orifices so that the cloud of droplets can be evenly distributed throughout the duct. The interaction between droplets when injected through many orifices, where opposite clouds of atomized liquid can reach each other, is to be expected. This work presents experimental measurements of droplet size measured in situ and the evidence of cloud interaction within a Venturi scrubber operating with multi-orifice jet injection. The influence of gas velocity, liquid flow rate and droplet size variation in the axial position after the point of the injection of the liquid were also evaluated for the different injection configurations. The experimental results showed that an increase in the liquid flow rate generated greater interaction between jets. The number of orifices had a significant influence on droplet size. In general, the increase in the velocity of the liquid jet and in the gas velocity favored the atomization process by reducing the size of the droplets.

Acyl-CoA synthetase 3 promotes lipid droplet biogenesis in ER microdomains

PubMed Central

Kassan, Adam; Herms, Albert; Fernández-Vidal, Andrea; Bosch, Marta; Schieber, Nicole L.; Reddy, Babu J.N.; Fajardo, Alba; Gelabert-Baldrich, Mariona; Tebar, Francesc; Enrich, Carlos; Gross, Steven P.

2013-01-01

Control of lipid droplet (LD) nucleation and copy number are critical, yet poorly understood, processes. We use model peptides that shift from the endoplasmic reticulum (ER) to LDs in response to fatty acids to characterize the initial steps of LD formation occurring in lipid-starved cells. Initially, arriving lipids are rapidly packed in LDs that are resistant to starvation (pre-LDs). Pre-LDs are restricted ER microdomains with a stable core of neutral lipids. Subsequently, a first round of “emerging” LDs is nucleated, providing additional lipid storage capacity. Finally, in proportion to lipid concentration, new rounds of LDs progressively assemble. Confocal microscopy and electron tomography suggest that emerging LDs are nucleated in a limited number of ER microdomains after a synchronized stepwise process of protein gathering, lipid packaging, and recognition by Plin3 and Plin2. A comparative analysis demonstrates that the acyl-CoA synthetase 3 is recruited early to the assembly sites, where it is required for efficient LD nucleation and lipid storage. PMID:24368806

New High-Performance Droplet Freezing Assay (HP-DFA) for the Analysis of Ice Nuclei with Complex Composition

NASA Astrophysics Data System (ADS)

Kunert, Anna Theresa; Scheel, Jan Frederik; Helleis, Frank; Klimach, Thomas; Pöschl, Ulrich; Fröhlich-Nowoisky, Janine

2016-04-01

Freezing of water above homogeneous freezing is catalyzed by ice nucleation active (INA) particles called ice nuclei (IN), which can be of various inorganic or biological origin. The freezing temperatures reach up to -1 °C for some biological samples and are dependent on the chemical composition of the IN. The standard method to analyze IN in solution is the droplet freezing assay (DFA) established by Gabor Vali in 1970. Several modifications and improvements were already made within the last decades, but they are still limited by either small droplet numbers, large droplet volumes or inadequate separation of the single droplets resulting in mutual interferences and therefore improper measurements. The probability that miscellaneous IN are concentrated together in one droplet increases with the volume of the droplet, which can be described by the Poisson distribution. At a given concentration, the partition of a droplet into several smaller droplets leads to finely dispersed IN resulting in better statistics and therefore in a better resolution of the nucleation spectrum. We designed a new customized high-performance droplet freezing assay (HP-DFA), which represents an upgrade of the previously existing DFAs in terms of temperature range and statistics. The necessity of observing freezing events at temperatures lower than homogeneous freezing due to freezing point depression, requires high-performance thermostats combined with an optimal insulation. Furthermore, we developed a cooling setup, which allows both huge and tiny temperature changes within a very short period of time. Besides that, the new DFA provides the analysis of more than 750 droplets per run with a small droplet volume of 5 μL. This enables a fast and more precise analysis of biological samples with complex IN composition as well as better statistics for every sample at the same time.

Impingement of Cloud Droplets on 36.5-Percent-Thick Joukowski Airfoil at Zero Angle of Attack and Discussion of Use as Cloud Measuring Instrument in Dye-Tracer Technique

NASA Technical Reports Server (NTRS)

Brun, R. J.; Vogt, Dorothea E.

1957-01-01

The trajectories of droplets i n the air flowing past a 36.5-percent-thick Joukowski airfoil at zero angle of attack were determined. The amount of water i n droplet form impinging on the airfoil, the area of droplet impingement, and the rate of droplet impingement per unit area on the airfoil surface were calculated from the trajectories and cover a large range of flight and atmospheric conditions. With the detailed impingement information available, the 36.5-percent-thick Joukowski airfoil can serve the dual purpose of use as the principal element in instruments for making measurements in clouds and of a basic shape for estimating impingement on a thick streamlined body. Methods and examples are presented for illustrating some limitations when the airfoil is used as the principal element in the dye-tracer technique.

Bridging the condensation-collision size gap: a direct numerical simulation of continuous droplet growth in turbulent clouds

NASA Astrophysics Data System (ADS)

Chen, Sisi; Yau, Man-Kong; Bartello, Peter; Xue, Lulin

2018-05-01

In most previous direct numerical simulation (DNS) studies on droplet growth in turbulence, condensational growth and collisional growth were treated separately. Studies in recent decades have postulated that small-scale turbulence may accelerate droplet collisions when droplets are still small when condensational growth is effective. This implies that both processes should be considered simultaneously to unveil the full history of droplet growth and rain formation. This paper introduces the first direct numerical simulation approach to explicitly study the continuous droplet growth by condensation and collisions inside an adiabatic ascending cloud parcel. Results from the condensation-only, collision-only, and condensation-collision experiments are compared to examine the contribution to the broadening of droplet size distribution (DSD) by the individual process and by the combined processes. Simulations of different turbulent intensities are conducted to investigate the impact of turbulence on each process and on the condensation-induced collisions. The results show that the condensational process promotes the collisions in a turbulent environment and reduces the collisions when in still air, indicating a positive impact of condensation on turbulent collisions. This work suggests the necessity of including both processes simultaneously when studying droplet-turbulence interaction to quantify the turbulence effect on the evolution of cloud droplet spectrum and rain formation.

Accuracy Assessments of Cloud Droplet Size Retrievals from Polarized Reflectance Measurements by the Research Scanning Polarimeter

NASA Technical Reports Server (NTRS)

Alexandrov, Mikhail Dmitrievic; Cairns, Brian; Emde, Claudia; Ackerman, Andrew S.; vanDiedenhove, Bastiaan

2012-01-01

We present an algorithm for the retrieval of cloud droplet size distribution parameters (effective radius and variance) from the Research Scanning Polarimeter (RSP) measurements. The RSP is an airborne prototype for the Aerosol Polarimetery Sensor (APS), which was on-board of the NASA Glory satellite. This instrument measures both polarized and total reflectance in 9 spectral channels with central wavelengths ranging from 410 to 2260 nm. The cloud droplet size retrievals use the polarized reflectance in the scattering angle range between 135deg and 165deg, where they exhibit the sharply defined structure known as the rain- or cloud-bow. The shape of the rainbow is determined mainly by the single scattering properties of cloud particles. This significantly simplifies both forward modeling and inversions, while also substantially reducing uncertainties caused by the aerosol loading and possible presence of undetected clouds nearby. In this study we present the accuracy evaluation of our algorithm based on the results of sensitivity tests performed using realistic simulated cloud radiation fields.

Role of Microphysical Parameterizations with Droplet Relative Dispersion in IAP AGCM 4.1

DOE PAGES

Xie, Xiaoning; Zhang, He; Liu, Xiaodong; ...

2018-01-10

In previous studies we see that accurate descriptions of the cloud droplet effective radius (Re) and the autoconversion process of cloud droplets to raindrops (Au) can effectively improve simulated clouds and surface precipitation, and reduce the uncertainty of aerosol indirect effects in global climate models (GCMs). In this paper, we implement cloud microphysical schemes including two-moment Au and R e considering relative dispersion of the cloud droplet size distribution into version 4.1 of the Institute of Atmospheric Physics atmospheric GCM (IAP AGCM 4.1), which is the atmospheric component of the Chinese Academy of Sciences-Earth System model (CAS-ESM 1.0). An analysismore » of the effects of different schemes shows that the newly implemented schemes can improve both the simulated shortwave (SWCF) and longwave cloud radiative forcings (LWCF) as compared to the standard scheme in IAP AGCM 4.1. The new schemes also effectively enhance the large-scale precipitation, especially over low latitudes, although the influences of total precipitation are insignificant for different schemes. Further studies show that similar results can be found with the Community Atmosphere Model 5.1 (CAM5.1).« less

Role of Microphysical Parameterizations with Droplet Relative Dispersion in IAP AGCM 4.1

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

Xie, Xiaoning; Zhang, He; Liu, Xiaodong

In previous studies we see that accurate descriptions of the cloud droplet effective radius (Re) and the autoconversion process of cloud droplets to raindrops (Au) can effectively improve simulated clouds and surface precipitation, and reduce the uncertainty of aerosol indirect effects in global climate models (GCMs). In this paper, we implement cloud microphysical schemes including two-moment Au and R e considering relative dispersion of the cloud droplet size distribution into version 4.1 of the Institute of Atmospheric Physics atmospheric GCM (IAP AGCM 4.1), which is the atmospheric component of the Chinese Academy of Sciences-Earth System model (CAS-ESM 1.0). An analysismore » of the effects of different schemes shows that the newly implemented schemes can improve both the simulated shortwave (SWCF) and longwave cloud radiative forcings (LWCF) as compared to the standard scheme in IAP AGCM 4.1. The new schemes also effectively enhance the large-scale precipitation, especially over low latitudes, although the influences of total precipitation are insignificant for different schemes. Further studies show that similar results can be found with the Community Atmosphere Model 5.1 (CAM5.1).« less

Merging magnetic droplets by a magnetic field pulse

NASA Astrophysics Data System (ADS)

Wang, Chengjie; Xiao, Dun; Liu, Yaowen

2018-05-01

Reliable manipulation of magnetic droplets is of immense importance for their applications in spin torque oscillators. Using micromagnetic simulations, we find that the antiphase precession state, which originates in the dynamic dipolar interaction effect, is a favorable stable state for two magnetic droplets nucleated at two identical nano-contacts. A magnetic field pulse can be used to destroy their stability and merge them into a big droplet. The merging process strongly depends on the pulse width as well as the pulse strength.

International Workshop on Comparing Ice Nucleation Measuring Systems 2014

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

Cziczo, Daniel

The relationship of ambient aerosol particles to the formation of ice-containing clouds is one of the largest uncertainties in understanding the Earth’s climate. The uncertainty is due to several poorly understood processes and measurements including, but not limited to: (1) the microphysics of how particles nucleate ice, (2) the number of ice forming particles as a function of atmospheric properties such as temperature and relative humidity, (3) the atmospheric distribution of ice forming particles and (4) the role of anthropogenic activities in producing or changing the behavior of ice forming particles. The ways in which ice forming particles can impactmore » climate is also multi-faceted. More ice forming particles can lead to clouds with more ice crystals and different optical properties than clouds with less ice forming particles. More effective ice forming particles can lead to ice at higher temperature and/or lower saturation, resulting in clouds at lower altitude or latitude which also changes the Earth’s radiative balance. Ice nucleation also initiates most of the Earth’s precipitation, even in the mid- and low-latitudes, since cloud-top temperatures are often below freezing. The limited measurements and lack of understanding directly translates to restrictions in our ability to model atmospheric ice formation and project changes into the future. The importance of ice nucleation research is further exemplified by Figure 1 which shows the publications per decade and citations per year on the topic of ice nucleation [DeMott et al., 2011]. After a lull at the end of the last century, there has been a dramatic increase in both publications and citations related to ice nucleation; this directly corresponds to the importance of ice nucleation on the Earth’s climate and the uncertainty in this area noted by the Solomon [2007].« 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

Biogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud water

NASA Astrophysics Data System (ADS)

Cook, Ryan D.; Lin, Ying-Hsuan; Peng, Zhuoyu; Boone, Eric; Chu, Rosalie K.; Dukett, James E.; Gunsch, Matthew J.; Zhang, Wuliang; Tolic, Nikola; Laskin, Alexander; Pratt, Kerri A.

2017-12-01

Organic aerosol formation and transformation occurs within aqueous aerosol and cloud droplets, yet little is known about the composition of high molecular weight organic compounds in cloud water. Cloud water samples collected at Whiteface Mountain, New York, during August-September 2014 were analyzed by ultra-high-resolution mass spectrometry to investigate the molecular composition of dissolved organic carbon, with a focus on sulfur- and nitrogen-containing compounds. Organic molecular composition was evaluated in the context of cloud water inorganic ion concentrations, pH, and total organic carbon concentrations to gain insights into the sources and aqueous-phase processes of the observed high molecular weight organic compounds. Cloud water acidity was positively correlated with the average oxygen : carbon ratio of the organic constituents, suggesting the possibility for aqueous acid-catalyzed (prior to cloud droplet activation or during/after cloud droplet evaporation) and/or radical (within cloud droplets) oxidation processes. Many tracer compounds recently identified in laboratory studies of bulk aqueous-phase reactions were identified in the cloud water. Organosulfate compounds, with both biogenic and anthropogenic volatile organic compound precursors, were detected for cloud water samples influenced by air masses that had traveled over forested and populated areas. Oxidation products of long-chain (C10-12) alkane precursors were detected during urban influence. Influence of Canadian wildfires resulted in increased numbers of identified sulfur-containing compounds and oligomeric species, including those formed through aqueous-phase reactions involving methylglyoxal. Light-absorbing aqueous-phase products of syringol and guaiacol oxidation were observed in the wildfire-influenced samples, and dinitroaromatic compounds were observed in all cloud water samples (wildfire, biogenic, and urban-influenced). Overall, the cloud water molecular composition depended on air mass source influence and reflected aqueous-phase reactions involving biogenic, urban, and biomass burning precursors.

Bimodal SLD Ice Accretion on a NACA 0012 Airfoil Model

NASA Technical Reports Server (NTRS)

Potapczuk, Mark; Tsao, Jen-Ching; King-Steen, Laura

2016-01-01

This presentation describes the results of ice accretion measurements on a NACA 0012 airfoil model, from the NASA Icing Research Tunnel, using an icing cloud composed of a bimodal distribution of Supercooled Large Droplets. The data consists of photographs, laser scans of the ice surface, and measurements of the mass of ice for each icing condition. The results of ice shapes accumulated as a result of exposure to an icing cloud with a bimodal droplet distribution were compared to the ice shapes resulting from an equivalent cloud composed of a droplet distribution with a standard bell curve shape.

Multi-year ground-based observations of aerosol-cloud interactions in the Mid-Atlantic of the United States

NASA Astrophysics Data System (ADS)

Li, Siwei; Joseph, Everette; Min, Qilong; Yin, Bangsheng

2017-02-01

The U.S. Mid-Atlantic region experiences a wide variability of aerosol loading and frequent episodes of elevated anthropogenic aerosol loading associated with urban pollution conditions during summer months. In this study, multi-year ground-based observations (2006 to 2010) of aerosol and cloud properties from passive, active and in situ measurements at an atmospheric measurement field station in the Baltimore-Washington corridor operated by Howard University were analyzed to examine aerosol indirect effect on single-layer warm clouds including cloud optical depth (COD), liquid water path (LWP), cloud droplet effective radius (Re) and cloud droplet number concentration (Nd) in this region. A greater occurrence of polluted episodes and cloud cases with smaller Re (<7 μm) were found during the polluted year summers (2006, 2007 and 2008) than the clean year summers (2009 and 2010). The measurements of aerosol particulate matter with aerodynamic diameter≤2.5 μm (PM2.5) were used to represent the aerosol loading under cloudy conditions. Significant negative relationships between cloud droplet Re and PM2.5 were observed. Cloud cases were separated into clean and polluted groups based on the value of PM2.5. The cloud droplet Re was found proportional to LWP under clean conditions but weakly dependent on LWP under polluted conditions. The Nd was proportional to LWP under polluted condition but weakly dependent on LWP under clean conditions. Moreover, the effects of increasing fine aerosol particles on modifying cloud microphysical properties were found more significant under large LWP than small LWP in this region.

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.