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.

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

NASA Astrophysics Data System (ADS)

DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.; Sullivan, R. C.; Petters, M. D.; Tobo, Y.; Niemand, M.; Möhler, O.; Snider, J. R.; Wang, Z.; Kreidenweis, S. M.

2015-01-01

Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RHw) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RHw of 105% vs. maximum fractions active at higher RHw. Instrumental factors that affect activation behavior vs. RHw in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

DOE PAGES

DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.; ...

2015-01-13

Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RH w) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. Themore » parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RH w of 105% vs. maximum fractions active at higher RH w. Instrumental factors that affect activation behavior vs. RH w in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.« less

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.

What have we learned from HaChi (HAZE IN CHINA) project?

NASA Astrophysics Data System (ADS)

Zhao, Chunsheng; Wiedensohler, Alfred

2016-04-01

HaChi (Haze in China) project, a joint research between Chinese NSFC and German DFG, focuses on investigating the aerosol hygroscopic properties in the North China Plain and their relationships to aerosol optics, radiation, cloud physics and ozone photochemistry. As we know, Eastern China has suffered from severe pollution caused by large concentrations of aerosol particles resulting from emissions from fossil fuel and biomass burning, transportation and some other combustion sources. Low visibility events are frequently encountered and mainly accompanied with haze as a result of either high aerosol loading or the strong hygroscopic growth of the aerosol particles. Especially at relative humidities between 90 and 99%, the aerosol particles grow exponentially. The hygroscopic behaviors at relative humidities close to 100% are also strongly linked to the particles ability to grow into cloud droplets at supersaturation. In my talk, I will present an overview of the up to date results from a serial of intensive and comprehensive field campaigns conducted at the sites of Wuqing and Xianghe, China, between 2009 and 2014. The measurements of the ambient aerosol hygroscopic properties at high RH between 90 and 98.5% are reported first. These in situ field measurements of atmospheric aerosol are unique with respect to their high RH range and especially of importance to better understand the widespread anthropogenic haze over the North China Plain. Then I will introduce the methods for calculating of aerosol hygroscopicity and their parameterization schemes derived from size-segregated chemical composition and the light scattering enhancement factor measurements in the North China Plain. A new method was proposed to retrieve the ratio of the externally mixed light absorbing carbon mass to the total mass of light absorbing carbon. A new parameterization scheme of light extinction for low visibilities on hazy days is proposed based on visibility, relative humidity, aerosol hygroscopic growth factors and particle number size distributions measured. Cloud Condensation Nuclei (CCN) closure study is conducted with bulk CCN number concentration and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties. An evaluation of various methods for CCN parameterization is presented based on in situ measurements of aerosol activation properties within HaChi project. Hygroscopic growth of aerosol particles can significantly affect their single-scattering albedo, and consequently alters the aerosol effect on tropospheric photochemistry. At last, I will introduce the results on the relationship between aerosol hygroscopic properties and aerosol radiation including impacts of aerosol hygroscopic growth on the NO2 photolysis rate coefficient and the estimation of direct aerosol radiative effect in the North China Plan.

Introducing Convective Cloud Microphysics to a Deep Convection Parameterization Facilitating Aerosol Indirect Effects

NASA Astrophysics Data System (ADS)

Alapaty, K.; Zhang, G. J.; Song, X.; Kain, J. S.; Herwehe, J. A.

2012-12-01

Short lived pollutants such as aerosols play an important role in modulating not only the radiative balance but also cloud microphysical properties and precipitation rates. In the past, to understand the interactions of aerosols with clouds, several cloud-resolving modeling studies were conducted. These studies indicated that in the presence of anthropogenic aerosols, single-phase deep convection precipitation is reduced or suppressed. On the other hand, anthropogenic aerosol pollution led to enhanced precipitation for mixed-phase deep convective clouds. To date, there have not been many efforts to incorporate such aerosol indirect effects (AIE) in mesoscale models or global models that use parameterization schemes for deep convection. Thus, the objective of this work is to implement a diagnostic cloud microphysical scheme directly into a deep convection parameterization facilitating aerosol indirect effects in the WRF-CMAQ integrated modeling systems. Major research issues addressed in this study are: What is the sensitivity of a deep convection scheme to cloud microphysical processes represented by a bulk double-moment scheme? How close are the simulated cloud water paths as compared to observations? Does increased aerosol pollution lead to increased precipitation for mixed-phase clouds? These research questions are addressed by performing several WRF simulations using the Kain-Fritsch convection parameterization and a diagnostic cloud microphysical scheme. In the first set of simulations (control simulations) the WRF model is used to simulate two scenarios of deep convection over the continental U.S. during two summer periods at 36 km grid resolution. In the second set, these simulations are repeated after incorporating a diagnostic cloud microphysical scheme to study the impacts of inclusion of cloud microphysical processes. Finally, in the third set, aerosol concentrations simulated by the CMAQ modeling system are supplied to the embedded cloud microphysical scheme to study impacts of aerosol concentrations on precipitation and radiation fields. Observations available from the ARM microbase data, the SURFRAD network, GOES imagery, and other reanalysis and measurements will be used to analyze the impacts of a cloud microphysical scheme and aerosol concentrations on parameterized convection.

Improving Calculation Accuracies of Accumulation-Mode Fractions Based on Spectral of Aerosol Optical Depths

NASA Astrophysics Data System (ADS)

Ying, Zhang; Zhengqiang, Li; Yan, Wang

2014-03-01

Anthropogenic aerosols are released into the atmosphere, which cause scattering and absorption of incoming solar radiation, thus exerting a direct radiative forcing on the climate system. Anthropogenic Aerosol Optical Depth (AOD) calculations are important in the research of climate changes. Accumulation-Mode Fractions (AMFs) as an anthropogenic aerosol parameter, which are the fractions of AODs between the particulates with diameters smaller than 1μm and total particulates, could be calculated by AOD spectral deconvolution algorithm, and then the anthropogenic AODs are obtained using AMFs. In this study, we present a parameterization method coupled with an AOD spectral deconvolution algorithm to calculate AMFs in Beijing over 2011. All of data are derived from AErosol RObotic NETwork (AERONET) website. The parameterization method is used to improve the accuracies of AMFs compared with constant truncation radius method. We find a good correlation using parameterization method with the square relation coefficient of 0.96, and mean deviation of AMFs is 0.028. The parameterization method could also effectively solve AMF underestimate in winter. It is suggested that the variations of Angstrom indexes in coarse mode have significant impacts on AMF inversions.

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

NASA Astrophysics Data System (ADS)

Zhang, K.; O'Donnell, D.; Kazil, J.; Stier, P.; Kinne, S.; Lohmann, U.; Ferrachat, S.; Croft, B.; Quaas, J.; Wan, H.; Rast, S.; Feichter, J.

2012-03-01

This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Sensitivity experiments are carried out to analyse the effects of these improvements in the process representation on the simulated aerosol properties and global distribution. The new parameterizations that have largest impact on the global mean aerosol optical depth and radiative effects turn out to be the water uptake scheme and cloud microphysics. The former leads to a significant decrease of aerosol water contents in the lower troposphere, and consequently smaller optical depth; the latter results in higher aerosol loading and longer lifetime due to weaker in-cloud scavenging. The combined effects of the new/updated parameterizations are demonstrated by comparing the new model results with those from the earlier version, and against observations. Model simulations are evaluated in terms of aerosol number concentrations against measurements collected from twenty field campaigns as well as from fixed measurement sites, and in terms of optical properties against the AERONET measurements. Results indicate a general improvement with respect to the earlier version. The aerosol size distribution and spatial-temporal variance simulated by HAM2 are in better agreement with the observations. Biases in the earlier model version in aerosol optical depth and in the Ångström parameter have been reduced. The paper also points out the remaining model deficiencies that need to be addressed in the future.

Ice nucleation by soil dust compared to desert dust aerosols

NASA Astrophysics Data System (ADS)

Moehler, O.; Steinke, I.; Ullrich, R.; Höhler, K.; Schiebel, T.; Hoose, C.; Funk, R.

2015-12-01

A minor fraction of atmospheric aerosol particles, so-called ice-nucleating particles (INPs), initiates the formation of the ice phase in tropospheric clouds and thereby markedly influences the Earth's weather and climate systems. Whether an aerosol particle acts as an INP depends on its size, morphology and chemical compositions. The INP fraction of certain aerosol types also strongly depends on the temperature and the relative humidity. Because both desert dust and soil dust aerosols typically comprise a variety of different particles, it is difficult to assess and predict their contribution to the atmospheric INP abundance. This requires both accurate modelling of the sources and atmospheric distribution of atmospheric dust components and detailed investigations of their ice nucleation activities. The latter can be achieved in laboratory experiments and parameterized for use in weather and climate models as a function of temperature and particle surface area, a parameter called ice-nucleation active site (INAS) density. Concerning ice nucleation activity studies, the soil dust is of particular interest because it contains a significant fraction of organics and biological components, both with the potential for contributing to the atmospheric INP abundance at relatively high temperatures compared to mineral components. First laboratory ice nucleation experiments with a few soil dust samples indicated their INP fraction to be comparable or slightly enhanced to that of desert dust. We have used the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber to study the immersion freezing ability of four different arable soil dusts, sampled in Germany, China and Argentina. For temperatures higher than about -20°C, we found the INP fraction of aerosols generated from these samples by a dry dispersion technique to be significantly higher compared to various desert dust aerosols also investigated in AIDA experiments. In this contribution, we will summarize the experimental results, introduce related INP parameterizations for use in weather and climate models, and briefly discuss possible reasons for the discrepancy between the INP fraction of desert and soil dust aerosols.

A physically-based approach of treating dust-water cloud interactions in climate models

NASA Astrophysics Data System (ADS)

Kumar, P.; Karydis, V.; Barahona, D.; Sokolik, I. N.; Nenes, A.

2011-12-01

All aerosol-cloud-climate assessment studies to date assume that the ability of dust (and other insoluble species) to act as a Cloud Condensation Nuclei (CCN) is determined solely by their dry size and amount of soluble material. Recent evidence however clearly shows that dust can act as efficient CCN (even if lacking appreciable amounts of soluble material) through adsorption of water vapor onto the surface of the particle. This "inherent" CCN activity is augmented as the dust accumulates soluble material through atmospheric aging. A comprehensive treatment of dust-cloud interactions therefore requires including both of these sources of CCN activity in atmospheric models. This study presents a "unified" theory of CCN activity that considers both effects of adsorption and solute. The theory is corroborated and constrained with experiments of CCN activity of mineral aerosols generated from clays, calcite, quartz, dry lake beds and desert soil samples from Northern Africa, East Asia/China, and Northern America. The unified activation theory then is included within the mechanistic droplet activation parameterization of Kumar et al. (2009) (including the giant CCN correction of Barahona et al., 2010), for a comprehensive treatment of dust impacts on global CCN and cloud droplet number. The parameterization is demonstrated with the NASA Global Modeling Initiative (GMI) Chemical Transport Model using wind fields computed with the Goddard Institute for Space Studies (GISS) general circulation model. References Barahona, D. et al. (2010) Comprehensively Accounting for the Effect of Giant CCN in Cloud Activation Parameterizations, Atmos.Chem.Phys., 10, 2467-2473 Kumar, P., I.N. Sokolik, and A. Nenes (2009), Parameterization of cloud droplet formation for global and regional models: including adsorption activation from insoluble CCN, Atmos.Chem.Phys., 9, 2517- 2532

Impact of capturing rainfall scavenging intermittency using cloud superparameterization on simulated continental scale wildfire smoke transport

NASA Astrophysics Data System (ADS)

Pritchard, M. S.; Kooperman, G. J.; Zhao, Z.; Wang, M.; Russell, L. M.; Somerville, R. C.; Ghan, S. J.

2011-12-01

Evaluating the fidelity of new aerosol physics in climate models is confounded by uncertainties in source emissions, systematic error in cloud parameterizations, and inadequate sampling of long-range plume concentrations. To explore the degree to which cloud parameterizations distort aerosol processing and scavenging, the Pacific Northwest National Laboratory (PNNL) Aerosol-Enabled Multi-Scale Modeling Framework (AE-MMF), a superparameterized branch of the Community Atmosphere Model Version 5 (CAM5), is applied to represent the unusually active and well sampled North American wildfire season in 2004. In the AE-MMF approach, the evolution of double moment aerosols in the exterior global resolved scale is linked explicitly to convective statistics harvested from an interior cloud resolving scale. The model is configured in retroactive nudged mode to observationally constrain synoptic meteorology, and Arctic wildfire activity is prescribed at high space/time resolution using data from the Global Fire Emissions Database. Comparisons against standard CAM5 bracket the effect of superparameterization to isolate the role of capturing rainfall intermittency on the bulk characteristics of 2004 Arctic plume transport. Ground based lidar and in situ aircraft wildfire plume constraints from the International Consortium for Atmospheric Research on Transport and Transformation field campaign are used as a baseline for model evaluation.

Externally mixed aerosol : simulation of ice nucleation in a parcel model

NASA Astrophysics Data System (ADS)

Anquetil-Deck, Candy; Hoose, Corinna; Conolly, Paul

2014-05-01

The effect of different aerosol (mineral dust, bacteria and soot) acting as immersion ice nuclei is investigated using ACPIM (AerosolCloud Precipitation Interaction Model) [1]. ACPIM is a powerful tool which can be used in two different ways. This box model can be, either, driven by experimental data (experiments carried out at the AIDA cloud chamber facility) or used as an air parcel in order to examine different ice nucleation parameterizations under specific conditions. This adiabatic air parcel model was employed for the simulation of a convective cloud. The study consists here in the investigation of how two externally mixed aerosols interact with one another. The initial study concentrates on mineral dust aerosol and biological aerosol without any background in order to fully understand the interaction between the different types of aerosol. Immersion freezing is described for the mineral dust aerosol by Niemand et al. 's parameterization [2], which was derived from laboratory studies in AIDA and is an extension of surface site density approach suggested by Connolly et al. [1]. Regarding bioaerosol, we introduce Hummel et al. 's parameterization [3] : f(in) = f(max)(1 - exp(- Ap *n(s)(T))) With an empirically fitted ice nucleation active site density n s based on AIDA measurements of Pseudomonas syringae bacteria [4]. This initial study is conducted for different proportion of each aerosol (the total number of aerosol being constant throughout all the simulation runs) at different vertical velocities. We then extented this study with different backgrounds (urban, marine, rural) in order to get a full picture. We found that there is not only a CCN competition but an IN competition as well. References : [1] Connolly, P. J., Möhler O., Field P. R., Saathoff H., Burgess, R., Choularton, T. and Gallagher, M., Atmos. Chem. Phys 9, 2805-2824 (2009). [2] Niemand, M., Möhler, O., Vogel B., Vogel, H., Hoose, C., Connolly, P., Klein, H., Bingemer, H., DeMott,P., Skrotzki, J. and Leisner T., J. Atmos. Sci. 69, 3077-3092 (2012). [3] Hummel, M. et al., In preparation, (2014). [4] Oehm, C. et al., In preparation, (2014).

Assessing the CAM5 Physics Suite in the WRF-Chem Model: Implementation, Resolution Sensitivity, and a First Evaluation for a Regional Case Study

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

Ma, Po-Lun; Rasch, Philip J.; Fast, Jerome D.

A suite of physical parameterizations (deep and shallow convection, turbulent boundary layer, aerosols, cloud microphysics, and cloud fraction) from the global climate model Community Atmosphere Model version 5.1 (CAM5) has been implemented in the regional model Weather Research and Forecasting with chemistry (WRF-Chem). A downscaling modeling framework with consistent physics has also been established in which both global and regional simulations use the same emissions and surface fluxes. The WRF-Chem model with the CAM5 physics suite is run at multiple horizontal resolutions over a domain encompassing the northern Pacific Ocean, northeast Asia, and northwest North America for April 2008 whenmore » the ARCTAS, ARCPAC, and ISDAC field campaigns took place. These simulations are evaluated against field campaign measurements, satellite retrievals, and ground-based observations, and are compared with simulations that use a set of common WRF-Chem Parameterizations. This manuscript describes the implementation of the CAM5 physics suite in WRF-Chem provides an overview of the modeling framework and an initial evaluation of the simulated meteorology, clouds, and aerosols, and quantifies the resolution dependence of the cloud and aerosol parameterizations. We demonstrate that some of the CAM5 biases, such as high estimates of cloud susceptibility to aerosols and the underestimation of aerosol concentrations in the Arctic, can be reduced simply by increasing horizontal resolution. We also show that the CAM5 physics suite performs similarly to a set of parameterizations commonly used in WRF-Chem, but produces higher ice and liquid water condensate amounts and near-surface black carbon concentration. Further evaluations that use other mesoscale model parameterizations and perform other case studies are needed to infer whether one parameterization consistently produces results more consistent with observations.« less

Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

EPA Pesticide Factsheets

The uploaded data consists of the BRACE Na aerosol observations paired with CMAQ model output, the updated model's parameterization of sea salt aerosol emission size distribution, and the model's parameterization of the sea salt emission factor as a function of sea surface temperature. This dataset is associated with the following publication:Gantt , B., J. Kelly , and J. Bash. Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2. Geoscientific Model Development. Copernicus Publications, Katlenburg-Lindau, GERMANY, 8: 3733-3746, (2015).

COMPUTATIONAL CHEMISTRY METHOD FOR PREDICTING VAPOR PRESSURES AND ACTIVITY COEFFICIENTS OF POLAR ORGANIC OXYGENATES IN PM2.5

EPA Science Inventory

Parameterizations of interactions of polar multifunctional organic oxygenates in PM2.5 must be included in aerosol chemistry models for evaluating control strategies for reducing ambient concentrations of PM2.5 compounds. Vapor pressures and activity coefficients of these compo...

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

NASA Astrophysics Data System (ADS)

Yun, Yuxing; Penner, Joyce E.

2012-04-01

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

Simulating Aerosol Indirect Effects with Improved Aerosol-Cloud- Precipitation Representations in a Coupled Regional Climate Model

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

Zhang, Yang; Leung, L. Ruby; Fan, Jiwen

This is a collaborative project among North Carolina State University, Pacific Northwest National Laboratory, and Scripps Institution of Oceanography, University of California at San Diego to address the critical need for an accurate representation of aerosol indirect effect in climate and Earth system models. In this project, we propose to develop and improve parameterizations of aerosol-cloud-precipitation feedbacks in climate models and apply them to study the effect of aerosols and clouds on radiation and hydrologic cycle. Our overall objective is to develop, improve, and evaluate parameterizations to enable more accurate simulations of these feedbacks in high resolution regional and globalmore » climate models.« less

Raman lidar and sun photometer measurements of aerosols and water vapor during the ARM RCS experiment

NASA Technical Reports Server (NTRS)

Ferrare, R. A.; Whiteman, D. N.; Melfi, S. H.; Evans, K. D.; Holben, B. N.

1995-01-01

The first Atmospheric Radiation Measurement (ARM) Remote Cloud Study (RCS) Intensive Operations Period (IOP) was held during April 1994 at the Southern Great Plains (SGP) Cloud and Radiation Testbed (CART) site near Lamont, Oklahoma. This experiment was conducted to evaluate and calibrate state-of-the-art, ground based remote sensing instruments and to use the data acquired by these instruments to validate retrieval algorithms developed under the ARM program. These activities are part of an overall plan to assess general circulation model (GCM) parameterization research. Since radiation processes are one of the key areas included in this parameterization research, measurements of water vapor and aerosols are required because of the important roles these atmospheric constituents play in radiative transfer. Two instruments were deployed during this IOP to measure water vapor and aerosols and study their relationship. The NASA/Goddard Space Flight Center (GSFC) Scanning Raman Lidar (SRL) acquired water vapor and aerosol profile data during 15 nights of operations. The lidar acquired vertical profiles as well as nearly horizontal profiles directed near an instrumented 60 meter tower. Aerosol optical thickness, phase function, size distribution, and integrated water vapor were derived from measurements with a multiband automatic sun and sky scanning radiometer deployed at this site.

A Physically Based Framework for Modelling the Organic Fractionation of Sea Spray Aerosol from Bubble Film Langmuir Equilibria

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

Burrows, Susannah M.; Ogunro, O.; Frossard, Amanda

2014-12-19

The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely-sensed chlorophyll-a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll-a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel frameworkmore » for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semi-labile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecule. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll-\\textit{a} and organic fraction are similar to existing empirical parameterizations, but can vary between biologically productive and non-productive regions, and seasonally within a given region. Major uncertainties include the bubble film thickness at bursting and the variability of organic surfactant activity in the ocean, which is poorly constrained. In addition, marine colloids and cooperative adsorption of polysaccharides may make important contributions to the aerosol, but are not included here. This organic fractionation framework is an initial step towards a closer linking of ocean biogeochemistry and aerosol chemical composition in Earth system models. Future work should focus on improving constraints on model parameters through new laboratory experiments or through empirical fitting to observed relationships in the real ocean and atmosphere, as well as on atmospheric implications of the variable composition of organic matter in sea spray.« less

Modeling particle nucleation and growth over northern California during the 2010 CARES campaign

NASA Astrophysics Data System (ADS)

Lupascu, A.; Easter, R.; Zaveri, R.; Shrivastava, M.; Pekour, M.; Tomlinson, J.; Yang, Q.; Matsui, H.; Hodzic, A.; Zhang, Q.; Fast, J. D.

2015-11-01

Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4, while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapor parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates are predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary-layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10-40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. We found that newly formed particles could explain up to 20-30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ~ 36 %.

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

NASA Astrophysics Data System (ADS)

DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.; Sullivan, R. C.; Petters, M. D.; Tobo, Y.; Niemand, M.; Möhler, O.; Snider, J. R.; Wang, Z.; Kreidenweis, S. M.

2014-06-01

Data from both laboratory studies and atmospheric measurements are used to develop a simple parametric description for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RHw) are taken to approximate the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A correction factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RHw of 105% vs. maximum fractions active at higher RHw. Instrumental factors that affect activation behavior vs. RHw in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this correction factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization to the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically-relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first order approximation in numerical modeling investigations.

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

Importance of Physico-Chemical Properties of Aerosols in the Formation of Arctic Ice Clouds

NASA Astrophysics Data System (ADS)

Keita, S. A.; Girard, E.

2014-12-01

Ice clouds play an important role in the Arctic weather and climate system but interactions between aerosols, clouds and radiation are 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. TIC-1 are composed by non-precipitating very small (radar-unseen) ice crystals whereas TIC-2 are detected by both sensors and are characterized by a low concentration of large precipitating ice crystals. It is hypothesized that TIC-2 formation is linked to the acidification of aerosols, which inhibit the ice nucleating properties of ice nuclei (IN). As a result, the IN concentration is reduced in these regions, resulting to a smaller concentration of larger ice crystals. Over the past 10 years, several parameterizations of homogeneous and heterogeneous ice nucleation have been developed to reflect the various physical and chemical properties of aerosols. These parameterizations are derived from laboratory studies on aerosols of different chemical compositions. The parameterizations are also developed according to two main approaches: stochastic (that nucleation is a probabilistic process, which is time dependent) and singular (that nucleation occurs at fixed conditions of temperature and humidity and time-independent). This research aims to better understand the formation process of TICs using a newly-developed ice nucleation parameterizations. For this purpose, we implement some parameterizations (2 approaches) 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 Arctic Cloud (ISDAC) in Alaska. We use both approaches but special attention is focused on the new parameterizations of the singular approach. Simulation results of the TICs-2 observed on April 15th and 25th (polluted or acidic cases) and TICs-1 observed on April 5th (non-polluted cases) will be presented.

Radiative flux and forcing parameterization error in aerosol-free clear skies

DOE PAGES

Pincus, Robert; Mlawer, Eli J.; Oreopoulos, Lazaros; ...

2015-07-03

This article reports on the accuracy in aerosol- and cloud-free conditions of the radiation parameterizations used in climate models. Accuracy is assessed relative to observationally validated reference models for fluxes under present-day conditions and forcing (flux changes) from quadrupled concentrations of carbon dioxide. Agreement among reference models is typically within 1 W/m 2, while parameterized calculations are roughly half as accurate in the longwave and even less accurate, and more variable, in the shortwave. Absorption of shortwave radiation is underestimated by most parameterizations in the present day and has relatively large errors in forcing. Error in present-day conditions is essentiallymore » unrelated to error in forcing calculations. Recent revisions to parameterizations have reduced error in most cases. As a result, a dependence on atmospheric conditions, including integrated water vapor, means that global estimates of parameterization error relevant for the radiative forcing of climate change will require much more ambitious calculations.« less

Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions

PubMed Central

Che, H. C.; Zhang, X. Y.; Wang, Y. Q.; Zhang, L.; Shen, X. J.; Zhang, Y. M.; Ma, Q. L.; Sun, J. Y.; Zhang, Y. W.; Wang, T. T.

2016-01-01

To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate. PMID:27075947

Modeling particle nucleation and growth over northern California during the 2010 CARES campaign

NASA Astrophysics Data System (ADS)

Lupascu, A.; Easter, R.; Zaveri, R.; Shrivastava, M.; Pekour, M.; Tomlinson, J.; Yang, Q.; Matsui, H.; Hodzic, A.; Zhang, Q.; Fast, J. D.

2015-07-01

Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4 while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapors parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates were predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10-40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. Differences among the three simulations for the 40-100 nm particle diameter range are mostly associated with the timing of the peak total tendencies that shift the morning increase and afternoon decrease in particle number concentration by up to two hours. We found that newly formed particles could explain up to 20-30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ∼ 36 %.

Sensitivity studies of different aerosol indirect effects in mixed-phase clouds

NASA Astrophysics Data System (ADS)

Lohmann, U.; Hoose, C.

2009-11-01

Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO4-crit), which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m-2. This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.

Sensitivity studies of different aerosol indirect effects in mixed-phase clouds

NASA Astrophysics Data System (ADS)

Lohmann, U.; Hoose, C.

2009-07-01

Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO4-crit), which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m-2. This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.

Modeling of the Wegener Bergeron Findeisen process—implications for aerosol indirect effects

NASA Astrophysics Data System (ADS)

Storelvmo, T.; Kristjánsson, J. E.; Lohmann, U.; Iversen, T.; Kirkevåg, A.; Seland, Ø.

2008-10-01

A new parameterization of the Wegener-Bergeron-Findeisen (WBF) process has been developed, and implemented in the general circulation model CAM-Oslo. The new parameterization scheme has important implications for the process of phase transition in mixed-phase clouds. The new treatment of the WBF process replaces a previous formulation, in which the onset of the WBF effect depended on a threshold value of the mixing ratio of cloud ice. As no observational guidance for such a threshold value exists, the previous treatment added uncertainty to estimates of aerosol effects on mixed-phase clouds. The new scheme takes subgrid variability into account when simulating the WBF process, allowing for smoother phase transitions in mixed-phase clouds compared to the previous approach. The new parameterization yields a model state which gives reasonable agreement with observed quantities, allowing for calculations of aerosol effects on mixed-phase clouds involving a reduced number of tunable parameters. Furthermore, we find a significant sensitivity to perturbations in ice nuclei concentrations with the new parameterization, which leads to a reversal of the traditional cloud lifetime effect.

Current state of aerosol nucleation parameterizations for air-quality and climate modeling

NASA Astrophysics Data System (ADS)

Semeniuk, Kirill; Dastoor, Ashu

2018-04-01

Aerosol nucleation parameterization models commonly used in 3-D air quality and climate models have serious limitations. This includes classical nucleation theory based variants, empirical models and other formulations. Recent work based on detailed and extensive laboratory measurements and improved quantum chemistry computation has substantially advanced the state of nucleation parameterizations. In terms of inorganic nucleation involving BHN and THN including ion effects these new models should be considered as worthwhile replacements for the old models. However, the contribution of organic species to nucleation remains poorly quantified. New particle formation consists of a distinct post-nucleation growth regime which is characterized by a strong Kelvin curvature effect and is thus dependent on availability of very low volatility organic species or sulfuric acid. There have been advances in the understanding of the multiphase chemistry of biogenic and anthropogenic organic compounds which facilitate to overcome the initial aerosol growth barrier. Implementation of processes influencing new particle formation is challenging in 3-D models and there is a lack of comprehensive parameterizations. This review considers the existing models and recent innovations.

Improved parameterization for the vertical flux of dust aerosols emitted by an eroding soil

USDA-ARS?s Scientific Manuscript database

The representation of the dust cycle in atmospheric circulation models hinges on an accurate parameterization of the vertical dust flux at emission. However, existing parameterizations of the vertical dust flux vary substantially in their scaling with wind friction velocity, require input parameters...

From Global to Cloud Resolving Scale: Experiments with a Scale- and Aerosol-Aware Physics Package and Impact on Tracer Transport

NASA Astrophysics Data System (ADS)

Grell, G. A.; Freitas, S. R.; Olson, J.; Bela, M.

2017-12-01

We will start by providing a summary of the latest cumulus parameterization modeling efforts at NOAA's Earth System Research Laboratory (ESRL) will be presented on both regional and global scales. The physics package includes a scale-aware parameterization of subgrid cloudiness feedback to radiation (coupled PBL, microphysics, radiation, shallow and congestus type convection), the stochastic Grell-Freitas (GF) scale- and aerosol-aware convective parameterization, and an aerosol aware microphysics package. GF is based on a stochastic approach originally implemented by Grell and Devenyi (2002) and described in more detail in Grell and Freitas (2014, ACP). It was expanded to include PDF's for vertical mass flux, as well as modifications to improve the diurnal cycle. This physics package will be used on different scales, spanning global to cloud resolving, to look at the impact on scalar transport and numerical weather prediction.

The Impact of Aerosol Sources and Aging on CCN Formation in the Houston-Galveston-Gulf of Mexico Region

NASA Astrophysics Data System (ADS)

Quinn, P.; Bates, T.; Coffman, D.; Covert, D.

2007-12-01

The impact of anthropogenic aerosol on cloud properties, cloud lifetime, and precipitation processes is one of the largest uncertainties in our current understanding of climate change. Aerosols affect cloud properties by serving as cloud condensation nuclei (CCN) thereby leading to the formation of cloud droplets. The process of cloud drop activation is a function of both the size and chemistry of the aerosol particles which, in turn, depend on the source of the aerosol and transformations that occur downwind. In situ field measurements that can lead to an improved understanding of the process of cloud drop formation and simplifying parameterizations for improving the accuracy of climate models are highly desirable. During the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), the NOAA RV Ronald H. Brown encountered a wide variety of aerosol types ranging from marine near the Florida panhandle to urban and industrial in the Houston-Galveston area. These varied sources provided an opportunity to investigate the role of aerosol sources, aging, chemistry, and size in the activation of particles to form cloud droplets. Here, we use the correlation between variability in critical diameter for activation (determined empirically from measured CCN concentrations and the number size distribution) and aerosol composition to quantify the impact of composition on particle activation. Variability in aerosol composition is parameterized by the mass fraction of Hydrocarbon-like Organic Aerosol (HOA) for particle diameters less than 200 nm (vacuum aerodynamic). The HOA mass fraction in this size range is lowest for marine aerosol and higher for aerosol impacted by anthropogenic emissions. Combining all data collected at 0.44 percent supersaturation (SS) reveals that composition (defined in this way) explains 40 percent of the variance in the critical diameter. As expected, the dependence of activation on composition is strongest at lower SS. At the same time, correlations between HOA mass fraction and aerosol mean diameter show that these two parameters are essentially independent of one another for this data set. We conclude that, based on the variability of the HOA mass fraction observed during GoMACCS, composition plays a dominant role in determining the fraction of particles that are activated to form cloud droplets. Using Kohler theory, we estimate the error that results in calculated CCN concentrations if the organic fraction of the aerosol is neglected (i.e., a fully soluble composition of ammonium sulfate is assumed) for the range of organic mass fractions and mean diameters observed during GoMACCS. We then relate this error to the source and age of the aerosol. At 0.22 and 0.44 percent SS, the error is considerable for anthropogenic aerosol sampled near the source region as this aerosol has, on average, a high POM mass fraction and smaller particle mean diameter. The error is lower for more aged aerosol as it has a lower POM mass fraction and larger mean particle diameter. Hence, the percent error in calculated CCN concentration is expected to be larger for younger, organic- rich aerosol and smaller for aged, sulfate rich aerosol and for marine aerosol. We extend this analysis to continental and marine data sets recently reported by Dusek et al. [Science, 312, 1375, 2006] and Hudson [Geophys. Res., Lett., 34, L08801, 2007].

Role of clouds, aerosols, and aerosol-cloud interaction in 20th century simulations with GISS ModelE2

NASA Astrophysics Data System (ADS)

Nazarenko, L.; Rind, D. H.; Bauer, S.; Del Genio, A. D.

2015-12-01

Simulations of aerosols, clouds and their interaction contribute to the major source of uncertainty in predicting the changing Earth's energy and in estimating future climate. Anthropogenic contribution of aerosols affects the properties of clouds through aerosol indirect effects. Three different versions of NASA GISS global climate model are presented for simulation of the twentieth century climate change. All versions have fully interactive tracers of aerosols and chemistry in both the troposphere and stratosphere. All chemical species are simulated prognostically consistent with atmospheric physics in the model and the emissions of short-lived precursors [Shindell et al., 2006]. One version does not include the aerosol indirect effect on clouds. The other two versions include a parameterization of the interactive first indirect aerosol effect on clouds following Menon et al. [2010]. One of these two models has the Multiconfiguration Aerosol Tracker of Mixing state (MATRIX) that permits detailed treatment of aerosol mixing state, size, and aerosol-cloud activation. The main purpose of this study is evaluation of aerosol-clouds interactions and feedbacks, as well as cloud and aerosol radiative forcings, for the twentieth century climate under different assumptions and parameterizations for aerosol, clouds and their interactions in the climate models. The change of global surface air temperature based on linear trend ranges from +0.8°C to +1.2°C between 1850 and 2012. Water cloud optical thickness increases with increasing temperature in all versions with the largest increase in models with interactive indirect effect of aerosols on clouds, which leads to the total (shortwave and longwave) cloud radiative cooling trend at the top of the atmosphere. Menon, S., D. Koch, G. Beig, S. Sahu, J. Fasullo, and D. Orlikowski (2010), Black carbon aerosols and the third polar ice cap, Atmos. Chem. Phys., 10,4559-4571, doi:10.5194/acp-10-4559-2010. Shindell, D., G. Faluvegi, N. Unger, E. Aguilar, G.A. Schmidt, D.M. Koch, S.E. Bauer, and J.R. Miller (2006), Simulations of preindustrial, present-day, and 2100 conditions in the NASA GISS composition and climate model G-PUCCINI, Atmos. Chem. Phys., 6, 4427-4459.

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.

Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

NASA Astrophysics Data System (ADS)

Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

2012-04-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. Decreases in NOx emissions without simultaneous decreases in SO2 emissions increase new-particle formation and growth due to increased oxidation of SO2. The parameterization we describe here should allow for more accurate predictions of aerosol size distributions and a greater confidence in the effects of aerosols in climate and health studies.

Cloud microphysics modification with an online coupled COSMO-MUSCAT regional model

NASA Astrophysics Data System (ADS)

Sudhakar, D.; Quaas, J.; Wolke, R.; Stoll, J.; Muehlbauer, A. D.; Tegen, I.

2015-12-01

Abstract: The quantification of clouds, aerosols, and aerosol-cloud interactions in models, continues to be a challenge (IPCC, 2013). In this scenario two-moment bulk microphysical scheme is used to understand the aerosol-cloud interactions in the regional model COSMO (Consortium for Small Scale Modeling). The two-moment scheme in COSMO has been especially designed to represent aerosol effects on the microphysics of mixed-phase clouds (Seifert et al., 2006). To improve the model predictability, the radiation scheme has been coupled with two-moment microphysical scheme. Further, the cloud microphysics parameterization has been modified via coupling COSMO with MUSCAT (MultiScale Chemistry Aerosol Transport model, Wolke et al., 2004). In this study, we will be discussing the initial result from the online-coupled COSMO-MUSCAT model system with modified two-moment parameterization scheme along with COSP (CFMIP Observational Simulator Package) satellite simulator. This online coupled model system aims to improve the sub-grid scale process in the regional weather prediction scenario. The constant aerosol concentration used in the Seifert and Beheng, (2006) parameterizations in COSMO model has been replaced by aerosol concentration derived from MUSCAT model. The cloud microphysical process from the modified two-moment scheme is compared with stand-alone COSMO model. To validate the robustness of the model simulation, the coupled model system is integrated with COSP satellite simulator (Muhlbauer et al., 2012). Further, the simulations are compared with MODIS (Moderate Resolution Imaging Spectroradiometer) and ISCCP (International Satellite Cloud Climatology Project) satellite products.

A parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: improvement of particulate nitrate prediction

NASA Astrophysics Data System (ADS)

Chen, Ying; Wolke, Ralf; Ran, Liang; Birmili, Wolfram; Spindler, Gerald; Schröder, Wolfram; Su, Hang; Cheng, Yafang; Tegen, Ina; Wiedensohler, Alfred

2018-01-01

The heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R = 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO-MUSCAT, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10-25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5-19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ˜ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17-18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3-] of less than 2 % on average and 20 % at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.

The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization

NASA Astrophysics Data System (ADS)

Sakamoto, Kimiko M.; Laing, James R.; Stevens, Robin G.; Jaffe, Daniel A.; Pierce, Jeffrey R.

2016-06-01

Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA) evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, accurately accounting for biomass-burning aerosol size in global models requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emission-inventory and meteorological parameters. In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA) to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations and yields R2 values of 0.83 and 0.89 for Dpm and modal width, respectively. The size distribution is particularly sensitive to the mass emissions flux, fire area, wind speed, and time, and we provide simplified fits of the aged size distribution to just these input variables. The simplified fits were tested against 11 aged biomass-burning size distributions observed at the Mt. Bachelor Observatory in August 2015. The simple fits captured over half of the variability in observed Dpm and modal width even though the freshly emitted Dpm and modal widths were unknown. These fits may be used in global and regional aerosol models. Finally, we show that coagulation generally leads to greater changes in the particle size distribution than OA evaporation/formation does, using estimates of OA production/loss from the literature.

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.

Temporal and spatial characteristics of dust devils and their contribution to the aerosol budget in East Asia-An analysis using a new parameterization scheme for dust devils

NASA Astrophysics Data System (ADS)

Tang, Yaoguo; Han, Yongxiang; Liu, Zhaohuan

2018-06-01

Dust aerosols are the main aerosol components of the atmosphere that affect climate change, but the contribution of dust devils to the atmospheric dust aerosol budget is uncertain. In this study, a new parameterization scheme for dust devils was established and coupled with WRF-Chem, and the diurnal and monthly variations and the contribution of dust devils to the atmospheric dust aerosol budget in East Asia was simulated. The results show that 1) both the diurnal and monthly variations in dust devil emissions in East Asia had unimodal distributions, with peaks in the afternoon and the summer that were similar to the observations; 2) the simulated dust devils occurred frequently in deserts, including the Gobi. The distributed area and the intensity center of the dust devil moved from east to west during the day; 3) the ratio between the availability of convective buoyancy relative to the frictional dissipation was the main factor that limited the presence of dust devils. The position of the dust devil formation, the surface temperature, and the boundary layer height determined the dust devil intensity; 4) the contribution of dust devils to atmospheric dust aerosols determined in East Asia was 30.4 ± 13%, thereby suggesting that dust devils contribute significantly to the total amount of atmospheric dust aerosols. Although the new parameterization scheme for dust devils was rough, it was helpful for understanding the distribution of dust devils and their contribution to the dust aerosol budget.

FY 2010 Fourth Quarter Report: Evaluation of the Dependency of Drizzle Formation on Aerosol Properties

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

Lin, W; McGraw, R; Liu, Y

Metric for Quarter 4: Report results of implementation of composite parameterization in single-column model (SCM) to explore the dependency of drizzle formation on aerosol properties. To better represent VOCALS conditions during a test flight, the Liu-Duam-McGraw (LDM) drizzle parameterization is implemented in the high-resolution Weather Research and Forecasting (WRF) model, as well as in the single-column Community Atmosphere Model (CAM), to explore this dependency.

Fine-scale application of WRF-CAM5 during a dust storm episode over East Asia: Sensitivity to grid resolutions and aerosol activation parameterizations

NASA Astrophysics Data System (ADS)

Wang, Kai; Zhang, Yang; Zhang, Xin; Fan, Jiwen; Leung, L. Ruby; Zheng, Bo; Zhang, Qiang; He, Kebin

2018-03-01

An advanced online-coupled meteorology and chemistry model WRF-CAM5 has been applied to East Asia using triple-nested domains at different grid resolutions (i.e., 36-, 12-, and 4-km) to simulate a severe dust storm period in spring 2010. Analyses are performed to evaluate the model performance and investigate model sensitivity to different horizontal grid sizes and aerosol activation parameterizations and to examine aerosol-cloud interactions and their impacts on the air quality. A comprehensive model evaluation of the baseline simulations using the default Abdul-Razzak and Ghan (AG) aerosol activation scheme shows that the model can well predict major meteorological variables such as 2-m temperature (T2), water vapor mixing ratio (Q2), 10-m wind speed (WS10) and wind direction (WD10), and shortwave and longwave radiation across different resolutions with domain-average normalized mean biases typically within ±15%. The baseline simulations also show moderate biases for precipitation and moderate-to-large underpredictions for other major variables associated with aerosol-cloud interactions such as cloud droplet number concentration (CDNC), cloud optical thickness (COT), and cloud liquid water path (LWP) due to uncertainties or limitations in the aerosol-cloud treatments. The model performance is sensitive to grid resolutions, especially for surface meteorological variables such as T2, Q2, WS10, and WD10, with the performance generally improving at finer grid resolutions for those variables. Comparison of the sensitivity simulations with an alternative (i.e., the Fountoukis and Nenes (FN) series scheme) and the default (i.e., AG scheme) aerosol activation scheme shows that the former predicts larger values for cloud variables such as CDNC and COT across all grid resolutions and improves the overall domain-average model performance for many cloud/radiation variables and precipitation. Sensitivity simulations using the FN series scheme also have large impacts on radiations, T2, precipitation, and air quality (e.g., decreasing O3) through complex aerosol-radiation-cloud-chemistry feedbacks. The inclusion of adsorptive activation of dust particles in the FN series scheme has similar impacts on the meteorology and air quality but to lesser extent as compared to differences between the FN series and AG schemes. Compared to the overall differences between the FN series and AG schemes, impacts of adsorptive activation of dust particles can contribute significantly to the increase of total CDNC (∼45%) during dust storm events and indicate their importance in modulating regional climate over East Asia.

Combining laboratory results, numerical modeling, and in situ measurements to investigate the relative contributions of homogeneous and heterogeneous nucleation to ice formation in the tropical tropopause layer

NASA Astrophysics Data System (ADS)

Jensen, E. J.; Karcher, B.; Ueyama, R.; Pfister, L.; Bui, T. V.; Diskin, G. S.; DiGangi, J. P.; Woods, S.; Lawson, P.; Froyd, K. D.; Murphy, D. M.

2017-12-01

Laboratory experiments over the past decade have advanced our understanding of the physical state and ice nucleation efficacy of aerosols with atmospherically-relevant compositions at low temperatures. We use these laboratory results along with measurements of upper-tropospheric aerosol composition to develop a parameterization if the ice nuclei number, and activity dependence on ice supersaturation and temperature in the cold tropical tropopause layer (TTL, 13-18 km). We show that leading candidates for aerosol types serving as effective ice nuclei are glassy organic-containing aerosols, crystalline ammonium sulfate, and mineral dust. We apply the low-temperature heterogeneous ice nucleation parameterization in a detailed model of TTL transport and cirrus formation. The model treats heterogeneous ice nucleation and homogeneous freezing of aqueous aerosols, deposition growth and sublimation of ice crystals, and sedimentation of ice crystals. The model is driven by meteorological fields with high-frequency waves superimposed, and simulated cirrus microphysical properties are statistically compared with recent measurements of TTL cirrus microphysical properties and ice supersaturation from recent high-altitude aircraft campaigns. We show that effective ice nuclei concentrations on the order of 50-100/L can dominate over homogeneous freezing production of TTL cirrus ice crystals. Glassy organic-containing aerosols or crystalline ammonium sulfate could conceivably provide more abundant sources of ice nuclei, but the simulations indicate that high concentrations of effective IN would prevent observed occurrence of large supersaturations and high ice concentrations. We will also show the impact of heterogeneous ice nuclei on TTL cirrus microphysical properties and occurrence frequencies.

Impact of aerosol size representation on modeling aerosol-cloud interactions

DOE PAGES

Zhang, Y.; Easter, R. C.; Ghan, S. J.; ...

2002-11-07

In this study, we use a 1-D version of a climate-aerosol-chemistry model with both modal and sectional aerosol size representations to evaluate the impact of aerosol size representation on modeling aerosol-cloud interactions in shallow stratiform clouds observed during the 2nd Aerosol Characterization Experiment. Both the modal (with prognostic aerosol number and mass or prognostic aerosol number, surface area and mass, referred to as the Modal-NM and Modal-NSM) and the sectional approaches (with 12 and 36 sections) predict total number and mass for interstitial and activated particles that are generally within several percent of references from a high resolution 108-section approach.more » The modal approach with prognostic aerosol mass but diagnostic number (referred to as the Modal-M) cannot accurately predict the total particle number and surface areas, with deviations from the references ranging from 7-161%. The particle size distributions are sensitive to size representations, with normalized absolute differences of up to 12% and 37% for the 36- and 12-section approaches, and 30%, 39%, and 179% for the Modal-NSM, Modal-NM, and Modal-M, respectively. For the Modal-NSM and Modal-NM, differences from the references are primarily due to the inherent assumptions and limitations of the modal approach. In particular, they cannot resolve the abrupt size transition between the interstitial and activated aerosol fractions. For the 12- and 36-section approaches, differences are largely due to limitations of the parameterized activation for non-log-normal size distributions, plus the coarse resolution for the 12-section case. Differences are larger both with higher aerosol (i.e., less complete activation) and higher SO2 concentrations (i.e., greater modification of the initial aerosol distribution).« less

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

NASA Astrophysics Data System (ADS)

Liu, X.; Shi, X.

2018-02-01

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

A simple parameterization of aerosol emissions in RAMS

NASA Astrophysics Data System (ADS)

Letcher, Theodore

Throughout the past decade, a high degree of attention has been focused on determining the microphysical impact of anthropogenically enhanced concentrations of Cloud Condensation Nuclei (CCN) on orographic snowfall in the mountains of the western United States. This area has garnered a lot of attention due to the implications this effect may have on local water resource distribution within the Region. Recent advances in computing power and the development of highly advanced microphysical schemes within numerical models have provided an estimation of the sensitivity that orographic snowfall has to changes in atmospheric CCN concentrations. However, what is still lacking is a coupling between these advanced microphysical schemes and a real-world representation of CCN sources. Previously, an attempt to representation the heterogeneous evolution of aerosol was made by coupling three-dimensional aerosol output from the WRF Chemistry model to the Colorado State University (CSU) Regional Atmospheric Modeling System (RAMS) (Ward et al. 2011). The biggest problem associated with this scheme was the computational expense. In fact, the computational expense associated with this scheme was so high, that it was prohibitive for simulations with fine enough resolution to accurately represent microphysical processes. To improve upon this method, a new parameterization for aerosol emission was developed in such a way that it was fully contained within RAMS. Several assumptions went into generating a computationally efficient aerosol emissions parameterization in RAMS. The most notable assumption was the decision to neglect the chemical processes in formed in the formation of Secondary Aerosol (SA), and instead treat SA as primary aerosol via short-term WRF-CHEM simulations. While, SA makes up a substantial portion of the total aerosol burden (much of which is made up of organic material), the representation of this process is highly complex and highly expensive within a numerical model. Furthermore, SA formation is greatly reduced during the winter months due to the lack of naturally produced organic VOC's. Because of these reasons, it was felt that neglecting SOA within the model was the best course of action. The actual parameterization uses a prescribed source map to add aerosol to the model at two vertical levels that surround an arbitrary height decided by the user. To best represent the real-world, the WRF Chemistry model was run using the National Emissions Inventory (NEI2005) to represent anthropogenic emissions and the Model Emissions of Gases and Aerosols from Nature (MEGAN) to represent natural contributions to aerosol. WRF Chemistry was run for one hour, after which the aerosol output along with the hygroscopicity parameter (κ) were saved into a data file that had the capacity to be interpolated to an arbitrary grid used in RAMS. The comparison of this parameterization to observations collected at Mesa Verde National Park (MVNP) during the Inhibition of Snowfall from Pollution Aerosol (ISPA-III) field campaign yielded promising results. The model was able to simulate the variability in near surface aerosol concentration with reasonable accuracy, though with a general low bias. Furthermore, this model compared much better to the observations than did the WRF Chemistry model using a fraction of the computational expense. This emissions scheme was able to show reasonable solutions regarding the aerosol concentrations and can therefore be used to provide an estimate of the seasonal impact of increased CCN on water resources in Western Colorado with relatively low computational expense.

Linking Aerosol Optical Properties Between Laboratory, Field, and Model Studies

NASA Astrophysics Data System (ADS)

Murphy, S. M.; Pokhrel, R. P.; Foster, K. A.; Brown, H.; Liu, X.

2017-12-01

The optical properties of aerosol emissions from biomass burning have a significant impact on the Earth's radiative balance. Based on measurements made during the Fourth Fire Lab in Missoula Experiment, our group published a series of parameterizations that related optical properties (single scattering albedo and absorption due to brown carbon at multiple wavelengths) to the elemental to total carbon ratio of aerosols emitted from biomass burning. In this presentation, the ability of these parameterizations to simulate the optical properties of ambient aerosol is assessed using observations collected in 2017 from our mobile laboratory chasing wildfires in the Western United States. The ambient data includes measurements of multi-wavelength absorption, scattering, and extinction, size distribution, chemical composition, and volatility. In addition to testing the laboratory parameterizations, this combination of measurements allows us to assess the ability of core-shell Mie Theory to replicate observations and to assess the impact of brown carbon and mixing state on optical properties. Finally, both laboratory and ambient data are compared to the optical properties generated by a prominent climate model (Community Earth System Model (CESM) coupled with the Community Atmosphere Model (CAM 5)). The discrepancies between lab observations, ambient observations and model output will be 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.

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.

Radiative flux and forcing parameterization error in aerosol-free clear skies.

PubMed

Pincus, Robert; Mlawer, Eli J; Oreopoulos, Lazaros; Ackerman, Andrew S; Baek, Sunghye; Brath, Manfred; Buehler, Stefan A; Cady-Pereira, Karen E; Cole, Jason N S; Dufresne, Jean-Louis; Kelley, Maxwell; Li, Jiangnan; Manners, James; Paynter, David J; Roehrig, Romain; Sekiguchi, Miho; Schwarzkopf, Daniel M

2015-07-16

Radiation parameterizations in GCMs are more accurate than their predecessorsErrors in estimates of 4 ×CO 2 forcing are large, especially for solar radiationErrors depend on atmospheric state, so global mean error is unknown.

Campaign datasets for Two-Column Aerosol Project (TCAP)

DOE Data Explorer

Berg,Larry; Mei,Fan; Cairns,Brian; Chand,Duli; Comstock,Jennifer; Cziczo,Daniel; Hostetler,Chris; Hubbe,John; Long,Chuck; Michalsky,Joseph; Pekour,Mikhail; Russell,Phil; Scott,Herman; Sedlacek,Arthur; Shilling,John; Springston,Stephen; Tomlinson,Jason; Watson,Thomas; Zelenyuk-Imre,Alla

2013-12-30

This campaign was designed to provide a detailed set of observations with which to 1) perform radiative and cloud condensation nuclei (CCN) closure studies, 2) evaluate a new retrieval algorithm for aerosol optical depth (AOD) in the presence of clouds using passive remote sensing 3) extend a previously developed technique to investigate aerosol indirect effects, and 4) evaluate the performance of a detailed regional-scale model and a more parameterized global-scale model in simulating particle activation and AOD associated with the aging of anthropogenic aerosols. To meet these science objectives, the ARM Mobile Facility (AMF) and the Mobile Aerosol Observing System (MAOS) was deployed on Cape Cod, Massachusetts for a 12-month period starting in the summer of 2012 in order to quantify aerosol properties, radiation and cloud characteristics at a location subject to both clear- and cloudy- conditions, and clean- and polluted-conditions. These observations were supplemented by two aircraft intensive observation periods (IOPS), one in the summer and a second in the winter. Each IOP required two aircraft.

Uncertainty in Predicting CCN Activity of Aged and Primary Aerosols

NASA Astrophysics Data System (ADS)

Zhang, Fang; Wang, Yuying; Peng, Jianfei; Ren, Jingye; Collins, Don; Zhang, Renyi; Sun, Yele; Yang, Xin; Li, Zhanqing

2017-11-01

Understanding particle CCN activity in diverse atmospheres is crucial when evaluating aerosol indirect effects. Here aerosols measured at three sites in China were categorized as different types for attributing uncertainties in CCN prediction in terms of a comprehensive data set including size-resolved CCN activity, size-resolved hygroscopic growth factor, and chemical composition. We show that CCN activity for aged aerosols is unexpectedly underestimated 22% at a supersaturation (S) of 0.2% when using κ-Kohler theory with an assumption of an internal mixture with measured bulk composition that has typically resulted in an overestimate of the CCN activity in previous studies. We conclude that the underestimation stems from neglect of the effect of aging/coating on particle hygroscopicity, which is not considered properly in most current models. This effect enhanced the hygroscopicity parameter (κ) by between 11% (polluted conditions) and 30% (clean days), as indicated in diurnal cycles of κ based on measurements by different instruments. In the urban Beijing atmosphere heavily influenced by fresh emissions, the CCN activity was overestimated by 45% at S = 0.2%, likely because of inaccurate assumptions of particle mixing state and because of variability of chemical composition over the particle size range. For both fresh and aged aerosols, CCN prediction exhibits very limited sensitivity to κSOA, implying a critical role of other factors like mixing of aerosol components within and between particles in regulating CCN activity. Our findings could help improving CCN parameterization in climate models.

A Global Data Assimilation System for Atmospheric Aerosol

NASA Technical Reports Server (NTRS)

daSilva, Arlindo

1999-01-01

We will give an overview of an aerosol data assimilation system which combines advances in remote sensing of atmospheric aerosols, aerosol modeling and data assimilation methodology to produce high spatial and temporal resolution 3D aerosol fields. Initially, the Goddard Aerosol Assimilation System (GAAS) will assimilate TOMS, AVHRR and AERONET observations; later we will include MODIS and MISR. This data assimilation capability will allows us to integrate complementing aerosol observations from these platforms, enabling the development of an assimilated aerosol climatology as well as a global aerosol forecasting system in support of field campaigns. Furthermore, this system provides an interactive retrieval framework for each aerosol observing satellites, in particular TOMS and AVHRR. The Goddard Aerosol Assimilation System (GAAS) takes advantage of recent advances in constituent data assimilation at DAO, including flow dependent parameterizations of error covariances and the proper consideration of model bias. For its prognostic transport model, GAAS will utilize the Goddard Ozone, Chemistry, Aerosol, Radiation and Transport (GOCART) model developed at NASA/GSFC Codes 916 and 910.3. GOCART includes the Lin-Rood flux-form, semi-Langrangian transport model with parameterized aerosol chemistry and physical processes for absorbing (dust and black carbon) and non-absorbing aerosols (sulfate and organic carbon). Observations and model fields are combined using a constituent version of DAO's Physical-space Statistical Analysis System (PSAS), including its adaptive quality control system. In this talk we describe the main components of this assimilation system and present preliminary results obtained by assimilating TOMS data.

Coupling Spectral-bin Cloud Microphysics with the MOSAIC Aerosol Model in WRF-Chem: Methodology and Results for Marine Stratocumulus Clouds

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

Gao, Wenhua; Fan, Jiwen; Easter, Richard C.

Aerosol-cloud interaction processes can be represented more physically with bin cloud microphysics relative to bulk microphysical parameterizations. However, due to computational power limitations in the past, bin cloud microphysics was often run with very simple aerosol treatments. The purpose of this study is to represent better aerosol-cloud interaction processes in the Chemistry version of Weather Research and Forecast model (WRF-Chem) at convection-permitting scales by coupling spectral-bin cloud microphysics (SBM) with the MOSAIC sectional aerosol model. A flexible interface is built that exchanges cloud and aerosol information between them. The interface contains a new bin aerosol activation approach, which replaces themore » treatments in the original SBM. It also includes the modified aerosol resuspension and in-cloud wet removal processes with the droplet loss tendencies and precipitation fluxes from SBM. The newly coupled system is evaluated for two marine stratocumulus cases over the Southeast Pacific Ocean with either a simplified aerosol setup or full-chemistry. We compare the aerosol activation process in the newly-coupled SBM-MOSAIC against the SBM simulation without chemistry using a simplified aerosol setup, and the results show consistent activation rates. A longer time simulation reinforces that aerosol resuspension through cloud drop evaporation plays an important role in replenishing aerosols and impacts cloud and precipitation in marine stratocumulus clouds. Evaluation of the coupled SBM-MOSAIC with full-chemistry using aircraft measurements suggests that the new model works realistically for the marine stratocumulus clouds, and improves the simulation of cloud microphysical properties compared to a simulation using MOSAIC coupled with the Morrison two-moment microphysics.« less

Coupling spectral-bin cloud microphysics with the MOSAIC aerosol model in WRF-Chem: Methodology and results for marine stratocumulus clouds

NASA Astrophysics Data System (ADS)

Gao, Wenhua; Fan, Jiwen; Easter, R. C.; Yang, Qing; Zhao, Chun; Ghan, Steven J.

2016-09-01

Aerosol-cloud interaction processes can be represented more physically with bin cloud microphysics relative to bulk microphysical parameterizations. However, due to computational power limitations in the past, bin cloud microphysics was often run with very simple aerosol treatments. The purpose of this study is to represent better aerosol-cloud interaction processes in the Chemistry version of Weather Research and Forecast model (WRF-Chem) at convection-permitting scales by coupling spectral-bin cloud microphysics (SBM) with the MOSAIC sectional aerosol model. A flexible interface is built that exchanges cloud and aerosol information between them. The interface contains a new bin aerosol activation approach, which replaces the treatments in the original SBM. It also includes the modified aerosol resuspension and in-cloud wet removal processes with the droplet loss tendencies and precipitation fluxes from SBM. The newly coupled system is evaluated for two marine stratocumulus cases over the Southeast Pacific Ocean with either a simplified aerosol setup or full-chemistry. We compare the aerosol activation process in the newly coupled SBM-MOSAIC against the SBM simulation without chemistry using a simplified aerosol setup, and the results show consistent activation rates. A longer time simulation reinforces that aerosol resuspension through cloud drop evaporation plays an important role in replenishing aerosols and impacts cloud and precipitation in marine stratocumulus clouds. Evaluation of the coupled SBM-MOSAIC with full-chemistry using aircraft measurements suggests that the new model works realistically for the marine stratocumulus clouds, and improves the simulation of cloud microphysical properties compared to a simulation using MOSAIC coupled with the Morrison two-moment microphysics.

Aerosol indirect effects on summer precipitation in a regional climate model for the Euro-Mediterranean region

NASA Astrophysics Data System (ADS)

Da Silva, Nicolas; Mailler, Sylvain; Drobinski, Philippe

2018-03-01

Aerosols affect atmospheric dynamics through their direct and semi-direct effects as well as through their effects on cloud microphysics (indirect effects). The present study investigates the indirect effects of aerosols on summer precipitation in the Euro-Mediterranean region, which is located at the crossroads of air masses carrying both natural and anthropogenic aerosols. While it is difficult to disentangle the indirect effects of aerosols from the direct and semi-direct effects in reality, a numerical sensitivity experiment is carried out using the Weather Research and Forecasting (WRF) model, which allows us to isolate indirect effects, all other effects being equal. The Mediterranean hydrological cycle has often been studied using regional climate model (RCM) simulations with parameterized convection, which is the approach we adopt in the present study. For this purpose, the Thompson aerosol-aware microphysics scheme is used in a pair of simulations run at 50 km resolution with extremely high and low aerosol concentrations. An additional pair of simulations has been performed at a convection-permitting resolution (3.3 km) to examine these effects without the use of parameterized convection. While the reduced radiative flux due to the direct effects of the aerosols is already known to reduce precipitation amounts, there is still no general agreement on the sign and magnitude of the aerosol indirect forcing effect on precipitation, with various processes competing with each other. Although some processes tend to enhance precipitation amounts, some others tend to reduce them. In these simulations, increased aerosol loads lead to weaker precipitation in the parameterized (low-resolution) configuration. The fact that a similar result is obtained for a selected area in the convection-permitting (high-resolution) configuration allows for physical interpretations. By examining the key variables in the model outputs, we propose a causal chain that links the aerosol effects on microphysics to their simulated effect on precipitation, essentially through reduction of the radiative heating of the surface and corresponding reductions of surface temperature, resulting in increased atmospheric stability in the presence of high aerosol loads.

Whitecaps, sea-salt aerosols, and climate

NASA Astrophysics Data System (ADS)

Anguelova, Magdalena Dimitrova

Oceanic whitecaps are the major source of sea-salt aerosols. Because these aerosols are dominant in remote marine air, they control the radiative properties of the clean background atmosphere by scattering sunlight, changing cloud properties and lifetime, and providing media for chemical reactions. Including sea-salt effects in climate models improves predictions, but simulating their generation is first necessary. To make the sea-salt generation function currently used in climate models more relevant for aerosol investigations, this study proposes two modifications. First, the conventional relation between whitecap coverage, W, and the 10-meter wind speed, U10, used in typical generation functions is expanded to include additional factors that affect whitecaps and sea-salt aerosol formation. Second, the sea-salt generation function is extended to smaller sizes; sea-salt aerosol with initial radii from 0.4 to 20 mum can now be modeled. To achieve these goals, this thesis develops a new method for estimating whitecap coverage on a global scale using satellite measurements of the brightness temperature of the ocean surface. Whitecap coverage evaluated with this method incorporates the effects of atmospheric stability, sea-surface temperature, salinity, wind fetch, wind duration, and the amount of surface-active material. Assimilating satellite-derived values for whitecap coverage in the sea-salt generation function incorporates the effects of all environmental factors on sea-salt production and predicts realistic sea-salt aerosol loadings into the atmosphere. An extensive database of whitecap coverage and sea-salt aerosol fluxes has been compiled with the new method and is used to investigate their spatial and temporal characteristics. The composite effect of all environmental factors suggests a more uniform latitudinal distribution of whitecaps and sea-salt aerosols than that predicted from wind speed alone. The effect of sea-surface temperature, TS, is parameterized for the first time using regression analysis. The resulting parameterization W( U10, TS) is a better predictor of whitecap coverage than the conventional W(U 10) relation. This thesis also considers the contribution of oceanic whitecaps to ocean albedo and CO2 transfer and evaluates the direct effect of sea-salt aerosols on climate, the sea-salt contribution to CCN formation, and the role of sea-salt aerosols in atmospheric chemistry.

Effects of a polar stratosphere cloud parameterization on ozone depletion due to stratospheric aircraft in a two-dimensional model

NASA Technical Reports Server (NTRS)

Considine, David B.; Douglass, Anne R.; Jackman, Charles H.

1994-01-01

A parameterization of Type 1 and 2 polar stratospheric cloud (PSC) formation is presented which is appropriate for use in two-dimensional (2-D) photochemical models of the stratosphere. The calculations of PSC frequency of occurrence and surface area density uses climatological temperature probability distributions obtained from National Meteorological Center data to avoid using zonal mean temperatures, which are not good predictors of PSC behavior. The parameterization does not attempt to model the microphysics of PSCs. The parameterization predicts changes in PSC formation and heterogeneous processing due to perturbations of stratospheric trace constituents. It is therefore useful in assessing the potential effects of a fleet of stratospheric aircraft (high speed civil transports, or HSCTs) on stratospheric composition. the model calculated frequency of PSC occurrence agrees well with a climatology based on stratospheric aerosol measurement (SAM) 2 observations. PSCs are predicted to occur in the tropics. Their vertical range is narrow, however, and their impact on model O3 fields is small. When PSC and sulfate aerosol heterogeneous processes are included in the model calculations, the O3 change for 1980 - 1990 is in substantially better agreement with the total ozone mapping spectrometer (TOMS)-derived O3 trend than otherwise. The overall changes in model O3 response to standard HSCT perturbation scenarios produced by the parameterization are small and tend to decrease the model sensitivity to the HSCT perturbation. However, in the southern hemisphere spring a significant increase in O3 sensitivity to HSCT perturbations is found. At this location and time, increased PSC formation leads to increased levels of active chlorine, which produce the O3 decreases.

Effect of Terrestrial and Marine Organic Aerosol on Regional and Global Climate: Model Development, Application, and Verification with Satellite Data

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

Meskhidze, Nicholas; Zhang, Yang; Kamykowski, Daniel

2012-03-28

In this DOE project the improvements to parameterization of marine primary organic matter (POM) emissions, hygroscopic properties of marine POM, marine isoprene derived secondary organic aerosol (SOA) emissions, surfactant effects, new cloud droplet activation parameterization have been implemented into Community Atmosphere Model (CAM 5.0), with a seven mode aerosol module from the Pacific Northwest National Laboratory (PNNL)'s Modal Aerosol Model (MAM7). The effects of marine aerosols derived from sea spray and ocean emitted biogenic volatile organic compounds (BVOCs) on microphysical properties of clouds were explored by conducting 10 year CAM5.0-MAM7 model simulations at a grid resolution 1.9° by 2.5° withmore » 30 vertical layers. Model-predicted relationship between ocean physical and biological systems and the abundance of CCN in remote marine atmosphere was compared to data from the A-Train satellites (MODIS, CALIPSO, AMSR-E). Model simulations show that on average, primary and secondary organic aerosol emissions from the ocean can yield up to 20% increase in Cloud Condensation Nuclei (CCN) at 0.2% Supersaturation, and up to 5% increases in droplet number concentration of global maritime shallow clouds. Marine organics were treated as internally or externally mixed with sea salt. Changes associated with cloud properties reduced (absolute value) the model-predicted short wave cloud forcing from -1.35 Wm-2 to -0.25 Wm-2. By using different emission scenarios, and droplet activation parameterizations, this study suggests that addition of marine primary aerosols and biologically generated reactive gases makes an important difference in radiative forcing assessments. All baseline and sensitivity simulations for 2001 and 2050 using global-through-urban WRF/Chem (GU-WRF) were completed. The main objective of these simulations was to evaluate the capability of GU-WRF for an accurate representation of the global atmosphere by exploring the most accurate configuration of physics options in GWRF for global scale modeling in 2001 at a horizontal grid resolution of 1° x 1°. GU-WRF model output was evaluated using observational datasets from a variety of sources including surface based observations (NCDC and BSRN), model reanalysis (NCEP/ NCAR Reanalysis and CMAP), and remotely-sensed data (TRMM) to evaluate the ability of GU-WRF to simulate atmospheric variables at the surface as well as aloft. Explicit treatment of nanoparticles produced from new particle formation in GU-WRF/Chem-MADRID was achieved by expanding particle size sections from 8 to 12 to cover particles with the size range of 1.16 nm to 11.6m. Simulations with two different nucleation parameterizations were conducted for August 2002 over a global domain at a 4º by 5º horizontal resolution. The results are evaluated against field measurement data from the 2002 Aerosol Nucleation and Real Time Characterization Experiment (ANARChE) in Atlanta, Georgia, as well as satellite and reanalysis data. We have also explored the relationship between clean marine aerosol optical properties and ocean surface wind speed using remotely sensed data from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the CALIPSO satellite and the Advanced Microwave Scanning Radiometer (AMSR-E) on board the AQUA satellite. Detailed data analyses were carried out over 15 regions selected to be representative of different areas of the global ocean for the time period from June 2006 to April 2011. We show that for very low (less than 4 m s-1) and very high (more than 12 m s-1) wind speed conditions the mean CALIPSO-derived aerosol optical depth (AOD) has little dependency on the surface wind speed. For an intermediate (between 4 and 12 m s-1) marine AOD was linearly correlated with the surface wind speed values, with a slope of 0.0062 s m-1. Results of our study suggest that considerable improvements to both optical properties of marine aerosols and their production mechanisms can be achieved by discriminating clean marine aerosols (or sea salt particles) from all other types of aerosols present over the ocean.« less

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

A consistent prescription of stratospheric aerosol for both radiation and chemistry in the Community Earth System Model (CESM1)

DOE PAGES

Neely, III, Ryan Reynolds; Conley, Andrew J.; Vitt, Francis; ...

2016-07-25

Here we describe an updated parameterization for prescribing stratospheric aerosol in the National Center for Atmospheric Research (NCAR) Community Earth System Model (CESM1). The need for a new parameterization is motivated by the poor response of the CESM1 (formerly referred to as the Community Climate System Model, version 4, CCSM4) simulations contributed to the Coupled Model Intercomparison Project 5 (CMIP5) to colossal volcanic perturbations to the stratospheric aerosol layer (such as the 1991 Pinatubo eruption or the 1883 Krakatau eruption) in comparison to observations. In particular, the scheme used in the CMIP5 simulations by CESM1 simulated a global mean surface temperature decreasemore » that was inconsistent with the GISS Surface Temperature Analysis (GISTEMP), NOAA's National Climatic Data Center, and the Hadley Centre of the UK Met Office (HADCRUT4). The new parameterization takes advantage of recent improvements in historical stratospheric aerosol databases to allow for variations in both the mass loading and size of the prescribed aerosol. An ensemble of simulations utilizing the old and new schemes shows CESM1's improved response to the 1991 Pinatubo eruption. Most significantly, the new scheme more accurately simulates the temperature response of the stratosphere due to local aerosol heating. Here, results also indicate that the new scheme decreases the global mean temperature response to the 1991 Pinatubo eruption by half of the observed temperature change, and modelled climate variability precludes statements as to the significance of this change.« 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

Simulation of semi-explicit mechanisms of SOA formation from glyoxal in a 3D model

NASA Astrophysics Data System (ADS)

Knote, C. J.; Hodzic, A.; Jimenez, J. L.; Volkamer, R.; Orlando, J. J.; Baidar, S.; Brioude, J. F.; Fast, J. D.; Gentner, D. R.; Goldstein, A. H.; Hayes, P. L.; Knighton, W. B.; Oetjen, H.; Setyan, A.; Stark, H.; Thalman, R. M.; Tyndall, G. S.; Washenfelder, R. A.; Waxman, E.; Zhang, Q.

2013-12-01

Formation of secondary organic aerosols (SOA) through multi-phase processing of glyoxal has been proposed recently as a relevant contributor to SOA mass. Glyoxal has both anthropogenic and biogenic sources, and readily partitions into the aqueous-phase of cloud droplets and aerosols. Both reversible and irreversible chemistry in the liquid-phase has been observed. A recent laboratory study indicates that the presence of salts in the liquid-phase strongly enhances the Henry';s law constant of glyoxal, allowing for much more effective multi-phase processing. In our work we investigate the contribution of glyoxal to SOA formation on the regional scale. We employ the regional chemistry transport model WRF-chem with MOZART gas-phase chemistry and MOSAIC aerosols, which we both extended to improve the description of glyoxal formation in the gas-phase, and its interactions with aerosols. The detailed description of aerosols in our setup allows us to compare very simple (uptake coefficient) parameterizations of SOA formation from glyoxal, as has been used in previous modeling studies, with much more detailed descriptions of the various pathways postulated based on laboratory studies. Measurements taken during the CARES and CalNex campaigns in California in summer 2010 allowed us to constrain the model, including the major direct precursors of glyoxal. Simulations at convection-permitting resolution over a 2 week period in June 2010 have been conducted to assess the effect of the different ways to parameterize SOA formation from glyoxal and investigate its regional variability. We find that depending on the parameterization used the contribution of glyoxal to SOA is between 1 and 15% in the LA basin during this period, and that simple parameterizations based on uptake coefficients derived from box model studies lead to higher contributions (15%) than parameterizations based on lab experiments (1%). A kinetic limitation found in experiments hinders substantial contribution of volume-based pathways to total SOA formation from glyoxal. Once removed, 5% of total SOA can be formed from glyoxal through these channels. Results from a year-long simulation over the continental US will give a broader picture of the contribution of glyoxal to SOA formation.

Stochastic Convection Parameterizations

NASA Technical Reports Server (NTRS)

Teixeira, Joao; Reynolds, Carolyn; Suselj, Kay; Matheou, Georgios

2012-01-01

computational fluid dynamics, radiation, clouds, turbulence, convection, gravity waves, surface interaction, radiation interaction, cloud and aerosol microphysics, complexity (vegetation, biogeochemistry, radiation versus turbulence/convection stochastic approach, non-linearities, Monte Carlo, high resolutions, large-Eddy Simulations, cloud structure, plumes, saturation in tropics, forecasting, parameterizations, stochastic, radiation-clod interaction, hurricane forecasts

Aerosol indirect effect on the grid-scale clouds in the two-way coupled WRF-CMAQ: model description, development, evaluation and regional analysis

EPA Science Inventory

This study implemented first, second and glaciations aerosol indirect effects (AIE) on resolved clouds in the two-way coupled WRF-CMAQ modeling system by including parameterizations for both cloud drop and ice number concentrations on the basis of CMAQ predicted aerosol distribu...

Grid-scale Indirect Radiative Forcing of Climate due to aerosols over the northern hemisphere simulated by the integrated WRF-CMAQ model: Preliminary results

EPA Science Inventory

In this study, indirect aerosol effects on grid-scale clouds were implemented in the integrated WRF3.3-CMAQ5.0 modeling system by including parameterizations for both cloud droplet and ice number concentrations calculated from the CMAQ-predicted aerosol particles. The resulting c...

Observational Constraints on Ephemeral Wind Gusts that MobilizeSoil Dust Aerosols

NASA Astrophysics Data System (ADS)

Miller, R. L.; Leung, M. F.

2017-12-01

Dust aerosol models resolve the planetary scale winds that disperse particles throughout the globe, but the winds raising dust are often organized on smaller scales that are below the resolution of the model. These winds, including ephemeral wind gusts associated with boundary layer mixing, are typically parameterized. For example, gusts by dry convective eddies are related to the sensible heat flux. What remains is to constrain the magnitude of the wind gusts using boundary layer measurements, so that dust emission has the correct sensitivity to these gusts, relative to the resolved wind. Here, we use a year of ARM measurements with high temporal resolution from Niamey, Niger in the Sahel to evaluate our parameterization. This evaluation is important for dust aerosol models that use 'nudging' to reproduce observed transport patterns.

Limited Effect of Anthropogenic Nitrogen Oxides on Secondary Organic Aerosol Formation

NASA Astrophysics Data System (ADS)

Zheng, Y.; Unger, N.; Hodzic, A.; Knote, C. J.; Tilmes, S.; Emmons, L. K.; Lamarque, J. F.; Yu, P.

2014-12-01

Globally secondary organic aerosol (SOA) is mostly formed from biogenic vegetation emissions and as such is regarded as natural aerosol that cannot be reduced by emission control legislation. However, recent research implies that human activities facilitate SOA formation by affecting the amount of precursor emission, the chemical processing and the partitioning into the aerosol phase. Among the multiple human influences, nitrogen oxides (NO + NO2 = NOx) have been assumed to play a critical role in the chemical formation of low volatile compounds. The goal of this study is to improve the SOA scheme in the global NCAR Community Atmospheric Model version 4 with chemistry (CAM4-Chem) by implementing an updated 4-product Volatility Basis Set (VBS) scheme, and apply it to investigate the impact of anthropogenic NOx on SOA. We first compare three different SOA parameterizations: a 2-product model and the updated VBS model both with and without a SOA aging parameterization. Secondly we evaluate predicted organic aerosol amounts against surface measurement from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network and Aerosol Mass Spectrometer (AMS) measurements from 13 aircraft-based field campaigns. We then perform sensitivity experiments to examine how the SOA loading responds to a 50% reduction in anthropogenic NOx in different regions. We find limited SOA reductions of -2.3%, -5.6% and -4.0% for global, southeastern U.S. and Amazon NOx perturbations, respectively. To investigate the chemical processes in more detail, we also use a simplified box model with the same gas-phase chemistry and gas-aerosol partitioning mechanism as in CAM4-Chem to examine the SOA yields dependence on initial precursor emissions and background NOx level. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to buffering in chemical pathways (low- versus high-NOx pathways, OH versus NO3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.

Modeling regional air quality and climate: improving organic aerosol and aerosol activation processes in WRF/Chem version 3.7.1

NASA Astrophysics Data System (ADS)

Yahya, Khairunnisa; Glotfelty, Timothy; Wang, Kai; Zhang, Yang; Nenes, Athanasios

2017-06-01

Air quality and climate influence each other through the uncertain processes of aerosol formation and cloud droplet activation. In this study, both processes are improved in the Weather, Research and Forecasting model with Chemistry (WRF/Chem) version 3.7.1. The existing Volatility Basis Set (VBS) treatments for organic aerosol (OA) formation in WRF/Chem are improved by considering the following: the secondary OA (SOA) formation from semi-volatile primary organic aerosol (POA), a semi-empirical formulation for the enthalpy of vaporization of SOA, and functionalization and fragmentation reactions for multiple generations of products from the oxidation of VOCs. Over the continental US, 2-month-long simulations (May to June 2010) are conducted and results are evaluated against surface and aircraft observations during the Nexus of Air Quality and Climate Change (CalNex) campaign. Among all the configurations considered, the best performance is found for the simulation with the 2005 Carbon Bond mechanism (CB05) and the VBS SOA module with semivolatile POA treatment, 25 % fragmentation, and the emissions of semi-volatile and intermediate volatile organic compounds being 3 times the original POA emissions. Among the three gas-phase mechanisms (CB05, CB6, and SAPRC07) used, CB05 gives the best performance for surface ozone and PM2. 5 concentrations. Differences in SOA predictions are larger for the simulations with different VBS treatments (e.g., nonvolatile POA versus semivolatile POA) compared to the simulations with different gas-phase mechanisms. Compared to the simulation with CB05 and the default SOA module, the simulations with the VBS treatment improve cloud droplet number concentration (CDNC) predictions (normalized mean biases from -40.8 % to a range of -34.6 to -27.7 %), with large differences between CB05-CB6 and SAPRC07 due to large differences in their OH and HO2 predictions. An advanced aerosol activation parameterization based on the Fountoukis and Nenes (2005) series reduces the large negative CDNC bias associated with the default Abdul Razzak and Ghan (2000) parameterization from -35.4 % to a range of -0.8 to 7.1 %. However, it increases the errors due to overpredictions of CDNC, mainly over the northeastern US. This work indicates a need to improve other aerosol-cloud-radiation processes in the model, such as the spatial distribution of aerosol optical depth and cloud condensation nuclei, in order to further improve CDNC predictions.

Assessing the Performance of Computationally Simple and Complex Representations of Aerosol Processes using a Testbed Methodology

NASA Astrophysics Data System (ADS)

Fast, J. D.; Ma, P.; Easter, R. C.; Liu, X.; Zaveri, R. A.; Rasch, P.

2012-12-01

Predictions of aerosol radiative forcing in climate models still contain large uncertainties, resulting from a poor understanding of certain aerosol processes, the level of complexity of aerosol processes represented in models, and the ability of models to account for sub-grid scale variability of aerosols and processes affecting them. In addition, comparing the performance and computational efficiency of new aerosol process modules used in various studies is problematic because different studies often employ different grid configurations, meteorology, trace gas chemistry, and emissions that affect the temporal and spatial evolution of aerosols. To address this issue, we have developed an Aerosol Modeling Testbed (AMT) to systematically and objectively evaluate aerosol process modules. The AMT consists of the modular Weather Research and Forecasting (WRF) model, a series of testbed cases for which extensive in situ and remote sensing measurements of meteorological, trace gas, and aerosol properties are available, and a suite of tools to evaluate the performance of meteorological, chemical, aerosol process modules. WRF contains various parameterizations of meteorological, chemical, and aerosol processes and includes interactive aerosol-cloud-radiation treatments similar to those employed by climate models. In addition, the physics suite from a global climate model, Community Atmosphere Model version 5 (CAM5), has also been ported to WRF so that these parameterizations can be tested at various spatial scales and compared directly with field campaign data and other parameterizations commonly used by the mesoscale modeling community. In this study, we evaluate simple and complex treatments of the aerosol size distribution and secondary organic aerosols using the AMT and measurements collected during three field campaigns: the Megacities Initiative Local and Global Observations (MILAGRO) campaign conducted in the vicinity of Mexico City during March 2006, the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento California during June 2010, and the California Nexus (CalNex) campaign conducted in southern California during May and June of 2010. For the aerosol size distribution, we compare the predictions from the GOCART bulk aerosol model, the MADE/SORGAM modal aerosol model, the Modal Aerosol Model (MAM) employed by CAM5, and the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) which uses a sectional representation. For secondary organic aerosols, we compare simple fixed mass yield approaches with the numerically complex volatility basis set approach. All simulations employ the same emissions, meteorology, trace gas chemistry (except for that involving condensable organic species), and initial and boundary conditions. Performance metrics from the AMT are used to assess performance in terms of simulated mass, composition, size distribution (except for GOCART), and aerosol optical properties in relation to computational expense. In addition to statistical measures, qualitative differences among the different aerosol models over the computational domain are presented to examine variations in how aerosols age among the aerosol models.

A critical role for autoxidation in the alpha-pinene + OH aerosol system

EPA Science Inventory

Oxidation of monoterpenes results in efficient formation of secondary organic aerosol (SOA) and is included as an SOA source in most chemical transport models. However, current model parameterizations lack a mechanistic dependence of monoterpene SOA on NOx and oxidant identity (e...

Investigating the Use of a Simplified Aerosol Parameterization in Space-Based XCO2 Retrievals from OCO-2

NASA Astrophysics Data System (ADS)

Nelson, R. R.; O'Dell, C.

2017-12-01

The primary goal of OCO-2 is to use hyperspectral measurements of reflected near-infrared sunlight to retrieve the column-averaged dry-air mole fraction of carbon dioxide (XCO2) with high accuracy. This is only possible for measurements of scenes nearly free of optically thick clouds and aerosols. As some cloud or aerosol contamination will always be present, the OCO-2 retrieval algorithm includes clouds and aerosols as retrieved properties in its state vector. Information content analyses demonstrate that there are only 2-6 pieces of information about aerosols in the OCO-2 radiances. However, the upcoming OCO-2 algorithm (B8) attempts to retrieve 9 aerosol parameters; this over-fitting can hinder convergence and produce multiple solutions. In this work, we develop a simplified cloud and aerosol parameterization that intelligently reduces the number of retrieved parameters to 5 by only retrieving information about two aerosol layers: a lower tropospheric layer and an upper tropospheric / stratospheric layer. We retrieve the optical depth of each layer and the height of the lower tropospheric layer. Each of these layers contains a mixture of fine and coarse mode aerosol. In comparisons between OCO-2 XCO2 estimates and validation sources including TCCON, this scheme performs about as well as the more complicated OCO-2 retrieval algorithm, but has the potential benefits of more interpretable aerosol results, faster convergence, less nonlinearity, and greater throughput. We also investigate the dependence of our results on the optical properties of the fine and coarse mode aerosol types, such as their effective radii and the environmental relative humidity.

Assimilation of MODIS and VIIRS AOD to improve aerosols forecasts with FV3-GOCART

NASA Astrophysics Data System (ADS)

Pagowski, M.

2017-12-01

In 2016 NOAA chose the FV3 dynamical core as a basis for its future global modeling system. We present an implementation of aerosol module in the FV3 model and its assimilation framework. The parameterization of aerosols is based on the GOCART scheme. The assimilation methodology relies on hybrid 3D-Var and EnKF methods. Aerosol observations include aerosol optical depth at 550 nm from VIIRS satellite. Results and evaluation of the system against independent observations and NASA's MERRA-2 is shown.

GCM Simulations of the Aerosol Indirect Effect: Sensitivity to Cloud Parameterization and Aerosol Burden

NASA Technical Reports Server (NTRS)

Menon, Surabi; DelGenio, Anthony D.; Koch, Dorothy; Tselioudis, George; Hansen, James E. (Technical Monitor)

2001-01-01

We describe the coupling of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to an online sulfur chemistry model and source models for organic matter and sea-salt that is used to estimate the aerosol indirect effect. The cloud droplet number concentration is diagnosed empirically from field experiment datasets over land and ocean that observe droplet number and all three aerosol types simultaneously; corrections are made for implied variations in cloud turbulence levels. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to predict aerosol effects on cloud optical thickness and microphysical process rates. We calculate the aerosol indirect effect by differencing the top-of-the-atmosphere net cloud radiative forcing for simulations with present-day vs. pre-industrial emissions. Both the first (radiative) and second (microphysical) indirect effects are explored. We test the sensitivity of our results to cloud parameterization assumptions that control the vertical distribution of cloud occurrence, the autoconversion rate, and the aerosol scavenging rate, each of which feeds back significantly on the model aerosol burden. The global mean aerosol indirect effect for all three aerosol types ranges from -1.55 to -4.36 W m(exp -2) in our simulations. The results are quite sensitive to the pre-industrial background aerosol burden, with low pre-industrial burdens giving strong indirect effects, and to a lesser extent to the anthropogenic aerosol burden, with large burdens giving somewhat larger indirect effects. Because of this dependence on the background aerosol, model diagnostics such as albedo-particle size correlations and column cloud susceptibility, for which satellite validation products are available, are not good predictors of the resulting indirect effect.

GCM Simulations of the Aerosol Indirect Effect: Sensitivity to Cloud Parameterization and Aerosol Burden

NASA Technical Reports Server (NTRS)

Menon, Surabi; DelGenio, Anthony D.; Koch, Dorothy; Tselioudis, George; Hansen, James E. (Technical Monitor)

2001-01-01

We describe the coupling of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to an online sulfur chemistry model and source models for organic matter and sea-salt that is used to estimate the aerosol indirect effect. The cloud droplet number concentration is diagnosed empirically from field experiment datasets over land and ocean that observe droplet number and all three aerosol types simultaneously; corrections are made for implied variations in cloud turbulence levels. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to predict aerosol effects on cloud optical thickness and microphysical process rates. We calculate the aerosol indirect effect by differencing the top-of-the-atmosphere net cloud radiative forcing for simulations with present-day vs. pre-industrial emissions. Both the first (radiative) and second (microphysical) indirect effects are explored. We test the sensitivity of our results to cloud parameterization assumptions that control the vertical distribution of cloud occurrence, the autoconversion rate, and the aerosol scavenging rate, each of which feeds back significantly on the model aerosol burden. The global mean aerosol indirect effect for all three aerosol types ranges from -1.55 to -4.36 W/sq m in our simulations. The results are quite sensitive to the pre-industrial background aerosol burden, with low pre-industrial burdens giving strong indirect effects, and to a lesser extent to the anthropogenic aerosol burden, with large burdens giving somewhat larger indirect effects. Because of this dependence on the background aerosol, model diagnostics such as albedo-particle size correlations and column cloud susceptibility, for which satellite validation products are available, are not good predictors of the resulting indirect effect.

Aerosol indirect effect on tropospheric ozone via lightning

NASA Astrophysics Data System (ADS)

Yuan, Tianle; Remer, Lorraine A.; Bian, Huisheng; Ziemke, Jerald R.; Albrecht, Rachel; Pickering, Kenneth E.; Oreopoulos, Lazaros; Goodman, Steven J.; Yu, Hongbin; Allen, Dale J.

2012-09-01

Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. Inadequate understanding of processes related to O3 production, in particular those natural ones such as lightning, contributes to this uncertainty. Here we demonstrate a new effect of aerosol particles on O3production by affecting lightning activity and lightning-generated NOx (LNOx). We find that lightning flash rate increases at a remarkable rate of 30 times or more per unit of aerosol optical depth. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses show O3is increased as a result of aerosol-induced increase in lightning and LNOx, which is supported by modle simulations with prescribed lightning change. O3production increase from this aerosol-lightning-ozone link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. In the face of anthropogenic aerosol increase our findings suggest that lightning activity, LNOx and O3, especially in the upper troposphere, have all increased substantially since preindustrial time due to the proposed aerosol-lightning-ozone link, which implies a stronger O3 historical radiative forcing. Aerosol forcing therefore has a warming component via its effect on O3 production and this component has mostly been ignored in previous studies of climate forcing related to O3and aerosols. Sensitivity simulations suggest that 4-8% increase of column tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications for understanding past and projecting future tropospheric O3forcing as well as wildfire changes and call for integrated investigations of the coupled aerosol-cloud-chemistry system.

Aerosol indirect effect on tropospheric ozone via lightning

NASA Astrophysics Data System (ADS)

Yuan, T.; Remer, L. A.; Bian, H.; Ziemke, J. R.; Albrecht, R. I.; Pickering, K. E.; Oreopoulos, L.; Goodman, S. J.; Yu, H.; Allen, D. J.

2012-12-01

Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. The unresolved difference between modeled and observed natural background O3 concentrations is a key source of the uncertainty. Here we demonstrate remarkable sensitivity of lightning activity to aerosol loading with lightning activity increasing more than 30 times per unit of aerosol optical depth over our study area. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses suggest O3 is increased as a result of aerosol-induced increase in lightning and lightning produced NOx. Model simulations with prescribed lightning change corroborate the satellite data analysis. This aerosol-O3 connection is achieved via aerosol increasing lightning and thus lightning produced nitrogen oxides. This aerosol-lightning-ozone link provides a potential physical mechanism that may account for a part of the model-observation difference in background O3 concentration. More importantly, O3 production increase from this link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. Both of these implications suggest a stronger O3 historical radiative forcing. This introduces a new pathway, through which increasing in aerosols from pre-industrial time to present day enhances tropospheric O3 production. Aerosol forcing thus has a warming component via its effect on O3 production. Sensitivity simulations suggest that 4-8% increase of tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications for understanding past and projecting future tropospheric O3 forcing as well as wildfire changes and call for integrated investigations of the coupled aerosol-cloud-chemistry system.

High Resolution Electro-Optical Aerosol Phase Function Database PFNDAT2006

DTIC Science & Technology

2006-08-01

snow models use the gamma distribution (equation 12) with m = 0. 3.4.1 Rain Model The most widely used analytical parameterization for raindrop size ...Uijlenhoet and Stricker (22), as the result of an analytical derivation based on a theoretical parameterization for the raindrop size distribution ...6 2.2 Particle Size Distribution Models

A Thermal Infrared Radiation Parameterization for Atmospheric Studies

NASA Technical Reports Server (NTRS)

Chou, Ming-Dah; Suarez, Max J.; Liang, Xin-Zhong; Yan, Michael M.-H.; Cote, Charles (Technical Monitor)

2001-01-01

This technical memorandum documents the longwave radiation parameterization developed at the Climate and Radiation Branch, NASA Goddard Space Flight Center, for a wide variety of weather and climate applications. Based on the 1996-version of the Air Force Geophysical Laboratory HITRAN data, the parameterization includes the absorption due to major gaseous absorption (water vapor, CO2, O3) and most of the minor trace gases (N2O, CH4, CFCs), as well as clouds and aerosols. The thermal infrared spectrum is divided into nine bands. To achieve a high degree of accuracy and speed, various approaches of computing the transmission function are applied to different spectral bands and gases. The gaseous transmission function is computed either using the k-distribution method or the table look-up method. To include the effect of scattering due to clouds and aerosols, the optical thickness is scaled by the single-scattering albedo and asymmetry factor. The parameterization can accurately compute fluxes to within 1% of the high spectral-resolution line-by-line calculations. The cooling rate can be accurately computed in the region extending from the surface to the 0.01-hPa level.

Dependence of stratocumulus-topped boundary-layer entrainment on cloud-water sedimentation: Impact on global aerosol indirect effect in GISS ModelE3 single column model and global simulations

NASA Astrophysics Data System (ADS)

Ackerman, A. S.; Kelley, M.; Cheng, Y.; Fridlind, A. M.; Del Genio, A. D.; Bauer, S.

2017-12-01

Reduction in cloud-water sedimentation induced by increasing droplet concentrations has been shown in large-eddy simulations (LES) and direct numerical simulation (DNS) to enhance boundary-layer entrainment, thereby reducing cloud liquid water path and offsetting the Twomey effect when the overlying air is sufficiently dry, which is typical. Among recent upgrades to ModelE3, the latest version of the NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM), are a two-moment stratiform cloud microphysics treatment with prognostic precipitation and a moist turbulence scheme that includes an option in its entrainment closure of a simple parameterization for the effect of cloud-water sedimentation. Single column model (SCM) simulations are compared to LES results for a stratocumulus case study and show that invoking the sedimentation-entrainment parameterization option indeed reduces the dependence of cloud liquid water path on increasing aerosol concentrations. Impacts of variations of the SCM configuration and the sedimentation-entrainment parameterization will be explored. Its impact on global aerosol indirect forcing in the framework of idealized atmospheric GCM simulations will also be assessed.

Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

PubMed Central

Jathar, Shantanu H.; Gordon, Timothy D.; Hennigan, Christopher J.; Pye, Havala O. T.; Pouliot, George; Adams, Peter J.; Donahue, Neil M.; Robinson, Allen L.

2014-01-01

Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles, and biomass burning. About 10–20% of NMOG emissions from these major combustion sources are not routinely speciated and therefore are currently misclassified in emission inventories and chemical transport models. The smog chamber data demonstrate that this misclassification biases model predictions of SOA production low because the unspeciated NMOG produce more SOA per unit mass than the speciated NMOG. We present new source-specific SOA yield parameterizations for these unspeciated emissions. These parameterizations and associated source profiles are designed for implementation in chemical transport models. Box model calculations using these new parameterizations predict that NMOG emissions from the top six combustion sources form 0.7 Tg y−1 of first-generation SOA in the United States, almost 90% of which is from biomass burning and gasoline vehicles. About 85% of this SOA comes from unspeciated NMOG, demonstrating that chemical transport models need improved treatment of combustion emissions to accurately predict ambient SOA concentrations. PMID:25002466

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

DOE PAGES

DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.; ...

2014-06-27

Data from both laboratory studies and atmospheric measurements are used to develop a simple parametric description for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RH w) are taken to approximate the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterizationmore » developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A correction factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RH w of 105% vs. maximum fractions active at higher RH w. Instrumental factors that affect activation behavior vs. RH w in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this correction factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization to the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically-relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first order approximation in numerical modeling investigations.« less

Validation of Satellite Aerosol Retrievals from AERONET Ground-Based Measurements

NASA Technical Reports Server (NTRS)

Holben, Brent; Remer, Lorraine; Torres, Omar; Zhao, Tom; Smith, David E. (Technical Monitor)

2001-01-01

Accurate and comprehensive assessment of the parameters that control key atmospheric and biospheric processes including assessment of anthropogenic effects on climate change is a fundamental measurement objective of NASA's EOS program (King and Greenstone, 1999). Satellite assessment programs and associated global climate models require validation and additional parameterization with frequent reliable ground-based observations. A critical and highly uncertain element of the measurement program is characterization of tropospheric aerosols requiring basic observations of aerosols optical and microphysical properties. Unfortunately as yet we do not know the aerosol burden man is contributing to the atmosphere and thus we will have no definitive measure of change for the future. This lack of aerosol assessment is the impetus for some of the EOS measurement activities (Kaufman et al., 1997; King et al., 1999) and the formation of the AERONET program (Holben et al., 1998). The goals of the AERONET program are to develop long term monitoring at globally distributed sites providing critical data for multiannual trend changes in aerosol loading and optical properties with the specific goal of providing a data base for validation of satellite derived aerosol optical properties. The AERONET program has evolved into an international federated network of approximately 100 ground-based remote sensing monitoring stations to characterize the optical and microphysical properties of aerosols.

A new parameterization of the UV irradiance altitude dependence for clear-sky conditions and its application in the on-line UV tool over Northern Eurasia

NASA Astrophysics Data System (ADS)

Chubarova, Nataly; Zhdanova, Yekaterina; Nezval, Yelena

2016-09-01

A new method for calculating the altitude UV dependence is proposed for different types of biologically active UV radiation (erythemally weighted, vitamin-D-weighted and cataract-weighted types). We show that for the specified groups of parameters the altitude UV amplification (AUV) can be presented as a composite of independent contributions of UV amplification from different factors within a wide range of their changes with mean uncertainty of 1 % and standard deviation of 3 % compared with the exact model simulations with the same input parameters. The parameterization takes into account for the altitude dependence of molecular number density, ozone content, aerosol and spatial surface albedo. We also provide generalized altitude dependencies of the parameters for evaluating the AUV. The resulting comparison of the altitude UV effects using the proposed method shows a good agreement with the accurate 8-stream DISORT model simulations with correlation coefficient r > 0.996. A satisfactory agreement was also obtained with the experimental UV data in mountain regions. Using this parameterization we analyzed the role of different geophysical parameters in UV variations with altitude. The decrease in molecular number density, especially at high altitudes, and the increase in surface albedo play the most significant role in the UV growth. Typical aerosol and ozone altitude UV effects do not exceed 10-20 %. Using the proposed parameterization implemented in the on-line UV tool (http://momsu.ru/uv/) for Northern Eurasia over the PEEX domain we analyzed the altitude UV increase and its possible effects on human health considering different skin types and various open body fraction for January and April conditions in the Alpine region.

Assessment of State-of-the-Art Dust Emission Scheme in GEOS

NASA Technical Reports Server (NTRS)

Darmenov, Anton; Liu, Xiaohong; Prigent, Catherine

2017-01-01

The GEOS modeling system has been extended with state of the art parameterization of dust emissions based on the vertical flux formulation described in Kok et al 2014. The new dust scheme was coupled with the GOCART and MAM aerosol models. In the present study we compare dust emissions, aerosol optical depth (AOD) and radiative fluxes from GEOS experiments with the standard and new dust emissions. AOD from the model experiments are also compared with AERONET and satellite based data. Based on this comparative analysis we concluded that the new parameterization improves the GEOS capability to model dust aerosols originating from African sources, however it lead to overestimation of dust emissions from Asian and Arabian sources. Further regional tuning of key parameters controlling the threshold friction velocity may be required in order to achieve more definitive and uniform improvement in the dust modeling skill.

Changes in organic aerosol composition with aging inferred from aerosol mass spectra

NASA Astrophysics Data System (ADS)

Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.; Chhabra, P. S.; Seinfeld, J. H.; Worsnop, D. R.

2011-07-01

Organic aerosols (OA) can be separated with factor analysis of aerosol mass spectrometer (AMS) data into hydrocarbon-like OA (HOA) and oxygenated OA (OOA). We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum). Such parameterization allows for the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups) vs. f43 space ("triangle plot") (Ng et al., 2010) into the Van Krevelen diagram (H:C vs. O:C) (Van Krevelen, 1950). Heald et al. (2010) examined the evolution of total OA in the Van Krevelen diagram. In this work total OA is deconvolved into components that correspond to primary (HOA and others) and secondary (OOA) organic aerosols. By deconvolving total OA into different components, we remove physical mixing effects between secondary and primary aerosols which allows for examination of the evolution of OOA components alone in the Van Krevelen space. This provides a unique means of following ambient secondary OA evolution that is analogous to and can be compared with trends observed in chamber studies of secondary organic aerosol formation. The triangle plot in Ng et al. (2010) indicates that f44 of OOA components increases with photochemical age, suggesting the importance of acid formation in OOA evolution. Once they are transformed with the new parameterization, the triangle plot of the OOA components from all sites occupy an area in Van Krevelen space which follows a ΔH:C/ΔO:C slope of ~ -0.5. This slope suggests that ambient OOA aging results in net changes in chemical composition that are equivalent to the addition of both acid and alcohol/peroxide functional groups without fragmentation (i.e. C-C bond breakage), and/or the addition of acid groups with fragmentation. These results provide a framework for linking the bulk aerosol chemical composition evolution to molecular-level studies.

Assessing the impact of aerosol-atmosphere interactions in convection-permitting regional climate simulations: the Rolf medicane in 2011

NASA Astrophysics Data System (ADS)

José Gómez-Navarro, Juan; María López-Romero, José; Palacios-Peña, Laura; Montávez, Juan Pedro; Jiménez-Guerrero, Pedro

2017-04-01

A critical challenge for assessing regional climate change projections relies on improving the estimate of atmospheric aerosol impact on clouds and reducing the uncertainty associated with the use of parameterizations. In this sense, the horizontal grid spacing implemented in state-of-the-art regional climate simulations is typically 10-25 kilometers, meaning that very important processes such as convective precipitation are smaller than a grid box, and therefore need to be parameterized. This causes large uncertainties, as closure assumptions and a number of parameters have to be established by model tuning. Convection is a physical process that may be strongly conditioned by atmospheric aerosols, although the solution of aerosol-cloud interactions in warm convective clouds remains nowadays a very important scientific challenge, rendering parametrization of these complex processes an important bottleneck that is responsible from a great part of the uncertainty in current climate change projections. Therefore, the explicit simulation of convective processes might improve the quality and reliability of the simulations of the aerosol-cloud interactions in a wide range of atmospheric phenomena. Particularly over the Mediterranean, the role of aerosol particles is very important, being this a crossroad that fuels the mixing of particles from different sources (sea-salt, biomass burning, anthropogenic, Saharan dust, etc). Still, the role of aerosols in extreme events in this area such as medicanes has been barely addressed. This work aims at assessing the role of aerosol-atmosphere interaction in medicanes with the help of the regional chemistry/climate on-line coupled model WRF-CHEM run at a convection-permitting resolution. The analysis is exemplary based on the "Rolf" medicane (6-8 November 2011). Using this case study as reference, four sets of simulations are run with two spatial resolutions: one at a convection-permitting configuration of 4 km, and other at the lower resolution of 12 km, in whose case the convection has to be parameterized. Each configuration is used to produce two simulations, including and not including aerosol-radiation-cloud interactions. The comparison of the simulated output at different scales allows to evaluate the impact of sub-grid scale mixing of precursors on aerosol production. By focusing on these processes at different resolutions, the differences between convection-permitting models running at resolutions of 4 km to 12 km can be explored. Preliminary results indicate that the inclusion of aerosol effects may indeed impact the severity of this simulated medicane, especially sea salt aerosols, and leads to important spatial shifts and differences in intensity of surface precipitation.

Modeling the Complex Photochemistry of Biomass Burning Plumes in Plume-Scale, Regional, and Global Air Quality Models

NASA Astrophysics Data System (ADS)

Alvarado, M. J.; Lonsdale, C. R.; Yokelson, R. J.; Travis, K.; Fischer, E. V.; Lin, J. C.

2014-12-01

Forecasting the impacts of biomass burning (BB) plumes on air quality is difficult due to the complex photochemistry that takes place in the concentrated young BB plumes. The spatial grid of global and regional scale Eulerian models is generally too large to resolve BB photochemistry, which can lead to errors in predicting the formation of secondary organic aerosol (SOA) and O3, as well as the partitioning of NOyspecies. AER's Aerosol Simulation Program (ASP v2.1) can be used within plume-scale Lagrangian models to simulate this complex photochemistry. We will present results of validation studies of the ASP model against aircraft observations of young BB smoke plumes. We will also present initial results from the coupling of ASP v2.1 into the Lagrangian particle dispersion model STILT-Chem in order to better examine the interactions between BB plume chemistry and dispersion. In addition, we have used ASP to develop a sub-grid scale parameterization of the near-source chemistry of BB plumes for use in regional and global air quality models. The parameterization takes inputs from the host model, such as solar zenith angle, temperature, and fire fuel type, and calculates enhancement ratios of O3, NOx, PAN, aerosol nitrate, and other NOy species, as well as organic aerosol (OA). We will present results from the ASP-based BB parameterization as well as its implementation into the global atmospheric composition model GEOS-Chem for the SEAC4RS campaign.

Quantifying the uncertainties of aerosol indirect effects and impacts on decadal-scale climate variability in NCAR CAM5 and CESM1

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

Park, Sungsu

2014-12-12

The main goal of this project is to systematically quantify the major uncertainties of aerosol indirect effects due to the treatment of moist turbulent processes that drive aerosol activation, cloud macrophysics and microphysics in response to anthropogenic aerosol perturbations using the CAM5/CESM1. To achieve this goal, the P.I. hired a postdoctoral research scientist (Dr. Anna Fitch) who started her work from the Nov.1st.2012. In order to achieve the project goal, the first task that the Postdoc. and the P.I. did was to quantify the role of subgrid vertical velocity variance on the activation and nucleation of cloud liquid droplets andmore » ice crystals and its impact on the aerosol indirect effect in CAM5. First, we analyzed various LES cases (from dry stable to cloud-topped PBL) to check whether this isotropic turbulence assumption used in CAM5 is really valid. It turned out that this isotropic turbulence assumption is not universally valid. Consequently, from the analysis of LES, we derived an empirical formulation relaxing the isotropic turbulence assumption used for the CAM5 aerosol activation and ice nucleation, and implemented the empirical formulation into CAM5/CESM1, and tested in the single-column and global simulation modes, and examined how it changed aerosol indirect effects in the CAM5/CESM1. These results were reported in the poster section in the 18th Annual CESM workshop held in Breckenridge, CO during Jun.17-20.2013. While we derived an empirical formulation from the analysis of couple of LES from the first task, the general applicability of that empirical formulation was questionable, because it was obtained from the limited number of LES simulations. The second task we did was to derive a more fundamental analytical formulation relating vertical velocity variance to TKE using other information starting from basic physical principles. This was a somewhat challenging subject, but if this could be done in a successful way, it could be directly implemented into the CAM5 as a practical parameterization, and substantially contributes to achieving the project goal. Through an intensive research for about one year, we found appropriate mathematical formulation and tried to implement it into the CAM5 PBL and activation routine as a practical parameterized numerical code. During these processes, however, the Postdoc applied for another position in Sweden, Europe, and accepted a job offer there, and left NCAR in August 2014. In Sweden, Dr. Anna Fitch is still working on this subject in a part time, planning to finalize the research and to write the paper in a near future.« less

Modeling the formamtion and aging of secondary organic aerosols in Los Angeles during CalNex 2010

EPA Science Inventory

Four different literature parameterizations for the formation and evolution of urban secondary organic aerosol (SOA) frequently used in 3-D models are evaluated using a 0-D box model representing the Los Angeles metropolitan region during the California Research at the Nexus of A...

Linking Global to Regional Models to Assess Future Climate Impacts on Surface Ozone Concentrations in the United States

EPA Science Inventory

The UCD sectional aerosol model has been coupled to the CMAQ air quality model and used to simulate air quality in Tampa, Florida. Sea salt emissions are parameterized as a function of modeled wind speed and relative humidity. Modeled aerosol sulfate, nitrate, ammonium, sodium,...

Statistical analysis and parameterization of the hygroscopic growth of the sub-micrometer urban background aerosol in Beijing

NASA Astrophysics Data System (ADS)

Wang, Yu; Wu, Zhijun; Ma, Nan; Wu, Yusheng; Zeng, Limin; Zhao, Chunsheng; Wiedensohler, Alfred

2018-02-01

The take-up of water of aerosol particles plays an important role in heavy haze formation over North China Plain, since it is related with particle mass concentration, visibility degradation, and particle chemistry. In the present study, we investigated the size-resolved hygroscopic growth factor (HGF) of sub-micrometer aerosol particles (smaller than 350 nm) on a basis of 9-month Hygroscopicity-Tandem Differential Mobility Analyzer measurement in the urban background atmosphere of Beijing. The mean hygroscopicity parameter (κ) values derived from averaging over the entire sampling period for particles of 50 nm, 75 nm, 100 nm, 150 nm, 250 nm, and 350 nm in diameters were 0.14 ± 0.07, 0.17 ± 0.05, 0.18 ± 0.06, 0.20 ± 0.07, 0.21 ± 0.09, and 0.23 ± 0.12, respectively, indicating the dominance of organics in the sub-micrometer urban aerosols. In the spring, summer, and autumn, the number fraction of hydrophilic particles increased with increasing particle size, resulting in an increasing trend of overall particle hygroscopicity with enhanced particle size. Differently, the overall mean κ values peaked in the range of 75-150 nm and decreased for particles larger than 150 nm in diameter during wintertime. Such size-dependency of κ in winter was related to the strong primary particle emissions from coal combustion during domestic heating period. The number fraction of hydrophobic particles such as freshly emitted soot decreased with increasing PM2.5 mass concentration, indicating aged and internal mixed particles were dominant in the severe particulate matter pollution. Parameterization schemes of the HGF as a function of relative humidity (RH) and particle size between 50 and 350 nm were determined for different seasons and pollution levels. The HGFs calculated from the parameterizations agree well with the measured HGFs at 20-90% RH. The parameterizations can be applied to determine the hygroscopic growth of aerosol particles at ambient conditions for the area of Beijing (ultrafine and fine particles) and the North China plain (fine particles).

A simple analytical formula to compute clear sky total and photosynthetically available solar irradiance at the ocean surface

NASA Technical Reports Server (NTRS)

Frouin, Robert; Lingner, David W.; Gautier, Catherine; Baker, Karen S.; Smith, Ray C.

1989-01-01

A simple but accurate analytical formula was developed for computing the total and the photosynthetically available solar irradiances at the ocean surface under clear skies, which takes into account the processes of scattering by molecules and aerosols within the atmosphere and of absorption by the water vapor, ozone, and aerosols. These processes are parameterized as a function of solar zenith angle, aerosol type, atmospheric visibility, and vertically integrated water-vapor and ozone amounts. Comparisons of the calculated and measured total and photosynthetically available solar irradiances for several experiments in tropical and mid-latitude ocean regions show 39 and 14 Wm/sq m rms errors (6.5 and 4.7 percent of the average measured values) on an hourly time scale, respectively. The proposed forumula is unique in its ability to predict surface solar irradiance in the photosynthetically active spectral interval.

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

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

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

2010-02-22

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

Potential of polarization lidar to provide profiles of CCN- and INP-relevant aerosol parameters

NASA Astrophysics Data System (ADS)

Mamouri, R. E.; Ansmann, A.

2015-12-01

We investigate the potential of polarization lidar to provide vertical profiles of aerosol parameters from which cloud condensation nucleus (CCN) and ice nucleating particle (INP) number concentrations can be estimated. We show that height profiles of number concentrations of aerosol particles with radius > 50 nm (APC50, reservoir of favorable CCN) and with radius > 250 nm (APC250, reservoir of favorable INP), as well as profiles of the aerosol particle surface area concentration (ASC, used in INP parameterization) can be retrieved from lidar-derived aerosol extinction coefficients (AEC) with relative uncertainties of a factor of around 2 (APC50), and of about 25-50 % (APC250, ASC). Of key importance is the potential of polarization lidar to identify mineral dust particles and to distinguish and separate the aerosol properties of basic aerosol types such as mineral dust and continental pollution (haze, smoke). We investigate the relationship between AEC and APC50, APC250, and ASC for the main lidar wavelengths of 355, 532 and 1064 nm and main aerosol types (dust, pollution, marine). Our study is based on multiyear Aerosol Robotic Network (AERONET) photometer observations of aerosol optical thickness and column-integrated particle size distribution at Leipzig, Germany, and Limassol, Cyprus, which cover all realistic aerosol mixtures of continental pollution, mineral dust, and marine aerosol. We further include AERONET data from field campaigns in Morocco, Cabo Verde, and Barbados, which provide pure dust and pure marine aerosol scenarios. By means of a simple relationship between APC50 and the CCN-reservoir particles (APCCCN) and published INP parameterization schemes (with APC250 and ASC as input) we finally compute APCCCN and INP concentration profiles. We apply the full methodology to a lidar observation of a heavy dust outbreak crossing Cyprus with dust up to 8 km height and to a case during which anthropogenic pollution dominated.

A study of aerosol indirect effects and feedbacks on convective precipitation

NASA Astrophysics Data System (ADS)

Da Silva, Nicolas; Mailler, Sylvain; Drobinski, Philippe

2017-04-01

Atmospheric aerosols from natural and anthropogenic origin are present in the troposphere of the Mediterranean basin and continental Europe, occasionnally reaching very high concentrations in air masses with a strong content of aerosols related to mineral dust emissions, wildfires, or anthropogenic contamination [1]. On the other hand precipitations in the Mediterranean basin need to be understood precisely since drought and extreme precipitation events are a part of Mediterranean climate which can strongly affect the people and the economic activity in the Mediterranean basin [2]. The present study is a contribution to the investigations on the effects of aerosols on precipitation in the Mediterranean basin and continental Europe. For that purpose, we used the Weather Research and Forecasting Model (WRF) parameterized with the Thompson aerosol-aware microphysics schemes, performing two sensitivity simulations forced with two different aerosol climatologies during six months covering an entire summer season on a domain, covering the Mediterranean basin and continental Europe at 50 km resolution. Aerosols may affect atmospheric dynamics through their direct and semidirect radiative effects as well as through their indirect effects (through the changes of cloud microphysics). While it is difficult to disentangle these differents effects in reality, numerical modelling with the WRF model make it possible to isolate indirect effects by modifying them without affecting the direct or semidirect effects of aerosols in an attempt to examine the effect of aerosols on precipitations through microphysical effects only. Our first results have shown two opposite responses depending whether the precipitation are convective or large-scale. Since convective precipitations seem to be clearly inhibited by increased concentrations of cloud-condensation nuclei, we attempted to understand which processes and feedbacks are involved in this reduction of parameterized convective precipitations when the concentrations of cloud-condensation nuclei are increased. We diagnosed a complex feedback chain beginning from the reduction of mean droplet radii, yielding an increase of atmospheric stability and also lowering the humidity available in the planetary boundary layer for the formation of convective clouds and precipitations. These results suggest that the microphysical effect of aerosols may contribute to a reduction of convective precipitation mostly through modifications in thermodynamic vertical profiles. References [1] G. Rea, S. Turquety, L. Menut, R. Briant, S. Mailler, and G. Siour. Source contributions to 2012 summertime aerosols in the euro-mediterranean region. Atmospheric Chemistry and Physics, 15(14):8013-8036, 2015. [2] F. Giorgi. Climate change hot-spots. Geophysical Research Letters, 33(8): L08707, 2006.

Aerosol optical properties in the southeastern United States in summer - Part 1: Hygroscopic growth

NASA Astrophysics Data System (ADS)

Brock, C. A.; Wagner, N. L.; Anderson, B. E.; Attwood, A. R.; Beyersdorf, A.; Campuzano-Jost, P.; Carlton, A. G.; Day, D. A.; Diskin, G. S.; Gordon, T. D.; Jimenez, J. L.; Lack, D. A.; Liao, J.; Markovic, M. Z.; Middlebrook, A. M.; Ng, N. L.; Perring, A. E.; Richardson, M. S.; Schwarz, J. P.; Washenfelder, R. A.; Welti, A.; Xu, L.; Ziemba, L. D.; Murphy, D. M.

2015-09-01

Aircraft observations of meteorological, trace gas, and aerosol properties were made during May-September 2013 in the southeastern United States (US) under fair-weather, afternoon conditions with well-defined planetary boundary layer structure. Optical extinction at 532 nm was directly measured at three relative humidities and compared with extinction calculated from measurements of aerosol composition and size distribution using the κ-Köhler approximation for hygroscopic growth. Using this approach, the hygroscopicity parameter κ for the organic fraction of the aerosol must have been < 0.10 to be consistent with 75 % of the observations within uncertainties. This subsaturated κ value for the organic aerosol in the southeastern US is consistent with several field studies in rural environments. We present a new parameterization of the change in aerosol extinction as a function of relative humidity that better describes the observations than does the widely used power-law (gamma, γ) parameterization. This new single-parameter κext formulation is based upon κ-Köhler and Mie theories and relies upon the well-known approximately linear relationship between particle volume (or mass) and optical extinction (Charlson et al., 1967). The fitted parameter, κext, is nonlinearly related to the chemically derived κ parameter used in κ-Köhler theory. The values of κext we determined from airborne measurements are consistent with independent observations at a nearby ground site.

New insights into modeling an organic mass fraction of sea spray aerosol

NASA Astrophysics Data System (ADS)

Meskhidze, N.; Gantt, B.

2010-12-01

As the study of climate change progresses, a need to separate the effects of natural and anthropogenic processes becomes essential in order to correctly forecast the future climate. Due to their massive source regions underlying an atmosphere with low aerosol concentration, marine aerosols derived from sea spray and ocean emitted biogenic volatile organic compounds (BVOCs) are extremely important for the Earth’s radiative budget, regional air quality and biogeochemical cycling of elements. Measurements of freshly-emitted sea spray have revealed that bubble bursting processes, largely responsible for the production of sea salt aerosol, also control sea-to-air transfer of marine organic matter. It has been established that the organic mass fraction of sea spray can be a function of sea-water composition (e.g., concentrations of Chlorophyll-a, [Chl-a], dissolved organic carbon, [DOC], particulate organic carbon, [POC], types of organic carbon, and the amount of surfactants). Current paramaterizations of marine primary organic aerosol emissions use remotely sensed [Chl-a] data as a proxy for oceanic biological activity. However, it has also been shown that the path length, size, and lifetime of bubbles in seawater as well as spatial coverage of seawater surface by streaks or slicks (visible film of a roughly 50 μm thick layer, highly enriched in organics) can have dramatic effect on organic mass fraction of sea spray (OCss). Dynamics of bubble entrainment and the level of microlayer enrichment by organics relative to the underlying bulk water can be controlled by surface wind speed. For bubble entrainment, high winds can increase rising bubble path length and therefore the amount of organics scavenged by the bubble. However, when the surface wind speeds exceed 8 m s-1 breaking of ocean waves can entirely destroy surface organic films and diminish the amount of organics leaving the sea. Despite the probable impact of wind speed, existing parameterizations do not consider the wind speed dependence of OCss. In this study we use remotely sensed data for ocean slick coverage and surface wind speed in conjunction with an upwind averaged concentrations of [Chl-a], [DOC] and [POC] to derive marine primary organic aerosol emission function. Derived empirical relationships between the aerosol and ocean/meteorological data are then compared to observed OCss at Mace Head and Point Reyes National Seashore. MATLAB curve fitting tool revealed that multi-variable regression analysis (with both wind speed and [Chl-a]) yields a significant improvement between model predicted and observed submicron fraction of OCss. The coefficient of determination increased from R2=0.1 for previous parameterizations to R2=0.6. Based on the results of this study we propose that in addition to sea-water composition, future parameterizations of marine primary organic aerosol emissions should include sea spray organic mass fraction dependence on surface wind speed.

Optical Extinction and Aerosol Hygroscopicity in the Southeastern United States

NASA Astrophysics Data System (ADS)

Brock, C. A.; Gordon, T.; Wagner, N.; Lack, D. A.; Richardson, M.; Middlebrook, A. M.; Liao, J.; Murphy, D. M.; Attwood, A. R.; Washenfelder, R. A.; Campuzano Jost, P.; Day, D. A.; Jimenez, J. L.; Carlton, A. M. G.

2015-12-01

Most aerosol particles take up water and grow as relative humidity increases, leading to increased optical extinction, reduced visibility, greater aerosol optical depths (AODs), and altered radiative forcing, even while dry particulate mass remains constant. Relative humidity varies greatly temporally, horizontally, and especially vertically. Thus hygroscopicity is a confounding factor when attempting to link satellite-based observations of AOD to surface measurements of particulate mass or to model predictions of aerosol mass concentrations. Airborne observations of aerosol optical, chemical, and microphysical properties were made in the southeastern United States in the daytime in summer 2013 during the NOAA SENEX and NASA SEAC4RS projects. Applying κ-Köhler theory for hygroscopic growth to these data, the inferred hygroscopicity parameter κ for the organic fraction of the aerosol was <0.11. This κ for organics is toward the lower end of values found from laboratory studies of the aerosol formed from oxidation of biogenic precursors and from several field studies in rural environments. The gamma (γ) parameterization is commonly used to describe the change in aerosol extinction as a function of relative humidity. Because this formulation did not fit the airborne data well, a new parameterization was developed that better describes the observations. This new single-parameter κext formulation is physically based and relies upon the well-known approximately linear relationship between particle volume and optical extinction. The fitted parameter, κext, is nonlinearly related to the chemically derived κ parameter used in κ-Köhler theory. The values of κext determined from the airborne measurements are consistent with independent observations at a nearby ground site.

The Radiative Forcing Model Intercomparison Project (RFMIP): Experimental protocol for CMIP6

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

Pincus, Robert; Forster, Piers M.; Stevens, Bjorn

The phrasing of the first of three questions motivating CMIP6 – “How does the Earth system respond to forcing?” – suggests that forcing is always well-known, yet the radiative forcing to which this question refers has historically been uncertain in coordinated experiments even as understanding of how best to infer radiative forcing has evolved. The Radiative Forcing Model Intercomparison Project (RFMIP) endorsed by CMIP6 seeks to provide a foundation for answering the question through three related activities: (i) accurate characterization of the effective radiative forcing relative to a near-preindustrial baseline and careful diagnosis of the components of this forcing; (ii) assessment ofmore » the absolute accuracy of clear-sky radiative transfer parameterizations against reference models on the global scales relevant for climate modeling; and (iii) identification of robust model responses to tightly specified aerosol radiative forcing from 1850 to present. Complete characterization of effective radiative forcing can be accomplished with 180 years (Tier 1) of atmosphere-only simulation using a sea-surface temperature and sea ice concentration climatology derived from the host model's preindustrial control simulation. Assessment of parameterization error requires trivial amounts of computation but the development of small amounts of infrastructure: new, spectrally detailed diagnostic output requested as two snapshots at present-day and preindustrial conditions, and results from the model's radiation code applied to specified atmospheric conditions. In conclusion, the search for robust responses to aerosol changes relies on the CMIP6 specification of anthropogenic aerosol properties; models using this specification can contribute to RFMIP with no additional simulation, while those using a full aerosol model are requested to perform at least one and up to four 165-year coupled ocean–atmosphere simulations at Tier 1.« less

The Radiative Forcing Model Intercomparison Project (RFMIP): Experimental protocol for CMIP6

DOE PAGES

Pincus, Robert; Forster, Piers M.; Stevens, Bjorn

2016-09-27

The phrasing of the first of three questions motivating CMIP6 – “How does the Earth system respond to forcing?” – suggests that forcing is always well-known, yet the radiative forcing to which this question refers has historically been uncertain in coordinated experiments even as understanding of how best to infer radiative forcing has evolved. The Radiative Forcing Model Intercomparison Project (RFMIP) endorsed by CMIP6 seeks to provide a foundation for answering the question through three related activities: (i) accurate characterization of the effective radiative forcing relative to a near-preindustrial baseline and careful diagnosis of the components of this forcing; (ii) assessment ofmore » the absolute accuracy of clear-sky radiative transfer parameterizations against reference models on the global scales relevant for climate modeling; and (iii) identification of robust model responses to tightly specified aerosol radiative forcing from 1850 to present. Complete characterization of effective radiative forcing can be accomplished with 180 years (Tier 1) of atmosphere-only simulation using a sea-surface temperature and sea ice concentration climatology derived from the host model's preindustrial control simulation. Assessment of parameterization error requires trivial amounts of computation but the development of small amounts of infrastructure: new, spectrally detailed diagnostic output requested as two snapshots at present-day and preindustrial conditions, and results from the model's radiation code applied to specified atmospheric conditions. In conclusion, the search for robust responses to aerosol changes relies on the CMIP6 specification of anthropogenic aerosol properties; models using this specification can contribute to RFMIP with no additional simulation, while those using a full aerosol model are requested to perform at least one and up to four 165-year coupled ocean–atmosphere simulations at Tier 1.« less

Synthesis and Surface-Specific Analysis of Molecular Constituents Relevant to Biogenic Secondary Organic Aerosol Material

NASA Astrophysics Data System (ADS)

Be, A. G.; Upshur, M. A.; Chase, H. M.; Geiger, F.; Thomson, R. J.

2017-12-01

Secondary organic aerosol (SOA) particles formed from the oxidation of biogenic volatile organic compounds (BVOCs) remain a principal, yet elusive, class of airborne particulate matter that impacts the Earth's radiation budget. Given the characteristic molecular complexity comprising biogenic SOA particles, chemical information selective to the gas-aerosol interface may be valuable in the investigation of such systems, as surface considerations likely dictate the phenomena driving particle evolution mechanisms and climate effects. In particular, cloud activation processes may be parameterized using the surface tension depression that coincides with partitioning of surface-active organic species to the gas-droplet interface. However, the extent to which surface chemical processes, such as cloud droplet condensation, are influenced by the chemical structure and reactivity of individual surface-active molecules in SOA particles is largely unknown. We seek to study terpene-derived organic species relevant to the surfaces of biogenic SOA particles via synthesis of putative oxidation products followed by analysis using surface-selective physicochemical measurements. Using dynamic surface tension measurements, considerable differences are observed in the surface tension depression of aqueous pendant droplets that contain synthetically prepared ozonolysis products derived from abundant terpene precursors. Furthermore, sum frequency generation spectroscopy is utilized for comparison of the surface vibrational spectral responses of synthesized reference compounds with those observed for laboratory aerosol toward probing the surface composition of SOA material. Such ongoing findings highlight the underlying importance of molecular structure and reactivity when considering the surface chemistry of biogenic terpene-derived atmospheric aerosols.

An Investigation of the Radiative Effects and Climate Feedbacks of Sea Ice Sources of Sea Salt Aerosol

NASA Astrophysics Data System (ADS)

Horowitz, H. M.; Alexander, B.; Bitz, C. M.; Jaegle, L.; Burrows, S. M.

2017-12-01

In polar regions, sea ice is a major source of sea salt aerosol through lofting of saline frost flowers or blowing saline snow from the sea ice surface. Under continued climate warming, an ice-free Arctic in summer with only first-year, more saline sea ice in winter is likely. Previous work has focused on climate impacts in summer from increasing open ocean sea salt aerosol emissions following complete sea ice loss in the Arctic, with conflicting results suggesting no net radiative effect or a negative climate feedback resulting from a strong first aerosol indirect effect. However, the radiative forcing from changes to the sea ice sources of sea salt aerosol in a future, warmer climate has not previously been explored. Understanding how sea ice loss affects the Arctic climate system requires investigating both open-ocean and sea ice sources of sea-salt aerosol and their potential interactions. Here, we implement a blowing snow source of sea salt aerosol into the Community Earth System Model (CESM) dynamically coupled to the latest version of the Los Alamos sea ice model (CICE5). Snow salinity is a key parameter affecting blowing snow sea salt emissions and previous work has assumed constant regional snow salinity over sea ice. We develop a parameterization for dynamic snow salinity in the sea ice model and examine how its spatial and temporal variability impacts the production of sea salt from blowing snow. We evaluate and constrain the snow salinity parameterization using available observations. Present-day coupled CESM-CICE5 simulations of sea salt aerosol concentrations including sea ice sources are evaluated against in situ and satellite (CALIOP) observations in polar regions. We then quantify the present-day radiative forcing from the addition of blowing snow sea salt aerosol with respect to aerosol-radiation and aerosol-cloud interactions. The relative contributions of sea ice vs. open ocean sources of sea salt aerosol to radiative forcing in polar regions is discussed.

Sensitivity of aerosol indirect forcing and autoconversion to cloud droplet parameterization: an assessment with the NASA Global Modeling Initiative.

NASA Astrophysics Data System (ADS)

Sotiropoulou, R. P.; Meshkhidze, N.; Nenes, A.

2006-12-01

The aerosol indirect forcing is one of the largest sources of uncertainty in assessments of anthropogenic climate change [IPCC, 2001]. Much of this uncertainty arises from the approach used for linking cloud droplet number concentration (CDNC) to precursor aerosol. Global Climate Models (GCM) use a wide range of cloud droplet activation mechanisms ranging from empirical [Boucher and Lohmann, 1995] to detailed physically- based formulations [e.g., Abdul-Razzak and Ghan, 2000; Fountoukis and Nenes, 2005]. The objective of this study is to assess the uncertainties in indirect forcing and autoconversion of cloud water to rain caused by the application of different cloud droplet parameterization mechanisms; this is an important step towards constraining the aerosol indirect effects (AIE). Here we estimate the uncertainty in indirect forcing and autoconversion rate using the NASA Global Model Initiative (GMI). The GMI allows easy interchange of meteorological fields, chemical mechanisms and the aerosol microphysical packages. Therefore, it is an ideal tool for assessing the effect of different parameters on aerosol indirect forcing. The aerosol module includes primary emissions, chemical production of sulfate in clear air and in-cloud aqueous phase, gravitational sedimentation, dry deposition, wet scavenging in and below clouds, and hygroscopic growth. Model inputs include SO2 (fossil fuel and natural), black carbon (BC), organic carbon (OC), mineral dust and sea salt. The meteorological data used in this work were taken from the NASA Data Assimilation Office (DAO) and two different GCMs: the NASA GEOS4 finite volume GCM (FVGCM) and the Goddard Institute for Space Studies version II' (GISS II') GCM. Simulations were carried out for "present day" and "preindustrial" emissions using different meteorological fields (i.e. DAO, FVGCM, GISS II'); cloud droplet number concentration is computed from the correlations of Boucher and Lohmann [1995], Abdul-Razzak and Ghan [2000], Feingold and Heymsfield [1992], Fountoukis and Nenes [2005] and Segal and Khain [2006]. Computed CDNC is used to calculate the cloud optical depth, the autoconversion rate and the mean top-of-the-atmosphere (TOA) short-wave radiative forcing using modified FAST-J algorithm [Meshkhidze et al., 2006]. Autoconversion of cloud water to precipitation is parameterized following the formulation of Khairoutdinov and Kogan [2000]. References Abdul-Razzak, H., and S. J. Ghan (2000), J. Geophys. Res., 105, 6837-6844. Boucher, O., and U. Lohmann (1995), Tellus, Ser. B, 47, 281- 300. Feingold, G. and A. Heymsfield (1992), J. Atmos. Sci., 49, 2325-2342. Fountoukis, C., and A. Nenes (2005), J. Geophys. Res., 110, D11212, doi:10.1029/ 2004JD005591. Intergovernmental Panel on Climate Change - IPCC (2001), Climate Change, The Scientific Basis, Cambridge University Press, UK. Khairoutdinov, M. and Y. Kogan (2000), Mon. Weather Rev., 128 (1), 229-243. Meshkhidze, N., A Nenes, J. Kouatchou, B. Das and J. Rodriguez, 7th International Aerosol Conference, American Association for Aerosol Research (IAC 2006), St. Paul, Minnesota, October 2006 Nenes, A., and J. H. Seinfeld (2003), J. Geophys. Res., 108, 4415, doi:10.1029/ 2002JD002911. Segal, Y., and A. Khain (2006), J. Geophys. Res., 111, D15204, doi:10.1029/2005JD006561.

Representation of Nucleation Mode Microphysics in a Global Aerosol Model with Sectional Microphysics

NASA Technical Reports Server (NTRS)

Lee, Y. H.; Pierce, J. R.; Adams, P. J.

2013-01-01

In models, nucleation mode (1 nm

Ensemble projections of wildfire activity and carbonaceous aerosol concentrations over the western United States in the mid-21st century

PubMed Central

Yue, Xu; Mickley, Loretta J.; Logan, Jennifer A.; Kaplan, Jed O.

2013-01-01

We estimate future wildfire activity over the western United States during the mid-21st century (2046–2065), based on results from 15 climate models following the A1B scenario. We develop fire prediction models by regressing meteorological variables from the current and previous years together with fire indexes onto observed regional area burned. The regressions explain 0.25–0.60 of the variance in observed annual area burned during 1980–2004, depending on the ecoregion. We also parameterize daily area burned with temperature, precipitation, and relative humidity. This approach explains ~0.5 of the variance in observed area burned over forest ecoregions but shows no predictive capability in the semi-arid regions of Nevada and California. By applying the meteorological fields from 15 climate models to our fire prediction models, we quantify the robustness of our wildfire projections at mid-century. We calculate increases of 24–124% in area burned using regressions and 63–169% with the parameterization. Our projections are most robust in the southwestern desert, where all GCMs predict significant (p<0.05) meteorological changes. For forested ecoregions, more GCMs predict significant increases in future area burned with the parameterization than with the regressions, because the latter approach is sensitive to hydrological variables that show large inter-model variability in the climate projections. The parameterization predicts that the fire season lengthens by 23 days in the warmer and drier climate at mid-century. Using a chemical transport model, we find that wildfire emissions will increase summertime surface organic carbon aerosol over the western United States by 46–70% and black carbon by 20–27% at midcentury, relative to the present day. The pollution is most enhanced during extreme episodes: above the 84th percentile of concentrations, OC increases by ~90% and BC by ~50%, while visibility decreases from 130 km to 100 km in 32 Federal Class 1 areas in Rocky Mountains Forest. PMID:24015109

Influence of Convection and Aerosol Pollution on Ice Cloud Particle Effective Radius

NASA Technical Reports Server (NTRS)

Jiang, J. H.; Su, H.; Zhai, C.; Massie, S. T.; Schoeberl, M. R.; Colarco, P. R.; Platnick, S.; Gu, Y.; Liou, K.-N.

2011-01-01

Satellite observations show that ice cloud effective radius (r(sub e)) increases with ice water content (IWC) but decreases with aerosol optical thickness (AOT). Using least-squares fitting to the observed data, we obtain an analytical formula to describe the variations of r(sub e) with IWC and AOT for several regions with distinct characteristics of r(sub e) -IWC-AOT relationships. As IWC directly relates to convective strength and AOT represents aerosol loading, our empirical formula provides a means to quantify the relative roles of dynamics and aerosols in controlling r(sub e) in different geographical regions, and to establish a framework for parameterization of aerosol effects on r(sub e) in climate models.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores: OPTICAL AND CHEMICAL PROPERTIES OF BROWN CARBON AEROSOLS

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

Bluvshtein, Nir; Lin, Peng; Flores, J. Michel

The radiative effects of biomass burning aerosols on regional and global scale is substantial. Accurate modeling of the radiative effects of smoke aerosols require wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass burning aerosols between 300 and 650 nm wavelength during a regional bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about two orders ofmore » magnitude, changing the size-weighted single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and aged biomass burning aerosols. In addition, PM2.5 filter samples were collected for detailed off-line chemical analysis of the water soluble organics that contribute to light absorption. Nitrophenols were identified as the main organic species responsible for the increased absorption at 400-500 nm. These include species such as 4- nitrocatechol, 4-nitrophenol, nitro-syringol and nitro-guaiacol; oxidation-nitration products of methoxyphenols, known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosol from biomass burning in absorption of solar radiation and in effective radiative forcing.« less

Global direct radiative forcing by process-parameterized aerosol optical properties

NASA Astrophysics Data System (ADS)

KirkevâG, Alf; Iversen, Trond

2002-10-01

A parameterization of aerosol optical parameters is developed and implemented in an extended version of the community climate model version 3.2 (CCM3) of the U.S. National Center for Atmospheric Research. Direct radiative forcing (DRF) by monthly averaged calculated concentrations of non-sea-salt sulfate and black carbon (BC) is estimated. Inputs are production-specific BC and sulfate from [2002] and background aerosol size distribution and composition. The scheme interpolates between tabulated values to obtain the aerosol single scattering albedo, asymmetry factor, extinction coefficient, and specific extinction coefficient. The tables are constructed by full calculations of optical properties for an array of aerosol input values, for which size-distributed aerosol properties are estimated from theory for condensation and Brownian coagulation, assumed distribution of cloud-droplet residuals from aqueous phase oxidation, and prescribed properties of the background aerosols. Humidity swelling is estimated from the Köhler equation, and Mie calculations finally yield spectrally resolved aerosol optical parameters for 13 solar bands. The scheme is shown to give excellent agreement with nonparameterized DRF calculations for a wide range of situations. Using IPCC emission scenarios for the years 2000 and 2100, calculations with an atmospheric global cliamte model (AFCM) yield a global net anthropogenic DRF of -0.11 and 0.11 W m-2, respectively, when 90% of BC from biomass burning is assumed anthropogenic. In the 2000 scenario, the individual DRF due to sulfate and BC has separately been estimated to -0.29 and 0.19 W m-2, respectively. Our estimates of DRF by BC per BC mass burden are lower than earlier published estimates. Some sensitivity tests are included to investigate to what extent uncertain assumptions may influence these results.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores

NASA Astrophysics Data System (ADS)

Bluvshtein, Nir; Lin, Peng; Flores, J. Michel; Segev, Lior; Mazar, Yinon; Tas, Eran; Snider, Graydon; Weagle, Crystal; Brown, Steven S.; Laskin, Alexander; Rudich, Yinon

2017-05-01

The radiative effects of biomass-burning aerosols on regional and global scales can be substantial. Accurate modeling of the radiative effects of smoke aerosols requires wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass-burning aerosols from 300 to 650 nm wavelengths during a regional nighttime bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about 2 orders of magnitude, changing the single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and slightly aged biomass-burning aerosols. In addition, PM2.5 filter samples were collected for detailed offline chemical analysis of the water-soluble organics that contribute to light absorption. Nitroaromatics were identified as major organic species responsible for the increased absorption at 400 to 500 nm. Typical chromophores include 4-nitrocatechol, 4-nitrophenol, nitrosyringol, and nitroguaiacol; oxidation-nitration products of methoxyphenols; and known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosols from biomass burning in absorption of solar radiation and in effective radiative forcing.

Aerosol-cloud interactions in a multi-scale modeling framework

NASA Astrophysics Data System (ADS)

Lin, G.; Ghan, S. J.

2017-12-01

Atmospheric aerosols play an important role in changing the Earth's climate through scattering/absorbing solar and terrestrial radiation and interacting with clouds. However, quantification of the aerosol effects remains one of the most uncertain aspects of current and future climate projection. Much of the uncertainty results from the multi-scale nature of aerosol-cloud interactions, which is very challenging to represent in traditional global climate models (GCMs). In contrast, the multi-scale modeling framework (MMF) provides a viable solution, which explicitly resolves the cloud/precipitation in the cloud resolved model (CRM) embedded in the GCM grid column. In the MMF version of community atmospheric model version 5 (CAM5), aerosol processes are treated with a parameterization, called the Explicit Clouds Parameterized Pollutants (ECPP). It uses the cloud/precipitation statistics derived from the CRM to treat the cloud processing of aerosols on the GCM grid. However, this treatment treats clouds on the CRM grid but aerosols on the GCM grid, which is inconsistent with the reality that cloud-aerosol interactions occur on the cloud scale. To overcome the limitation, here, we propose a new aerosol treatment in the MMF: Explicit Clouds Explicit Aerosols (ECEP), in which we resolve both clouds and aerosols explicitly on the CRM grid. We first applied the MMF with ECPP to the Accelerated Climate Modeling for Energy (ACME) model to have an MMF version of ACME. Further, we also developed an alternative version of ACME-MMF with ECEP. Based on these two models, we have conducted two simulations: one with the ECPP and the other with ECEP. Preliminary results showed that the ECEP simulations tend to predict higher aerosol concentrations than ECPP simulations, because of the more efficient vertical transport from the surface to the higher atmosphere but the less efficient wet removal. We also found that the cloud droplet number concentrations are also different between the two simulations due to the difference in the cloud droplet lifetime. Next, we will explore how the ECEP treatment affects the anthropogenic aerosol forcing, particularly the aerosol indirect forcing, by comparing present-day and pre-industrial simulations.

Laboratory Studies of the Cloud Droplet Activation Properties and Corresponding Chemistry of Saline Playa Dust.

PubMed

Gaston, Cassandra J; Pratt, Kerri A; Suski, Kaitlyn J; May, Nathaniel W; Gill, Thomas E; Prather, Kimberly A

2017-02-07

Playas emit large quantities of dust that can facilitate the activation of cloud droplets. Despite the potential importance of playa dusts for cloud formation, most climate models assume that all dust is nonhygroscopic; however, measurements are needed to clarify the role of dusts in aerosol-cloud interactions. Here, we report measurements of CCN activation from playa dusts and parameterize these results in terms of both κ-Köhler theory and adsorption activation theory for inclusion in atmospheric models. κ ranged from 0.002 ± 0.001 to 0.818 ± 0.094, whereas Frankel-Halsey-Hill (FHH) adsorption parameters of A FHH = 2.20 ± 0.60 and B FHH = 1.24 ± 0.14 described the water uptake properties of the dusts. Measurements made using aerosol time-of-flight mass spectrometry (ATOFMS) revealed the presence of halite, sodium sulfates, and sodium carbonates that were strongly correlated with κ underscoring the role that mineralogy, including salts, plays in water uptake by dust. Predictions of κ made using bulk chemical techniques generally showed good agreement with measured values. However, several samples were poorly predicted suggesting that chemical heterogeneities as a function of size or chemically distinct particle surfaces can determine the hygroscopicity of playa dusts. Our results further demonstrate the importance of dust in aerosol-cloud interactions.

The Grell-Freitas Convection Parameterization: Recent Developments and Applications Within the NASA GEOS Global Model

NASA Technical Reports Server (NTRS)

Freitas, Saulo R.; Grell, Georg; Molod, Andrea; Thompson, Matthew A.

2017-01-01

We implemented and began to evaluate an alternative convection parameterization for the NASA Goddard Earth Observing System (GEOS) global model. The parameterization is based on the mass flux approach with several closures, for equilibrium and non-equilibrium convection, and includes scale and aerosol awareness functionalities. Recently, the scheme has been extended to a tri-modal spectral size approach to simulate the transition from shallow, mid, and deep convection regimes. In addition, the inclusion of a new closure for non-equilibrium convection resulted in a substantial gain of realism in model simulation of the diurnal cycle of convection over the land. Here, we briefly introduce the recent developments, implementation, and preliminary results of this parameterization in the NASA GEOS modeling system.

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.

Implementation of a Brown Carbon Parameterization in the Community Earth System Model (CESM): Model Validation, Estimation of Brown Carbon Radiative Effect, and Climate Impact

NASA Astrophysics Data System (ADS)

Brown, Hunter Y.

A recent development in the representation of aerosols in climate models is the realization that some components of organic carbon (OC), emitted from biomass and biofuel burning, can have a significant contribution to short-wave radiation absorption in the atmosphere. The absorbing fraction of OC is referred to as brown carbon (BrC). This study introduces one of the first implementations of BrC into the Community Earth System Model (CESM), using a parameterization for BrC absorption described in Saleh et al. (2014). 9-year experiments are run (2003-2011) with prescribed emissions and sea surface temperatures to analyze the effect of BrC in the atmosphere. Model validation is conducted via model comparison to single-scatter albedo (SSA) and aerosol optical depth from the Aerosol Robotic Network (AERONET), as well as comparison with a laboratory derived parameterization for SSA dependent on the (black carbon (BC))/(BC+OC) ratio in biomass burning emissions. These comparisons reveal a model underestimation of SSA in biomass burning regions for both default and BrC model runs. Global annual average radiative effects are calculated due to aerosol-radiation interactions (REari; 0.13+/-0.021 W m -2), aerosol-cloud interactions (REaci; 0.07+/-0.056 W m -2), and surface albedo change (REsac; -0.06+/-0.035 W m -2). REari is similar to other studies' estimations of BrC direct radiative effect, while REaci indicates a global reduction in low clouds due to the BrC semi-direct effect. REsac suggests increased surface albedo with BrC implementation due to modified snowfall, but does not take into account the warming effect of BrC on snow. Lastly, comparisons of BrC implementation approaches find that this implementation may do a better job of estimating BrC radiative effect in the Arctic regions than previous studies with CESM.

Potential sea salt aerosol sources from frost flowers in the pan-Arctic region

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

Xu, Li; Russell, Lynn M.; Burrows, Susannah M.

In order to better represent observed wintertime aerosol concentrations at Barrow, Alaska, we implemented an observationally-based parameterization for estimating sea salt production from frost flowers in the Community Earth System Model (CESM). In this work, we evaluate the potential influence of this sea salt source on the pan-Arctic (60ºN-90ºN) climate. Results show that frost flower salt emissions substantially increase the modeled surface sea salt aerosol concentration in the winter months when new sea ice and frost flowers are present. The parameterization reproduces both the magnitude and seasonal variation of the observed submicron sea salt aerosol concentration at surface in Barrowmore » during winter much better than the standard CESM simulation without a frost-flower salt particle source. Adding these frost flower salt particle emissions increases aerosol optical depth by 10% and results in a small cooling at surface. The increase in salt particle mass concentrations of a factor of 8 provides nearly two times the cloud condensation nuclei concentration, as well as 10% increases in cloud droplet number and 40% increases in liquid water content near coastal regions adjacent to continents. These cloud changes reduce longwave cloud forcing by 3% and cause a small surface warming, increasing the downward longwave flux at the surface by 2 W m-2 in the pan-Arctic under the present-day climate.« less

A Solar Radiation Parameterization for Atmospheric Studies. Volume 15

NASA Technical Reports Server (NTRS)

Chou, Ming-Dah; Suarez, Max J. (Editor)

1999-01-01

The solar radiation parameterization (CLIRAD-SW) developed at the Goddard Climate and Radiation Branch for application to atmospheric models are described. It includes the absorption by water vapor, O3, O2, CO2, clouds, and aerosols and the scattering by clouds, aerosols, and gases. Depending upon the nature of absorption, different approaches are applied to different absorbers. In the ultraviolet and visible regions, the spectrum is divided into 8 bands, and single O3 absorption coefficient and Rayleigh scattering coefficient are used for each band. In the infrared, the spectrum is divided into 3 bands, and the k-distribution method is applied for water vapor absorption. The flux reduction due to O2 is derived from a simple function, while the flux reduction due to CO2 is derived from precomputed tables. Cloud single-scattering properties are parameterized, separately for liquid drops and ice, as functions of water amount and effective particle size. A maximum-random approximation is adopted for the overlapping of clouds at different heights. Fluxes are computed using the Delta-Eddington approximation.

The Grell-Freitas Convective Parameterization: Recent Developments and Applications Within the NASA GEOS Global Model

NASA Astrophysics Data System (ADS)

Freitas, S.; Grell, G. A.; Molod, A.

2017-12-01

We implemented and began to evaluate an alternative convection parameterization for the NASA Goddard Earth Observing System (GEOS) global model. The parameterization (Grell and Freitas, 2014) is based on the mass flux approach with several closures, for equilibrium and non-equilibrium convection, and includes scale and aerosol awareness functionalities. Scale dependence for deep convection is implemented either through using the method described by Arakawa et al (2011), or through lateral spreading of the subsidence terms. Aerosol effects are included though the dependence of autoconversion and evaporation on the CCN number concentration.Recently, the scheme has been extended to a tri-modal spectral size approach to simulate the transition from shallow, congestus, and deep convection regimes. In addition, the inclusion of a new closure for non-equilibrium convection resulted in a substantial gain of realism in model simulation of the diurnal cycle of convection over the land. Also, a beta-pdf is employed now to represent the normalized mass flux profile. This opens up an additional venue to apply stochasticism in the scheme.

Evaluation of Simulated Marine Aerosol Production Using the WaveWatchIII Prognostic Wave Model Coupled to the Community Atmosphere Model within the Community Earth System Model

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

Long, M. S.; Keene, William C.; Zhang, J.

2016-11-08

Primary marine aerosol (PMA) is emitted into the atmosphere via breaking wind waves on the ocean surface. Most parameterizations of PMA emissions use 10-meter wind speed as a proxy for wave action. This investigation coupled the 3 rd generation prognostic WAVEWATCH-III wind-wave model within a coupled Earth system model (ESM) to drive PMA production using wave energy dissipation rate – analogous to whitecapping – in place of 10-meter wind speed. The wind speed parameterization did not capture basin-scale variability in relations between wind and wave fields. Overall, the wave parameterization did not improve comparison between simulated versus measured AOD ormore » Na +, thus highlighting large remaining uncertainties in model physics. Results confirm the efficacy of prognostic wind-wave models for air-sea exchange studies coupled with laboratory- and field-based characterizations of the primary physical drivers of PMA production. No discernible correlations were evident between simulated PMA fields and observed chlorophyll or sea surface temperature.« less

Sensitivity study of cloud parameterizations with relative dispersion in CAM5.1: impacts on aerosol indirect effects

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

Xie, Xiaoning; Zhang, He; Liu, Xiaodong

Aerosol-induced increase of relative dispersion of cloud droplet size distribution ε exerts a warming effect and partly offsets the cooling of aerosol indirect radiative forcing (AIF) associated with increased droplet concentration by increasing the cloud droplet effective radius ( R e) and enhancing the cloud-to-rain autoconversion rate (Au) (labeled aBut, the total dispersion effects on both R e and Au are not fully considered in most GCMs, especially in different versions of the Community Atmospheric Model (CAM). Furthermore, in order to accurately evaluate the dispersion effect on AIF, the new complete cloud parameterizations of R e and Au explicitly accountingmore » for ε are implemented into the CAM version 5.1 (CAM5.1), and a suite of sensitivity experiments is conducted with different representations of ε reported in the literature. It is shown that the shortwave cloud radiative forcing is much better simulated with the new cloud parameterizations as compared to the standard scheme in CAM5.1, whereas the influences on longwave cloud radiative forcing and surface precipitation are minimal. In addition, consideration of the dispersion effect can significantly reduce the changes induced by anthropogenic aerosols in the cloud-top effective radius and the liquid water path, especially in the Northern Hemisphere. The corresponding AIF with the dispersion effect considered can also be reduced substantially by a range of 0.10 to 0.21 W m -2 at the global scale and by a much bigger margin of 0.25 to 0.39 W m -2 for the Northern Hemisphere in comparison with that of fixed relative dispersion, mainly dependent on the change of relative dispersion and droplet concentrations (Δε/ΔN).« less

Sensitivity study of cloud parameterizations with relative dispersion in CAM5.1: impacts on aerosol indirect effects

NASA Astrophysics Data System (ADS)

Xie, Xiaoning; Zhang, He; Liu, Xiaodong; Peng, Yiran; Liu, Yangang

2017-05-01

Aerosol-induced increase of relative dispersion of cloud droplet size distribution ɛ exerts a warming effect and partly offsets the cooling of aerosol indirect radiative forcing (AIF) associated with increased droplet concentration by increasing the cloud droplet effective radius (Re) and enhancing the cloud-to-rain autoconversion rate (Au) (labeled as the dispersion effect), which can help reconcile global climate models (GCMs) with the satellite observations. However, the total dispersion effects on both Re and Au are not fully considered in most GCMs, especially in different versions of the Community Atmospheric Model (CAM). In order to accurately evaluate the dispersion effect on AIF, the new complete cloud parameterizations of Re and Au explicitly accounting for ɛ are implemented into the CAM version 5.1 (CAM5.1), and a suite of sensitivity experiments is conducted with different representations of ɛ reported in the literature. It is shown that the shortwave cloud radiative forcing is much better simulated with the new cloud parameterizations as compared to the standard scheme in CAM5.1, whereas the influences on longwave cloud radiative forcing and surface precipitation are minimal. Additionally, consideration of the dispersion effect can significantly reduce the changes induced by anthropogenic aerosols in the cloud-top effective radius and the liquid water path, especially in the Northern Hemisphere. The corresponding AIF with the dispersion effect considered can also be reduced substantially by a range of 0.10 to 0.21 W m-2 at the global scale and by a much bigger margin of 0.25 to 0.39 W m-2 for the Northern Hemisphere in comparison with that of fixed relative dispersion, mainly dependent on the change of relative dispersion and droplet concentrations (Δɛ/ΔNc).

Sensitivity study of cloud parameterizations with relative dispersion in CAM5.1: impacts on aerosol indirect effects

DOE PAGES

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

2017-05-12

Aerosol-induced increase of relative dispersion of cloud droplet size distribution ε exerts a warming effect and partly offsets the cooling of aerosol indirect radiative forcing (AIF) associated with increased droplet concentration by increasing the cloud droplet effective radius ( R e) and enhancing the cloud-to-rain autoconversion rate (Au) (labeled aBut, the total dispersion effects on both R e and Au are not fully considered in most GCMs, especially in different versions of the Community Atmospheric Model (CAM). Furthermore, in order to accurately evaluate the dispersion effect on AIF, the new complete cloud parameterizations of R e and Au explicitly accountingmore » for ε are implemented into the CAM version 5.1 (CAM5.1), and a suite of sensitivity experiments is conducted with different representations of ε reported in the literature. It is shown that the shortwave cloud radiative forcing is much better simulated with the new cloud parameterizations as compared to the standard scheme in CAM5.1, whereas the influences on longwave cloud radiative forcing and surface precipitation are minimal. In addition, consideration of the dispersion effect can significantly reduce the changes induced by anthropogenic aerosols in the cloud-top effective radius and the liquid water path, especially in the Northern Hemisphere. The corresponding AIF with the dispersion effect considered can also be reduced substantially by a range of 0.10 to 0.21 W m -2 at the global scale and by a much bigger margin of 0.25 to 0.39 W m -2 for the Northern Hemisphere in comparison with that of fixed relative dispersion, mainly dependent on the change of relative dispersion and droplet concentrations (Δε/ΔN).« less

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Toward Quantifying the Mass-Based Hygroscopicity of Individual Submicron Atmospheric Aerosol Particles with STXM/NEXAFS and SEM/EDX

NASA Astrophysics Data System (ADS)

Yancey Piens, D.; Kelly, S. T.; OBrien, R. E.; Wang, B.; Petters, M. D.; Laskin, A.; Gilles, M. K.

2014-12-01

The hygroscopic behavior of atmospheric aerosols influences their optical and cloud-nucleation properties, and therefore affects climate. Although changes in particle size as a function of relative humidity have often been used to quantify the hygroscopic behavior of submicron aerosol particles, it has been noted that calculations of hygroscopicity based on size contain error due to particle porosity, non-ideal volume additivity and changes in surface tension. We will present a method to quantify the hygroscopic behavior of submicron aerosol particles based on changes in mass, rather than size, as a function of relative humidity. This method results from a novel experimental approach combining scanning transmission x-ray microscopy with near-edge x-ray absorption fine spectroscopy (STXM/NEXAFS), as well as scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM/EDX) on the same individual particles. First, using STXM/NEXAFS, our methods are applied to aerosol particles of known composition ‒ for instance ammonium sulfate, sodium bromide and levoglucosan ‒ and validated by theory. Then, using STXM/NEXAFS and SEM/EDX, these methods are extended to mixed atmospheric aerosol particles collected in the field at the DOE Atmospheric Radiation Measurement (ARM) Climate Research Facility at the Southern Great Planes sampling site in Oklahoma, USA. We have observed and quantified a range of hygroscopic behaviors which are correlated to the composition and morphology of individual aerosol particles. These methods will have implications for parameterizing aerosol mixing state and cloud-nucleation activity in atmospheric models.

Evaluating Aerosol Process Modules within the Framework of the Aerosol Modeling Testbed

NASA Astrophysics Data System (ADS)

Fast, J. D.; Velu, V.; Gustafson, W. I.; Chapman, E.; Easter, R. C.; Shrivastava, M.; Singh, B.

2012-12-01

Factors that influence predictions of aerosol direct and indirect forcing, such as aerosol mass, composition, size distribution, hygroscopicity, and optical properties, still contain large uncertainties in both regional and global models. New aerosol treatments are usually implemented into a 3-D atmospheric model and evaluated using a limited number of measurements from a specific case study. Under this modeling paradigm, the performance and computational efficiency of several treatments for a specific aerosol process cannot be adequately quantified because many other processes among various modeling studies (e.g. grid configuration, meteorology, emission rates) are different as well. The scientific community needs to know the advantages and disadvantages of specific aerosol treatments when the meteorology, chemistry, and other aerosol processes are identical in order to reduce the uncertainties associated with aerosols predictions. To address these issues, an Aerosol Modeling Testbed (AMT) has been developed that systematically and objectively evaluates new aerosol treatments for use in regional and global models. The AMT consists of the modular Weather Research and Forecasting (WRF) model, a series testbed cases for which extensive in situ and remote sensing measurements of meteorological, trace gas, and aerosol properties are available, and a suite of tools to evaluate the performance of meteorological, chemical, aerosol process modules. WRF contains various parameterizations of meteorological, chemical, and aerosol processes and includes interactive aerosol-cloud-radiation treatments similar to those employed by climate models. In addition, the physics suite from the Community Atmosphere Model version 5 (CAM5) have also been ported to WRF so that they can be tested at various spatial scales and compared directly with field campaign data and other parameterizations commonly used by the mesoscale modeling community. Data from several campaigns, including the 2006 MILAGRO, 2008 ISDAC, 2008 VOCALS, 2010 CARES, and 2010 CalNex campaigns, have been incorporated into the AMT as testbed cases. Data from operational networks (e.g. air quality, meteorology, satellite) are also included in the testbed cases to supplement the field campaign data. The CARES and CalNex testbed cases are used to demonstrate how the AMT can be used to assess the strengths and weaknesses of simple and complex representations of aerosol processes in relation to computational cost. Anticipated enhancements to the AMT and how this type of testbed can be used by the scientific community to foster collaborations and coordinate aerosol modeling research will also be discussed.

An Aerosol Physical Chemistry Model for the Upper Troposphere

NASA Technical Reports Server (NTRS)

Lin, Jin-Sheng

2001-01-01

This report is the final report for the Cooperative Agreement NCC2-1000. The tasks outlined in the various proposals are listed with a brief comment as to the research performed. The publications titles are: The effects of particle size and nitric acid uptake on the homogenous freezing of sulfate aerosols; Parameterization of an aerosol physical chemistry model (APCM) for the NH3/H2SO4/HNO3/H2O system at cold temperatures; and The onset, extent and duration of dehydration in the Southern Hemisphere polar vortex.

MAP-oriented research in the People's Republic of China

NASA Technical Reports Server (NTRS)

Lu, D.

1985-01-01

A brief accounting of MAP oriented research in the Republic of China is given. A stratosphere balloon launching facility and its capabilities are reviewed. Observations of the stratospheric aerosols with a balloon-borne aerosol computer were made. Long term monitoring of stratospheric aerosols induced by volcanic eruptions are made with a ruby lidar. The main parameters of an ST radar system are given. The ionospheric D region is investigated with the method of ionospheric absorption. And photochemical modeling and radiation parameterization of the middle atmosphere are made.

Double-moment cloud microphysics scheme for the deep convection parameterization in the GFDL AM3

NASA Astrophysics Data System (ADS)

Belochitski, A.; Donner, L.

2014-12-01

A double-moment cloud microphysical scheme originally developed by Morrision and Gettelman (2008) for the stratiform clouds and later adopted for the deep convection by Song and Zhang (2011) has been implemented in to the Geophysical Fluid Dynamics Laboratory's atmospheric general circulation model AM3. The scheme treats cloud drop, cloud ice, rain, and snow number concentrations and mixing ratios as diagnostic variables and incorporates processes of autoconversion, self-collection, collection between hydrometeor species, sedimentation, ice nucleation, drop activation, homogeneous and heterogeneous freezing, and the Bergeron-Findeisen process. Such detailed representation of microphysical processes makes the scheme suitable for studying the interactions between aerosols and convection, as well as aerosols' indirect effects on clouds and their roles in climate change. The scheme is first tested in the single column version of the GFDL AM3 using forcing data obtained at the U.S. Department of Energy Atmospheric Radiation Measurment project's Southern Great Planes site. Scheme's impact on SCM simulations is discussed. As the next step, runs of the full atmospheric GCM incorporating the new parameterization are compared to the unmodified version of GFDL AM3. Global climatological fields and their variability are contrasted with those of the original version of the GCM. Impact on cloud radiative forcing and climate sensitivity is investigated.

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

NASA Astrophysics Data System (ADS)

Belochitski, A.; Donner, L.

2013-12-01

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

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

Seinfeld, John H.

This project addressed the following research need in the Atmospheric System Research (ASR) Science and Program Plan: "Measurements downwind of urban sources of aerosol particles and precursor gases have shown that the mass concentration of secondary organic aerosol (SOA) can be several-fold greater than can be explained on the basis of current model calculations using observed precursor concentrations. ASR will continue conducting laboratory experiments on both gas-phase and aqueous-phase SOA formation to characterize the particle formation and the organic gases that react to form new organic aerosol material on aerosol seeds. ASR will use these experiments to guide the developmentmore » of comprehensive chemical mechanisms... to guide the development of parameterizations that are simple enough to be applied to aerosol life cycle models."« less

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

Assessment of biomass burning smoke influence on environmental conditions for multi-year tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints.

PubMed

Saide, Pablo E; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M; Pierce, R Bradley; Carmichael, Gregory R

2016-09-16

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations.

Assessment of Biomass Burning Smoke Influence on Environmental Conditions for Multi-Year Tornado Outbreaks by Combining Aerosol-Aware Microphysics and Fire Emission Constraints

NASA Technical Reports Server (NTRS)

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; Da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2016-01-01

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRFChem for its use in applications such as NWP and cloud-resolving simulations.

Impact of anthropogenic aerosols on regional climate change in Beijing, China

NASA Astrophysics Data System (ADS)

Zhao, B.; Liou, K. N.; He, C.; Lee, W. L.; Gu, Y.; Li, Q.; Leung, L. R.

2015-12-01

Anthropogenic aerosols affect regional climate significantly through radiative (direct and semi-direct) and indirect effects, but the magnitude of these effects over megacities are subject to large uncertainty. In this study, we evaluated the effects of anthropogenic aerosols on regional climate change in Beijing, China using the online-coupled Weather Research and Forecasting/Chemistry Model (WRF/Chem) with the Fu-Liou-Gu radiation scheme and a spatial resolution of 4km. We further updated this radiation scheme with a geometric-optics surface-wave (GOS) approach for the computation of light absorption and scattering by black carbon (BC) particles in which aggregation shape and internal mixing properties are accounted for. In addition, we incorporated in WRF/Chem a 3D radiative transfer parameterization in conjunction with high-resolution digital data for city buildings and landscape to improve the simulation of boundary-layer, surface solar fluxes and associated sensible/latent heat fluxes. Preliminary simulated meteorological parameters, fine particles (PM2.5) and their chemical components agree well with observational data in terms of both magnitude and spatio-temporal variations. The effects of anthropogenic aerosols, including BC, on radiative forcing, surface temperature, wind speed, humidity, cloud water path, and precipitation are quantified on the basis of simulation results. With several preliminary sensitivity runs, we found that meteorological parameters and aerosol radiative effects simulated with the incorporation of improved BC absorption and 3-D radiation parameterizations deviate substantially from simulation results using the conventional homogeneous/core-shell configuration for BC and the plane-parallel model for radiative transfer. Understanding of the aerosol effects on regional climate change over megacities must consider the complex shape and mixing state of aerosol aggregates and 3D radiative transfer effects over city landscape.

Sea-State Dependence of Aerosol Concentration in the Marine Atmospheric Boundary Layer

NASA Astrophysics Data System (ADS)

Lenain, L.; Melville, W. K.

2016-02-01

While sea spray aerosols represent a large portion of the aerosols present in the marine environment, and despite evidence of the importance of surface wave and wave-breaking related processes in the coupling of the ocean with the atmosphere, sea spray source generation functions are traditionally parameterized by the wind speed at 10m. It is clear that unless the wind and wave field are fully developed, the source function will be a function of both wind and wave parameters. In this study, we report on an air-sea interaction experiment, the ONR phase-resolved High-Resolution Air-Sea Interaction experiments (HIRES), conducted off the coast of Northern California in June 2010. Detailed measurements of aerosol number concentration in the Marine Atmospheric Boundary Layer (MABL), at altitudes ranging from as low as 30m and up to 800m AMSL over a broad range of environmental conditions (significant wave height, Hs, of 2 to 4.5m and wind speed at 10m height, U10, of 10 to 18 m/s) collected from an instrumented research aircraft, are presented. Aerosol number densities and volume are computed over a range of particle diameters from 0.1 to 200 µm, while the surface conditions, i.e. significant wave height, moments of the breaker length distribution Λ(c), and wave breaking dissipation, were measured by a suite of electro-optical sensors that included the NASA Airborne Topographic Mapper (ATM). The sea-state dependence of the aerosol concentration in the MABL is evident, ultimately stressing the need to incorporate wave and wave kinematics in the spray source generation functions that are traditionally primarily parameterized by surface winds. A scaling of the measured aerosol volume distribution by wave and atmospheric state variables is proposed.

Application of WRF/Chem-MADRID and WRF/Polyphemus in Europe - Part 1: Model description, evaluation of meteorological predictions, and aerosol-meteorology interactions

NASA Astrophysics Data System (ADS)

Zhang, Y.; Sartelet, K.; Wu, S.-Y.; Seigneur, C.

2013-07-01

Comprehensive model evaluation and comparison of two 3-D air quality modeling systems (i.e., the Weather Research and Forecast model (WRF)/Polyphemus and WRF with chemistry and the Model of Aerosol Dynamics, Reaction, Ionization, and Dissolution (MADRID) (WRF/Chem-MADRID)) are conducted over Western Europe. Part 1 describes the background information for the model comparison and simulation design, the application of WRF for January and July 2001 over triple-nested domains in Western Europe at three horizontal grid resolutions: 0.5°, 0.125°, and 0.025°, and the effect of aerosol/meteorology interactions on meteorological predictions. Nine simulated meteorological variables (i.e., downward shortwave and longwave radiation fluxes (SWDOWN and LWDOWN), outgoing longwave radiation flux (OLR), temperature at 2 m (T2), specific humidity at 2 m (Q2), relative humidity at 2 m (RH2), wind speed at 10 m (WS10), wind direction at 10 m (WD10), and precipitation (Precip)) are evaluated using available observations in terms of spatial distribution, domainwide daily and site-specific hourly variations, and domainwide performance statistics. The vertical profiles of temperature, dew points, and wind speed/direction are also evaluated using sounding data. WRF demonstrates its capability in capturing diurnal/seasonal variations and spatial gradients and vertical profiles of major meteorological variables. While the domainwide performance of LWDOWN, OLR, T2, Q2, and RH2 at all three grid resolutions is satisfactory overall, large positive or negative biases occur in SWDOWN, WS10, and Precip even at 0.125° or 0.025° in both months and in WD10 in January. In addition, discrepancies between simulations and observations exist in T2, Q2, WS10, and Precip at mountain/high altitude sites and large urban center sites in both months, in particular, during snow events or thunderstorms. These results indicate the model's difficulty in capturing meteorological variables in complex terrain and subgrid-scale meteorological phenomena, due to inaccuracies in model initialization parameterization (e.g., lack of soil temperature and moisture nudging), limitations in the physical parameterizations (e.g., shortwave radiation, cloud microphysics, cumulus parameterizations, and ice nucleation treatments) as well as limitations in surface heat and moisture budget parameterizations (e.g., snow-related processes, subgrid-scale surface roughness elements, and urban canopy/heat island treatments and CO2 domes). While the use of finer grid resolutions of 0.125° and 0.025° shows some improvements for WS10, WD10, Precip, and some mesoscale events (e.g., strong forced convection and heavy precipitation), it does not significantly improve the overall statistical performance for all meteorological variables except for Precip. The WRF/Chem simulations with and without aerosols show that aerosols lead to reduced net shortwave radiation fluxes, 2 m temperature, 10 m wind speed, planetary boundary layer (PBL) height, and precipitation and increase aerosol optical depth, cloud condensation nuclei, cloud optical depth, and cloud droplet number concentrations over most of the domain. These results indicate a need to further improve the model representations of the above parameterizations as well as aerosol-meteorology interactions at all scales.

Probing aerosol indirect effect on deep convection using idealized cloud-resolving simulations with parameterized large-scale dynamics.

NASA Astrophysics Data System (ADS)

Anber, U.; Wang, S.; Gentine, P.; Jensen, M. P.

2017-12-01

A framework is introduced to investigate the indirect impact of aerosol loading on tropical deep convection using 3-dimentional idealized cloud-system resolving simulations with coupled large-scale circulation. The large scale dynamics is parameterized using a spectral weak temperature gradient approximation that utilizes the dominant balance in the tropics between adiabatic cooling and diabatic heating. Aerosol loading effect is examined by varying the number concentration of nuclei (CCN) to form cloud droplets in the bulk microphysics scheme over a wide range from 30 to 5000 without including any radiative effect as the radiative cooling is prescribed at a constant rate, to isolate the microphysical effect. Increasing aerosol number concentration causes mean precipitation to decrease monotonically, despite the increase in cloud condensates. Such reduction in precipitation efficiency is attributed to reduction in the surface enthalpy fluxes, and not to the divergent circulation, as the gross moist stability remains unchanged. We drive a simple scaling argument based on the moist static energy budget, that enables a direct estimation of changes in precipitation given known changes in surfaces enthalpy fluxes and the constant gross moist stability. The impact on cloud hydrometers and microphysical properties is also examined and is consistent with the macro-physical picture.

Aerosols and Aerosol-related haze forecasting in China Meteorological Adminstration

NASA Astrophysics Data System (ADS)

Zhou, Chunhong; Zhang, Xiaoye; Gong, Sunling; Liu, Hongli; Xue, Min

2017-04-01

CMA Unified Atmospheric Chemistry Environmental Forecasting System (CUACE) is a unified numerical chemical weather forecasting system with BC, OC, Sulfate, Nitrate, Ammonia, Dust and Sea-Salt aerosols and their sources, gas to particle processes, SOA, microphysics and transformation. With an open interface, CUACE has been online coupled to mesoscale model MM5 and the new NWP system GRAPES (Global/Regional Assimilation and Prediction Enhanced System)min CMA. With Chinese Emissions from Cao and Zhang(2012 and 2013), a forecasting system called CUACE/Haze-fog has been running in real time in CMA and issue 5-days PM10, O3 and Visibility forecasts. A comprehensive ACI scheme has also been developed in CUACE Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The results show that interactive aerosols with the WDM6 in CUACE obviously improve the clouds properties and the precipitation, showing 24% to 48% enhancements of TS scoring for 6-h precipitation .

The Fifth International Ice Nucleation Workshop Activities FIN-1 and FIN-2: Overview and Selected Results

NASA Astrophysics Data System (ADS)

Moehler, O.; Cziczo, D. J.; DeMott, P. J.; Hiranuma, N.; Petters, M. D.

2015-12-01

The role of aerosol particles for ice formation in clouds is one of the largest uncertainties in understanding the Earth's weather and climate systems, which is related to the poor knowledge of ice nucleation microphysics or of the nature and atmospheric abundance of ice nucleating particles (INPs). During the recent years, new mobile instruments were developed for measuring the concentration, size and chemical composition of INPs, which were tested during the three-part Fifth International Ice Nucleation (FIN) workshop. The FIN activities addressed not only instrument issues, but also important science topics like the nature of atmospheric INP and cloud ice residuals, the ice nucleation activity of relevant atmospheric aerosols, or the parameterization of ice formation in atmospheric weather and climate models. The first activity FIN-1 was conducted during November 2014 at the AIDA cloud chamber. It involved co-locating nine single particle mass spectrometers to evaluate how well they resolve the INP and ice residual composition and how spectra from different instruments compare for relevant atmospheric aerosols. We conducted about 90 experiments with mineral, carbonaceous and biological aerosol types, some also coated with organic and inorganic compounds. The second activity FIN-2 was conducted during March 2015 at the AIDA facility. A total of nine mobile INP instruments directly sampled from the AIDA aerosol chambers. Wet suspension and filter samples were also taken for offline INP processing. A refereed blind intercomparison was conducted during two days of the FIN-2 activity. The third activity FIN-3 will take place at the Desert Research Institute's Storm Peak Laboratory (SPL) in order to test the instruments' performance in the field. This contribution will introduce the FIN activities, summarize first results from the formal part of FIN-2, and discuss selected results, mainly from FIN-1 for the effect of coating on the ice nucleation (IN) by mineral aerosols. The coating with both secondary organic compounds and sulphuric acid was conducted in the AIDA chamber at relevant temperatures and precursor concentrations and was monitored with the particle mass spectrometers. Already very thin, atmospherically relevant coatings reduced deposition IN, but had little effect on immersion freezing.

Evaluating Model Parameterizations of Submicron Aerosol Scattering and Absorption with in situ Data from ARCTAS 2008

NASA Technical Reports Server (NTRS)

Alvarado, Matthew J.; Lonsdale, Chantelle R.; Macintyre, Helen L.; Bian, Huisheng; Chin, Mian; Ridley, David A.; Heald, Colette L.; Thornhill, Kenneth L.; Anderson, Bruce E.; Cubison, Michael J.;

Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

NASA Astrophysics Data System (ADS)

Alvarado, Matthew J.; Lonsdale, Chantelle R.; Macintyre, Helen L.; Bian, Huisheng; Chin, Mian; Ridley, David A.; Heald, Colette L.; Thornhill, Kenneth L.; Anderson, Bruce E.; Cubison, Michael J.; Jimenez, Jose L.; Kondo, Yutaka; Sahu, Lokesh K.; Dibb, Jack E.; Wang, Chien

2016-07-01

Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10-23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.

Impact of aerosols, dust, water vapor and clouds on fair weather PG and implications for the Carnegie curve

NASA Astrophysics Data System (ADS)

Kourtidis, Konstantinos; Georgoulias, Aristeidis

2017-04-01

We studied the impact of anthropogenic aerosols, fine mode natural aerosols, Saharan dust, atmospheric water vapor, cloud fraction, cloud optical depth and cloud top height on the magnitude of fair weather PG at the rural station of Xanthi. Fair weather PG was measured in situ while the other parameters were obtained from the MODIS instrument onboard the Terra and Aqua satellites. All of the above parameteres were found to impact fair weather PG magnitude. Regarding aerosols, the impact was larger for Saharan dust and fine mode natural aerosols whereas regarding clouds the impact was larger for cloud fraction while less than that of aerosols. Water vapour and ice precipitable water were also found to influence fair weather PG. Since aerosols and water are ubiquitous in the atmosphere and exhibit large spatial and temporal variability, we postulate that our understanding of the Carnegie curve might need revision.

Aerosol Modeling for the Global Model Initiative

NASA Technical Reports Server (NTRS)

Weisenstein, Debra K.; Ko, Malcolm K. W.

2001-01-01

The goal of this project is to develop an aerosol module to be used within the framework of the Global Modeling Initiative (GMI). The model development work will be preformed jointly by the University of Michigan and AER, using existing aerosol models at the two institutions as starting points. The GMI aerosol model will be tested, evaluated against observations, and then applied to assessment of the effects of aircraft sulfur emissions as needed by the NASA Subsonic Assessment in 2001. The work includes the following tasks: 1. Implementation of the sulfur cycle within GMI, including sources, sinks, and aqueous conversion of sulfur. Aerosol modules will be added as they are developed and the GMI schedule permits. 2. Addition of aerosol types other than sulfate particles, including dust, soot, organic carbon, and black carbon. 3. Development of new and more efficient parameterizations for treating sulfate aerosol nucleation, condensation, and coagulation among different particle sizes and types.

The dynamical core, physical parameterizations, and basic simulation characteristics of the atmospheric component AM3 of the GFDL global coupled model CM3

USGS Publications Warehouse

Donner, L.J.; Wyman, B.L.; Hemler, R.S.; Horowitz, L.W.; Ming, Y.; Zhao, M.; Golaz, J.-C.; Ginoux, P.; Lin, S.-J.; Schwarzkopf, M.D.; Austin, J.; Alaka, G.; Cooke, W.F.; Delworth, T.L.; Freidenreich, S.M.; Gordon, C.T.; Griffies, S.M.; Held, I.M.; Hurlin, W.J.; Klein, S.A.; Knutson, T.R.; Langenhorst, A.R.; Lee, H.-C.; Lin, Y.; Magi, B.I.; Malyshev, S.L.; Milly, P.C.D.; Naik, V.; Nath, M.J.; Pincus, R.; Ploshay, J.J.; Ramaswamy, V.; Seman, C.J.; Shevliakova, E.; Sirutis, J.J.; Stern, W.F.; Stouffer, R.J.; Wilson, R.J.; Winton, M.; Wittenberg, A.T.; Zeng, F.

2011-01-01

The Geophysical Fluid Dynamics Laboratory (GFDL) has developed a coupled general circulation model (CM3) for the atmosphere, oceans, land, and sea ice. The goal of CM3 is to address emerging issues in climate change, including aerosol-cloud interactions, chemistry-climate interactions, and coupling between the troposphere and stratosphere. The model is also designed to serve as the physical system component of earth system models and models for decadal prediction in the near-term future-for example, through improved simulations in tropical land precipitation relative to earlier-generation GFDL models. This paper describes the dynamical core, physical parameterizations, and basic simulation characteristics of the atmospheric component (AM3) of this model. Relative to GFDL AM2, AM3 includes new treatments of deep and shallow cumulus convection, cloud droplet activation by aerosols, subgrid variability of stratiform vertical velocities for droplet activation, and atmospheric chemistry driven by emissions with advective, convective, and turbulent transport. AM3 employs a cubed-sphere implementation of a finite-volume dynamical core and is coupled to LM3, a new land model with ecosystem dynamics and hydrology. Its horizontal resolution is approximately 200 km, and its vertical resolution ranges approximately from 70 m near the earth's surface to 1 to 1.5 km near the tropopause and 3 to 4 km in much of the stratosphere. Most basic circulation features in AM3 are simulated as realistically, or more so, as in AM2. In particular, dry biases have been reduced over South America. In coupled mode, the simulation of Arctic sea ice concentration has improved. AM3 aerosol optical depths, scattering properties, and surface clear-sky downward shortwave radiation are more realistic than in AM2. The simulation of marine stratocumulus decks remains problematic, as in AM2. The most intense 0.2% of precipitation rates occur less frequently in AM3 than observed. The last two decades of the twentieth century warm in CM3 by 0.328C relative to 1881-1920. The Climate Research Unit (CRU) and Goddard Institute for Space Studies analyses of observations show warming of 0.568 and 0.528C, respectively, over this period. CM3 includes anthropogenic cooling by aerosol-cloud interactions, and its warming by the late twentieth century is somewhat less realistic than in CM2.1, which warmed 0.668C but did not include aerosol-cloud interactions. The improved simulation of the direct aerosol effect (apparent in surface clear-sky downward radiation) in CM3 evidently acts in concert with its simulation of cloud-aerosol interactions to limit greenhouse gas warming. ?? 2011 American Meteorological Society.

Intercomparison between CMIP5 model and MODIS satellite-retrieved data of aerosol optical depth, cloud fraction, and cloud-aerosol interactions

NASA Astrophysics Data System (ADS)

Sockol, Alyssa; Small Griswold, Jennifer D.

2017-08-01

Aerosols are a critical component of the Earth's atmosphere and can affect the climate of the Earth through their interactions with solar radiation and clouds. Cloud fraction (CF) and aerosol optical depth (AOD) at 550 nm from the Moderate Resolution Imaging Spectroradiometer (MODIS) are used with analogous cloud and aerosol properties from Historical Phase 5 of the Coupled Model Intercomparison Project (CMIP5) model runs that explicitly include anthropogenic aerosols and parameterized cloud-aerosol interactions. The models underestimate AOD by approximately 15% and underestimate CF by approximately 10% overall on a global scale. A regional analysis is then used to evaluate model performance in two regions with known biomass burning activity and absorbing aerosol (South America (SAM) and South Africa (SAF)). In SAM, the models overestimate AOD by 4.8% and underestimate CF by 14%. In SAF, the models underestimate AOD by 35% and overestimate CF by 13.4%. Average annual cycles show that the monthly timing of AOD peaks closely match satellite data in both SAM and SAF for all except the Community Atmosphere Model 5 and Geophysical Fluid Dynamics Laboratory (GFDL) models. Monthly timing of CF peaks closely match for all models (except GFDL) for SAM and SAF. Sorting monthly averaged 2° × 2.5° model or MODIS CF as a function of AOD does not result in the previously observed "boomerang"-shaped CF versus AOD relationship characteristic of regions with absorbing aerosols from biomass burning. Cloud-aerosol interactions, as observed using daily (or higher) temporal resolution data, are not reproducible at the spatial or temporal resolution provided by the CMIP5 models.

Assessment of biomass burning smoke influence on environmental conditions for multiyear tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints

NASA Astrophysics Data System (ADS)

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2016-09-01

We use the Weather Research and Forecasting (WRF) system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the U.S. during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included, and smoke emissions are constrained using an inverse modeling technique and satellite-based aerosol optical depth observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low-level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics, and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations.

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

Changes in organic aerosol composition with aging inferred from aerosol mass spectra

NASA Astrophysics Data System (ADS)

Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.; Chhabra, P. S.; Seinfeld, J. H.; Worsnop, D. R.

2011-03-01

Organic aerosols (OA) can be separated with factor analysis of aerosol mass spectrometer (AMS) data into hydrocarbon-like OA (HOA) and oxygenated OA (OOA). We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum). Such parameterization allows the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups) vs. f43 space ("triangle plot") (Ng et al., 2010) into the Van Krevelen diagram (H:C vs. O:C). Heald et al. (2010) suggested that the bulk composition of OA line up in the Van Krevelen diagram with a slope ~ -1; such slope can potentially arise from the physical mixing of HOA and OOA, and/or from chemical aging of these components. In this study, we find that the OOA components from all sites occupy an area in the Van Krevelen space, with the evolution of OOA following a shallower slope of ~ -0.5, consistent with the additions of both acid and alcohol functional groups without fragmentation, and/or the addition of acid groups with C-C bond breakage. The importance of acid formation in OOA evolution is consistent with increasing f44 in the triangle plot with photochemical age. These results provide a framework for linking the bulk aerosol chemical composition evolution to molecular-level studies.

Quantification of Absorption Due to Black and Brown Carbon from Biomass Burning and Parameterizations for Comparison to Climate Models Result

NASA Astrophysics Data System (ADS)

Pokhrel, Rudra Prasad

This dissertation examines the optical properties of fresh and aged biomass burning aerosols, parameterization of these properties, and development of new instrumentation and calibration techniques to measure aerosol optical properties. Data sets were collected from the fourth Fire Lab at Missoula Experiment (FLAME-4) that took place from October 15 to November 16, 2012. Biomass collected from the various parts of the world were burned under controlled laboratory conditions and fresh emissions from different stages of burning were measured and analyzed. Optical properties of aged aerosol under different conditions was also explored. A photoacoustic absorption spectrometer (PAS) was built and integrated with a newly designed thermal denuder to improve upon observations made during Flame-4. A novel calibration technique for the PAS was developed. Single scattering albedo (SSA) and absorption Angstrom exponent (AAE) from 12 different fuels with 41 individual burns were estimated and parameterized with modified combustion efficiency (MCE) and the ratio of elemental carbon (EC) to organic carbon (OC) mass. The EC / OC ratio has better capability to parameterize SSA and AAE than MCE. The simple linear regression model proposed in this study accurately predicts SSA during the first few hours of plume aging with the ambient data from a biomass burning event. In addition, absorption due to brown carbon (BrC) can significantly lower the SSA at 405 nm resulting in a wavelength dependence of SSA. Furthermore, smoldering dominated burns have larger AAE values while flaming dominated burns have smaller AAE values indicating a large fraction of BrC is emitted during the smoldering stage of the burn. Enhancement in BC absorption (EAbs) due to coating by absorbing and non-absorbing substances is estimated at 405 nm and 660 nm. Relatively smaller values of EAbs at 660 nm compared to 405 nm suggests lensing is a less important contributor to biomass burning aerosol absorption at lower wavelengths. Multiple burns of the same fuel produced significantly different EAbs values at 405 nm, but show good correlation with the EC/OC ratio indicating less dependency on fuel type and more dependency on burn conditions. In addition, absorption due to BrC can contribute up to 92 % of the total biomass burning aerosol absorption at 405 nm and up to 58 % of the total absorption at 532 nm. Indicating BrC absorption in biomass burning emissions is equally or more important than the absorption due to BC at short wavelengths. Furthermore, fractional absorption due to BrC shows reasonably good correlation with EC/OC ratio and AAE. Primary organic aerosol is found to be more volatile than secondary organic aerosol and it is found that the thermal denuder deployed in this study removes less organic aerosol if secondary organic aerosol is present. SSA at 532 nm remains constant during different conditions of aging while SSA at 405 nm increases under certain conditions suggesting the degradation of BrC. Decreases in AAE under the same experiment further support the proposed BrC degradation. The novel thermal denuder designed completely removes non-refractory material and can be used under higher flow rates (maximum of 5 LPM) than the most commercially available thermal denuders. The new calibration techniques proposed for the photoacousitc absorption spectrometer will reduce uncertainty during calibration compared to the conventional calibration methods.

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

DeMott, PJ; Suski, KJ; Hill, TCJ

The first ever ice nucleating particle (INP) measurements to be collected at the Southern Great Plains site were made during a period from late April to June 2014, as a trial for possible longer-term measurements at the site. These measurements will also be used to lay the foundation for understanding and parameterizing (for cloud resolving modeling) the sources of these climatically important aerosols as well as to augment the existing database containing this knowledge. Siting the measurements during the spring was intended to capture INP sources in or to this region from plant, soil, dust transported over long distances, biomassmore » burning, and pollution aerosols at a time when they may influence warm-season convective clouds and precipitation. Data have been archived of real-time measurements of INP number concentrations as a function of processing conditions (temperature and relative humidity) during 18 days of sampling that spanned two distinctly different weather situations: a warm, dry and windy period with regional dust and biomass burning influences in early May, and a cooler period of frequent precipitation during early June. Precipitation delayed winter wheat harvesting, preventing intended sampling during that perturbation on atmospheric aerosols. INP concentrations were highest and most variable at all temperatures in the dry period, where we attribute the INP activity primarily to soil dust emissions. Additional offline INP analyses are underway to extend the characterization of INP to cover the entire mixed phase cloud regime from -5°C to -35°C during the full study. Initial comparisons between methods on four days show good agreement and excellent future promise. The additional offline immersion freezing data will be archived as soon as completed under separate funding. Analyses of additional specialized studies for specific attribution of INP to biological and smoke sources are continuing via the National Science Foundation and National Aeronautics and Space Administration funding that helped support instrumentation used for the measurements described herein. Aerosol Observing System aerosol data will be vital to the interpretation and parameterization of results as part of analyses for publications in preparation.« less

Assessing the Dynamics of Organic Aerosols over the North Atlantic Ocean

PubMed Central

Kasparian, Jérôme; Hassler, Christel; Ibelings, Bas; Berti, Nicolas; Bigorre, Sébastien; Djambazova, Violeta; Gascon-Diez, Elena; Giuliani, Grégory; Houlmann, Raphaël; Kiselev, Denis; de Laborie, Pierric; Le, Anh-Dao; Magouroux, Thibaud; Neri, Tristan; Palomino, Daniel; Pfändler, Stéfanie; Ray, Nicolas; Sousa, Gustavo; Staedler, Davide; Tettamanti, Federico; Wolf, Jean-Pierre; Beniston, Martin

2017-01-01

The influence of aerosols on climate is highly dependent on the particle size distribution, concentration, and composition. In particular, the latter influences their ability to act as cloud condensation nuclei, whereby they impact cloud coverage and precipitation. Here, we simultaneously measured the concentration of aerosols from sea spray over the North Atlantic on board the exhaust-free solar-powered vessel “PlanetSolar”, and the sea surface physico-chemical parameters. We identified organic-bearing particles based on individual particle fluorescence spectra. Organic-bearing aerosols display specific spatio-temporal distributions as compared to total aerosols. We propose an empirical parameterization of the organic-bearing particle concentration, with a dependence on water salinity and sea-surface temperature only. We also show that a very rich mixture of organic aerosols is emitted from the sea surface. Such data will certainly contribute to providing further insight into the influence of aerosols on cloud formation, and be used as input for the improved modeling of aerosols and their role in global climate processes. PMID:28361985

A sensitivity analysis of volcanic aerosol dispersion in the stratosphere. [Mt. Fuego, Guatemala eruptions

NASA Technical Reports Server (NTRS)

Butler, C. F.

1979-01-01

A computer sensitivity analysis was performed to determine the uncertainties involved in the calculation of volcanic aerosol dispersion in the stratosphere using a 2 dimensional model. The Fuego volcanic event of 1974 was used. Aerosol dispersion processes that were included are: transport, sedimentation, gas phase sulfur chemistry, and aerosol growth. Calculated uncertainties are established from variations in the stratospheric aerosol layer decay times at 37 latitude for each dispersion process. Model profiles are also compared with lidar measurements. Results of the computer study are quite sensitive (factor of 2) to the assumed volcanic aerosol source function and the large variations in the parameterized transport between 15 and 20 km at subtropical latitudes. Sedimentation effects are uncertain by up to a factor of 1.5 because of the lack of aerosol size distribution data. The aerosol chemistry and growth, assuming that the stated mechanisms are correct, are essentially complete in several months after the eruption and cannot explain the differences between measured and modeled results.

On the competition among aerosol number, size and composition in predicting CCN variability: a multi-annual field study in an urbanized desert.

PubMed

Crosbie, E; Youn, J-S; Balch, B; Wonaschütz, A; Shingler, T; Wang, Z; Conant, W C; Betterton, E A; Sorooshian, A

2015-02-10

A 2-year data set of measured CCN (cloud condensation nuclei) concentrations at 0.2 % supersaturation is combined with aerosol size distribution and aerosol composition data to probe the effects of aerosol number concentrations, size distribution and composition on CCN patterns. Data were collected over a period of 2 years (2012-2014) in central Tucson, Arizona: a significant urban area surrounded by a sparsely populated desert. Average CCN concentrations are typically lowest in spring (233 cm -3 ), highest in winter (430 cm -3 ) and have a secondary peak during the North American monsoon season (July to September; 372 cm -3 ). There is significant variability outside of seasonal patterns, with extreme concentrations (1 and 99 % levels) ranging from 56 to 1945 cm -3 as measured during the winter, the season with highest variability. Modeled CCN concentrations based on fixed chemical composition achieve better closure in winter, with size and number alone able to predict 82% of the variance in CCN concentration. Changes in aerosol chemical composition are typically aligned with changes in size and aerosol number, such that hygroscopicity can be parameterized even though it is still variable. In summer, models based on fixed chemical composition explain at best only 41% (pre-monsoon) and 36% (monsoon) of the variance. This is attributed to the effects of secondary organic aerosol (SOA) production, the competition between new particle formation and condensational growth, the complex interaction of meteorology, regional and local emissions and multi-phase chemistry during the North American monsoon. Chemical composition is found to be an important factor for improving predictability in spring and on longer timescales in winter. Parameterized models typically exhibit improved predictive skill when there are strong relationships between CCN concentrations and the prevailing meteorology and dominant aerosol physicochemical processes, suggesting that similar findings could be possible in other locations with comparable climates and geography.

Estimation of the Cloud condensation nuclei concentration(CCN) and aerosol optical depth(AOD) relation in the Arctic region

NASA Astrophysics Data System (ADS)

Jung, C. H.; Yoon, Y. J.; Ahn, S. H.; Kang, H. J.; Gim, Y. T.; Lee, B. Y.

2017-12-01

Information of the spatial and temporal variations of cloud condensation nuclei (CCN) concentrations is important in estimating aerosol indirect effects. Generally, CCN aerosol is difficult to estimate using remote sensing methods. Although there are many CCN measurements data, extensive measurements of CCN are not feasible because of the complex nature of the operation and high cost, especially in the Arctic region. Thus, there have been many attempts to estimate CCN concentrations from more easily obtainable parameters such as aerosol optical depth (AOD) because AOD has the advantage of being readily observed by remote sensing from space by several sensors. For example, some form of correlation was derived between AOD and the number concentration of cloud condensation nuclei (CCN) through the comparison results from AERONET network and CCN measurements (Andreae 2009). In this study, a parameterization of CCN concentration as a function of AOD at 500 nm is given in the Arctic region. CCN data was collected during the period 2007-2013 at the Zeppelin observatory (78.91° N, 11.89° E, 474 masl). The AERONET network and MODIS AOD data are compared with ground measured CCN measurement and the relations between AOD and CCN are parameterized. The seasonal characteristics as well as long term trends are also considered. Through the measurement, CCN concentration remains high during spring because of aerosol transportation from the mid-latitudes, known as Arctic Haze. Lowest CCN number densities were observed during Arctic autumn and early winter when aerosol long-range transport into the Arctic is not effective and new particle formation ceases. The results show that the relation between AOD and CCN shows a different parameter depending on the seasonal aerosol and CCN characteristics. This seasonal different CCN-AOD relation can be interpreted as many physico-chemical aerosol properties including aerosol size distribution, composition. ReferenceAndreae, M. O. (2009) Correlation between cloud condensation nuclei concentration and aerosol optical thickness in remote and polluted regions,2009, Atmos. Chem. Phys., 9, 543-556.

Assessment of biomass burning smoke influence on environmental conditions for multi-year tornado outbreaks by combining aerosol-aware microphysics and fire emission constraints

PubMed Central

Saide, Pablo E.; Thompson, Gregory; Eidhammer, Trude; da Silva, Arlindo M.; Pierce, R. Bradley; Carmichael, Gregory R.

2018-01-01

We use the WRF system to study the impacts of biomass burning smoke from Central America on several tornado outbreaks occurring in the US during spring. The model is configured with an aerosol-aware microphysics parameterization capable of resolving aerosol-cloud-radiation interactions in a cost-efficient way for numerical weather prediction (NWP) applications. Primary aerosol emissions are included and smoke emissions are constrained using an inverse modeling technique and satellite-based AOD observations. Simulations turning on and off fire emissions reveal smoke presence in all tornado outbreaks being studied and show an increase in aerosol number concentrations due to smoke. However, the likelihood of occurrence and intensification of tornadoes is higher due to smoke only in cases where cloud droplet number concentration in low level clouds increases considerably in a way that modifies the environmental conditions where the tornadoes are formed (shallower cloud bases and higher low-level wind shear). Smoke absorption and vertical extent also play a role, with smoke absorption at cloud-level tending to burn-off clouds and smoke absorption above clouds resulting in an increased capping inversion. Comparing these and WRF-Chem simulations configured with a more complex representation of aerosol size and composition and different optical properties, microphysics and activation schemes, we find similarities in terms of the simulated aerosol optical depths and aerosol impacts on near-storm environments. This provides reliability on the aerosol-aware microphysics scheme as a less computationally expensive alternative to WRF-Chem for its use in applications such as NWP and cloud-resolving simulations. PMID:29619287

How the Emitted Size Distribution and Mixing State of Feldspar Affect Ice Nucleating Particles in a Global Model

NASA Technical Reports Server (NTRS)

Perlwitz, Jan P.; Fridlind, Ann M.; Knopf, Daniel A.; Miller, Ron L.; García-Pando, Carlos Perez

2017-01-01

The effect of aerosol particles on ice nucleation and, in turn, the formation of ice and mixed phase clouds is recognized as one of the largest sources of uncertainty in climate prediction. We apply an improved dust mineral specific aerosol module in the NASA GISS Earth System ModelE, which takes into account soil aggregates and their fragmentation at emission as well as the emission of large particles. We calculate ice nucleating particle concentrations from K-feldspar abundance for an active site parameterization for a range of activation temperatures and external and internal mixing assumption. We find that the globally averaged INP concentration is reduced by a factor of two to three, compared to a simple assumption on the size distribution of emitted dust minerals. The decrease can amount to a factor of five in some geographical regions. The results vary little between external and internal mixing and different activation temperatures, except for the coldest temperatures. In the sectional size distribution, the size range 24 micrometer contributes the largest INP number.

How the Emitted Size Distribution and Mixing State of Feldspar Affect Ice Nucleating Particles in a Global Model

NASA Astrophysics Data System (ADS)

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

2017-12-01

The effect of aerosol particles on ice nucleation and, in turn, the formation of ice and mixed phase clouds is recognized as one of the largest sources of uncertainty in climate prediction. We apply an improved dust mineral specific aerosol module in the NASA GISS Earth System ModelE, which takes into account soil aggregates and their fragmentation at emission as well as the emission of large particles. We calculate ice nucleating particle concentrations from K-feldspar abundance for an active site parameterization for a range of activation temperatures and external and internal mixing assumption. We find that the globally averaged INP concentration is reduced by a factor of two to three, compared to a simple assumption on the size distribution of emitted dust minerals. The decrease can amount to a factor of five in some geographical regions. The results vary little between external and internal mixing and different activation temperatures, except for the coldest temperatures. In the sectional size distribution, the size range 2-4 μm contributes the largest INP number.

Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

NASA Astrophysics Data System (ADS)

Gunthe, S. S.; King, S. M.; Rose, D.; Chen, Q.; Roldin, P.; Farmer, D. K.; Jimenez, J. L.; Artaxo, P.; Andreae, M. O.; Martin, S. T.; Pöschl, U.

2009-10-01

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ≍0.1-0.4 (0.16±0.06 arithmetic mean and standard deviation). The overall median value of κ≍0.15 was by a factor of two lower than the values typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≍0.1 at D≍50 nm; κ≍0.2 at D≍200 nm), which is in agreement with earlier hygroscopicity tandem differential mobility analyzer (H-TDMA) studies. The CCN measurement results are consistent with aerosol mass spectrometry (AMS) data, showing that the organic mass fraction (forg) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≍200 nm). The κ values exhibited a negative linear correlation with forg (R2=0.81), and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≍0.1 which can be regarded as the effective hygroscopicity of biogenic secondary organic aerosol (SOA) and κinorg≍0.6 which is characteristic for ammonium sulfate and related salts. Both the size dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=κorg×forg +κinorg×finorg). The CCN number concentrations predicted with κp were in fair agreement with the measurement results (~20% average deviation). The median CCN number concentrations at S=0.1-0.82% ranged from NCCN,0.10≍35 cm-3 to NCCN,0.82≍160 cm-3, the median concentration of aerosol particles larger than 30 nm was NCN,30≍200 cm-3, and the corresponding integral CCN efficiencies were in the range of NCCN,0.10/NCN,30≍0.1 to NCCN,0.82/NCN,30≍0.8. Although the number concentrations and hygroscopicity parameters were much lower in pristine rainforest air, the integral CCN efficiencies observed were similar to those in highly polluted megacity air. Moreover, model calculations of NCCN,S assuming an approximate global average value of κ≍0.3 for continental aerosols led to systematic overpredictions, but the average deviations exceeded ~50% only at low water vapor supersaturation (0.1%) and low particle number concentrations (≤100 cm-3). Model calculations assuming a constant aerosol size distribution led to higher average deviations at all investigated levels of supersaturation: ~60% for the campaign average distribution and ~1600% for a generic remote continental size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this paper should enable efficient description of the CCN properties of pristine tropical rainforest aerosols of Amazonia in detailed process models as well as in large-scale atmospheric and climate models.

Simulation of Optical Properties and Direct and Indirect Radiative Effects of Smoke Aerosols Over Marine Stratocumulus Clouds During Summer 2008 in California With the Regional Climate Model RegCM

NASA Astrophysics Data System (ADS)

Mallet, M.; Solmon, F.; Roblou, L.; Peers, F.; Turquety, S.; Waquet, F.; Jethva, H.; Torres, O.

2017-10-01

The regional climate model RegCM has been modified to better account for the climatic effects of biomass-burning particles. Smoke aerosols are represented by new tracers with consistent radiative and hygroscopic properties to simulate the direct radiative forcing (DRF), and a new parameterization has been integrated for relating the droplet number concentration to the aerosol concentration for marine stratocumulus clouds (Sc). RegCM has been tested during the summer of 2008 over California, when extreme concentration of smoke, together with the presence of Sc, is observed. This work indicates that significant aerosol optical depth (AOD) ( 1-2 at 550 nm) is related to the intense 2008 fires. Compared to Ozone Monitoring Instrument (OMI) and Moderate Resolution Imaging Spectroradiometer, the regional pattern of RegCM AOD is well represented although the magnitude is lower than satellite observations. Comparisons with Polarization and Directionality of Earth Reflectances (POLDER) above-clouds aerosol optical depth (ACAOD) show the ability of RegCM to simulate realistic ACAOD during the transport of smoke above the Pacific Ocean. The simulated single scattering albedo is 0.90 (at 550 nm) near biomass-burning sources, consistent with OMI and POLDER, and smoke leads to shortwave heating rates 1.5-2°K d-1. RegCM is not able to correctly resolve the daily patterns in cloud properties notably due to its coarse horizontal resolutions. However, the changes in the sign of the DRF at top of atmosphere (TOA) (negative to positive) from clear-sky to all-sky conditions is well simulated. Finally, the "aerosol-cloud" parameterization allows simulating an increase of the cloud optical depth for significant concentrations, leading to large perturbations of radiative fluxes at TOA.

Improving the Understanding and Model Representation of Processes that Couple Shallow Clouds, Aerosols, and Land-Ecosystems

NASA Astrophysics Data System (ADS)

Fast, J. D.; Berg, L. K.; Schmid, B.; Alexander, M. L. L.; Bell, D.; D'Ambro, E.; Hubbe, J. M.; Liu, J.; Mei, F.; Pekour, M. S.; Pinterich, T.; Schobesberger, S.; Shilling, J.; Springston, S. R.; Thornton, J. A.; Tomlinson, J. M.; Wang, J.; Zelenyuk, A.

2016-12-01

Cumulus convection is an important component in the atmospheric radiation budget and hydrologic cycle over the southern Great Plains and over many regions of the world, particularly during the summertime growing season when intense turbulence induced by surface radiation couples the land surface to clouds. Current convective cloud parameterizations, however, contain uncertainties resulting from insufficient coincident data that couples cloud macrophysical and microphysical properties to inhomogeneity in surface layer, boundary layer, and aerosol properties. We describe the measurement strategy and preliminary findings from the recent Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign conducted in May and September of 2016 in the vicinity of the DOE's Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site located in Oklahoma. The goal of the HI-SCALE campaign is to provide a detailed set of aircraft and surface measurements needed to obtain a more complete understanding and improved parameterizations of the lifecycle of shallow clouds. The sampling is done in two periods, one in the spring and the other in the late summer to take advantage of variations in the "greenness" for various types of vegetation, new particle formation, anthropogenic enhancement of biogenic secondary organic aerosol (SOA), and other aerosol properties. The aircraft measurements will be coupled with extensive routine ARM SGP measurements as well as Large Eddy Simulation (LES), cloud resolving, and cloud-system resolving models. Through these integrated analyses and modeling studies, the affects of inhomogeneity in land use, vegetation, soil moisture, convective eddies, and aerosol properties on the evolution of shallow clouds will be determined, including the feedbacks of cloud radiative effects.

A theory-based parameterization for heterogeneous ice nucleation and implications for the simulation of ice processes in atmospheric models

NASA Astrophysics Data System (ADS)

Savre, J.; Ekman, A. M. L.

2015-05-01

A new parameterization for heterogeneous ice nucleation constrained by laboratory data and based on classical nucleation theory is introduced. Key features of the parameterization include the following: a consistent and modular modeling framework for treating condensation/immersion and deposition freezing, the possibility to consider various potential ice nucleating particle types (e.g., dust, black carbon, and bacteria), and the possibility to account for an aerosol size distribution. The ice nucleating ability of each aerosol type is described using a contact angle (θ) probability density function (PDF). A new modeling strategy is described to allow the θ PDF to evolve in time so that the most efficient ice nuclei (associated with the lowest θ values) are progressively removed as they nucleate ice. A computationally efficient quasi Monte Carlo method is used to integrate the computed ice nucleation rates over both size and contact angle distributions. The parameterization is employed in a parcel model, forced by an ensemble of Lagrangian trajectories extracted from a three-dimensional simulation of a springtime low-level Arctic mixed-phase cloud, in order to evaluate the accuracy and convergence of the method using different settings. The same model setup is then employed to examine the importance of various parameters for the simulated ice production. Modeling the time evolution of the θ PDF is found to be particularly crucial; assuming a time-independent θ PDF significantly overestimates the ice nucleation rates. It is stressed that the capacity of black carbon (BC) to form ice in the condensation/immersion freezing mode is highly uncertain, in particular at temperatures warmer than -20°C. In its current version, the parameterization most likely overestimates ice initiation by BC.

Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

NASA Astrophysics Data System (ADS)

Gunthe, S. S.; King, S. M.; Rose, D.; Chen, Q.; Roldin, P.; Farmer, D. K.; Jimenez, J. L.; Artaxo, P.; Andreae, M. O.; Martin, S. T.; Pöschl, U.

2009-02-01

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ=0.05-0.45. The overall median value of κ≍0.15 was only half of the value typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≍0.1 at D≍50 nm; κ≍0.2 at D≍200 nm). The CCN measurement results were fully consistent with aerosol mass spectrometry (AMS) data, which showed that the organic mass fraction (Xm,org) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≍200 nm). The κ values exhibited a close linear correlation with Xm,org and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≍0.1 which is consistent with laboratory measurements of secondary organic aerosols and κinorg≍0.6 which is characteristic for ammonium sulfate and related salts. Both the size-dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=0.1 Xm,org+0.6 Xm,inorg), and the CCN number concentrations predicted with κp were in fair agreement with the measurement results. The median CCN number concentrations at S=0.1-0.82% ranged from NCCN,0.10≍30 cm-3 to NCCN,0.82≍150 cm-3, the median concentration of aerosol particles larger than 30 nm was NCN,30≍180 cm-3, and the corresponding integral CCN efficiencies were in the range of NCCN,0.10/NCN,30≍0.1 to NCCN,0.82/NCN,30≍0.8. Although the number concentrations and hygroscopicity parameters were much lower, the integral CCN efficiencies observed in pristine rainforest air were similar to those in highly polluted mega-city air. Moreover, model calculations of NCCN,S with a global average value of κ=0.3 led to systematic overpredictions, but the relative deviations exceeded ~50% only at low water vapor supersaturation (0.1%) and low particle number concentrations (≤100 cm-3). These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this paper should enable efficient description of the CCN properties of pristine tropical rainforest aerosols in detailed process models as well as in large-scale atmospheric and climate models.

Scanning Backscatter Lidar Observations for Characterizing 4-D Cloud and Aerosol Fields to Improve Radiative Transfer Parameterizations

NASA Technical Reports Server (NTRS)

Schwemmer, Geary K.; Miller, David O.

2005-01-01

Clouds have a powerful influence on atmospheric radiative transfer and hence are crucial to understanding and interpreting the exchange of radiation between the Earth's surface, the atmosphere, and space. Because clouds are highly variable in space, time and physical makeup, it is important to be able to observe them in three dimensions (3-D) with sufficient resolution that the data can be used to generate and validate parameterizations of cloud fields at the resolution scale of global climate models (GCMs). Simulation of photon transport in three dimensionally inhomogeneous cloud fields show that spatial inhomogeneities tend to decrease cloud reflection and absorption and increase direct and diffuse transmission, Therefore it is an important task to characterize cloud spatial structures in three dimensions on the scale of GCM grid elements. In order to validate cloud parameterizations that represent the ensemble, or mean and variance of cloud properties within a GCM grid element, measurements of the parameters must be obtained on a much finer scale so that the statistics on those measurements are truly representative. High spatial sampling resolution is required, on the order of 1 km or less. Since the radiation fields respond almost instantaneously to changes in the cloud field, and clouds changes occur on scales of seconds and less when viewed on scales of approximately 100m, the temporal resolution of cloud properties should be measured and characterized on second time scales. GCM time steps are typically on the order of an hour, but in order to obtain sufficient statistical representations of cloud properties in the parameterizations that are used as model inputs, averaged values of cloud properties should be calculated on time scales on the order of 10-100 s. The Holographic Airborne Rotating Lidar Instrument Experiment (HARLIE) provides exceptional temporal (100 ms) and spatial (30 m) resolution measurements of aerosol and cloud backscatter in three dimensions. HARLIE was used in a ground-based configuration in several recent field campaigns. Principal data products include aerosol backscatter profiles, boundary layer heights, entrainment zone thickness, cloud fraction as a function of altitude and horizontal wind vector profiles based on correlating the motions of clouds and aerosol structures across portions of the scan. Comparisons will be made between various cloud detecting instruments to develop a baseline performance metric.

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

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

NASA Technical Reports Server (NTRS)

Penner, Joyce E.

1998-01-01

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

Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

NASA Astrophysics Data System (ADS)

Zhou, C.; Zhang, X.; Gong, S.

2015-12-01

A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under CMA chemical weather modeling system GRAPES/CUACE. Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred. The results show that interactive aerosols with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content and cloud droplet number concentrations while decrease the mean diameter of cloud droplets with varying magnitudes of the changes in each case and region. These interactive micro-physical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24% to 48% enhancements of TS scoring for 6-h precipitation in almost all regions. The interactive aerosols with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3°C.

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.

Impact of Improvements in Volcanic Implementation on Atmospheric Chemistry and Climate in the GISS-E2 Model

NASA Technical Reports Server (NTRS)

Tsigaridis, Kostas; LeGrande, Allegra; Bauer, Susanne

2015-01-01

The representation of volcanic eruptions in climate models introduces some of the largest errors when evaluating historical simulations, partly due to the crude model parameterizations. We will show preliminary results from the Goddard Institute for Space Studies (GISS)-E2 model comparing traditional highly parameterized volcanic implementation (specified Aerosol Optical Depth, Effective Radius) to deploying the full aerosol microphysics module MATRIX and directly emitting SO2 allowing us the prognosically determine the chemistry and climate impact. We show a reasonable match in aerosol optical depth, effective radius, and forcing between the full aerosol implementation and reconstructions/observations of the Mt. Pinatubo 1991 eruption, with a few areas as targets for future improvement. This allows us to investigate not only the climate impact of the injection of volcanic aerosols, but also influences on regional water vapor, O3, and OH distributions. With the skill of the MATRIX volcano implementation established, we explore (1) how the height of the injection column of SO2 influence atmospheric chemistry and climate response, (2) how the initial condition of the atmosphere influences the climate and chemistry impact of the eruption with a particular focus on how ENSO and QBO and (3) how the coupled chemistry could mitigate the climate signal for much larger eruptions (i.e. the 1258 eruption, reconstructed to be approximately 10x Pinatubo). During each sensitivity experiment we assess the impact on profiles of water vapor, O3, and OH, and assess how the eruption impacts the budget of each.

Local effects of partly-cloudy skies on solar and emitted radiations

NASA Technical Reports Server (NTRS)

Whitney, D. A.; Griffin, T. J.

1983-01-01

Atmospheric aerosol and turbidity measurements were analyzed and the results are presented. The correlation of global insolation with cloud cover fractions for the first complete year's data set was completed. A theoretical model was developed to parameterize the effects of local aerosols upon insolation received at the ground using satellite radiometric data and insolation measurements under clear sky conditions. A February data set, composed of one minute integrated global insolation and direct solar irradiances, cloud cover fractions, meteorological data from nearby weather stations, and GOES East satellite radiometric data was collected to test the model and used to calculate the effects of local aerosols.

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.

Evaluating WRF-Chem aerosol indirect effects in Southeast Pacific marine stratocumulus during VOCALS-REx

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

Saide P. E.; Springston S.; Spak, S. N.

2012-03-29

We evaluate a regional-scale simulation with the WRF-Chem model for the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx), which sampled the Southeast Pacific's persistent stratocumulus deck. Evaluation of VOCALS-REx ship-based and three aircraft observations focuses on analyzing how aerosol loading affects marine boundary layer (MBL) dynamics and cloud microphysics. We compare local time series and campaign-averaged longitudinal gradients, and highlight differences in model simulations with (W) and without (NW) wet deposition processes. The higher aerosol loadings in the NW case produce considerable changes in MBL dynamics and cloud microphysics, in accordance with the established conceptualmore » model of aerosol indirect effects. These include increase in cloud albedo, increase in MBL and cloud heights, drizzle suppression, increase in liquid water content, and increase in cloud lifetime. Moreover, better statistical representation of aerosol mass and number concentration improves model fidelity in reproducing observed spatial and temporal variability in cloud properties, including top and base height, droplet concentration, water content, rain rate, optical depth (COD) and liquid water path (LWP). Together, these help to quantify confidence in WRF-Chem's modeled aerosol-cloud interactions, especially in the activation parameterization, while identifying structural and parametric uncertainties including: irreversibility in rain wet removal; overestimation of marine DMS and sea salt emissions, and accelerated aqueous sulfate conversion. Our findings suggest that WRF-Chem simulates marine cloud-aerosol interactions at a level sufficient for applications in forecasting weather and air quality and studying aerosol climate forcing, and may do so with the reliability required for policy analysis.« less

Modeling organic aerosols in a megacity: potential contribution of semi-volatile and intermediate volatility primary organic compounds to secondary organic aerosol formation

NASA Astrophysics Data System (ADS)

Hodzic, A.; Jimenez, J. L.; Madronich, S.; Canagaratna, M. R.; Decarlo, P. F.; Kleinman, L.; Fast, J.

2010-06-01

It has been established that observed local and regional levels of secondary organic aerosols (SOA) in polluted areas cannot be explained by the oxidation and partitioning of anthropogenic and biogenic VOC precursors, at least using current mechanisms and parameterizations. In this study, the 3-D regional air quality model CHIMERE is applied to estimate the potential contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic precursors (S/IVOC) in and around Mexico City for the MILAGRO field experiment during March 2006. The model has been updated to include explicitly the volatility distribution of primary organic aerosols (POA), their gas-particle partitioning and the gas-phase oxidation of the vapors. Two recently proposed parameterizations, those of Robinson et al. (2007) ("ROB") and Grieshop et al. (2009) ("GRI") are compared and evaluated against surface and aircraft measurements. The 3-D model results are assessed by comparing with the concentrations of OA components from Positive Matrix Factorization of Aerosol Mass Spectrometer (AMS) data, and for the first time also with oxygen-to-carbon ratios derived from high-resolution AMS measurements. The results show a substantial enhancement in predicted SOA concentrations (2-4 times) with respect to the previously published base case without S/IVOCs (Hodzic et al., 2009), both within and downwind of the city leading to much reduced discrepancies with the total OA measurements. Model improvements in OA predictions are associated with the better-captured SOA magnitude and diurnal variability. The predicted production from anthropogenic and biomass burning S/IVOC represents 40-60% of the total measured SOA at the surface during the day and is somewhat larger than that from commonly measured aromatic VOCs, especially at the T1 site at the edge of the city. The SOA production from the continued multi-generation S/IVOC oxidation products continues actively downwind. Similar to aircraft observations, the predicted OA/ΔCO ratio for the ROB case increases from 20-30 μg sm-3 ppm-1 up to 60-70 μg sm-3 ppm-1 between a fresh and 1-day aged air mass, while the GRI case produces a 30% higher OA growth than observed. The predicted average O/C ratio of total OA for the ROB case is 0.16 at T0, substantially below observed value of 0.5. A much better agreement for O/C ratios and temporal variability (R2=0.63) is achieved with the updated GRI treatment. Both treatments show a deficiency in regard to POA ageing with a tendency to over-evaporate POA upon dilution of the urban plume suggesting that atmospheric HOA may be less volatile than assumed in these parameterizations. This study highlights the important potential role of S/IVOC chemistry in the SOA budget in this region, and highlights the need for further improvements in available parameterizations. The agreement observed in this study is not sufficient evidence to conclude that S/IVOC are the major missing SOA source in megacity environments. The model is still very underconstrained, and other possible pathways such as formation from very volatile species like glyoxal may explain some of the mass and especially increase the O/C ratio.

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.

The climate impacts of absorbing aerosols on and within the Arctic

NASA Astrophysics Data System (ADS)

Rasch, P.; Wang, H.; Ma, P.; Fast, J. D.; Wang, M.; Easter, R. C.; Liu, X.; Qian, Y.; Flanner, M. G.; Ghan, S.; Singh, B.

2011-12-01

Absorbing aerosols are receiving increasing attention as forcing agents in the climate system. By scattering and absorbing light they can reduce planetary albedo, particularly over bright surfaces (clouds, snow and ice). They also act as cloud condensation and/or ice nuclei, influencing the brightness, lifetime and precipitation properties of clouds. Atmospheric stability and primary circulation features respond to the changing vertical and horizontal patterns of heating, cooling, and surface fluxes produced by the aerosols, clouds and surface properties. These changes in meteorology have further impacts on aerosols and clouds producing a complex interplay between transport, forcings, and feedbacks involving absorbing aerosols and climate. The complexity of the processes and the interactions between them make it very challenging to represent aerosols realistically in large scale (global and regional) climate models. Simulations of important features of aerosols still contain easily identifiable biases. I will describe our efforts to identify the processes responsible for some of those biases and the deficiencies in model formulations that impede progress in treating aerosols and understanding their role in polar climate. I plan to summarize some studies performed with the NCAR CESM (global) and WRF-Chem (regional) Community models that examine the simulation sensitivity to treatments of physics, chemistry, and meteorology. Some of these simulations were allowed to evolve freely; others were strongly constrained to agree with observed meteorological fields. We have also altered the formulation of a number of the processes in the model to improve fidelity in the aerosol distributions. The parameterizations used in our global model have also been transferred to the regional model, allowing comparisons to be made between the simpler formulations used in the global model with more elaborate and costly formulations available in the regional model. The regional model can be run at higher resolution in order to explore the resolution dependence of the parameterizations and make comparisons to field experiments more straightforward. Aerosols sources have also been tagged by sector and geographic region to help in attribution and interpretation. The many variations mentioned here help in understanding how aerosols reach the arctic and how they produce changes in radiative forcing and Arctic climate. I will provide a brief overview of these studies, with more detail available in presentations submitted to this session and elsewhere.

Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions.

PubMed

Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, Ernest; Lohmann, Ulrike; Baltensperger, Urs; Cziczo, Daniel J

2009-09-28

Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of atmospheric interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation (SS) with respect to liquid water. In this study the subsaturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were investigated. Aerosols were generated both with a wet and a dry disperser. The water uptake was parameterized via the hygroscopicity parameter kappa. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived kappa values between 0.00 and 0.02 (the latter corresponds to a particle consisting of 96.7% by volume insoluble material and approximately 3.3% ammonium sulfate). Pure clay aerosols were generally found to be less hygroscopic than natural desert dust particles. The illite and montmorillonite samples had kappa approximately 0.003. The kaolinite samples were less hygroscopic and had kappa=0.001. SD (kappa=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (kappa=0.007) and ATD (kappa=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles. Thus, the generation method is critically important when presenting such data. These results indicate any atmospheric processing of a fresh mineral dust particle which leads to the addition of more than approximately 3% soluble material will significantly enhance its hygroscopicity and CCN activity.

Relating Aerosol Mass and Optical Depth in the Summertime Continental Boundary Layer

NASA Astrophysics Data System (ADS)

Brock, C. A.; Wagner, N.; Middlebrook, A. M.; Attwood, A. R.; Washenfelder, R. A.; Brown, S. S.; McComiskey, A. C.; Gordon, T. D.; Welti, A.; Carlton, A. G.; Murphy, D. M.

2014-12-01

Aerosol optical depth (AOD), the column-integrated ambient aerosol light extinction, is determined from satellite and ground-based remote sensing measurements. AOD is the parameter most often used to validate earth system model simulations of aerosol mass. Relating aerosol mass to AOD, however, is problematic due to issues including aerosol water uptake as a function of relative humidity (RH) and the complicated relationship between aerosol physicochemical properties and light extinction. Measurements of aerosol microphysical, chemical, and optical properties help to constrain the relationship between aerosol mass and optical depth because aerosol extinction at ambient RH is a function of the abundance, composition and size distribution of the aerosol. We use vertical profiles of humidity and dry aerosol extinction observed in the southeastern United States (U.S.) to examine the relationship between submicron aerosol mass concentration and extinction at ambient RH. We show that the κ-Köhler parameterization directly, and without additional Mie calculations, describes the change in extinction with varying RH as a function of composition for both aged aerosols typical of the polluted summertime continental boundary layer and the biomass burning aerosols we encountered. We calculate how AOD and the direct radiative effect in the eastern U.S. have likely changed due to trends in aerosol composition in recent decades. We also examine the sensitivity of AOD to the RH profile and to aerosol composition, size distribution and abundance.

Differences in ice nucleation behavior of arable and desert soil dust in deposition nucleation regime

NASA Astrophysics Data System (ADS)

Ullrich, Romy; Vogel, Franziska; Möhler, Ottmar; Höhler, Kristina; Schiebel, Thea

2017-04-01

Soil dust from arid and semi-arid regions is one of the most abundant aerosol types in the atmosphere with emission rates of about 1600 Tg per year (Andreae et al. (2009)). Therewith, soil dust plays an important role for the atmospheric radiative transfer and also for the formation of clouds. Soil dust refers to dust sampled from agricultural used areas, to dust from bare soil as well as to dust from desert regions. By mass-spectrometric measurements of the chemical composition of ice residuals, mineral dust as component of soil dust was found to be the major heterogeneous ice nucleating particle (INP) type (e.g. Cziczo et al. (2013)), in particular in the upper troposphere. Also in laboratory studies the ice nucleation efficiency of the different soil dusts was investigated. It was shown that desert dusts (Ullrich et al. (2017)) as well as soil dusts from arable regions (O'Sullivan et al. (2014), Tobo et al. (2014)) are efficient INP. However, there is still a lack of data for ice nucleation on soil dusts for temperatures below about 220 K. With the AIDA (Aerosol Interactions and Dynamics in the Atmosphere) cloud chamber, we are able to characterize the ice nucleation efficiency for different aerosol types to temperatures down to 180 K and high ice supersaturations. In order to extend the already existing AIDA data base for deposition nucleation on desert dusts and agricultural soil dusts, new experiments were done in the upper tropospheric temperature regime. This contribution will show the results of the new experiments with desert dust in comparison to existing data for higher temperatures. The first data analysis confirms the temperature dependent trend of the ice nucleation activity as discussed and parameterized in a recent paper by Ullrich et al. (2017). Furthermore, the update and extension of the recently published parameterization of deposition nucleation for desert dust to lower temperatures will be discussed. The experiments with agricultural soil dust will be compared to existing AIDA experiments at higher temperatures published by Steinke et al. (2016). Finally, the ice nucleation activity of both desert dust and agricultural soil dust will be compared for the upper tropospheric temperature regime. Andreae et al. (2009), Sources and Nature of Atmospheric Aerosols, in Aerosol Pollution Impact on Precipitation - A Scientific Review, Ch.3, Springer Netherlands, 45-89 Cziczo et al. (2013), Clarifying the Dominant Sources and Mechanisms of Cirrus Cloud Formation, Science, 340, 1320-1324 O'Sullivan et al. (2014), Ice nucleation by fertile soil dusts: relative importance of mineral and biogenic components, Atmos. Chem. Phys., 14, 1853-1867 Steinke et al. (2016), Ice nucleation activity of agricultural soil dust aerosols from Mongolia, Argentina and Germany, J. Geophys. Res., 121 Tobo et al. (2014), Organic matter matters for ice nuclei of agricultural soil origin, Atmos. Chem. Phys., 14, 8521-8531 Ullrich et al. (2017), A new ice nucleation active site parametrization for desert dust and soot, J. Atmos. Sci., in press

Ganges Valley Aerosol Experiment (GVAX) Final Campaign Report

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

Kotamarthi, VR

2013-12-01

In general, the Indian Summer Monsoon (ISM) as well as the and the tropical monsoon climate is influenced by a wide range of factors. Under various climate change scenarios, temperatures over land and into the mid troposphere are expected to increase, intensifying the summer pressure gradient differential between land and ocean and thus strengthening the ISM. However, increasing aerosol concentration, air pollution, and deforestation result in changes to surface albedo and insolation, potentially leading to low monsoon rainfall. Clear evidence points to increasing aerosol concentrations over the Indian subcontinent with time, and several hypotheses regarding the effect on monsoons havemore » been offered. The Ganges Valley Aerosol Experiment (GVAX) field study aimed to provide critical data to address these hypotheses and contribute to developing better parameterizations for tropical clouds, convection, and aerosol-cloud interactions. The primary science questions for the mission were as follows:« less

Balancing accuracy, efficiency, and flexibility in a radiative transfer parameterization for dynamical models

NASA Astrophysics Data System (ADS)

Pincus, R.; Mlawer, E. J.

2017-12-01

Radiation is key process in numerical models of the atmosphere. The problem is well-understood and the parameterization of radiation has seen relatively few conceptual advances in the past 15 years. It is nonthelss often the single most expensive component of all physical parameterizations despite being computed less frequently than other terms. This combination of cost and maturity suggests value in a single radiation parameterization that could be shared across models; devoting effort to a single parameterization might allow for fine tuning for efficiency. The challenge lies in the coupling of this parameterization to many disparate representations of clouds and aerosols. This talk will describe RRTMGP, a new radiation parameterization that seeks to balance efficiency and flexibility. This balance is struck by isolating computational tasks in "kernels" that expose as much fine-grained parallelism as possible. These have simple interfaces and are interoperable across programming languages so that they might be repalced by alternative implementations in domain-specific langauges. Coupling to the host model makes use of object-oriented features of Fortran 2003, minimizing branching within the kernels and the amount of data that must be transferred. We will show accuracy and efficiency results for a globally-representative set of atmospheric profiles using a relatively high-resolution spectral discretization.

A Comparison of Parameterizations of Secondary Organic Aerosol Production: Global Budget and Spatiotemporal Variability

NASA Astrophysics Data System (ADS)

Liu, J.; Chen, Z.; Horowitz, L. W.; Carlton, A. M. G.; Fan, S.; Cheng, Y.; Ervens, B.; Fu, T. M.; He, C.; Tao, S.

2014-12-01

Secondary organic aerosols (SOA) have a profound influence on air quality and climate, but large uncertainties exist in modeling SOA on the global scale. In this study, five SOA parameterization schemes, including a two-product model (TPM), volatility basis-set (VBS) and three cloud SOA schemes (Ervens et al. (2008, 2014), Fu et al. (2008) , and He et al. (2013)), are implemented into the global chemical transport model (MOZART-4). For each scheme, model simulations are conducted with identical boundary and initial conditions. The VBS scheme produces the highest global annual SOA production (close to 35 Tg·y-1), followed by three cloud schemes (26-30 Tg·y-1) and TPM (23 Tg·y-1). Though sharing a similar partitioning theory to the TPM scheme, the VBS approach simulates the chemical aging of multiple generations of VOCs oxidation products, resulting in a much larger SOA source, particularly from aromatic species, over Europe, the Middle East and Eastern America. The formation of SOA in VBS, which represents the net partitioning of semi-volatile organic compounds from vapor to condensed phase, is highly sensitivity to the aging and wet removal processes of vapor-phase organic compounds. The production of SOA from cloud processes (SOAcld) is constrained by the coincidence of liquid cloud water and water-soluble organic compounds. Therefore, all cloud schemes resolve a fairly similar spatial pattern over the tropical and the mid-latitude continents. The spatiotemporal diversity among SOA parameterizations is largely driven by differences in precursor inputs. Therefore, a deeper understanding of the evolution, wet removal, and phase partitioning of semi-volatile organic compounds, particularly above remote land and oceanic areas, is critical to better constrain the global-scale distribution and related climate forcing of secondary organic aerosols.

A New Paradigm for Diagnosing Contributions to Model Aerosol Forcing Error

NASA Astrophysics Data System (ADS)

Jones, A. L.; Feldman, D. R.; Freidenreich, S.; Paynter, D.; Ramaswamy, V.; Collins, W. D.; Pincus, R.

2017-12-01

A new paradigm in benchmark absorption-scattering radiative transfer is presented that enables both the globally averaged and spatially resolved testing of climate model radiation parameterizations in order to uncover persistent sources of biases in the aerosol instantaneous radiative effect (IRE). A proof of concept is demonstrated with the Geophysical Fluid Dynamics Laboratory AM4 and Community Earth System Model 1.2.2 climate models. Instead of prescribing atmospheric conditions and aerosols, as in prior intercomparisons, native snapshots of the atmospheric state and aerosol optical properties from the participating models are used as inputs to an accurate radiation solver to uncover model-relevant biases. These diagnostic results show that the models' aerosol IRE bias is of the same magnitude as the persistent range cited ( 1 W/m2) and also varies spatially and with intrinsic aerosol optical properties. The findings underscore the significance of native model error analysis and its dispositive ability to diagnose global biases, confirming its fundamental value for the Radiative Forcing Model Intercomparison Project.

General Circulation Model Simulations of the Annual Cycle of Martian Climate

NASA Astrophysics Data System (ADS)

Wilson, R.; Richardson, M.; Rodin, A.

Observations of the martian atmosphere have revealed a strong annual modulation of global mean atmospheric temperature that has been attributed to the pronounced seasonal asymmetry in solar radiation and the highly variable distribution of aerosol. These observations indicate little interannual variability during the relatively cool aphelion season and considerable variability in the perihelion season that is associated with the episodic occurrence of regional and major dust storms. The atmospheric circulation responds to the evolving spatial distribution of aerosol-induced heating and, in turn, plays a major role in determining the sources, sinks, and transport of radiatively active aerosol. We will present simulations employing the GFDL Mars General Circulation Model (MGCM) that show that aspects of the seasonally evolving climate may be simulated in a self-consistent manner using simple dust source parameterizations that represent the effects of lifting associated with local dust storms, dust devil activity, and other processes. Aerosol transport is accomplished, in large part, by elements of the large-scale circulation such as the Hadley circulation, baroclinic storms, tides, etc. A seasonal cycle of atmospheric opacity and temperature results from the variation in the strength and distribution of dust sources as well as from seasonal variations in the efficiency of atmospheric transport associated with changes in the circulation between solstice and equinox, and between perihelion and aphelion. We examine the efficiency of atmospheric transport of dust lifted along the perimeter of the polar caps to gauge the influence of these storms on the global circulation. We also consider the influence of water, as the formation of water ice clouds on dust nuclei may also affect the vertical distribution of dust and strongly influence the aerosol radiative properties.

The Secondary Organic Aerosol Processor (SOAP v1.0) model: a unified model with different ranges of complexity based on the molecular surrogate approach

NASA Astrophysics Data System (ADS)

Couvidat, F.; Sartelet, K.

2014-01-01

The Secondary Organic Aerosol Processor (SOAP v1.0) model is presented. This model is designed to be modular with different user options depending on the computing time and the complexity required by the user. This model is based on the molecular surrogate approach, in which each surrogate compound is associated with a molecular structure to estimate some properties and parameters (hygroscopicity, absorption on the aqueous phase of particles, activity coefficients, phase separation). Each surrogate can be hydrophilic (condenses only on the aqueous phase of particles), hydrophobic (condenses only on the organic phase of particles) or both (condenses on both the aqueous and the organic phases of particles). Activity coefficients are computed with the UNIFAC thermodynamic model for short-range interactions and with the AIOMFAC parameterization for medium and long-range interactions between electrolytes and organic compounds. Phase separation is determined by Gibbs energy minimization. The user can choose between an equilibrium and a dynamic representation of the organic aerosol. In the equilibrium representation, compounds in the particle phase are assumed to be at equilibrium with the gas phase. However, recent studies show that the organic aerosol (OA) is not at equilibrium with the gas phase because the organic phase could be semi-solid (very viscous liquid phase). The condensation or evaporation of organic compounds could then be limited by the diffusion in the organic phase due to the high viscosity. A dynamic representation of secondary organic aerosols (SOA) is used with OA divided into layers, the first layer at the center of the particle (slowly reaches equilibrium) and the final layer near the interface with the gas phase (quickly reaches equilibrium).

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.

Constraining Carbonaceous Aerosol Climate Forcing by Bridging Laboratory, Field and Modeling Studies

NASA Astrophysics Data System (ADS)

Dubey, M. K.; Aiken, A. C.; Liu, S.; Saleh, R.; Cappa, C. D.; Williams, L. R.; Donahue, N. M.; Gorkowski, K.; Ng, N. L.; Mazzoleni, C.; China, S.; Sharma, N.; Yokelson, R. J.; Allan, J. D.; Liu, D.

2014-12-01

Biomass and fossil fuel combustion emits black (BC) and brown carbon (BrC) aerosols that absorb sunlight to warm climate and organic carbon (OC) aerosols that scatter sunlight to cool climate. The net forcing depends strongly on the composition, mixing state and transformations of these carbonaceous aerosols. Complexities from large variability of fuel types, combustion conditions and aging processes have confounded their treatment in models. We analyse recent laboratory and field measurements to uncover fundamental mechanism that control the chemical, optical and microphysical properties of carbonaceous aerosols that are elaborated below: Wavelength dependence of absorption and the single scattering albedo (ω) of fresh biomass burning aerosols produced from many fuels during FLAME-4 was analysed to determine the factors that control the variability in ω. Results show that ω varies strongly with fire-integrated modified combustion efficiency (MCEFI)—higher MCEFI results in lower ω values and greater spectral dependence of ω (Liu et al GRL 2014). A parameterization of ω as a function of MCEFI for fresh BB aerosols is derived from the laboratory data and is evaluated by field data, including BBOP. Our laboratory studies also demonstrate that BrC production correlates with BC indicating that that they are produced by a common mechanism that is driven by MCEFI (Saleh et al NGeo 2014). We show that BrC absorption is concentrated in the extremely low volatility component that favours long-range transport. We observe substantial absorption enhancement for internally mixed BC from diesel and wood combustion near London during ClearFlo. While the absorption enhancement is due to BC particles coated by co-emitted OC in urban regions, it increases with photochemical age in rural areas and is simulated by core-shell models. We measure BrC absorption that is concentrated in the extremely low volatility components and attribute it to wood burning. Our results support enhanced light absorption by internally mixed BC parameterizations in models and identify mixed biomass and fossil combustion regions where this effect is large. We unify the treatment of carbonaceous aerosol components and their interactions to simplify and verify their representation in climate models, and re-evaluate their direct radiative forcing.

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

Boybeyi, Zafer

The Department of Energy (DOE) awarded George Mason University (GMU) with a research project. This project started on June, 2009 and ended July 2014. Main objectives of this research project are; a) to assess the indirect and semi-direct aerosol effects on microphysical structure and radiative properties of Arctic clouds, b) to assess the impact of feedback between the aerosol-cloud interactions and atmospheric boundary layer (ABL) processes on the surface energy balance, c) to better understand and characterize the important unresolved microphysical processes, aerosol effects, and ABL processes and feedbacks, over meso-γ spatial (~1-2 km) and temporal scales (a few minutesmore » to days), and d) to investigate the scale dependency of microphysical parameterizations and its effect on simulations.« less

Comparison of aerosol optical properties above clouds between POLDER and AeroCom models over the South East Atlantic Ocean during the fire season

NASA Astrophysics Data System (ADS)

Peers, F.; Bellouin, N.; Waquet, F.; Ducos, F.; Goloub, P.; Mollard, J.; Myhre, G.; Skeie, R. B.; Takemura, T.; Tanré, D.; Thieuleux, F.; Zhang, K.

2016-04-01

Aerosol properties above clouds have been retrieved over the South East Atlantic Ocean during the fire season 2006 using satellite observations from POLDER (Polarization and Directionality of Earth Reflectances). From June to October, POLDER has observed a mean Above-Cloud Aerosol Optical Thickness (ACAOT) of 0.28 and a mean Above-Clouds Single Scattering Albedo (ACSSA) of 0.87 at 550 nm. These results have been used to evaluate the simulation of aerosols above clouds in five Aerosol Comparisons between Observations and Models (Goddard Chemistry Aerosol Radiation and Transport (GOCART), Hadley Centre Global Environmental Model 3 (HadGEM3), European Centre Hamburg Model 5-Hamburg Aerosol Module 2 (ECHAM5-HAM2), Oslo-Chemical Transport Model 2 (OsloCTM2), and Spectral Radiation-Transport Model for Aerosol Species (SPRINTARS)). Most models do not reproduce the observed large aerosol load episodes. The comparison highlights the importance of the injection height and the vertical transport parameterizations to simulate the large ACAOT observed by POLDER. Furthermore, POLDER ACSSA is best reproduced by models with a high imaginary part of black carbon refractive index, in accordance with recent recommendations.

How much does sea spray aerosol organic matter impact clouds and radiation? Sensitivity studies in the Community Atmosphere Model

NASA Astrophysics Data System (ADS)

Burrows, S. M.; Liu, X.; Elliott, S.; Easter, R. C.; Singh, B.; Rasch, P. J.

2015-12-01

Submicron marine aerosol particles are frequently observed to contain substantial fractions of organic material, hypothesized to enter the atmosphere as part of the primary sea spray aerosol formed through bubble bursting. This organic matter in sea spray aerosol may affect cloud condensation nuclei and ice nuclei concentrations in the atmosphere, particularly in remote marine regions. Members of our team have developed a new, mechanistic representation of the enrichment of sea spray aerosol with organic matter, the OCEANFILMS parameterization (Burrows et al., 2014). This new representation uses fields from an ocean biogeochemistry model to predict properties of the emitted aerosol. We have recently implemented the OCEANFILMS representation of sea spray aerosol composition into the Community Atmosphere Model (CAM), and performed sensitivity experiments and comparisons with alternate formulations. Early results from these sensitivity simulations will be shown, including impacts on aerosols, clouds, and radiation. References: Burrows, S. M., Ogunro, O., Frossard, A. A., Russell, L. M., Rasch, P. J., and Elliott, S. M.: A physically based framework for modeling the organic fractionation of sea spray aerosol from bubble film Langmuir equilibria, Atmos. Chem. Phys., 14, 13601-13629, doi:10.5194/acp-14-13601-2014, 2014.

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Assessment of the first indirect radiative effect of ammonium-sulfate-nitrate aerosols in East Asia

NASA Astrophysics Data System (ADS)

Han, Xiao; Zhang, Meigen; Skorokhod, Andrei

2017-11-01

A physically based cloud nucleation parameterization was introduced into an optical properties/radiative transfer module incorporated with the off-line air quality modeling system Regional Atmospheric Modeling System (RAMS)-Models-3 Community Multi Scale Air Quality (CMAQ) to investigate the distribution features of the first indirect radiative effects of sulfate, nitrate, and ammonium-sulfate-nitrate (ASN) over East Asia for the years of 2005, 2010, and 2013. The relationship between aerosol particles and cloud droplet number concentration could be properly described by this parameterization because the simulated cloud fraction and cloud liquid water path were generally reliable compared with Moderate Resolution Imaging Spectroradiometer (MODIS) retrieved data. Simulation results showed that the strong effect of indirect forcing was mainly concentrated in Southeast China, the East China Sea, the Yellow Sea, and the Sea of Japan. The highest indirect radiative forcing of ASN reached -3.47 W m-2 over Southeast China and was obviously larger than the global mean of the indirect forcing of all anthropogenic aerosols. In addition, sulfate provided about half of the contribution to the ASN indirect forcing effect. However, the effect caused by nitrate was weak because the mass burden of nitrate was very low during summer, whereas the cloud fraction was the highest. The analysis indicated that even though the interannual variation of indirect forcing magnitude generally followed the trend of aerosol mass burden from 2005 to 2013, the cloud fraction was an important factor that determined the distribution pattern of indirect forcing. The heaviest aerosol loading in North China did not cause a strong radiative effect because of the low cloud fraction over this region.

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

NASA Technical Reports Server (NTRS)

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

2012-01-01

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

A New Paradigm for Diagnosing Contributions to Model Aerosol Forcing Error: Diagnosing Model Aerosol Forcing Error

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

Jones, A. L.; Feldman, D. R.; Freidenreich, S.

A new paradigm in benchmark absorption-scattering radiative transfer is presented that enables both the globally averaged and spatially resolved testing of climate model radiation parameterizations in order to uncover persistent sources of biases in the aerosol instantaneous radiative effect (IRE). A proof of concept is demonstrated with the Geophysical Fluid Dynamics Laboratory AM4 and Community Earth System Model 1.2.2 climate models. Instead of prescribing atmospheric conditions and aerosols, as in prior intercomparisons, native snapshots of the atmospheric state and aerosol optical properties from the participating models are used as inputs to an accurate radiation solver to uncover model-relevant biases. Thesemore » diagnostic results show that the models' aerosol IRE bias is of the same magnitude as the persistent range cited (~1 W/m 2) and also varies spatially and with intrinsic aerosol optical properties. The findings presented here underscore the significance of native model error analysis and its dispositive ability to diagnose global biases, confirming its fundamental value for the Radiative Forcing Model Intercomparison Project.« less

A New Paradigm for Diagnosing Contributions to Model Aerosol Forcing Error: Diagnosing Model Aerosol Forcing Error

DOE PAGES

Jones, A. L.; Feldman, D. R.; Freidenreich, S.; ...

2017-12-07

A new paradigm in benchmark absorption-scattering radiative transfer is presented that enables both the globally averaged and spatially resolved testing of climate model radiation parameterizations in order to uncover persistent sources of biases in the aerosol instantaneous radiative effect (IRE). A proof of concept is demonstrated with the Geophysical Fluid Dynamics Laboratory AM4 and Community Earth System Model 1.2.2 climate models. Instead of prescribing atmospheric conditions and aerosols, as in prior intercomparisons, native snapshots of the atmospheric state and aerosol optical properties from the participating models are used as inputs to an accurate radiation solver to uncover model-relevant biases. Thesemore » diagnostic results show that the models' aerosol IRE bias is of the same magnitude as the persistent range cited (~1 W/m 2) and also varies spatially and with intrinsic aerosol optical properties. The findings presented here underscore the significance of native model error analysis and its dispositive ability to diagnose global biases, confirming its fundamental value for the Radiative Forcing Model Intercomparison Project.« less

Investigation of cloud condensation nuclei properties and droplet growth kinetics of the water-soluble aerosol fraction in Mexico City

NASA Astrophysics Data System (ADS)

Padró, Luz T.; Tkacik, Daniel; Lathem, Terry; Hennigan, Chris J.; Sullivan, Amy P.; Weber, Rodney J.; Huey, L. Greg; Nenes, Athanasios

2010-05-01

We present hygroscopic and cloud condensation nuclei (CCN) relevant properties of the water-soluble fraction of Mexico City aerosol collected upon filters during the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) campaign. Application of κ-Köhler theory to the observed CCN activity gave a fairly constant hygroscopicity parameter (κ = 0.28 ± 0.06) regardless of location and organic fraction. Köhler theory analysis was used to understand this invariance by separating the molar volume and surfactant contributions to the CCN activity. Organics were found to depress surface tension (10-15%) from that of pure water. Daytime samples exhibited lower molar mass (˜200 amu) and surface tension depression than nighttime samples (˜400 amu); this is consistent with fresh hygroscopic secondary organic aerosol (SOA) condensing onto particles during peak photochemical hours, subsequently aging during nighttime periods of high relative humidity. Changes in surface tension partially compensate for shifts in average molar volume to give the constant hygroscopicity observed, which implies the amount (volume fraction) of soluble material in the parent aerosol is the key composition parameter required for CCN predictions. This finding, if applicable elsewhere, may explain why CCN predictions are often found to be insensitive to assumptions of chemical composition and provides a very simple way to parameterize organic hygroscopicity in atmospheric models (i.e., κorg = 0.28ɛWSOC). Special care should be given, however, to surface tension depression from organic surfactants, as its nonlinear dependence with organic fraction may introduce biases in observed (and predicted) hygroscopicity. Finally, threshold droplet growth analysis suggests the water-soluble organics do not affect activation kinetics.

Modelling winter organic aerosol at the European scale with CAMx: evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments

NASA Astrophysics Data System (ADS)

Ciarelli, Giancarlo; Aksoyoglu, Sebnem; El Haddad, Imad; Bruns, Emily A.; Crippa, Monica; Poulain, Laurent; Äijälä, Mikko; Carbone, Samara; Freney, Evelyn; O'Dowd, Colin; Baltensperger, Urs; Prévôt, André S. H.

2017-06-01

We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from -61 to -29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88 % (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64 % of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40 % to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60-70 %. Contributions to OA from residential combustion precursors in different volatility ranges were also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38 % with no specific gradient among the stations. Although the new parameterization leads to a better agreement between model results and observations, it still under-predicts the SOA fraction, suggesting that uncertainties in the new scheme and other sources and/or formation mechanisms remain to be elucidated. Moreover, a more detailed characterization of the semivolatile components of the emissions is needed.

Lidar Ice nuclei estimates and how they relate with airborne in-situ measurements

NASA Astrophysics Data System (ADS)

Marinou, Eleni; Amiridis, Vassilis; Ansmann, Albert; Nenes, Athanasios; Balis, Dimitris; Schrod, Jann; Binietoglou, Ioannis; Solomos, Stavros; Mamali, Dimitra; Engelmann, Ronny; Baars, Holger; Kottas, Michael; Tsekeri, Alexandra; Proestakis, Emmanouil; Kokkalis, Panagiotis; Goloub, Philippe; Cvetkovic, Bojan; Nichovic, Slobodan; Mamouri, Rodanthi; Pikridas, Michael; Stavroulas, Iasonas; Keleshis, Christos; Sciare, Jean

2018-04-01

By means of available ice nucleating particle (INP) parameterization schemes we compute profiles of dust INP number concentration utilizing Polly-XT and CALIPSO lidar observations during the INUIT-BACCHUS-ACTRIS 2016 campaign. The polarization-lidar photometer networking (POLIPHON) method is used to separate dust and non-dust aerosol backscatter, extinction, mass concentration, particle number concentration (for particles with radius > 250 nm) and surface area concentration. The INP final products are compared with aerosol samples collected from unmanned aircraft systems (UAS) and analyzed using the ice nucleus counter FRIDGE.

Final Report for Research Conducted at The Scripps Institution of Oceanography, University of California San Diego from 2/2002 to 8/2003 for ''Aerosol and Cloud-Field Radiative Effects in the Tropical Western Pacific: Analyses and General Circulation Model Parameterizations''

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

Vogelmann, A. M.

OAK-B135 Final report from the University of California San Diego for an ongoing research project that was moved to Brookhaven National Laboratory where proposed work will be completed. The research uses measurements made by the Atmospheric Radiation Measurement (ARM) Program to quantify the effects of aerosols and clouds on the Earth's energy balance in the climatically important Tropical Western Pacific.

On the Specification of Smoke Injection Heights for Aerosol Forecasting

NASA Astrophysics Data System (ADS)

da Silva, A.; Schaefer, C.; Randles, C. A.

2014-12-01

The proper forecasting of biomass burning (BB) aerosols in global or regional transport models requires not only the specification of emission rates with sufficient temporal resolution but also the injection layers of such emissions. While current near realtime biomass burning inventories such as GFAS, QFED, FINN, GBBEP and FLAMBE provide such emission rates, it is left for each modeling system to come up with its own scheme for distributing these emissions in the vertical. A number of operational aerosol forecasting models deposits BB emissions in the near surface model layers, relying on the model's parameterization of turbulent and convective transport to determine the vertical mass distribution of BB aerosols. Despite their simplicity such schemes have been relatively successful reproducing the vertical structure of BB aerosols, except for those large fires that produce enough buoyancy to puncture the PBL and deposit the smoke at higher layers. Plume Rise models such as the so-called 'Freitas model', parameterize this sub-grid buoyancy effect, but require the specification of fire size and heat fluxes, none of which is readily available in near real-time from current remotely-sensed products. In this talk we will introduce a bayesian algorithm for estimating file size and heat fluxes from MODIS brightness temperatures. For small to moderate fires the Freitas model driven by these heat flux estimates produces plume tops that are highly correlated with the GEOS-5 model estimate of PBL height. Comparison to MINX plume height estimates from MISR indicates moderate skill of this scheme predicting the injection height of large fires. As an alternative, we make use of OMPS UV aerosol index data in combination with estimates of Overshooting Convective Tops (from MODIS and Geo-stationary satellites) to detect PyCu events and specify the BB emission vertical mass distribution in such cases. We will present a discussion of case studies during the SEAC4RS field campaign in August-September 2013.

Modeling the formation and aging of secondary organic aerosols in the Los Angeles metropolitan region during the CalNex 2010 field campaign

NASA Astrophysics Data System (ADS)

Hayes, P. L.; Ma, P. K.; Jimenez, J. L.; Zhao, Y.; Robinson, A. L.; Carlton, A. M. G.; Baker, K. R.; Ahmadov, R.; Washenfelder, R. A.; Alvarez, S. L.; Rappenglück, B.; Gilman, J.; Kuster, W.; De Gouw, J. A.; Prevot, A. S.; Zotter, P.; Szidat, S.; Kleindienst, T. E.; Offenberg, J. H.

2015-12-01

Several different literature parameterizations for the formation and evolution of urban secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles Region during CalNex. The model SOA formed only from the oxidation of VOCs (V-SOA) is insufficient to explain the observed SOA concentrations, even when using SOA parameterizations with multi-generation oxidation that produce much higher yields than have been observed in chamber experiments, or when increasing yields to their upper limit estimates accounting for recently reported losses of vapors to chamber walls. Including SOA from primary semi-volatile and intermediate volatility organic compounds (P-S/IVOCs) following the parameterizations of Robinson et al. (2007), Grieshop et al. (2009), or Pye and Seinfeld (2010) improves model/measurement agreement for mass concentration at shorter photochemical ages (0.5 days). Our results strongly suggest that other precursors besides VOCs are needed to explain the observed SOA concentrations. In contrast, all of the literature P-S/IVOC parameterizations over-predict urban SOA formation at long photochemical ages (3 days) compared to observations from multiple sites, which can lead to problems in regional and global modeling. Sensitivity studies that reduce the IVOC emissions by one-half in the model improve SOA predictions at these long ages. In addition, when IVOC emissions in the Robinson et al. parameterization are constrained using recently reported measurements of these species model/measurement agreement is achieved. The amounts of SOA mass from diesel vehicles, gasoline vehicles, and cooking emissions are estimated to be 16 - 27%, 35 - 61%, and 19 - 35%, respectively, depending on the parameterization used, which is consistent with the observed fossil fraction of urban SOA, 71(±3)%. The percentage of SOA from diesel vehicle emissions is the same, within the estimated uncertainty, as reported in previous work that analyzed the weekly cycles in SOA concentrations (Bahreini et al., 2012; Hayes et al., 2013). However, the modeling work presented here suggests a strong anthropogenic source of modern carbon in urban SOA, possibly cooking emissions, that was not accounted for in those previous studies, and which is higher on weekends.

A new method for multicomponent activity coefficients of electrolytes in aqueous atmospheric aerosols

NASA Astrophysics Data System (ADS)

Zaveri, Rahul A.; Easter, Richard C.; Wexler, Anthony S.

2005-01-01

Three-dimensional models of atmospheric inorganic aerosols need accurate and computationally efficient parameterizations of activity coefficients of various electrolytes in multicomponent aqueous solutions. In this paper, we extend the Taylor's series expansion mixing rule used by C. Wagner in 1952 for estimating activity coefficients in dilute alloy solutions to aqueous electrolyte solutions at any concentration. The resulting method, called the multicomponent Taylor expansion method (MTEM), estimates the mean activity coefficient of an electrolyte in a multicomponent solution on the basis of its values in binary solutions of all the electrolytes present in the mixture at the solution water activity aw, assuming aw is equal to the ambient relative humidity. MTEM is applied here for atmospheric aerosol systems containing H+, NH4+, Na+, Ca2+, SO42-, HSO4-, NO3-, and Cl- ions. The aerosol water content is calculated using the Zdanovskii-Stokes-Robinson (ZSR) method. For self-consistency, most of the MTEM and ZSR parameters are derived using the comprehensive Pitzer-Simonson-Clegg model at 298.15 K and are valid for an aw range of 0.2-0.97. Because CaSO4 is sparingly soluble, it is treated as a solid in the model over the entire aw range. MTEM is evaluated for several multicomponent systems representing various continental and marine aerosols and is contrasted against the mixing rule of C. L. Kusik and H. P. Meissner and of L. A. Bromley and the newer approach of S. Metzger and colleagues. Predictions of MTEM are found to be generally within a factor of 0.8-1.25 of the comprehensive Pitzer-Simonson-Clegg model and are shown to be significantly more accurate than predictions of the other three methods. MTEM also yields a noniterative solution of the bisulfate ion dissociation in sulfate-rich systems: a major computational advantage over other ionic-strength-based methods that require an iterative solution. CPU time requirements of MTEM relative to other methods for sulfate-poor and sulfate-rich systems are also discussed.

Implementing Marine Organic Aerosols Into the GEOS-Chem Model

NASA Technical Reports Server (NTRS)

Johnson, Matthew S.

2015-01-01

Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

Derivation of Aerosol Columnar Mass from MODIS Optical Depth

NASA Technical Reports Server (NTRS)

Gasso, Santiago; Hegg, Dean A.

2003-01-01

In order to verify performance, aerosol transport models (ATM) compare aerosol columnar mass (ACM) with those derived from satellite measurements. The comparison is inherently indirect since satellites derive optical depths and they use a proportionality constant to derive the ACM. Analogously, ATMs output a four dimensional ACM distribution and the optical depth is linearly derived. In both cases, the proportionality constant requires a direct intervention of the user by prescribing the aerosol composition and size distribution. This study introduces a method that minimizes the direct user intervention by making use of the new aerosol products of MODIS. A parameterization is introduced for the derivation of columnar aerosol mass (AMC) and CCN concentration (CCNC) and comparisons between sunphotometer, MODIS Airborne Simulator (MAS) and in-measurements are shown. The method still relies on the scaling between AMC and optical depth but the proportionality constant is dependent on the MODIS derived r$_{eff}$,\\eta (contribution of the accumulation mode radiance to the total radiance), ambient RH and an assumed constant aerosol composition. The CCNC is derived fkom a recent parameterization of CCNC as a function of the retrieved aerosol volume. By comparing with in-situ data (ACE-2 and TARFOX campaigns), it is shown that retrievals in dry ambient conditions (dust) are improved when using a proportionality constant dependent on r$ {eff}$ and \\eta derived in the same pixel. In high humidity environments, the improvement inthe new method is inconclusive because of the difficulty in accounting for the uneven vertical distribution of relative humidity. Additionally, two detailed comparisons of AMC and CCNC retrieved by the MAS algorithm and the new method are shown. The new method and MAS retrievals of AMC are within the same order of magnitude with respect to the in-situ measurements of aerosol mass. However, the proposed method is closer to the in-situ measurements than the MODIS retrievals. The retrievals of CCNC are also within the same order of magnitude for both methods. The new method is applied to an actual MODIS retrieval and although no in-situ data is available to compare, it is shown that the proposed method yields more credible values than the MODIS retrievals. In addition, recent data available from the PRIDE (Puerto Rico Dust Experiment, July 2000) will be shown by comparing sunphotometer, MODIS and in-situ data.

Modeling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

NASA Astrophysics Data System (ADS)

Karl, Matthias; Kukkonen, Jaakko; Keuken, Menno P.; Lützenkirchen, Susanne; Pirjola, Liisa; Hussein, Tareq

2016-04-01

This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of 1 h, i.e., on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using the aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i) the coagulation of particles, (ii) the condensation and evaporation of two organic vapors, and (iii) dry deposition. The chemical transformation of gas-phase compounds was not taken into account. By choosing concentrations and particle size distributions at roadside as starting point of the computations, nucleation of gas-phase vapors from the exhaust has been regarded as post tail-pipe emission, avoiding the need to include nucleation in the process analysis. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The error of the contribution from dry deposition to PN losses due to the uncertainty of measured deposition velocities ranges from -76 to +64 %. The removal of nanoparticles by coagulation enhanced considerably when considering the fractal nature of soot aggregates and the combined effect of van der Waals and viscous interactions. The effect of condensation and evaporation of organic vapors emitted by vehicles on particle numbers and on particle size distributions was examined. Under inefficient dispersion conditions, the model predicts that condensational growth contributes to the evolution of PN from roadside to the neighborhood scale. The simplified parameterization of aerosol processes predicts the change in particle number concentrations between roadside and urban background within 10 % of that predicted by the fully size-resolved MAFOR model.

Modeling East Asian Dust and Its Radiative Feedbacks in CAM4-BAM

NASA Astrophysics Data System (ADS)

Xie, Xiaoning; Liu, Xiaodong; Che, Huizheng; Xie, Xiaoxun; Wang, Hongli; Li, Jiandong; Shi, Zhengguo; Liu, Yangang

2018-01-01

East Asian dust and its radiative feedbacks are analyzed by the use of the fourth version of the Community Atmosphere Model (CAM4) with a bulk aerosol model parameterization (BAM) for the dust size distribution (CAM4-BAM). Two numerical experiments are conducted and intercompared: one with (Active) and one without (Passive) the radiative effects of dust aerosols. This CAM4-BAM captures the main spatial distribution of the dust aerosol optical depth (AOD) and the dust surface concentrations over East Asia, with positive correlations with the local observational data on annual and seasonal means. A comparative analysis of the Active and Passive experiments reveals that consideration of the dust-radiation interaction can significantly reduce dust emissions, loading, transport, and dry and wet depositions over East Asia, which is opposite to the enhanced dust cycle over North Africa. Further analysis of the contrasting dust-radiation feedbacks between North Africa and East Asia shows that over North Africa, the dust radiative forcing significantly increases the surface temperature and 10 m wind speed, whereas it decreases the surface temperature and the surface wind speeds over East Asia. These contrasting radiative effects, in turn, result in distinct dust cycle changes over these two regions. Mechanistic analysis reveals that the radiative contrasts between East Asia and North Africa are mainly due to the differences in their regional surface albedo, dust vertical distribution, and size distribution.

CCN Activity of Organic Aerosols Observed Downwind of Urban Emissions during CARES

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

Mei, Fan; Setyan, Ari; Zhang, Qi

2013-12-17

During the Carbonaceous Aerosols and Radiative Effects Study (CARES), activation fraction of size-resolved aerosol particles and aerosol chemical composition were characterized at the T1 site (~60 km downwind of Sacramento, California) from 10 June to 28 June 2010. The hygroscopicity of CCN-active particles (K CCN) with diameter from 100 to 170 nm, derived from the size-resolved activated fraction, varied from 0.10 to 0.21, with an average of 0.15, which was substantially lower than that proposed for continental sites in earlier studies. The low K CCN value was due to the high organic volume fraction, averaged over 80% at the T1more » site. The derived K CCN exhibited little diurnal variation, consistent with the relatively constant organic volume fraction observed. At any time, over 90% of the size selected particles with diameter between 100 and 171nm were CCN active, suggesting most particles within this size range were aged background particles. Due to the large organic volume fraction, organic hygroscopicity (K org) strongly impacted particle hygroscopicity and therefore calculated CCN concentration. For vast majority of the cases, an increase of K org from 0.03 to 0.18, which are within the typical range, doubled the calculated CCN concentration. Organic hygroscopicity was derived from K CCN and aerosol chemical composition, and its variations with the fraction of total organic mass spectral signal at m/z 44 (f 44) and O:C were compared to results from previous studies. Overall, the relationships between K org and f 44 are quite consistent for organic aerosol (OA) observed during field studies and those formed in smog chamber. Compared to the relationship between K org and f 44, the relationship between K org and O:C exhibits more significant differences among different studies, suggesting korg may be better parameterized using f 44. A least squares fit yielded K org = 2.10 (±0.07) × f 44 -0.11 (±0.01) with the Pearson R 2 value of 0.71. One possible explanation for the stronger correlation between K org and f 44 is that the m/z 44 signal (mostly contributed by the CO 2 + ion) is more closely related to organic acids, which may dominate the overall korg due to their relatively high water solubility and hygroscopicity.« less

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.

Chemical Imaging of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

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

O'Brien, Rachel; Wang, Bingbing; Laskin, Alexander

2015-09-28

A new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission x-ray microscopy/near edge x-ray absorption fine structure (STXM/NEXAFS) and computer controlled scanning electron microscopy/energy dispersive x-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on June 27th and 28th during the 2010 Carbonaceous Aerosols and Radiative Effects (CARES) study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierramore » Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. Both microscopy imaging techniques showed more changes over these two days in the mixing state at the T0 site than at the T1 site. The STXM data showed evidence of changes in the mixing state associated with a build-up of organic matter confirmed by collocated measurements and the largest impact on the mixing state was due to an increase in soot dominant particles during this build-up. The CCSEM/EDX analysis showed the presence of two types of particle populations; the first was dominated by aged sea salt particles and had a higher mixing state index (indicating a more homogeneous population), the second was dominated by carbonaceous particles and had a lower mixing state index.« less

Comparison of aerosol optical properties above clouds between POLDER and AeroCom models over the South East Atlantic Ocean during the fire season: POLDER/AeroCom Comparison Above Clouds

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

Peers, F.; Bellouin, N.; Waquet, F.

Aerosol properties above clouds have been retrieved over the South East Atlantic Ocean during the fire season 2006 using satellite observations from POLDER (Polarization and Directionality of Earth Reflectances). From June to October, POLDER has observed a mean Above-Cloud Aerosol Optical Thickness (ACAOT) of 0.28 and a mean Above-Clouds Single Scattering Albedo (ACSSA) of 0.87 at 550nm. These results have been used to evaluate the simulation of aerosols above clouds in 5 AeroCom (Aerosol Comparisons between Observations and Models) models (GOCART, HadGEM3, ECHAM5-HAM2, OsloCTM2 and SPRINTARS). Most models do not reproduce the observed large aerosol load episodes. The comparison highlightsmore » the importance of the injection height and the vertical transport parameterizations to simulate the large ACAOT observed by POLDER. Furthermore, some models overestimate the ACSSA. In accordance with recent recommendations of the black carbon refractive index, a higher prescription of the imaginary part allows a better comparison with POLDER’s ACSSA.« less

Modeling the formation and aging of secondary organic aerosols in Los Angeles during CalNex 2010

NASA Astrophysics Data System (ADS)

Hayes, P. L.; Carlton, A. G.; Baker, K. R.; Ahmadov, R.; Washenfelder, R. A.; Alvarez, S.; Rappenglück, B.; Gilman, J. B.; Kuster, W. C.; de Gouw, J. A.; Zotter, P.; Prévôt, A. S. H.; Szidat, S.; Kleindienst, T. E.; Offenberg, J. H.; Jimenez, J. L.

2014-12-01

Four different parameterizations for the formation and evolution of secondary organic aerosol (SOA) are evaluated using a 0-D box model representing the Los Angeles Metropolitan Region during the CalNex 2010 field campaign. We constrain the model predictions with measurements from several platforms and compare predictions with particle and gas-phase observations from the CalNex Pasadena ground site. That site provides a unique opportunity to study aerosol formation close to anthropogenic emission sources with limited recirculation. The model SOA formed only from the oxidation of VOCs (V-SOA) is insufficient to explain the observed SOA concentrations, even when using SOA parameterizations with multi-generation oxidation that produce much higher yields than have been observed in chamber experiments, or when increasing yields to their upper limit estimates accounting for recently reported losses of vapors to chamber walls. The Community Multiscale Air Quality (WRF-CMAQ) model (version 5.0.1) provides excellent predictions of secondary inorganic particle species but underestimates the observed SOA mass by a factor of 25 when an older VOC-only parameterization is used, which is consistent with many previous model-measurement comparisons for pre-2007 anthropogenic SOA modules in urban areas. Including SOA from primary semi-volatile and intermediate volatility organic compounds (P-S/IVOCs) following the parameterizations of Robinson et al. (2007), Grieshop et al. (2009), or Pye and Seinfeld (2010) improves model/measurement agreement for mass concentration. When comparing the three parameterizations, the Grieshop et al. (2009) parameterization more accurately reproduces both the SOA mass concentration and oxygen-to-carbon ratio inside the urban area. Our results strongly suggest that other precursors besides VOCs, such as P-S/IVOCs, are needed to explain the observed SOA concentrations in Pasadena. All the parameterizations over-predict urban SOA formation at long photochemical ages (≈ 3 days) compared to observations from multiple sites, which can lead to problems in regional and global modeling. Among the explicitly modeled VOCs, the precursor compounds that contribute the greatest SOA mass are methylbenzenes. Polycyclic aromatic hydrocarbons (PAHs) are less important precursors and contribute less than 4% of the SOA mass. The amounts of SOA mass from diesel vehicles, gasoline vehicles, and cooking emissions are estimated to be 16-27, 35-61, and 19-35%, respectively, depending on the parameterization used, which is consistent with the observed fossil fraction of urban SOA, 71 (±3) %. In-basin biogenic VOCs are predicted to contribute only a few percent to SOA. A regional SOA background of approximately 2.1 μg m-3 is also present due to the long distance transport of highly aged OA. The percentage of SOA from diesel vehicle emissions is the same, within the estimated uncertainty, as reported in previous work that analyzed the weekly cycles in OA concentrations (Bahreini et al., 2012; Hayes et al., 2013). However, the modeling work presented here suggests a strong anthropogenic source of modern carbon in SOA, due to cooking emissions, which was not accounted for in those previous studies. Lastly, this work adapts a simple two-parameter model to predict SOA concentration and O/C from urban emissions. This model successfully predicts SOA concentration, and the optimal parameter combination is very similar to that found for Mexico City. This approach provides a computationally inexpensive method for predicting urban SOA in global and climate models. We estimate pollution SOA to account for 26 Tg yr-1 of SOA globally, or 17% of global SOA, 1/3 of which is likely to be non-fossil.

Heterogeneous formation of nitryl chloride and its role as a nocturnal NOx reservoir species during CalNex-LA 2010

NASA Astrophysics Data System (ADS)

Mielke, L. H.; Stutz, J.; Tsai, C.; Hurlock, S. C.; Roberts, J. M.; Veres, P. R.; Froyd, K. D.; Hayes, P. L.; Cubison, M. J.; Jimenez, J. L.; Washenfelder, R. A.; Young, C. J.; Gilman, J. B.; de Gouw, J. A.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Liu, J.; Weber, R. J.; Osthoff, H. D.

2013-09-01

nocturnal conversion of dinitrogen pentoxide (N2O5) to nitryl chloride (ClNO2) on chloride-containing aerosol can be a regionally important NOx (= NO + NO2) recycling and halogen activation pathway that affects oxidant photochemistry the following day. Here we present a comprehensive measurement data set acquired at Pasadena, California, during the CalNex-LA campaign 2010 that included measurements of odd nitrogen and its major components (NOy = NOx + NO3 + 2N2O5 + ClNO2 + HNO3 + HONO + peroxyacyl, alkyl, and aerosol nitrates) and aerosol size distribution and composition. Nitryl chloride was present during every night of the study (median mixing ratio at sunrise 800 pptv) and was usually a more significant nocturnal NOx and odd oxygen (Ox = O3 + NO2 + 3N2O5 + ClNO2) reservoir species than N2O5 (whose concentrations were calculated from its equilibrium with NO2 and NO3). At sunrise, ClNO2 accounted for 21% of NOz (=NOy - NOx), 4% of NOy, and 2.5% of Ox, respectively (median values). Kinetic parameters for the N2O5 to ClNO2 conversion were estimated by relating ClNO2 concentrations to their time-integrated heterogeneous production from N2O5 and were highly variable between nights. Production of ClNO2 required conversion of N2O5 on submicron aerosol with average yield (φ) and N2O5 reactive uptake probability (γ) of γφ = 0.008 (maximum 0.04), scaled with submicron aerosol chloride content, and was suppressed by aerosol organic matter and liquid water content. Not all of the observed variability of ClNO2 production efficiency could be rationalized using current literature parameterizations.

Characterization of Ice Nucleating Particles at the Western US Coast

NASA Astrophysics Data System (ADS)

Rocci, K.; McCluskey, C. S.; Hill, T. C. J.; DeMott, P. J.; Kreidenweis, S. M.

2015-12-01

In temperate climates, ice nucleating particles (INPs) are vital for precipitation initiation. Because INPs may affect precipitation efficiency, and thereby the supply of water resources, it is paramount to have a clear understanding of both natural and anthropogenic sources of INPs. This is especially important to understand in California where drought continues to be a major problem. The CalWater 2015 field campaign, which took place in California from January 15 - March 9, 2015, included comprehensive characterizations of aerosols and their ice nucleating ability via ground-, air-, and ship-based measurements. As part of this campaign, we characterized and analyzed the intra-air mass differences of INPs at a coastal site (Bodega Bay) using immersion freezing measurements of particles collected on filters. Aerosol filters collected throughout the campaign were characterized by their loading and dominant type using meteorology, aerosol size distributions, aerosol composition, and trace gas concentration data. Samples contained a variety of aerosol influences, including biomass burning, nitrogen pollution, sulfur pollution, and sea spray. This study had a particular focus on the INP activity spectra of sea spray aerosol (SSA). We used the online aerosol data to infer variations in SSA types and heat-treated specific samples to look for the presence of heat-labile biological INPs. Furthermore, we ran the NOAA HYSPLIT model to obtain back trajectories for samples dominated by SSA. We found that air masses dominated by distinct terrestrial source types are not well distinguished by their INP number concentrations. However, we did see significantly higher (up to 5000-fold) INP number concentrations in SSA samples taken at the coast compared with number concentrations in samples obtained over open ocean. This difference could be attributable to differences in overall aerosol abundance, which will be evaluated in future studies. Overall, our findings suggest that an ocean-specific INP parameterization is needed for oceanic emissions and that terrestrial INP sources strongly impact the ice nucleating ability of marine boundary air.

Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions

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

Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona

2009-11-01

Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of particular interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation with respect to liquid water similar to atmospheric conditions. In this study the sub-saturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols was determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as wellmore » as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were used. Aerosols were generated both with a wet and a dry disperser and the water uptake was parameterized via the hygroscopicity parameter, κ. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived κ values between 0.00 and 0.02. The latter value can be idealized as a particle consisting of 96.7% (by volume) insoluble material and ~3.3% ammonium sulfate. Pure clay aerosols were found to be generally less hygroscopic than real desert dust particles. All illite and montmorillonite samples had κ~0.003, kaolinites were least hygroscopic and had κ=0.001. SD (κ=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (κ=0.007) and ATD (κ=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles while immersed in an aqueous medium during atomization, thus indicating that specification of the generation method is critically important when presenting such data. Any atmospheric processing of fresh mineral dust which leads to the addition of more than ~3% soluble material is expected to significantly enhance hygroscopicity and CCN activity.« less

What We Can Say About the Roles of Natural and Anthropogenic Aerosols in Climate Change

NASA Astrophysics Data System (ADS)

Kahn, Ralph

2016-07-01

Although particles from natural sources dominate the globally averaged aerosol load, it is widely understood that human activity has added significantly to the atmospheric aerosol inventory in many regions. Anthropogenic contributions include pollution particles from industrial activity, transportation, cook-stoves, and other combustion sources, smoke from agricultural fires and those wildfires that result from land-management practices, soil and mineral dust mobilized in regions where overgrazing, severe tilling, or overuse of surface water resources have occurred, and biogenic particles from vegetation planted and maintained by the populance. The history of human influence is complex - in the 18th and 19th centuries agricultural burning tended to dominate the anthropogenic component in most places, whereas more recently, fossil fuel combustion leads the human contribution is many areas. However, identifying and quantifying the anthropogenic aerosol component on global scales is a challenging endeavor at present. Most estimates of the anthropogenic component come from aerosol transport models that are initialized with aerosol and precursor-gas source locations, emission strengths, and injection heights. The aerosol is then advected based on meteorological modeling, possibly modified chemically or physically, and removed by parameterized wet or dry deposition processes. Aerosol effects on clouds are also represented in some climate models, but with even greater uncertainty than the direct aerosol effects on Earth's radiation balance. Even for present conditions, aerosol source inventories are deduced from whatever constraints can be found, along with much creativity and many assumptions. Aerosol amount (i.e., aerosol optical depth) is routinely measured globally from space, but observational constraints on the anthropogenic component require some knowledge of the aerosol type as well, a much more difficult quantity to derive. As large-swath, multi-spectral, single-view instruments such as MODIS can provide some information about fine-mode vs. coarse-mode dominated aerosol over dark water, early efforts to constrain aerosol type assumed that some or all the fine-mode fraction is anthropogenic. However, this information is not sufficient to make the key anthropogenic vs. natural distinction in most places where the likely answer is not already known. Instruments providing more detailed measurements, such as multi-spectral, multi-angle and polarimetric imagers and multi-channel lidars, can offer tighter aerosol-type constraints in some circumstances, though generally not enough to specifically identify anthropogenic aerosols. The best we seem to be able to do with current data is to combine satellite and suborbital observations with models. And for the "pre-industrial" period, the analogy is usually made to the "natural" component of present-day aerosol, although there are ambiguities in our ability to distinguish natural from anthropogenic particles on regional-to-global scales, and the natural component itself might have changed over time. This talk will review where we stand, and what might be possible to say in the future.

Aerosol Retrievals Using Channel 1 and 2 AVHRR Data

NASA Technical Reports Server (NTRS)

Mishchenko, Michael I.; Geogdzhayev, Igor V.; Cairns, Brian; Rossow, William B.

1999-01-01

The effect of tropospheric aerosols on global climate via the direct and indirect radiative forcings is one of the largest remaining uncertainties in climate change studies. Current assessments of the direct aerosol radiative effect mainly focus on sulfate aerosols. It has become clear, however, that other aerosol types like soil dust and smoke from biomass burning are also likely to be important climate forcing factors. The magnitude and even the sign of the climate forcing caused by these aerosol types is still unknown. General circulation models (GCMs) can be used to estimate the climatic effect of the direct radiative forcing by tropospheric and stratospheric aerosols. Aerosol optical properties are already parameterized in the Goddard Institute for Space Studies GCM. Once the global distribution of aerosol properties (optical thickness, size distribution, and chemical composition) is available, the calculation of the direct aerosol forcing is rather straighfforward. However, estimates of the indirect aerosol effect require additional knowledge of the physics and chemistry of aerosol-cloud interactions which are still poorly understood. One of the main objectives of the Global Aerosol Climatology Project, established in 1998 as a joint initiative of NASA's Radiation Science Program and GEWEX, is to infer the global distribution of aerosols, their properties, and their seasonal and interannual variations for the full period of available satellite data. This will be accomplished primarily through a systematic application of multichannel aerosol retrieval algorithms to existing satellite data and advanced 3-dimensional aerosol chemistry/transport models. In this paper we outline the methodology of analyzing channel 1 and 2 AVHRR radiance data over the oceans and describe preliminary retrieval results.

On the controls of deep convection and lightning in the Amazon

NASA Astrophysics Data System (ADS)

Albrecht, R. I.; Giangrande, S. E.; Wang, D.; Morales, C. A.; Pereira, R. F. O.; Machado, L.; Silva Dias, M. A. F.

2017-12-01

Local observations and remote sensing have been extensively used to unravel cloud distribution and life cycle but yet their representativeness in cloud resolve models (CRMs) and global climate models (GCMs) are still very poor. In addition, the complex cloud-aerosol-precipitation interactions (CAPI), as well as thermodynamics, dynamics and large scale controls on convection have been the focus of many studies in the last two decades but still no final answer has been reached on the overall impacts of these interactions and controls on clouds, especially on deep convection. To understand the environmental and CAPI controls of deep convection, cloud electrification and lightning activity in the pristine region of Amazon basin, in this study we use long term satellite and field campaign measurements to depict the characteristics of deep convection and the relationships between lightning and convective fluxes in this region. Precipitation and lightning activity from the Tropical Rainfall Measuring Mission (TRMM) satellite are combined with estimates of aerosol concentrations and reanalysis data to delineate the overall controls on thunderstorms. A more detailed analysis is obtained studying these controls on the relationship between lightning activity and convective mass fluxes using radar wind profiler and 3D total lightning during GoAmazon 2014/15 field campaign. We find evidences that the large scale conditions control the distribution of the precipitation, with widespread and more frequent mass fluxes of moderate intensity during the wet season, resulting in less vigorous convection and lower lightning activity. Under higher convective available potential energy, lightning is enhanced in polluted and background aerosol conditions. The relationships found in this study can be used in model parameterizations and ensemble evaluations of both lightning activity and lightning NOx from seasonal forecasting to climate projections and in a broader sense to Earth Climate System Modeling.

Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

NASA Astrophysics Data System (ADS)

Zhou, C.; Zhang, X.; Gong, S.; Wang, Y.; Xue, M.

2016-01-01

A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under a China Meteorological Administration (CMA) chemical weather modeling system, GRAPES/CUACE (Global/Regional Assimilation and PrEdiction System, CMA Unified Atmospheric Chemistry Environment). Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) are interactively fed online into a two-moment cloud scheme (WRF Double-Moment 6-class scheme - WDM6) and a convective parameterization to drive cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred.

The results show that aerosols that interact with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content, and cloud droplet number concentrations, while decreasing the mean diameters of cloud droplets with varying magnitudes of the changes in each case and region. These interactive microphysical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24 to 48 % enhancements of threat score for 6 h precipitation in almost all regions. The aerosols that interact with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3 °C.

Simulated cold bias being improved by using MODIS time-varying albedo in the Tibetan Plateau in WRF model

NASA Astrophysics Data System (ADS)

Meng, X.; Lyu, S.; Zhang, T.; Zhao, L.; Li, Z.; Han, B.; Li, S.; Ma, D.; Chen, H.; Ao, Y.; Luo, S.; Shen, Y.; Guo, J.; Wen, L.

2018-04-01

Systematic cold biases exist in the simulation for 2 m air temperature in the Tibetan Plateau (TP) when using regional climate models and global atmospheric general circulation models. We updated the albedo in the Weather Research and Forecasting (WRF) Model lower boundary condition using the Global LAnd Surface Satellite Moderate-Resolution Imaging Spectroradiometer albedo products and demonstrated evident improvement for cold temperature biases in the TP. It is the large overestimation of albedo in winter and spring in the WRF model that resulted in the large cold temperature biases. The overestimated albedo was caused by the simulated precipitation biases and over-parameterization of snow albedo. Furthermore, light-absorbing aerosols can result in a large reduction of albedo in snow and ice cover. The results suggest the necessity of developing snow albedo parameterization using observations in the TP, where snow cover and melting are very different from other low-elevation regions, and the influence of aerosols should be considered as well. In addition to defining snow albedo, our results show an urgent call for improving precipitation simulation in the TP.

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.

Easy Volcanic Aerosol (EVA v1.0): an idealized forcing generator for climate simulations

NASA Astrophysics Data System (ADS)

Toohey, Matthew; Stevens, Bjorn; Schmidt, Hauke; Timmreck, Claudia

2016-11-01

Stratospheric sulfate aerosols from volcanic eruptions have a significant impact on the Earth's climate. To include the effects of volcanic eruptions in climate model simulations, the Easy Volcanic Aerosol (EVA) forcing generator provides stratospheric aerosol optical properties as a function of time, latitude, height, and wavelength for a given input list of volcanic eruption attributes. EVA is based on a parameterized three-box model of stratospheric transport and simple scaling relationships used to derive mid-visible (550 nm) aerosol optical depth and aerosol effective radius from stratospheric sulfate mass. Precalculated look-up tables computed from Mie theory are used to produce wavelength-dependent aerosol extinction, single scattering albedo, and scattering asymmetry factor values. The structural form of EVA and the tuning of its parameters are chosen to produce best agreement with the satellite-based reconstruction of stratospheric aerosol properties following the 1991 Pinatubo eruption, and with prior millennial-timescale forcing reconstructions, including the 1815 eruption of Tambora. EVA can be used to produce volcanic forcing for climate models which is based on recent observations and physical understanding but internally self-consistent over any timescale of choice. In addition, EVA is constructed so as to allow for easy modification of different aspects of aerosol properties, in order to be used in model experiments to help advance understanding of what aspects of the volcanic aerosol are important for the climate system.

The Secondary Organic Aerosol Processor (SOAP v1.0) model: a unified model with different ranges of complexity based on the molecular surrogate approach

NASA Astrophysics Data System (ADS)

Couvidat, F.; Sartelet, K.

2015-04-01

In this paper the Secondary Organic Aerosol Processor (SOAP v1.0) model is presented. This model determines the partitioning of organic compounds between the gas and particle phases. It is designed to be modular with different user options depending on the computation time and the complexity required by the user. This model is based on the molecular surrogate approach, in which each surrogate compound is associated with a molecular structure to estimate some properties and parameters (hygroscopicity, absorption into the aqueous phase of particles, activity coefficients and phase separation). Each surrogate can be hydrophilic (condenses only into the aqueous phase of particles), hydrophobic (condenses only into the organic phases of particles) or both (condenses into both the aqueous and the organic phases of particles). Activity coefficients are computed with the UNIFAC (UNIversal Functional group Activity Coefficient; Fredenslund et al., 1975) thermodynamic model for short-range interactions and with the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) parameterization for medium- and long-range interactions between electrolytes and organic compounds. Phase separation is determined by Gibbs energy minimization. The user can choose between an equilibrium representation and a dynamic representation of organic aerosols (OAs). In the equilibrium representation, compounds in the particle phase are assumed to be at equilibrium with the gas phase. However, recent studies show that the organic aerosol is not at equilibrium with the gas phase because the organic phases could be semi-solid (very viscous liquid phase). The condensation-evaporation of organic compounds could then be limited by the diffusion in the organic phases due to the high viscosity. An implicit dynamic representation of secondary organic aerosols (SOAs) is available in SOAP with OAs divided into layers, the first layer being at the center of the particle (slowly reaches equilibrium) and the final layer being near the interface with the gas phase (quickly reaches equilibrium). Although this dynamic implicit representation is a simplified approach to model condensation-evaporation with a low number of layers and short CPU (central processing unit) time, it shows good agreements with an explicit representation of condensation-evaporation (no significant differences after a few hours of condensation).

Constraining Aerosol-Cloud-Precipitation Interactions of Orographic Mixed-Phase Clouds with Trajectory Budgets

NASA Astrophysics Data System (ADS)

Glassmeier, F.; Lohmann, U.

2016-12-01

Orographic precipitation is prone to strong aerosol-cloud-precipitation interactions because the time for precipitation development is limited to the ascending section of mountain flow. At the same time, cloud microphysical development is constraint by the strong dynamical forcing of the orography. In this contribution, we discuss how changes in the amount and composition of droplet- and ice-forming aerosols influence precipitation in idealized simulations of stratiform orographic mixed-phase clouds. We find that aerosol perturbations trigger compensating responses of different precipitation formation pathways. The effect of aerosols is thus buffered. We explain this buffering by the requirement to fulfill aerosol-independent dynamical constraints. For our simulations, we use the regional atmospheric model COSMO-ART-M7 in a 2D setup with a bell-shaped mountain. The model is coupled to a 2-moment warm and cold cloud microphysics scheme. Activation and freezing rates are parameterized based on prescribed aerosol fields that are varied in number, size and composition. Our analysis is based on the budget of droplet water along trajectories of cloud parcels. The budget equates condensation as source term with precipitation formation from autoconversion, accretion, riming and the Wegener-Bergeron-Findeisen process as sink terms. Condensation, and consequently precipitation formation, is determined by dynamics and largely independent of the aerosol conditions. An aerosol-induced change in the number of droplets or crystals perturbs the droplet budget by affecting precipitation formation processes. We observe that this perturbation triggers adjustments in liquid and ice water content that re-equilibrate the budget. As an example, an increase in crystal number triggers a stronger glaciation of the cloud and redistributes precipitation formation from collision-coalescence to riming and from riming to vapor deposition. We theoretically confirm the dominant effect of water content adjustments over number changes by estimating susceptibilities d ln P / d ln N of precipitation formation P to droplet or crystal number N from the budget equation. The susceptibility analysis also reveals that aerosol perturbations to droplet and crystal number compensate each other.

Analysis of CCN activity of Remote and Combustion Aerosol over the South East Pacific during autumn 2008 and links to Sc cloud properties

NASA Astrophysics Data System (ADS)

Freitag, S.; Clarke, A. D.; Howell, S. G.; Twohy, C. H.; Snider, J. R.; Toohey, D. W.; Shank, L.; McNaughton, C. S.; Brekhovskikh, V.; Kapustin, V.

2013-12-01

The earth's most extensive Stratocumulus (Sc) deck, situated off the coast of Northern Chile and Southern Peru, strongly influences the radiation budget and climate over the South East Pacific (SEP) by enhancing solar reflection. This feature makes Sc clouds an important constituent for climate modeling, yet these clouds are poorly represented in models. A large uncertainty in understanding the variability in these low cloud fields arises from our deficit in understanding the role of aerosol. Hence, a major goal of the VOCALS (www.eol.ucar.edu/projects/vocals) campaign in 2008 was to further explore and assess interactions of natural and anthropogenic aerosol with Sc clouds in both the more polluted coastal environment and west of 80W where we encountered nearly pristine boundary layer clouds often exposed to cloud-top entrainment of pollution aerosol from the free troposphere. Extensive airborne measurements of size-resolved aerosol volatility and chemical composition collected aboard the NCAR C-130 were analyzed with an aerosol mass spectrometer (AMS) and a single particle soot photometer (SP2) to calculate aerosol hygroscopicity (κ) and predict cloud condensation nuclei (CCN) concentration for all observed air mass types above and below cloud utilizing estimated Sc cloud supersaturations deduced from cloud-processed aerosol size distribution information. The predicted CCN agree to within 10% to measured CCN. Results from this analysis are presented here and CCN variability observed along VOCALS flight tracks is discussed in conjunction with size-resolved cloud droplet information. This includes assessing the impact of aerosol perturbations on the shape of the cloud droplet size distribution parameterized in models and satellite algorithms such as cloud top effective radius retrievals. We will further discuss cloud droplet residual composition collected using a counterflow virtual impactor (CVI) and analyzed with the AMS and SP2. Size resolved variations in residual composition and its relation to CCN composition measured outside the cloud will be examined in terms of the influence of aerosol concentration, size, and chemical composition on Sc clouds.

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

NASA Astrophysics Data System (ADS)

Zhang, K.; O'Donnell, D.; Kazil, J.; Stier, P.; Kinne, S.; Lohmann, U.; Ferrachat, S.; Croft, B.; Quaas, J.; Wan, H.; Rast, S.; Feichter, J.

2012-10-01

This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Nudged simulations of the year 2000 are carried out to compare the aerosol properties and global distribution in HAM1 and HAM2, and to evaluate them against various observations. Sensitivity experiments are performed to help identify the impact of each individual update in model formulation. Results indicate that from HAM1 to HAM2 there is a marked weakening of aerosol water uptake in the lower troposphere, reducing the total aerosol water burden from 75 Tg to 51 Tg. The main reason is the newly introduced κ-Köhler-theory-based water uptake scheme uses a lower value for the maximum relative humidity cutoff. Particulate organic matter loading in HAM2 is considerably higher in the upper troposphere, because the explicit treatment of secondary organic aerosols allows highly volatile oxidation products of the precursors to be vertically transported to regions of very low temperature and to form aerosols there. Sulfate, black carbon, particulate organic matter and mineral dust in HAM2 have longer lifetimes than in HAM1 because of weaker in-cloud scavenging, which is in turn related to lower autoconversion efficiency in the newly introduced two-moment cloud microphysics scheme. Modification in the sea salt emission scheme causes a significant increase in the ratio (from 1.6 to 7.7) between accumulation mode and coarse mode emission fluxes of aerosol number concentration. This leads to a general increase in the number concentration of smaller particles over the oceans in HAM2, as reflected by the higher Ångström parameters. Evaluation against observation reveals that in terms of model performance, main improvements in HAM2 include a marked decrease of the systematic negative bias in the absorption aerosol optical depth, as well as smaller biases over the oceans in Ångström parameter and in the accumulation mode number concentration. The simulated geographical distribution of aerosol optical depth (AOD) is better correlated with the MODIS data, while the surface aerosol mass concentrations are very similar to those in the old version. The total aerosol water content in HAM2 is considerably closer to the multi-model average from Phase I of the AeroCom intercomparison project. Model deficiencies that require further efforts in the future include (i) positive biases in AOD over the ocean, (ii) negative biases in AOD and aerosol mass concentration in high-latitude regions, and (iii) negative biases in particle number concentration, especially that of the Aitken mode, in the lower troposphere in heavily polluted regions.

Potential contribution of semi-volatile and intermediate volatility primary organic compounds to secondary organic aerosol in the Mexico City region

NASA Astrophysics Data System (ADS)

Hodzic, A.; Jimenez, J. L.; Madronich, S.; Canagaratna, M. R.; Decarlo, P. F.; Kleinman, L.; Fast, J.

2010-01-01

It has been established that observed local and regional levels of secondary organic aerosols (SOA) in polluted areas cannot be explained by the oxidation and partitioning of anthropogenic and biogenic VOC precursors, at least using current mechanisms and parameterizations. In this study, the 3-D regional air quality model CHIMERE is applied to quantify the contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic vapors (S/IVOC) in and around Mexico City for the MILAGRO field experiment during March 2006. The model has been updated to include explicitly the volatility distribution of primary organic aerosols (POA), their gas-particle partitioning and the gas-phase oxidation of the vapors. Two recently proposed parameterizations, those of Robinson et al. (2007) ("ROB") and Grieshop et al. (2009) ("GRI") are compared and evaluated against surface and aircraft measurements. The 3-D model results are assessed by comparing with the concentrations of OA components from Positive Matrix Factorization of Aerosol Mass Spectrometer (AMS) data, and for the first time also with oxygen-to-carbon ratios derived from high-resolution AMS measurements. The results show a substantial enhancement in predicted SOA concentrations (3-6 times) with respect to the previously published base case without S/IVOCs (Hodzic et al., 2009), both within and downwind of the city leading to much reduced discrepancies with the total OA measurements. The predicted anthropogenic POA levels are found to agree within 20% with the observed HOA concentrations for both the ROB and GRI simulations, consistent with the interpretation of the emissions inventory by previous studies. The impact of biomass burning POA within the city is underestimated in comparison to the AMS BBOA, presumably due to insufficient nighttime smoldering emissions. Model improvements in OA predictions are associated with the better-captured SOA magnitude and diurnal variability. The predicted production from anthropogenic and biomass burning S/IVOC represents 40-60% of the total SOA at the surface during the day and is somewhat larger than that from aromatics, especially at the T1 site at the edge of the city. The SOA production from the continued multi-generation S/IVOC oxidation products continues actively downwind. Similar to aircraft observations, the predicted OA/ΔCO ratio for the ROB case increases from 20-30 μg sm-3 ppm-1 up to 60-70 μg sm-3 ppm-1 between a fresh and 1-day aged air mass, while the GRI case produces a 30-40% higher OA growth than observed. The predicted average O/C ratio of total OA for the ROB case is 0.16 at T0, substantially below observed value of 0.5. A much better agreement for O/C ratios and temporal variability (R2=0.63) is achieved with the updated GRI treatment. Both treatments show a deficiency in regard to POA evolution with a tendency to over-evaporate POA upon dilution of the urban plume suggesting that atmospheric HOA may be less volatile than assumed in these parameterizations. This study highlights the important potential role of S/IVOC chemistry in the SOA budget in this region, and highlights the need for improvements in current parameterizations. We note that our simulations did not include other proposed pathways of SOA formation such as formation from very volatile species like glyoxal, which can also contribute SOA mass and especially increase the O/C ratio.

An Overview of Atmospheric Composition OSSE Activities at NASA's Global Modeling and Assimilation Office

NASA Technical Reports Server (NTRS)

daSilva, Arlinda

2012-01-01

A model-based Observing System Simulation Experiment (OSSE) is a framework for numerical experimentation in which observables are simulated from fields generated by an earth system model, including a parameterized description of observational error characteristics. Simulated observations can be used for sampling studies, quantifying errors in analysis or retrieval algorithms, and ultimately being a planning tool for designing new observing missions. While this framework has traditionally been used to assess the impact of observations on numerical weather prediction, it has a much broader applicability, in particular to aerosols and chemical constituents. In this talk we will give a general overview of Observing System Simulation Experiments (OSSE) activities at NASA's Global Modeling and Assimilation Office, with focus on its emerging atmospheric composition component.

Season-dependent size distribution of aerosols over the tropical coastal environment of south-west India

NASA Astrophysics Data System (ADS)

Aryasree, S.; Nair, Prabha R.

2018-01-01

This paper presents the results of a detailed study on the size characteristics of aerosols at the tropical coastal site Thiruvananthapuram based on the in-situ measurements of size resolved aerosol number density using an aerosol spectrometer, covering a period of 28 months from September 2011 to December 2013. The diurnal pattern of aerosol number density is characterized by day time low and a two-fold increase during nighttime and these changes are closely associated with the strong mesoscale features namely the sea breeze and land breeze prevailing at the site. Aerosol Number Size Distribution (NSD) depicts a multi-modal nature with two prominent modes, one ≤0.1 μm and other ∼1 μm. Two other less pronounced modes are also observed in the NSD, one ∼0.3-0.5 μm and other ∼5-8 μm. The NSDs also exhibited strong seasonal changes linked with the synoptic meteorological feature of this region namely the South Asian monsoon. The seasonal NSDs were parameterized and analyzed. In addition to this, the effects of meteorological parameters temperature, relative humidity, and wind speed and airflow patterns on aerosol number density as revealed by partial correlation analysis were found to be aerosol size dependent.

Implementing marine organic aerosols into the GEOS-Chem model

DOE PAGES

Gantt, B.; Johnson, M. S.; Crippa, M.; ...

2015-03-17

Marine-sourced organic aerosols (MOAs) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem (Global Earth Observing System Chemistry) model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Modelmore » predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOAs observed during the summertime at an inland site near Paris, France. Our study shows that MOAs have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having >10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.« less

Indian summer monsoon rainfall: Dancing with the tunes of the sun

NASA Astrophysics Data System (ADS)

Hiremath, K. M.; Manjunath, Hegde; Soon, Willie

2015-02-01

There is strong statistical evidence that solar activity influences the Indian summer monsoon rainfall. To search for a physical link between the two, we consider the coupled cloud hydrodynamic equations, and derive an equation for the rate of precipitation that is similar to the equation of a forced harmonic oscillator, with cloud and rain water mixing ratios as forcing variables. Those internal forcing variables are parameterized in terms of the combined effect of external forcing as measured by sunspot and coronal hole activities with several well known solar periods (9, 13 and 27 days; 1.3, 5, 11 and 22 years). The equation is then numerically solved and the results show that the variability of the simulated rate of precipitation captures very well the actual variability of the Indian monsoon rainfall, yielding vital clues for a physical understanding that has so far eluded analyses based on statistical correlations alone. We also solved the precipitation equation by allowing for the effects of long-term variation of aerosols. We tentatively conclude that the net effects of aerosols variation are small, when compared to the solar factors, in terms of explaining the observed rainfall variability covering the full Indian monsoonal geographical domains.

Uncertainty in Modeling Dust Mass Balance and Radiative Forcing from Size Parameterization

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

Zhao, Chun; Chen, Siyu; Leung, Lai-Yung R.

2013-11-05

This study examines the uncertainties in simulating mass balance and radiative forcing of mineral dust due to biases in the aerosol size parameterization. Simulations are conducted quasi-globally (180oW-180oE and 60oS-70oN) using the WRF24 Chem model with three different approaches to represent aerosol size distribution (8-bin, 4-bin, and 3-mode). The biases in the 3-mode or 4-bin approaches against a relatively more accurate 8-bin approach in simulating dust mass balance and radiative forcing are identified. Compared to the 8-bin approach, the 4-bin approach simulates similar but coarser size distributions of dust particles in the atmosphere, while the 3-mode pproach retains more finemore » dust particles but fewer coarse dust particles due to its prescribed og of each mode. Although the 3-mode approach yields up to 10 days longer dust mass lifetime over the remote oceanic regions than the 8-bin approach, the three size approaches produce similar dust mass lifetime (3.2 days to 3.5 days) on quasi-global average, reflecting that the global dust mass lifetime is mainly determined by the dust mass lifetime near the dust source regions. With the same global dust emission (~6000 Tg yr-1), the 8-bin approach produces a dust mass loading of 39 Tg, while the 4-bin and 3-mode approaches produce 3% (40.2 Tg) and 25% (49.1 Tg) higher dust mass loading, respectively. The difference in dust mass loading between the 8-bin approach and the 4-bin or 3-mode approaches has large spatial variations, with generally smaller relative difference (<10%) near the surface over the dust source regions. The three size approaches also result in significantly different dry and wet deposition fluxes and number concentrations of dust. The difference in dust aerosol optical depth (AOD) (a factor of 3) among the three size approaches is much larger than their difference (25%) in dust mass loading. Compared to the 8-bin approach, the 4-bin approach yields stronger dust absorptivity, while the 3-mode approach yields weaker dust absorptivity. Overall, on quasi-global average, the three size parameterizations result in a significant difference of a factor of 2~3 in dust surface cooling (-1.02~-2.87 W m-2) and atmospheric warming (0.39~0.96 W m-2) and in a tremendous difference of a factor of ~10 in dust TOA cooling (-0.24~-2.20 W m-2). An uncertainty of a factor of 2 is quantified in dust emission estimation due to the different size parameterizations. This study also highlights the uncertainties in modeling dust mass and number loading, deposition fluxes, and radiative forcing resulting from different size parameterizations, and motivates further investigation of the impact of size parameterizations on modeling dust impacts on air quality, climate, and ecosystem.« 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.

Vertical Transport Processes for Inert and Scavenged Species: TRACE-A Measurements

NASA Technical Reports Server (NTRS)

Chatfield, Robert B.; Chan, K. Roland (Technical Monitor)

1997-01-01

The TRACE-A mission of the NASA DC-8 aircraft made a large-scale survey of the tropical and subtropical atmosphere in September and October of 1992. Both In-situ measurements of CO (G. Sachsen NASA Langley) and aerosol size (J. Browell group, NASA Langley) provide excellent data sets with which to constrain vertical transport by planetary boundary layer mixing and deep-cloud cumulus convection. Lidar profiles of aerosol-induced scattering and ozone (also by Bremen) are somewhat require more subtle interpretation as tracers, but the vertical information on layering largely compensates for these complexities. The reason this DC-8 dataset is so useful is that very large areas of biomass burning over Africa and South America provide surface sources of appropriate sizes with which to characterize vertical and horizontal motions; the major limitation of our source description is that biomass burning patterns move considerably every few days, and daily burning inventories are a matter of concurrent, intensive research. We use the Penn State / NCAR MM5 model in an assimilation mode on the synoptic and intercontinental scale, and assess the success it shows in vertical transport descriptions. We find that the general level of emissions suggested by the climatological approach (Will. Has, U. of Montana) appears to be approximately correct, possibly a bit low, for this October, 1992, time period. Vertical transport in planetary boundary layer mixing to 5.5 kin was observed and reproduced in our simulations. Furthermore we find evidence that Blackader "transilient" or matrix-transport scheme is needed, but may require some adaptation in our tracer model: CO seems to exhibit very high values at the top of the planetary boundary layer, a process that stretches the eddy-diffusion parameterization. We will report on progress in improving the deep convective transport of carbon monoxide: the Grail scheme as we used it at 100 kin resolution did not transport enough material to the upper troposphere. We expect to be able to attribute this to either parameterization reasons (inadequacy of this parameterization at the large 100km scale) or other reasons. Nevertheless, the qualitative nature of deep transport by clouds shows up well in the simulations. As for scavengable species, the simulations predict tens of micrograms per standard cubic meter of smoke aerosol in the boundary layer. In a straightforward illustration of our simple bulk-mass scavenging parameterization, to one or two micrograms per standard cubic meter of smoke aerosol in the free troposphere just above the source regions: very high concentrations for the free troposphere. We expect to report on comparisons of these predictions to a variety of observations.

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.

Multi-sensor cloud and aerosol retrieval simulator and remote sensing from model parameters - Part 2: Aerosols

NASA Astrophysics Data System (ADS)

Wind, Galina; da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-07-01

The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a "simulated radiance" product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land-ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers.This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled.In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model subgrid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to operational remote-sensing algorithms.Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (M{O/Y}D04). The M{O/Y}D04 product is of course normally produced from M{O/Y}D021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a M{O/Y}D021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source.We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters . Part 2; Aerosols

NASA Technical Reports Server (NTRS)

Wind, Galina; Da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-01-01

The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a simulated radiance product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers. This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled. In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model sub grid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to operational remote-sensing algorithms. Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (MOYD04). TheMOYD04 product is of course normally produced from MOYD021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a MOYD021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source. We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

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

NASA Technical Reports Server (NTRS)

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

2016-01-01

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

Assessing the aerosol direct and first indirect effects using ACM/GCM simulation results

NASA Astrophysics Data System (ADS)

Huang, H.; Gu, Y.; Xue, Y.; Lu, C. H.

2016-12-01

Atmospheric aerosols have been found to play an important role in global climate change but there are still large uncertainty in evaluating its role in the climate system. The aerosols generally affect global and regional climate through the scattering and the absorption of solar radiation (direct effect) and through their influences on cloud particle, number and sizes (first indirect effect). The indirect effect will further affects cloud water content, cloud top albedo and surface precipitations. In this study, we investigate the global climatic effect of aerosols using a coupled NCEP Global Forecast System (GFS) and a land surface model (SSiB2) The OPAC (Optical Properties of Aerosols and Clouds) database is used for aerosol effect. The OPAC data provides the optical properties (i.e., the extinction, scattering and absorption coefficient, single-scattering albedo, asymmetry factor and phase function) of ten types of aerosols under various relative humidity conditions for investigating the global direct and first indirect effects of dust aerosols. For indirect forcings due to liquid water, we follow the approach presented by Jiang et al (2011), in which a parameterization of cloud effective radius was calculated to describe its variance with convective strength and aerosol concentration. Since the oceans also play an important role on aerosol climatic effect, we also design a set of simulations using a coupled atmosphere/ocean model (CFS) to evaluate the sensitivity of aerosol effect with two-way atmosphere-ocean interactions.

Secondary organic aerosol formation by limonene ozonolysis: Parameterizing multi-generational chemistry in ozone- and residence time-limited indoor environments

NASA Astrophysics Data System (ADS)

Waring, Michael S.

2016-11-01

Terpene ozonolysis reactions can be a strong source of secondary organic aerosol (SOA) indoors. SOA formation can be parameterized and predicted using the aerosol mass fraction (AMF), also known as the SOA yield, which quantifies the mass ratio of generated SOA to oxidized terpene. Limonene is a monoterpene that is at sufficient concentrations such that it reacts meaningfully with ozone indoors. It has two unsaturated bonds, and the magnitude of the limonene ozonolysis AMF varies by a factor of ∼4 depending on whether one or both of its unsaturated bonds are ozonated, which depends on whether ozone is in excess compared to limonene as well as the available time for reactions indoors. Hence, this study developed a framework to predict the limonene AMF as a function of the ozone [O3] and limonene [lim] concentrations and the air exchange rate (AER, h-1), which is the inverse of the residence time. Empirical AMF data were used to calculate a mixing coefficient, β, that would yield a 'resultant AMF' as the combination of the AMFs due to ozonolysis of one or both of limonene's unsaturated bonds, within the volatility basis set (VBS) organic aerosol framework. Then, β was regressed against predictors of log10([O3]/[lim]) and AER (R2 = 0.74). The β increased as the log10([O3]/[lim]) increased and as AER decreased, having the physical meaning of driving the resultant AMF to the upper AMF condition when both unsaturated bonds of limonene are ozonated. Modeling demonstrates that using the correct resultant AMF to simulate SOA formation owing to limonene ozonolysis is crucial for accurate indoor prediction.

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.

Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

DOE PAGES

O'Brien, Rachel E.; Wang, Bingbing; Laskin, Alexander; ...

2015-08-26

In this study, a new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission X-ray microscopy/near edge X-ray absorption fine structure (STXM/NEXAFS) and computer-controlled scanning electron microscopy/energy dispersive X-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on 27 and 28 June during the 2010 Carbonaceous Aerosols and Radiative Effects study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near themore » Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. The STXM data showed evidence of changes in the mixing state associated with a buildup of organic matter confirmed by collocated measurements, and the largest impact on the mixing state was due to an increase in soot dominant particles during this buildup. The mixing state from STXM was similar between T0 and T1, indicating that the increased organic fraction at T1 had a small effect on the mixing state of the population. The CCSEM/EDX analysis showed the presence of two types of particle populations: the first was dominated by aged sea-salt particles and had a higher mixing state index (indicating a more homogeneous population); the second was dominated by carbonaceous particles and had a lower mixing state index.« less

Modeling East Asian Dust and Its Radiative Feedbacks in CAM4-BAM

DOE PAGES

Xie, Xiaoning; Liu, Xiaodong; Che, Huizheng; ...

2018-01-18

East Asian dust and its radiative feedbacks are analyzed by the use of the fourth version of the Community Atmosphere Model (CAM4) with a bulk aerosol model parameterization (BAM) for the dust size distribution (CAM4-BAM). Two numerical experiments are conducted and intercompared: one with (Active) and one without (Passive) the radiative effects of dust aerosols. This CAM4-BAM captures the main spatial distribution of the dust aerosol optical depth (AOD) and the dust surface concentrations over East Asia, with positive correlations with the local observational data on annual and seasonal means. A comparative analysis of the Active and Passive experiments revealsmore » that consideration of the dust-radiation interaction can significantly reduce dust emissions, loading, transport, and dry and wet depositions over East Asia, which is opposite to the enhanced dust cycle over North Africa. Further analysis of the contrasting dust-radiation feedbacks between North Africa and East Asia shows that over North Africa, the dust radiative forcing significantly increases the surface temperature and 10-m wind speed, whereas it decreases the surface temperature and the surface wind speeds over East Asia. These contrasting radiative effects, in turn, result in distinct dust cycle changes over these two regions. Thus, mechanistic analysis reveals that the radiative contrasts between East Asia and North Africa are mainly due to the differences in their regional surface albedo, dust vertical distribution and size distribution.« less

Modeling East Asian Dust and Its Radiative Feedbacks in CAM4-BAM

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

Xie, Xiaoning; Liu, Xiaodong; Che, Huizheng

East Asian dust and its radiative feedbacks are analyzed by the use of the fourth version of the Community Atmosphere Model (CAM4) with a bulk aerosol model parameterization (BAM) for the dust size distribution (CAM4-BAM). Two numerical experiments are conducted and intercompared: one with (Active) and one without (Passive) the radiative effects of dust aerosols. This CAM4-BAM captures the main spatial distribution of the dust aerosol optical depth (AOD) and the dust surface concentrations over East Asia, with positive correlations with the local observational data on annual and seasonal means. A comparative analysis of the Active and Passive experiments revealsmore » that consideration of the dust-radiation interaction can significantly reduce dust emissions, loading, transport, and dry and wet depositions over East Asia, which is opposite to the enhanced dust cycle over North Africa. Further analysis of the contrasting dust-radiation feedbacks between North Africa and East Asia shows that over North Africa, the dust radiative forcing significantly increases the surface temperature and 10-m wind speed, whereas it decreases the surface temperature and the surface wind speeds over East Asia. These contrasting radiative effects, in turn, result in distinct dust cycle changes over these two regions. Thus, mechanistic analysis reveals that the radiative contrasts between East Asia and North Africa are mainly due to the differences in their regional surface albedo, dust vertical distribution and size distribution.« 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.

Global Climate Models Intercomparison of Anthropogenic Aerosols Effects on Regional Climate over North Pacific

NASA Astrophysics Data System (ADS)

Hu, J.; Zhang, R.; Wang, Y.; Ming, Y.; Lin, Y.; Pan, B.

2015-12-01

Aerosols can alter atmospheric radiation and cloud physics, which further exert impacts on weather and global climate. With the development and industrialization of the developing Asian countries, anthropogenic aerosols have received considerable attentions and remain to be the largest uncertainty in the climate projection. Here we assess the performance of two stat-of-art global climate models (National Center for Atmospheric Research-Community Atmosphere Model 5 (CAM5) and Geophysical Fluid Dynamics Laboratory Atmosphere Model 3 (AM3)) in simulating the impacts of anthropogenic aerosols on North Pacific storm track region. By contrasting two aerosol scenarios, i.e. present day (PD) and pre-industrial (PI), both models show aerosol optical depth (AOD) enhanced by about 22%, with CAM5 AOD 40% lower in magnitude due to the long range transport of anthropogenic aerosols. Aerosol effects on the ice water path (IWP), stratiform precipitation, convergence and convection strengths in the two models are distinctive in patterns and magnitudes. AM3 shows qualitatively good agreement with long-term satellite observations, while CAM5 overestimates convection and liquid water path resulting in an underestimation of large-scale precipitation and IWP. Due to coarse resolution and parameterization in convection schemes, both models' performance on convection needs to be improved. Aerosols performance on large-scale circulation and radiative budget are also examined in this study.

Limited effect of anthropogenic nitrogen oxides on Secondary Organic Aerosol formation

NASA Astrophysics Data System (ADS)

Zheng, Y.; Unger, N.; Hodzic, A.; Emmons, L.; Knote, C.; Tilmes, S.; Lamarque, J.-F.; Yu, P.

2015-08-01

Globally, secondary organic aerosol (SOA) is mostly formed from emissions of biogenic volatile organic compounds (VOCs) by vegetation, but can be modified by human activities as demonstrated in recent research. Specifically, nitrogen oxides (NOx = NO + NO2) have been shown to play a critical role in the chemical formation of low volatility compounds. We have updated the SOA scheme in the global NCAR Community Atmospheric Model version 4 with chemistry (CAM4-chem) by implementing a 4-product Volatility Basis Set (VBS) scheme, including NOx-dependent SOA yields and aging parameterizations. The predicted organic aerosol amounts capture both the magnitude and distribution of US surface annual mean measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network by 50 %, and the simulated vertical profiles are within a factor of two compared to Aerosol Mass Spectrometer (AMS) measurements from 13 aircraft-based field campaigns across different region and seasons. We then perform sensitivity experiments to examine how the SOA loading responds to a 50 % reduction in anthropogenic nitric oxide (NO) emissions in different regions. We find limited SOA reductions of 0.9 to 5.6, 6.4 to 12.0 and 0.9 to 2.8 % for global, the southeast US and the Amazon NOx perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to buffering in chemical pathways (low- and high-NOx pathways, O3 versus NO3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.

Feedbacks between Air-Quality, Meteorology, and the Forest Environment

NASA Astrophysics Data System (ADS)

Makar, Paul; Akingunola, Ayodeji; Stroud, Craig; Zhang, Junhua; Gong, Wanmin; Moran, Michael; Zheng, Qiong; Brook, Jeffrey; Sills, David

2017-04-01

The outcome of air quality forecasts depend in part on how the local environment surrounding the emissions regions influences chemical reaction rates and transport from those regions to the larger spatial scales. Forested areas alter atmospheric chemistry through reducing photolysis rates and vertical diffusivities within the forest canopy. The emitted pollutants, and their reaction products, are in turn capable of altering meteorology, through the well-known direct and indirect effects of particulate matter on radiative transfer. The combination of these factors was examined using version 2 of the Global Environmental Multiscale - Modelling Air-quality and CHemistry (GEM-MACH) on-line air pollution model. The model configuration used for this study included 12 aerosol size bins, eight aerosol species, homogeneous core Mie scattering, the Milbrandt-Yao two-moment cloud microphysics scheme with cloud condensation nuclei generated from model aerosols using the scheme of Abdul-Razzak and Ghan, and a new parameterization for forest canopy shading and turbulence. The model was nested to 2.5km resolution for a domain encompassing the lower Great Lakes, for simulations of a period in August of 2015 during the Pan American Games, held in Toronto, Canada. Four scenarios were carried out: (1) a "Base Case" scenario (the original model, in which coupling between chemistry and weather is not permitted; instead, the meteorological model's internal climatologies for aerosol optical and cloud condensation properties are used for direct and indirect effect calculations); (2) a "Feedback" scenario (the aerosol properties were derived from the internally simulated chemistry, and coupled to the meteorological model's radiative transfer and cloud formation modules); (3) a "Forest" scenario (canopy shading and turbulence were added to the Base Case); (4) a "Combined" scenario (including both direct and indirect effect coupling between meteorology and chemistry, as well as the forest canopy parameterization). The simulations suggest that the feedbacks between simulated aerosols and meteorology may strengthen the existing lake breeze circulation, modifying the resulting meteorological and air-quality forecasts, while the forest canopy's influence may extend throughout the planetary boundary layer, and may also influence the weather. The simulations will be compared to available observations, in order to determine their relative impact on model performance.

Prediction of cloud condensation nuclei activity for organic compounds using functional group contribution methods

DOE PAGES

Petters, M. D.; Kreidenweis, S. M.; Ziemann, P. J.

2016-01-19

A wealth of recent laboratory and field experiments demonstrate that organic aerosol composition evolves with time in the atmosphere, leading to changes in the influence of the organic fraction to cloud condensation nuclei (CCN) spectra. There is a need for tools that can realistically represent the evolution of CCN activity to better predict indirect effects of organic aerosol on clouds and climate. This work describes a model to predict the CCN activity of organic compounds from functional group composition. Following previous methods in the literature, we test the ability of semi-empirical group contribution methods in Kohler theory to predict themore » effective hygroscopicity parameter, kappa. However, in our approach we also account for liquid–liquid phase boundaries to simulate phase-limited activation behavior. Model evaluation against a selected database of published laboratory measurements demonstrates that kappa can be predicted within a factor of 2. Simulation of homologous series is used to identify the relative effectiveness of different functional groups in increasing the CCN activity of weakly functionalized organic compounds. Hydroxyl, carboxyl, aldehyde, hydroperoxide, carbonyl, and ether moieties promote CCN activity while methylene and nitrate moieties inhibit CCN activity. Furthermore, the model can be incorporated into scale-bridging test beds such as the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) to evaluate the evolution of kappa for a complex mix of organic compounds and to develop suitable parameterizations of CCN evolution for larger-scale models.« less

Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate

DOE PAGES

Rastak, N.; Pajunoja, A.; Acosta Navarro, J. C.; ...

2017-04-28

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient datamore » with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.« less

Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate

NASA Astrophysics Data System (ADS)

Rastak, N.; Pajunoja, A.; Acosta Navarro, J. C.; Ma, J.; Song, M.; Partridge, D. G.; Kirkevâg, A.; Leong, Y.; Hu, W. W.; Taylor, N. F.; Lambe, A.; Cerully, K.; Bougiatioti, A.; Liu, P.; Krejci, R.; Petäjä, T.; Percival, C.; Davidovits, P.; Worsnop, D. R.; Ekman, A. M. L.; Nenes, A.; Martin, S.; Jimenez, J. L.; Collins, D. R.; Topping, D. O.; Bertram, A. K.; Zuend, A.; Virtanen, A.; Riipinen, I.

2017-05-01

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.

Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate.

PubMed

Rastak, N; Pajunoja, A; Acosta Navarro, J C; Ma, J; Song, M; Partridge, D G; Kirkevåg, A; Leong, Y; Hu, W W; Taylor, N F; Lambe, A; Cerully, K; Bougiatioti, A; Liu, P; Krejci, R; Petäjä, T; Percival, C; Davidovits, P; Worsnop, D R; Ekman, A M L; Nenes, A; Martin, S; Jimenez, J L; Collins, D R; Topping, D O; Bertram, A K; Zuend, A; Virtanen, A; Riipinen, I

2017-05-28

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.

Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate

PubMed Central

Rastak, N.; Pajunoja, A.; Acosta Navarro, J. C.; Ma, J.; Song, M.; Partridge, D. G.; Kirkevåg, A.; Leong, Y.; Hu, W. W.; Taylor, N. F.; Lambe, A.; Cerully, K.; Bougiatioti, A.; Liu, P.; Krejci, R.; Petäjä, T.; Percival, C.; Davidovits, P.; Worsnop, D. R.; Ekman, A. M. L.; Nenes, A.; Martin, S.; Jimenez, J. L.; Collins, D. R.; Topping, D.O.; Bertram, A. K.; Zuend, A.; Virtanen, A.

2017-01-01

Abstract A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH‐dependent SOA water‐uptake with solubility and phase separation; (2) show that laboratory data on IP‐ and MT‐SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single‐parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources. PMID:28781391

Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate

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

Rastak, N.; Pajunoja, A.; Acosta Navarro, J. C.

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient datamore » with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.« less

A51F-0123: Model Analysis of Tropospheric Aerosol Variability and Sources over the North Atlantic During NAAMES 2015-2016

NASA Technical Reports Server (NTRS)

Liu, Hongyu; Moore, Richard; Hostetler, Chris A.; Ferrare, Richard Anthony; Fairlie, Thomas Duncan; Hu, Youngxiang; Chen, Gao; Hair, Johnathan W.; Johnson, Matthew S.

2016-01-01

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is a five-year Earth-Venture Suborbital-2 Mission to characterize the plankton ecosystems and their influences on remote marine aerosols, boundary layer clouds, and their implications for climate in the North Atlantic. While marine-sourced aerosols have been shown to make important contributions to surface aerosol loading, cloud condensation nuclei and ice nuclei concentrations over remote marine and coastal regions, it is still a challenge to differentiate the marine biogenic aerosol signal from the strong influence of continental pollution outflow. We examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during the first two phases (November 2015 and May-June 2016) of NAAMES using a state-of-the-art chemical transport model (GEOS-Chem). The model is driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) from the NASA Global Modeling and Assimilation Office (GMAO). It includes sulfate-nitrate-ammonium aerosol thermodynamics coupled to ozone-NOx-hydrocarbon-aerosol chemistry, mineral dust, sea salt, elemental and organic carbon aerosols, and especially a recently implemented parameterization for the marine primary organic aerosol emission. The simulated aerosols over the North Atlantic are evaluated with available satellite (e.g., MODIS) observations of aerosol optical depths (AOD), and aircraft and ship aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. We also conduct model perturbation experiments to quantify the relative contributions of terrestrial and oceanic sources to the aerosol loading, AOD, and their variability over the North Atlantic.

Modelling absorbing aerosol with ECHAM-HAM: Insights from regional studies

NASA Astrophysics Data System (ADS)

Tegen, Ina; Heinold, Bernd; Schepanski, Kerstin; Banks, Jamie; Kubin, Anne; Schacht, Jacob

2017-04-01

Quantifying distributions and properties of absorbing aerosol is a basis for investigations of interactions of aerosol particles with radiation and climate. While evaluations of aerosol models by field measurements can be particularly successful at the regional scale, such results need to be put into a global context for climate studies. We present an overview over studies performed at the Leibniz Institute for Tropospheric Research aiming at constraining the properties of mineral dust and soot aerosol in the global aerosol model ECHAM6-HAM2 based on different regional studies. An example is the impact of different sources for dust transported to central Asia, which is influenced, by far-range transport of dust from Arabia and the Sahara together with dust from local sources. Dust types from these different source regions were investigated in the context of the CADEX project and are expected to have different optical properties. For Saharan dust, satellite retrievals from MSG SEVIRI are used to constrain Saharan dust sources and optical properties. In the Arctic region, on one hand dust aerosol is simulated in the framework of the PalMod project. On the other hand aerosol measurements that will be taken during the DFG-funded (AC)3 field campaigns will be used to evaluate the simulated transport pathways of soot aerosol from European, North American and Asian sources, as well as the parameterization of soot ageing processes in ECHAM6-HAM2. Ultimately, results from these studies will improve the representation of aerosol absorption in the global model.

Evaluating the Impact of Aerosols on Numerical Weather Prediction

NASA Astrophysics Data System (ADS)

Freitas, Saulo; Silva, Arlindo; Benedetti, Angela; Grell, Georg; Members, Wgne; Zarzur, Mauricio

2015-04-01

The Working Group on Numerical Experimentation (WMO, http://www.wmo.int/pages/about/sec/rescrosscut/resdept_wgne.html) has organized an exercise to evaluate the impact of aerosols on NWP. This exercise will involve regional and global models currently used for weather forecast by the operational centers worldwide and aims at addressing the following questions: a) How important are aerosols for predicting the physical system (NWP, seasonal, climate) as distinct from predicting the aerosols themselves? b) How important is atmospheric model quality for air quality forecasting? c) What are the current capabilities of NWP models to simulate aerosol impacts on weather prediction? Toward this goal we have selected 3 strong or persistent events of aerosol pollution worldwide that could be fairly represented in current NWP models and that allowed for an evaluation of the aerosol impact on weather prediction. The selected events includes a strong dust storm that blew off the coast of Libya and over the Mediterranean, an extremely severe episode of air pollution in Beijing and surrounding areas, and an extreme case of biomass burning smoke in Brazil. The experimental design calls for simulations with and without explicitly accounting for aerosol feedbacks in the cloud and radiation parameterizations. In this presentation we will summarize the results of this study focusing on the evaluation of model performance in terms of its ability to faithfully simulate aerosol optical depth, and the assessment of the aerosol impact on the predictions of near surface wind, temperature, humidity, rainfall and the surface energy budget.

Comparative Analysis of Aerosol Retrievals from MODIS, OMI and MISR Over Sahara Region

NASA Technical Reports Server (NTRS)

Lyapustin, A.; Wang, Y.; Hsu, C.; Terres, O.; Leptoukh, G.; Kalashnikova, O.; Korkin, S.

2011-01-01

MODIS is a wide field-of-view sensor providing daily global observations of the Earth. Currently, global MODIS aerosol retrievals over land are performed with the main Dark Target algorithm complimented with the Deep Blue (DB) Algorithm over bright deserts. The Dark Target algorithm relies on surface parameterization which relates reflectance in MODIS visible bands with the 2.1 micrometer region, whereas the Deep Blue algorithm uses an ancillary angular distribution model of surface reflectance developed from the time series of clear-sky MODIS observations. Recently, a new Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm has been developed for MODIS. MAIAC uses a time series and an image based processing to perform simultaneous retrievals of aerosol properties and surface bidirectional reflectance. It is a generic algorithm which works over both dark vegetative surfaces and bright deserts and performs retrievals at 1 km resolution. In this work, we will provide a comparative analysis of DB, MAIAC, MISR and OMI aerosol products over bright deserts of northern Africa.

Aerosol direct and indirect radiative effect over Eastern Mediterranean

NASA Astrophysics Data System (ADS)

Georgoulias, Aristeidis; Alexandri, Georgia; Zanis, Prodromos; Ntogras, Christos; Poeschl, Ulrich; Kourtidis, Kostas

In this work, we present results from the QUADIEEMS project which is focused on the aerosol-cloud relations and the aerosol direct and indirect radiative effect over the region of Eastern Mediterranean. First, a gridded dataset at a resolution of 0.1x0.1 degrees (~10km) with aerosol and cloud related parameters was compiled, using level-2 satellite observations from MODIS TERRA (3/2000-12/2012) and AQUA (7/2002-12/2012). The aerosol gridded dataset has been validated against sunphotometric measurements from 12 AERONET ground stations, showing that generally MODIS overestimates aerosol optical depth (AOD550). Then, the AOD550 and fine mode ratio (FMR550) data from MODIS were combined with aerosol index (AI) data from the Earth Probe TOMS and OMI satellite sensors, wind field data from the ERA-interim reanalysis and AOD550 data for various aerosol types from the GOCART model and the MACC reanalysis to quantify the relative contribution of different aerosol types (marine, dust, anthropogenic, fine-mode natural) to the total AOD550. The aerosol-cloud relations over the region were investigated with the use of the joint high resolution aerosol-cloud gridded dataset. Specifically, we focused on the seasonal relations between the cloud droplet number concentration (CDNC) and AOD550. The aerosol direct and first indirect radiative effect was then calculated for each aerosol type separately making use of the aerosol relative contribution to the total AOD550, the CDND-AOD550 relations and satellite-based parameterizations. The direct radiative effect was also quantified using simulations from a regional climate model (REGCM4), simulations with a radiative transfer model (SBDART) and the three methods were finally intervalidated.

Characterizing the Spatial and Temporal Distribution of Aerosol Optical Thickness Over the Atlantic Basin Utilizing GOES-8 Multispectral Data

NASA Technical Reports Server (NTRS)

Fox, Robert; Prins, Elaine Mae; Feltz, Joleen M.

2001-01-01

In recent years, modeling and analysis efforts have suggested that the direct and indirect radiative effects of both anthropogenic and natural aerosols play a major role in the radiative balance of the earth and are an important factor in climate change calculations. The direct effects of aerosols on radiation and indirect effects on cloud properties are not well understood at this time. In order to improve the characterization of aerosols within climate models it is important to accurately parameterize aerosol forcing mechanisms at the local, regional, and global scales. This includes gaining information on the spatial and temporal distribution of aerosols, transport regimes and mechanisms, aerosol optical thickness, and size distributions. Although there is an expanding global network of ground measurements of aerosol optical thickness and size distribution at specific locations, satellite data must be utilized to characterize the spatial and temporal extent of aerosols and transport regimes on regional and global scales. This study was part of a collaborative effort to characterize aerosol radiative forcing over the Atlantic basin associated with the following three major aerosol components in this region: urban/sulfate, Saharan dust, and biomass burning. In-situ ground measurements obtained by a network of sun photometers during the Smoke Clouds and Radiation Experiment in Brazil (SCAR-B) and the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) were utilized to develop, calibrate, and validate a Geostationary Operational Environmental Satellite (GOES)-8 aerosol optical thickness (AOT) product. Regional implementation of the GOES-8 AOT product was used to augment point source measurements to gain a better understanding of the spatial and temporal distributions of Atlantic basin aerosols during SCAR-B and TARFOX.

Particle water and pH in the eastern Mediterranean: source variability and implications for nutrient availability

NASA Astrophysics Data System (ADS)

Bougiatioti, Aikaterini; Nikolaou, Panayiota; Stavroulas, Iasonas; Kouvarakis, Giorgos; Weber, Rodney; Nenes, Athanasios; Kanakidou, Maria; Mihalopoulos, Nikolaos

2016-04-01

Particle water (liquid water content, LWC) and aerosol pH are important parameters of the aerosol phase, affecting heterogeneous chemistry and bioavailability of nutrients that profoundly impact cloud formation, atmospheric composition, and atmospheric fluxes of nutrients to ecosystems. Few measurements of in situ LWC and pH, however, exist in the published literature. Using concurrent measurements of aerosol chemical composition, cloud condensation nuclei activity, and tandem light scattering coefficients, the particle water mass concentrations associated with the aerosol inorganic (Winorg) and organic (Worg) components are determined for measurements conducted at the Finokalia atmospheric observation station in the eastern Mediterranean between June and November 2012. These data are interpreted using the ISORROPIA-II thermodynamic model to predict the pH of aerosols originating from the various sources that influence air quality in the region. On average, closure between predicted aerosol water and that determined by comparison of ambient with dry light scattering coefficients was achieved to within 8 % (slope = 0.92, R2 = 0.8, n = 5201 points). Based on the scattering measurements, a parameterization is also derived, capable of reproducing the hygroscopic growth factor (f(RH)) within 15 % of the measured values. The highest aerosol water concentrations are observed during nighttime, when relative humidity is highest and the collapse of the boundary layer increases the aerosol concentration. A significant diurnal variability is found for Worg with morning and afternoon average mass concentrations being 10-15 times lower than nighttime concentrations, thus rendering Winorg the main form of particle water during daytime. The average value of total aerosol water was 2.19 ± 1.75 µg m-3, contributing on average up to 33 % of the total submicron mass concentration. Average aerosol water associated with organics, Worg, was equal to 0.56 ± 0.37 µg m-3; thus, organics contributed about 27.5 % to the total aerosol water, mostly during early morning, late evening, and nighttime hours.

The aerosol was found to be highly acidic with calculated aerosol pH varying from 0.5 to 2.8 throughout the study period. Biomass burning aerosol presented the highest values of pH in the submicron fraction and the lowest values in total water mass concentration. The low pH values observed in the submicron mode and independently of air mass origin could increase nutrient availability and especially P solubility, which is the nutrient limiting sea water productivity of the eastern Mediterranean.

Particle water and pH in the Eastern Mediterranean: sources variability and implications for nutrients availability

NASA Astrophysics Data System (ADS)

Nikolaou, P.; Bougiatioti, A.; Stavroulas, I.; Kouvarakis, G.; Nenes, A.; Weber, R.; Kanakidou, M.; Mihalopoulos, N.

2015-10-01

Particle water (LWC) and aerosol pH drive the aerosol phase, heterogeneous chemistry and bioavailability of nutrients that profoundly impact cloud formation, atmospheric composition and atmospheric fluxes of nutrients to ecosystems. Few measurements of in-situ LWC and pH however exist in the published literature. Using concurrent measurements of aerosol chemical composition, cloud condensation nuclei activity and tandem light scattering coefficients, the particle water mass concentrations associated with the aerosol inorganic (Winorg) and organic (Worg) components are determined for measurements conducted at the Finokalia atmospheric observation station in the eastern Mediterranean between August and November 2012. These data are interpreted using the ISORROPIA-II thermodynamic model to predict pH of aerosols originating from the various sources that influence air quality in the region. On average, closure between predicted aerosol water and that determined by comparison of ambient with dry light scattering coefficients was achieved to within 8 % (slope = 0.92, R2 = 0.8, n = 5201 points). Based on the scattering measurements a parameterization is also derived, capable of reproducing the hygroscopic growth factor (f(RH)) within 15 % of the measured values. The highest aerosol water concentrations are observed during nighttime, when relative humidity is highest and the collapse of the boundary layer increases the aerosol concentration. A significant diurnal variability is found for Worg with morning and afternoon average mass concentrations being 10-15 times lower than nighttime concentrations, thus rendering Winorg the main form of particle water during daytime. The average value of total aerosol water was 2.19 ± 1.75 μg m-3, contributing on average up to 33 % of the total submicron mass concentration. Average aerosol water associated with organics, Worg, was equal to 0.56 ± 0.37 μg m-3, thus organics contributed about 27.5 % to the total aerosol water, mostly during early morning, late evening and nighttime hours. The aerosol was found to be highly acidic with calculated aerosol pH varying from 0.5 to 2.8 throughout the study period. Biomass burning aerosol presented the highest values of pH in the submicron fraction and the lowest values in total water mass concentration. The low pH values observed in the submicron mode and independently of air masses origin could increase nutrient availability and especially P solubility, which is the nutrient limiting sea water productivity of the eastern Mediterranean.

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.

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.

Quantification of marine aerosol subgrid variability and its correlation with clouds based on high-resolution regional modeling: Quantifying Aerosol Subgrid Variability

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

Lin, Guangxing; Qian, Yun; Yan, Huiping

One limitation of most global climate models (GCMs) is that with the horizontal resolutions they typically employ, they cannot resolve the subgrid variability (SGV) of clouds and aerosols, adding extra uncertainties to the aerosol radiative forcing estimation. To inform the development of an aerosol subgrid variability parameterization, here we analyze the aerosol SGV over the southern Pacific Ocean simulated by the high-resolution Weather Research and Forecasting model coupled to Chemistry. We find that within a typical GCM grid, the aerosol mass subgrid standard deviation is 15% of the grid-box mean mass near the surface on a 1 month mean basis.more » The fraction can increase to 50% in the free troposphere. The relationships between the sea-salt mass concentration, meteorological variables, and sea-salt emission rate are investigated in both the clear and cloudy portion. Under clear-sky conditions, marine aerosol subgrid standard deviation is highly correlated with the standard deviations of vertical velocity, cloud water mixing ratio, and sea-salt emission rates near the surface. It is also strongly connected to the grid box mean aerosol in the free troposphere (between 2 km and 4 km). In the cloudy area, interstitial sea-salt aerosol mass concentrations are smaller, but higher correlation is found between the subgrid standard deviations of aerosol mass and vertical velocity. Additionally, we find that decreasing the model grid resolution can reduce the marine aerosol SGV but strengthen the correlations between the aerosol SGV and the total water mixing ratio (sum of water vapor, cloud liquid, and cloud ice mixing ratios).« less

A Monte-Carlo Analysis of Organic Volatility with Aerosol Microphysics

NASA Astrophysics Data System (ADS)

Gao, Chloe; Tsigaridis, Kostas; Bauer, Susanne E.

2017-04-01

A newly developed box model, MATRIX-VBS, includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves aerosol mass and number concentrations and aerosol mixing state. The new scheme advanced the representation of organic aerosols in models by improving the traditional and simplistic treatment of organic aerosols as non-volatile and with a fixed size distribution. Further development includes adding the condensation of organics on coarse mode aerosols - dust and sea salt, thus making all organics in the system semi-volatile. To test and simplify the model, a Monte-Carlo analysis is performed to pin point which processes affect organics the most under varied chemical and meteorological conditions. Since the model's parameterizations have the ability to capture a very wide range of conditions, all possible scenarios on Earth across the whole parameter space, including temperature, humidity, location, emissions and oxidant levels, are examined. The Monte-Carlo simulations provide quantitative information on the sensitivity of the newly developed model and help us understand how organics are affecting the size distribution, mixing state and volatility distribution at varying levels of meteorological conditions and pollution levels. In addition, these simulations give information on which parameters play a critical role in the aerosol distribution and evolution in the atmosphere and which do not, that will facilitate the simplification of the box model, an important step in its implementation in the global model GISS ModelE as a module.

Parameterization of In-Cloud Aerosol Scavenging Due To Atmospheric Ionization: 2. Effects of Varying Particle Density

NASA Astrophysics Data System (ADS)

Zhang, Liang; Tinsley, Brian A.

2018-03-01

Simulations and parameterization of collision rate coefficients for aerosol particles with 3 μm radius droplets have been extended to a range of particle densities up to 2,000 kg m-3 for midtropospheric ( 5 km) conditions (540 hPa, -17°C). The increasing weight has no effect on collisions for particle radii less than 0.2 μm, but for greater radii the weight effect becomes significant and usually decreases the collision rate coefficient. When increasing size and density of particles make the fall speed of the particle relative to undisturbed air approach to that of the droplet, the effect of the particle falling away in the stagnation region ahead of the droplet becomes important, and the probability of frontside collisions can decrease to zero. Collisions on the rear side of the droplet can be enhanced as particle weight increases, and for this the weight effect tends to increase the rate coefficients. For charges on the droplet and for large particles with density ρ < 1,000 kg m-3 the predominant effect increases in rate coefficient due to the short-range attractive image electric force. With density ρ above about 1,000 kg m-3, the stagnation region prevents particles moving close to the droplet and reduces the effect of these short-range forces. Together with previous work, it is now possible to obtain collision rate coefficients for realistic combinations of droplet charge, particle charge, droplet radius, particle radius, particle density, and relative humidity in clouds. The parameterization allows rapid access to these values for use in cloud models.

Dimensionless parameterization of lidar for laser remote sensing of the atmosphere and its application to systems with SiPM and PMT detectors.

PubMed

Agishev, Ravil; Comerón, Adolfo; Rodriguez, Alejandro; Sicard, Michaël

2014-05-20

In this paper, we show a renewed approach to the generalized methodology for atmospheric lidar assessment, which uses the dimensionless parameterization as a core component. It is based on a series of our previous works where the problem of universal parameterization over many lidar technologies were described and analyzed from different points of view. The modernized dimensionless parameterization concept applied to relatively new silicon photomultiplier detectors (SiPMs) and traditional photomultiplier (PMT) detectors for remote-sensing instruments allowed predicting the lidar receiver performance with sky background available. The renewed approach can be widely used to evaluate a broad range of lidar system capabilities for a variety of lidar remote-sensing applications as well as to serve as a basis for selection of appropriate lidar system parameters for a specific application. Such a modernized methodology provides a generalized, uniform, and objective approach for evaluation of a broad range of lidar types and systems (aerosol, Raman, DIAL) operating on different targets (backscatter or topographic) and under intense sky background conditions. It can be used within the lidar community to compare different lidar instruments.

Host Model Uncertainty in Aerosol Radiative Forcing Estimates - The AeroCom Prescribed Experiment

NASA Astrophysics Data System (ADS)

Stier, P.; Kinne, S.; Bellouin, N.; Myhre, G.; Takemura, T.; Yu, H.; Randles, C.; Chung, C. E.

2012-04-01

Anthropogenic and natural aerosol radiative effects are recognized to affect global and regional climate. However, even for the case of identical aerosol emissions, the simulated direct aerosol radiative forcings show significant diversity among the AeroCom models (Schulz et al., 2006). Our analysis of aerosol absorption in the AeroCom models indicates a larger diversity in the translation from given aerosol radiative properties (absorption optical depth) to actual atmospheric absorption than in the translation of a given atmospheric burden of black carbon to the radiative properties (absorption optical depth). The large diversity is caused by differences in the simulated cloud fields, radiative transfer, the relative vertical distribution of aerosols and clouds, and the effective surface albedo. This indicates that differences in host model (GCM or CTM hosting the aerosol module) parameterizations contribute significantly to the simulated diversity of aerosol radiative forcing. The magnitude of these host model effects in global aerosol model and satellites retrieved aerosol radiative forcing estimates cannot be estimated from the diagnostics of the "standard" AeroCom forcing experiments. To quantify the contribution of differences in the host models to the simulated aerosol radiative forcing and absorption we conduct the AeroCom Prescribed experiment, a simple aerosol model and satellite retrieval intercomparison with prescribed highly idealised aerosol fields. Quality checks, such as diagnostic output of the 3D aerosol fields as implemented in each model, ensure the comparability of the aerosol implementation in the participating models. The simulated forcing variability among the models and retrievals is a direct measure of the contribution of host model assumptions to the uncertainty in the assessment of the aerosol radiative effects. We will present the results from the AeroCom prescribed experiment with focus on the attribution to the simulated variability to parametric and structural model uncertainties. This work will help to prioritise areas for future model improvements and ultimately lead to uncertainty reduction.

Characterizing the Vertical Distribution of Aerosols using Ground-based Multiwavelength Lidar Data

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Thorsen, T. J.; Clayton, M.; Mueller, D.; Chemyakin, E.; Burton, S. P.; Goldsmith, J.; Holz, R.; Kuehn, R.; Eloranta, E. W.; Marais, W.; Newsom, R. K.; Liu, X.; Sawamura, P.; Holben, B. N.; Hostetler, C. A.

2016-12-01

Observations of aerosol optical and microphysical properties are critical for developing and evaluating aerosol transport model parameterizations and assessing global aerosol-radiation impacts on climate. During the Combined HSRL And Raman lidar Measurement Study (CHARMS), we investigated the synergistic use of ground-based Raman lidar and High Spectral Resolution Lidar (HSRL) measurements to retrieve aerosol properties aloft. Continuous (24/7) operation of these co-located lidars during the ten-week CHARMS mission (mid-July through September 2015) allowed the acquisition of a unique, multiwavelength ground-based lidar dataset for studying aerosol properties above the Southern Great Plains (SGP) site. The ARM Raman lidar measured profiles of aerosol backscatter, extinction and depolarization at 355 nm as well as profiles of water vapor mixing ratio and temperature. The University of Wisconsin HSRL simultaneously measured profiles of aerosol backscatter, extinction and depolarization at 532 nm and aerosol backscatter at 1064 nm. Recent advances in both lidar retrieval theory and algorithm development demonstrate that vertically-resolved retrievals using such multiwavelength lidar measurements of aerosol backscatter and extinction can help constrain both the aerosol optical (e.g. complex refractive index, scattering, etc.) and microphysical properties (e.g. effective radius, concentrations) as well as provide qualitative aerosol classification. Based on this work, the NASA Langley Research Center (LaRC) HSRL group developed automated algorithms for classifying and retrieving aerosol optical and microphysical properties, demonstrated these retrievals using data from the unique NASA/LaRC airborne multiwavelength HSRL-2 system, and validated the results using coincident airborne in situ data. We apply these algorithms to the CHARMS multiwavelength (Raman+HSRL) lidar dataset to retrieve aerosol properties above the SGP site. We present some profiles of aerosol effective radius and concentration retrieved from the CHARMS data and compare column-average aerosol properties derived from the multiwavelength lidar aerosol retrievals to corresponding values retrieved from AERONET measurements.

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

DeMott, Paul J; Hill, Thomas CJ

Measurements were sought to evaluate a hypotheses that sea-spray-sourced ice-nucleating particles (INPs) are of biological origin and represent a distinctly different INP population in comparison to long-range-transported desert or urban and regional land-sourced INP, and that the layering of marine within other aerosol layers feeding orographic storms over the mountains of California and the Western United States thereby leads to common and quantifiable scenarios that influence precipitation over the region. Aerosol collections on the National Oceanic and Atmospheric Administration (NOAA) research vessel (RV) Ronald H. Brown, for subsequent processing of INP immersion freezing activation temperature spectra and composition analyses, addedmore » a valuable measurement component to the ARM Cloud Aerosol Precipitation Experiment (ACAPEX) and related CalWater2 (NOAA) studies for use in parameterizing and modeling the impacts of marine boundary layer and other aerosols on climate and radiation via aerosol indirect effects on mixed-phase clouds. Twenty-five nominally 24-hour collections were made and have been processed for immersion freezing INP number concentrations versus temperature in the mixed-phase cloud temperature regime from -10 to -27°C. The similarity of INP number concentrations compared to typical marine boundary layer values attributed to sea-spray aerosols was noted. Nevertheless, variability of INP concentrations of up to 50 times was noted at individual temperatures over the course of the study. A particular analysis possible with this data set is to examine INP budgets over oceans inside versus outside of atmospheric river conditions. These INP measurements supplemented multiple airborne INP measurements on the ARM Aerial Facility (AAF), and others on the ground during ACAPEX and CalWater2, to provide extensive spatial and temporal analyses of INP immersion freezing spectra during winter storm periods. Future analyses will use thermal sensitivity to examine INP compositions as organic versus inorganic in these marine boundary layer samples. Data set integration is occurring under funding from an Atmospheric System Research (ASR) proposal.« less

Model representations of aerosol layers transported from North America over the Atlantic Ocean during the Two-Column Aerosol Project

NASA Astrophysics Data System (ADS)

Fast, Jerome D.; Berg, Larry K.; Zhang, Kai; Easter, Richard C.; Ferrare, Richard A.; Hair, Johnathan W.; Hostetler, Chris A.; Liu, Ying; Ortega, Ivan; Sedlacek, Arthur; Shilling, John E.; Shrivastava, Manish; Springston, Stephen R.; Tomlinson, Jason M.; Volkamer, Rainer; Wilson, Jacqueline; Zaveri, Rahul A.; Zelenyuk, Alla

2016-08-01

The ability of the Weather Research and Forecasting model with chemistry (WRF-Chem) version 3.7 and the Community Atmosphere Model version 5.3 (CAM5) in simulating profiles of aerosol properties is quantified using extensive in situ and remote sensing measurements from the Two-Column Aerosol Project (TCAP) conducted during July of 2012. TCAP was supported by the U.S. Department of Energy's Atmospheric Radiation Measurement program and was designed to obtain observations within two atmospheric columns; one fixed over Cape Cod, Massachusetts, and the other several hundred kilometers over the ocean. The performance is quantified using most of the available aircraft and surface measurements during July, and 2 days are examined in more detail to identify the processes responsible for the observed aerosol layers. The higher-resolution WRF-Chem model produced more aerosol mass in the free troposphere than the coarser-resolution CAM5 model so that the fraction of aerosol optical thickness above the residual layer from WRF-Chem was more consistent with lidar measurements. We found that the free troposphere layers are likely due to mean vertical motions associated with synoptic-scale convergence that lifts aerosols from the boundary layer. The vertical displacement and the time period associated with upward transport in the troposphere depend on the strength of the synoptic system and whether relatively high boundary layer aerosol concentrations are present where convergence occurs. While a parameterization of subgrid scale convective clouds applied in WRF-Chem modulated the concentrations of aerosols aloft, it did not significantly change the overall altitude and depth of the layers.

A Monte-Carlo Analysis of Organic Aerosol Volatility with Aerosol Microphysics

NASA Astrophysics Data System (ADS)

Gao, C. Y.; Tsigaridis, K.; Bauer, S. E.

2016-12-01

A newly developed box model scheme, MATRIX-VBS, includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves aerosol mass and number concentrations and aerosol mixing state. The new scheme advanced the representation of organic aerosols in Earth system models by improving the traditional and simplistic treatment of organic aerosols as non-volatile and with a fixed size distribution. Further development includes adding the condensation of organics on coarse mode aerosols - dust and sea salt, thus making all organics in the system semi-volatile. To test and simplify the model, a Monte-Carlo analysis is performed to pin point which processes affect organics the most under which chemical and meteorological conditions. Since the model's parameterizations have the ability to capture a very wide range of conditions, from very clean to very polluted and for a wide range of meteorological conditions, all possible scenarios on Earth across the whole parameter space, including temperature, location, emissions and oxidant levels, are examined. The Monte-Carlo simulations provide quantitative information on the sensitivity of the newly developed model and help us understand how organics are affecting the size distribution, mixing state and volatility distribution at varying levels of meteorological conditions and pollution levels. In addition, these simulations give information on which parameters play a critical role in the aerosol distribution and evolution in the atmosphere and which do not, that will facilitate the simplification of the box model, an important step in its implementation in the global model.

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.

Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol

PubMed Central

Zhang, Xuan; Cappa, Christopher D.; Jathar, Shantanu H.; McVay, Renee C.; Ensberg, Joseph J.; Kleeman, Michael J.; Seinfeld, John H.

2014-01-01

Secondary organic aerosol (SOA) constitutes a major fraction of submicrometer atmospheric particulate matter. Quantitative simulation of SOA within air-quality and climate models—and its resulting impacts—depends on the translation of SOA formation observed in laboratory chambers into robust parameterizations. Worldwide data have been accumulating indicating that model predictions of SOA are substantially lower than ambient observations. Although possible explanations for this mismatch have been advanced, none has addressed the laboratory chamber data themselves. Losses of particles to the walls of chambers are routinely accounted for, but there has been little evaluation of the effects on SOA formation of losses of semivolatile vapors to chamber walls. Here, we experimentally demonstrate that such vapor losses can lead to substantially underestimated SOA formation, by factors as much as 4. Accounting for such losses has the clear potential to bring model predictions and observations of organic aerosol levels into much closer agreement. PMID:24711404

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.

2005-01-01

Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds, Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., 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 many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.

Uncertainties of parameterized surface downward clear-sky shortwave and all-sky longwave radiation.

NASA Astrophysics Data System (ADS)

Gubler, S.; Gruber, S.; Purves, R. S.

2012-06-01

As many environmental models rely on simulating the energy balance at the Earth's surface based on parameterized radiative fluxes, knowledge of the inherent model uncertainties is important. In this study we evaluate one parameterization of clear-sky direct, diffuse and global shortwave downward radiation (SDR) and diverse parameterizations of clear-sky and all-sky longwave downward radiation (LDR). In a first step, SDR is estimated based on measured input variables and estimated atmospheric parameters for hourly time steps during the years 1996 to 2008. Model behaviour is validated using the high quality measurements of six Alpine Surface Radiation Budget (ASRB) stations in Switzerland covering different elevations, and measurements of the Swiss Alpine Climate Radiation Monitoring network (SACRaM) in Payerne. In a next step, twelve clear-sky LDR parameterizations are calibrated using the ASRB measurements. One of the best performing parameterizations is elected to estimate all-sky LDR, where cloud transmissivity is estimated using measured and modeled global SDR during daytime. In a last step, the performance of several interpolation methods is evaluated to determine the cloud transmissivity in the night. We show that clear-sky direct, diffuse and global SDR is adequately represented by the model when using measurements of the atmospheric parameters precipitable water and aerosol content at Payerne. If the atmospheric parameters are estimated and used as a fix value, the relative mean bias deviance (MBD) and the relative root mean squared deviance (RMSD) of the clear-sky global SDR scatter between between -2 and 5%, and 7 and 13% within the six locations. The small errors in clear-sky global SDR can be attributed to compensating effects of modeled direct and diffuse SDR since an overestimation of aerosol content in the atmosphere results in underestimating the direct, but overestimating the diffuse SDR. Calibration of LDR parameterizations to local conditions reduces MBD and RMSD strongly compared to using the published values of the parameters, resulting in relative MBD and RMSD of less than 5% respectively 10% for the best parameterizations. The best results to estimate cloud transmissivity during nighttime were obtained by linearly interpolating the average of the cloud transmissivity of the four hours of the preceeding afternoon and the following morning. Model uncertainty can be caused by different errors such as code implementation, errors in input data and in estimated parameters, etc. The influence of the latter (errors in input data and model parameter uncertainty) on model outputs is determined using Monte Carlo. Model uncertainty is provided as the relative standard deviation σrel of the simulated frequency distributions of the model outputs. An optimistic estimate of the relative uncertainty σrel resulted in 10% for the clear-sky direct, 30% for diffuse, 3% for global SDR, and 3% for the fitted all-sky LDR.

Limited effect of anthropogenic nitrogen oxides on Secondary Organic Aerosol formation

DOE PAGES

Zheng, Y.; Unger, N.; Hodzic, A.; ...

2015-08-28

Globally, secondary organic aerosol (SOA) is mostly formed from emissions of biogenic volatile organic compounds (VOCs) by vegetation, but can be modified by human activities as demonstrated in recent research. Specifically, nitrogen oxides (NO x = NO + NO 2) have been shown to play a critical role in the chemical formation of low volatility compounds. We have updated the SOA scheme in the global NCAR Community Atmospheric Model version 4 with chemistry (CAM4-chem) by implementing a 4-product Volatility Basis Set (VBS) scheme, including NO x-dependent SOA yields and aging parameterizations. The predicted organic aerosol amounts capture both the magnitudemore » and distribution of US surface annual mean measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network by 50 %, and the simulated vertical profiles are within a factor of two compared to Aerosol Mass Spectrometer (AMS) measurements from 13 aircraft-based field campaigns across different region and seasons. We then perform sensitivity experiments to examine how the SOA loading responds to a 50 % reduction in anthropogenic nitric oxide (NO) emissions in different regions. We find limited SOA reductions of 0.9 to 5.6, 6.4 to 12.0 and 0.9 to 2.8 % for global, the southeast US and the Amazon NO x perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NO x can be largely attributed to buffering in chemical pathways (low- and high-NO x pathways, O 3 versus NO 3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.« less

Hygroscopic growth of size-resolved, emission-source classified, aerosol particles sampled across the United States

NASA Astrophysics Data System (ADS)

Shingler, T.; Crosbie, E. C.; Ziemba, L. D.; Anderson, B. E.; Campuzano Jost, P.; Jimenez, J. L.; Mikoviny, T.; Wisthaler, A.; Sorooshian, A.

2014-12-01

The hygroscopic growth of atmospheric aerosol particles is a key air quality parameter, impacting the radiation budget, visibility, and cloud formation. During the DC3 and SEAC4RS field campaigns (>300 total flight hours), measurements were made over 32 US states, Canada, the Pacific Ocean, and the Gulf of Mexico, between the surface and 41,000 feet ASL. The aircraft research payloads included a suite of in-situ aerosol and gas phase instruments. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) and the Langley Aerosol Research Group Experiment (LARGE) humidified nephelometer instrument applied different techniques to measure water uptake by aerosol particles at prescribed relative humidity values. Size-resolved growth factor (GF ≡ Dp,wet/Dp,dry) measurements by the DASH-SP are compared to bulk scattering measurements (f(RH) ≡ σscat,wet/σscat,dry) by the LARGE instrument. Spatial location and volatile organic compound tracers such as isoprene and acetonitrile are used to classify the origin of distinct air masses, including: forest fires, biogenic-emitting forests, agricultural use lands, marine boundary layer, urban, and rural background. Analyses of GF results by air mass origin are reported and results are compared with f(RH) measurements. A parameterization between the f(RH) and GF measurements and its potential uses are discussed.

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

DOE PAGES

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

2016-03-03

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

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

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

Fan, Jiwen; Wang, Yuan; Rosenfeld, Daniel

2016-11-01

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

Large Contribution of Coarse Mode to Aerosol Microphysical and Optical Properties: Evidence from Ground-Based Observations of a Transpacific Dust Outbreak at a High-Elevation North American Site

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

Kassianov, E.; Pekour, M.; Flynn, C.

Our work is motivated by previous studies of the long-range trans-Atlantic transport of Saharan dust and the observed quasi-static nature of coarse mode aerosol with a volume median diameter (VMD) of approximately 3.5 µm. We examine coarse mode contributions from the trans-Pacific transport of Asian dust to North American aerosol microphysical and optical properties using a dataset collected at the high-elevation, mountain-top Storm Peak Laboratory (SPL, 3.22 km above sea level [ASL]) and the nearby Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF, 2.76 km ASL). Data collected during the SPL Cloud Property Validation Experiment (STORMVEX, March 2011) are complemented bymore » quasi-global high-resolution model simulations coupled with aerosol chemistry. We identify dust event associated mostly with Asian plume (about 70% of dust mass) where the coarse mode with moderate (~4 µm) VMD is distinct and contributes substantially to aerosol microphysical (up to 70% for total volume) and optical (up to 45% for total scattering and aerosol optical depth) properties. Our results, when compared with previous Saharan dust studies, suggest a fairly invariant behavior of coarse mode dust aerosols. If confirmed in additional studies, this invariant behavior may simplify considerably model parameterizations for complex and size-dependent processes associated with dust transport and removal.« less

Salting Constants of Small Organic Molecules in Aerosol-Relevant Salts and Application to Aerosol Formation in the Southeastern United States

NASA Astrophysics Data System (ADS)

Waxman, E.; Carlton, A. M. G.; Ziemann, P. J.; Volkamer, R. M.

2014-12-01

Secondary organic aerosol (SOA) formation from small water-soluble molecules such as glyoxal and methyl glyoxal is a topic of emerging interest. Results from recent field campaigns, e.g. Waxman et al. (2013, GRL) and Knote et al. (2014, ACP), show that these molecules can form significant SOA mass as a result of 'salting-in'. Salting-in happens when a molecule's solubility increases with salt concentration and salting-out is the reverse. Salting effects modify the solubility exponentially with increasing salt concentration, and thus the effective Henry's law constant can strongly modify partitioning, and multiphase chemical reaction rates in aerosol water. Moreover, the solubility in aerosol water cannot easily inferred based on the solubility in cloud water, as the salting effects could change the solubility by a factor of 104 or more. In this work, we have devised and applied a novel experimental setup to measure salting constants using an ion trap mass spectrometer. We focus on small, water soluble molecules like methyl glyoxal and similar compounds and measure salting constants for aerosol-relevant salts including ammonium sulfate, ammonium nitrate, and sodium chloride. The Setschenow salting-constant values are then used to parameterize the effects of salting in CMAQ. We present a series of sensitivity studies of the effects that inorganic aerosols have on the SOA formation from small soluble molecules in the southeastern United States.

Long term measurements of optical properties and their hygroscopic enhancement

NASA Astrophysics Data System (ADS)

Hervo, M.; Sellegri, K.; Pichon, J. M.; Roger, J. C.; Laj, P.

2014-11-01

Optical properties of aerosols were measured from the GAW Puy de Dôme station (1465 m) over a seven year period (2006-2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010-2011). The analysis of the spatial and temporal variability of the optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the PBL height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type. At 90% humidity, the scattering factor enhancement (fσsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH = 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type.

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).

Improvement of a snow albedo parameterization in the Snow-Atmosphere-Soil Transfer model: evaluation of impacts of aerosol on seasonal snow cover

NASA Astrophysics Data System (ADS)

Zhong, Efang; Li, Qian; Sun, Shufen; Chen, Wen; Chen, Shangfeng; Nath, Debashis

2017-11-01

The presence of light-absorbing aerosols (LAA) in snow profoundly influence the surface energy balance and water budget. However, most snow-process schemes in land-surface and climate models currently do not take this into consideration. To better represent the snow process and to evaluate the impacts of LAA on snow, this study presents an improved snow albedo parameterization in the Snow-Atmosphere-Soil Transfer (SAST) model, which includes the impacts of LAA on snow. Specifically, the Snow, Ice and Aerosol Radiation (SNICAR) model is incorporated into the SAST model with an LAA mass stratigraphy scheme. The new coupled model is validated against in-situ measurements at the Swamp Angel Study Plot (SASP), Colorado, USA. Results show that the snow albedo and snow depth are better reproduced than those in the original SAST, particularly during the period of snow ablation. Furthermore, the impacts of LAA on snow are estimated in the coupled model through case comparisons of the snowpack, with or without LAA. The LAA particles directly absorb extra solar radiation, which accelerates the growth rate of the snow grain size. Meanwhile, these larger snow particles favor more radiative absorption. The average total radiative forcing of the LAA at the SASP is 47.5 W m-2. This extra radiative absorption enhances the snowmelt rate. As a result, the peak runoff time and "snow all gone" day have shifted 18 and 19.5 days earlier, respectively, which could further impose substantial impacts on the hydrologic cycle and atmospheric processes.

Global Distribution of Cloud Droplet Number Concentration, Autoconversion Rate, and Aerosol Indirect Effect Under Diabatic Droplet Activation

NASA Technical Reports Server (NTRS)

Barahona, Donifan; Sotiropoulou, Rafaella; Nenes, Athanasios

2011-01-01

This study presents a global assessment of the sensitivity of droplet number to diabatic activation (i.e., including effects from entrainment of dry air) and its first-order tendency on indirect forcing and autoconversion. Simulations were carried out with the NASA Global Modeling Initiative (GMI) atmospheric and transport model using climatological metereorological fields derived from the former NASA Data Assimilation Office (DAO), the NASA Finite volume GCM (FVGCM) and the Goddard Institute for Space Studies version II (GISS) GCM. Cloud droplet number concentration (CDNC) is calculated using a physically based prognostic parameterization that explicitly includes entrainment effects on droplet formation. Diabatic activation results in lower CDNC, compared to adiabatic treatment of the process. The largest decrease in CDNC (by up to 75 percent) was found in the tropics and in zones of moderate CCN concentration. This leads to a global mean effective radius increase between 0.2-0.5 micrometers (up to 3.5 micrometers over the tropics), a global mean autoconversion rate increase by a factor of 1.1 to 1.7 (up to a factor of 4 in the tropics), and a 0.2-0.4 W m(exp -2) decrease in indirect forcing. The spatial patterns of entrainment effects on droplet activation tend to reduce biases in effective radius (particularly in the tropics) when compared to satellite retrievals. Considering the diabatic nature of ambient clouds, entrainment effects on CDNC need to be considered in GCM studies of the aerosol indirect effect.

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

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

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well-constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (N a). These terms are further parameterized, and by assuming that on seasonal timescales N a is in steady state, the budget equation is rearranged to form a diagnostic equation for Nmore » a based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter N a concentrations are made using the simplified steady-state model and seasonal mean observed variables, and are found to match well with the observed N a. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g. precipitation rate, free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in N a, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.« less

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

DOE PAGES

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy; ...

2018-01-21

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well-constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (N a). These terms are further parameterized, and by assuming that on seasonal timescales N a is in steady state, the budget equation is rearranged to form a diagnostic equation for Nmore » a based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter N a concentrations are made using the simplified steady-state model and seasonal mean observed variables, and are found to match well with the observed N a. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g. precipitation rate, free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in N a, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.« less

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

NASA Astrophysics Data System (ADS)

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy; Eastman, Ryan; Luke, Edward

2018-01-01

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (Na). These terms are then parameterized, and by assuming that on seasonal time scales Na is in steady state, the budget equation is rearranged to form a diagnostic equation for Na based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-Section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter Na concentrations are made using the simplified steady state model and seasonal mean observed variables. These are found to match well with the observed Na. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g., precipitation rate and free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in Na, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.

An attempt to quantify aerosol-cloud effects in fields of precipitating trade wind cumuli

NASA Astrophysics Data System (ADS)

Seifert, Axel; Heus, Thijs

2015-04-01

Aerosol indirect effects are notoriously difficult to understand and quantify. Using large-eddy simulations (LES) we attempt to quantify the impact of aerosols on the albedo and the precipitation formation in trade wind cumulus clouds. Having performed a set of large-domain Giga-LES runs we are able to capture the mesoscale self-organization of the cloud field. Our simulations show that self-organization is intrinsically tied to precipitation formation in this cloud regime making previous studies that did not consider cloud organization questionable. We find that aerosols, here modeled just as a perturbation in cloud droplet number concentration, have a significant impact on the transient behavior, i.e., how fast rain is formed and self-organization of the cloud field takes place. Though, for longer integration times, all simulations approach the same radiative-convective equilibrium and aerosol effects become small. The sensitivity to aerosols becomes even smaller when we include explicit cloud-radiation interaction as this leads to a much faster and more vigorous response of the cloud layer. Overall we find that aerosol-cloud interactions, like cloud lifetime effects etc., are small or even negative when the cloud field is close to equilibrium. Consequently, the Twomey effect does already provide an upper bound on the albedo effects of aerosol perturbations. Our analysis also highlights that current parameterizations that predict only the grid-box mean of the cloud field and do not take into account cloud organization are not able to describe aerosol indirect effects correctly, but overestimate them due to that lack of cloud dynamical and mesoscale buffering.

Global-scale combustion sources of organic aerosols: sensitivity to formation and removal mechanisms

NASA Astrophysics Data System (ADS)

Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Pandis, Spyros N.; Lelieveld, Jos

2017-06-01

Organic compounds from combustion sources such as biomass burning and fossil fuel use are major contributors to the global atmospheric load of aerosols. We analyzed the sensitivity of model-predicted global-scale organic aerosols (OA) to parameters that control primary emissions, photochemical aging, and the scavenging efficiency of organic vapors. We used a computationally efficient module for the description of OA composition and evolution in the atmosphere (ORACLE) of the global chemistry-climate model EMAC (ECHAM/MESSy Atmospheric Chemistry). A global dataset of aerosol mass spectrometer (AMS) measurements was used to evaluate simulated primary (POA) and secondary (SOA) OA concentrations. Model results are sensitive to the emission rates of intermediate-volatility organic compounds (IVOCs) and POA. Assuming enhanced reactivity of semi-volatile organic compounds (SVOCs) and IVOCs with OH substantially improved the model performance for SOA. The use of a hybrid approach for the parameterization of the aging of IVOCs had a small effect on predicted SOA levels. The model performance improved by assuming that freshly emitted organic compounds are relatively hydrophobic and become increasingly hygroscopic due to oxidation.

Determining Best Estimates and Uncertainties in Cloud Microphysical Parameters from ARM Field Data: Implications for Models, Retrieval Schemes and Aerosol-Cloud-Radiation Interactions

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

McFarquhar, Greg

We proposed to analyze in-situ cloud data collected during ARM/ASR field campaigns to create databases of cloud microphysical properties and their uncertainties as needed for the development of improved cloud parameterizations for models and remote sensing retrievals, and for evaluation of model simulations and retrievals. In particular, we proposed to analyze data collected over the Southern Great Plains (SGP) during the Mid-latitude Continental Convective Clouds Experiment (MC3E), the Storm Peak Laboratory Cloud Property Validation Experiment (STORMVEX), the Small Particles in Cirrus (SPARTICUS) Experiment and the Routine AAF Clouds with Low Optical Water Depths (CLOWD) Optical Radiative Observations (RACORO) field campaign,more » over the North Slope of Alaska during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) and the Mixed-Phase Arctic Cloud Experiment (M-PACE), and over the Tropical Western Pacific (TWP) during The Tropical Warm Pool International Cloud Experiment (TWP-ICE), to meet the following 3 objectives; derive statistical databases of single ice particle properties (aspect ratio AR, dominant habit, mass, projected area) and distributions of ice crystals (size distributions SDs, mass-dimension m-D, area-dimension A-D relations, mass-weighted fall speeds, single-scattering properties, total concentrations N, ice mass contents IWC), complete with uncertainty estimates; assess processes by which aerosols modulate cloud properties in arctic stratus and mid-latitude cumuli, and quantify aerosol’s influence in context of varying meteorological and surface conditions; and determine how ice cloud microphysical, single-scattering and fall-out properties and contributions of small ice crystals to such properties vary according to location, environment, surface, meteorological and aerosol conditions, and develop parameterizations of such effects.In this report we describe the accomplishments that we made on all 3 research objectives.« less

Experimental study of H2SO4 aerosol nucleation at high ionization levels

NASA Astrophysics Data System (ADS)

Tomicic, Maja; Bødker Enghoff, Martin; Svensmark, Henrik

2018-04-01

One hundred and ten direct measurements of aerosol nucleation rate at high ionization levels were performed in an 8 m3 reaction chamber. Neutral and ion-induced particle formation from sulfuric acid (H2SO4) was studied as a function of ionization and H2SO4 concentration. Other species that could have participated in the nucleation, such as NH3 or organic compounds, were not measured but assumed constant, and the concentration was estimated based on the parameterization by Gordon et al. (2017). Our parameter space is thus [H2SO4] = 4×106 - 3×107 cm-3, [NH3+ org] = 2.2 ppb, T = 295 K, RH = 38 %, and ion concentrations of 1700-19 000 cm-3. The ion concentrations, which correspond to levels caused by a nearby supernova, were achieved with gamma ray sources. Nucleation rates were directly measured with a particle size magnifier (PSM Airmodus A10) at a size close to critical cluster size (mobility diameter of ˜ 1.4 nm) and formation rates at a mobility diameter of ˜ 4 nm were measured with a CPC (TSI model 3775). The measurements show that nucleation increases by around an order of magnitude when the ionization increases from background to supernova levels under fixed gas conditions. The results expand the parameterization presented in Dunne et al. (2016) and Gordon et al. (2017) (for [NH3 + org] = 2.2 ppb and T = 295 K) to lower sulfuric acid concentrations and higher ion concentrations. The results make it possible to expand the parameterization presented in Dunne et al. (2016) and Gordon et al. (2017) to higher ionization levels.

Model representations of aerosol layers transported from North America over the Atlantic Ocean during the Two-Column Aerosol Project

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

Fast, Jerome D.; Berg, Larry K.; Zhang, Kai

2016-08-22

The ability of the Weather Research and Forecasting model with chemistry (WRF-Chem) version 3.7 and the Community Atmosphere Model version 5.3 (CAM5) in simulating profiles of aerosol properties is quantified using extensive in situ and remote sensing measurements from the Two Column Aerosol Project (TCAP) conducted during July of 2012. TCAP was supported by the U.S. Department of Energy’s Atmospheric Radiation Measurement program and was designed to obtain observations within two atmospheric columns; one fixed over Cape Cod, Massachusetts and the other several hundred kilometers over the ocean. The performance is quantified using most of the available aircraft and surfacemore » measurements during July, and two days are examined in more detail to identify the processes responsible for the observed aerosol layers. The higher resolution WRF-Chem model produced more aerosol mass in the free troposphere than the coarser resolution CAM5 model so that the fraction of aerosol optical thickness above the residual layer from WRF-Chem was more consistent with lidar measurements. We found that the free troposphere layers are likely due to mean vertical motions associated with synoptic-scale convergence that lifts aerosols from the boundary layer. The vertical displacement and the time period associated with upward transport in the troposphere depend on the strength of the synoptic system and whether relatively high boundary layer aerosol concentrations are present where convergence occurs. While a parameterization of subgrid scale convective clouds applied in WRF-Chem modulated the concentrations of aerosols aloft, it did not significantly change the overall altitude and depth of the layers.« less

Model representations of aerosol layers transported from North America over the Atlantic Ocean during the Two-Column Aerosol Project

DOE PAGES

Fast, Jerome D.; Berg, Larry K.; Zhang, Kai; ...

2016-08-22

The ability of the Weather Research and Forecasting model with chemistry (WRF-Chem) version 3.7 and the Community Atmosphere Model version 5.3 (CAM5) in simulating profiles of aerosol properties is quantified using extensive in situ and remote sensing measurements from the Two-Column Aerosol Project (TCAP) conducted during July of 2012. TCAP was supported by the U.S. Department of Energy's Atmospheric Radiation Measurement program and was designed to obtain observations within two atmospheric columns; one fixed over Cape Cod, Massachusetts, and the other several hundred kilometers over the ocean. The performance is quantified using most of the available aircraft and surface measurementsmore » during July, and 2 days are examined in more detail to identify the processes responsible for the observed aerosol layers. The higher-resolution WRF-Chem model produced more aerosol mass in the free troposphere than the coarser-resolution CAM5 model so that the fraction of aerosol optical thickness above the residual layer from WRF-Chem was more consistent with lidar measurements. We found that the free troposphere layers are likely due to mean vertical motions associated with synoptic-scale convergence that lifts aerosols from the boundary layer. The vertical displacement and the time period associated with upward transport in the troposphere depend on the strength of the synoptic system and whether relatively high boundary layer aerosol concentrations are present where convergence occurs. In conclusion, while a parameterization of subgrid scale convective clouds applied in WRF-Chem modulated the concentrations of aerosols aloft, it did not significantly change the overall altitude and depth of the layers.« less

A new approach to modeling aerosol effects on East Asian climate: Parametric uncertainties associated with emissions, cloud microphysics, and their interactions: AEROSOL EFFECTS ON EAST ASIAN CLIMATE

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

Yan, Huiping; Qian, Yun; Zhao, Chun

2015-09-09

In this study, we adopt a parametric sensitivity analysis framework that integrates the quasi-Monte Carlo parameter sampling approach and a surrogate model to examine aerosol effects on the East Asian Monsoon climate simulated in the Community Atmosphere Model (CAM5). A total number of 256 CAM5 simulations are conducted to quantify the model responses to the uncertain parameters associated with cloud microphysics parameterizations and aerosol (e.g., sulfate, black carbon (BC), and dust) emission factors and their interactions. Results show that the interaction terms among parameters are important for quantifying the sensitivity of fields of interest, especially precipitation, to the parameters. Themore » relative importance of cloud-microphysics parameters and emission factors (strength) depends on evaluation metrics or the model fields we focused on, and the presence of uncertainty in cloud microphysics imposes an additional challenge in quantifying the impact of aerosols on cloud and climate. Due to their different optical and microphysical properties and spatial distributions, sulfate, BC, and dust aerosols have very different impacts on East Asian Monsoon through aerosol-cloud-radiation interactions. The climatic effects of aerosol do not always have a monotonic response to the change of emission factors. The spatial patterns of both sign and magnitude of aerosol-induced changes in radiative fluxes, cloud, and precipitation could be different, depending on the aerosol types, when parameters are sampled in different ranges of values. We also identify the different cloud microphysical parameters that show the most significant impact on climatic effect induced by sulfate, BC and dust, respectively, in East Asia.« less

Studying Diurnal Variations of Aerosols with NASA MERRA-2 Reanalysis Data

NASA Technical Reports Server (NTRS)

Shen, Suhung; Ostrenga, Dana M.; Zeng, Jian; Vollmer, Bruce E.

2018-01-01

Aerosols play an important role in atmospheric dynamics, climate variations, and Earth's energy cycle by altering the radiation balance in the atmosphere through interaction with clouds, providing fertilizer for forests and canopy, and as a supply of iron to the ocean over long time periods. Studies suggest that much of the feedback between dust aerosols and dynamics is associated with diurnal and synoptic scale variability. However, the lack of sub-daily resolution of aerosols from satellite observations makes it difficult to study the diurnal characteristics, especially over tropical and subtropical regions. Investigation of this topic utilizes over 37 years of simulated global aerosol products from NASA atmospheric reanalysis, in the second Modern-Era Retrospective analysis for Research and Applications (MERRA-2) data set, available from NASA Goddard Earth Science Data and Information Services Center (GES DISC). MERRA-2 covers the period 1980-present, and is continuing as an ongoing climate analysis. Aerosol assimilation is included throughout the period, using data from MODIS, MISR, AERONET, and AVHRR (in the pre-EOS period). The aerosols are assimilated using the MERRA-2 aerosol model, which interacts directly with radiation parameterization, and is radiatively coupled with atmospheric model dynamics in the Goddard Earth Observing System Model, Version 5 (GEOS-5). Hourly, monthly, and monthly diurnal data are available at spatial resolution of 0.5o x 0.625o (latitude x longitude). By using MERRA-2 hourly and monthly diurnal products, different aerosol diurnal variabilities are observed over North America, Africa, Asia, and Australia, that may be due to different meteorological conditions and aerosol sources. The presentation will also provide an overview of MERRA-2 data services at GES DISC, such as how to find and download data, and how to quickly visualize and analyze data online with Giovanni.

Sensitivity of Simulated Warm Rain Formation to Collision and Coalescence Efficiencies, Breakup, and Turbulence: Comparison of Two Bin-Resolved Numerical Models

NASA Technical Reports Server (NTRS)

Fridlind, Ann; Seifert, Axel; Ackerman, Andrew; Jensen, Eric

2004-01-01

Numerical models that resolve cloud particles into discrete mass size distributions on an Eulerian grid provide a uniquely powerful means of studying the closely coupled interaction of aerosols, cloud microphysics, and transport that determine cloud properties and evolution. However, such models require many experimentally derived paramaterizations in order to properly represent the complex interactions of droplets within turbulent flow. Many of these parameterizations remain poorly quantified, and the numerical methods of solving the equations for temporal evolution of the mass size distribution can also vary considerably in terms of efficiency and accuracy. In this work, we compare results from two size-resolved microphysics models that employ various widely-used parameterizations and numerical solution methods for several aspects of stochastic collection.

Quantifying Sources and Sinks of Reactive Gases in the Lower Atmosphere Using Airborne Flux Observations

NASA Technical Reports Server (NTRS)

Wolfe, G. M.; Hanisco, T. F.; Arkinson, H. L.; Bui, T. P.; Crounse, J. D.; Dean-Day, J.; Goldstein, A.; Guenther, A.; Hall, S. R.; Huey, G.;

Parameterizing Sound: Design Considerations for an Environmental Sound Database

DTIC Science & Technology

2015-04-01

Accordion Car backfire Crushing a metal can Aerosol can Car crash Crushing a tin can Alarm clock Car ignition Crushing egg shells Alloette...top Coffee perking Eggs beaten in a bowl with a whisk Bowling Coffee pot whistling Elastic (snap) Bread cutting Coin dropping Electric...Bus Combination lock Female speaking Bus air break Cooking with fat Ferry Bus stop and go Cuckoo clock Ferry horn Camera Corduroy

CloudSat 2C-ICE product update with a new Ze parameterization in lidar-only region.

PubMed

Deng, Min; Mace, Gerald G; Wang, Zhien; Berry, Elizabeth

2015-12-16

The CloudSat 2C-ICE data product is derived from a synergetic ice cloud retrieval algorithm that takes as input a combination of CloudSat radar reflectivity ( Z e ) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation lidar attenuated backscatter profiles. The algorithm uses a variational method for retrieving profiles of visible extinction coefficient, ice water content, and ice particle effective radius in ice or mixed-phase clouds. Because of the nature of the measurements and to maintain consistency in the algorithm numerics, we choose to parameterize (with appropriately large specification of uncertainty) Z e and lidar attenuated backscatter in the regions of a cirrus layer where only the lidar provides data and where only the radar provides data, respectively. To improve the Z e parameterization in the lidar-only region, the relations among Z e , extinction, and temperature have been more thoroughly investigated using Atmospheric Radiation Measurement long-term millimeter cloud radar and Raman lidar measurements. This Z e parameterization provides a first-order estimation of Z e as a function extinction and temperature in the lidar-only regions of cirrus layers. The effects of this new parameterization have been evaluated for consistency using radiation closure methods where the radiative fluxes derived from retrieved cirrus profiles compare favorably with Clouds and the Earth's Radiant Energy System measurements. Results will be made publicly available for the entire CloudSat record (since 2006) in the most recent product release known as R05.

Chemical Thermodynamics of Aqueous Atmospheric Aerosols: Modeling and Microfluidic Measurements

NASA Astrophysics Data System (ADS)

Nandy, L.; Dutcher, C. S.

2017-12-01

Accurate predictions of gas-liquid-solid equilibrium phase partitioning of atmospheric aerosols by thermodynamic modeling and measurements is critical for determining particle composition and internal structure at conditions relevant to the atmosphere. Organic acids that originate from biomass burning, and direct biogenic emission make up a significant fraction of the organic mass in atmospheric aerosol particles. In addition, inorganic compounds like ammonium sulfate and sea salt also exist in atmospheric aerosols, that results in a mixture of single, double or triple charged ions, and non-dissociated and partially dissociated organic acids. Statistical mechanics based on a multilayer adsorption isotherm model can be applied to these complex aqueous environments for predictions of thermodynamic properties. In this work, thermodynamic analytic predictive models are developed for multicomponent aqueous solutions (consisting of partially dissociating organic and inorganic acids, fully dissociating symmetric and asymmetric electrolytes, and neutral organic compounds) over the entire relative humidity range, that represent a significant advancement towards a fully predictive model. The model is also developed at varied temperatures for electrolytes and organic compounds the data for which are available at different temperatures. In addition to the modeling approach, water loss of multicomponent aerosol particles is measured by microfluidic experiments to parameterize and validate the model. In the experimental microfluidic measurements, atmospheric aerosol droplet chemical mimics (organic acids and secondary organic aerosol (SOA) samples) are generated in microfluidic channels and stored and imaged in passive traps until dehydration to study the influence of relative humidity and water loss on phase behavior.

Climate Change and Impacts Research Experiences for Urban Students

NASA Astrophysics Data System (ADS)

Marchese, P.; Carlson, B. E.; Rosenzweig, C.; Austin, S. A.; Peteet, D. M.; Druyan, L.; Fulakeza, M.; Gaffin, S.; Scalzo, F.; Frost, J.; Moshary, F.; Greenbaum, S.; Cheung, T. K.; Howard, A.; Steiner, J. C.; Johnson, L. P.

2011-12-01

Climate change and impacts research for undergraduate urban students is the focus of the Center for Global Climate Research (CGCR). We describe student research and significant results obtained during the Summer 2011. The NSF REU site, is a collaboration between the City University of New York (CUNY) and the NASA Goddard Institute for Space Studies (GISS). The research teams are mentored by NASA scientists and CUNY faculty. Student projects include: Effects of Stratospheric Aerosols on Tropical Cyclone Activity in the North Atlantic Basin; Comparison of Aerosol Optical Depth and Angstrom Exponent Retrieved by AERONET, MISR, and MODIS Measurements; White Roofs to the Rescue: Combating the Urban Heat Island Effect; Tropospheric Ozone Investigations in New York City; Carbon Sequestration with Climate Change in Alaskan Peatlands; Validating Regional Climate Models for Western Sub-Sahara Africa; Bio-Remediation of Toxic Waste Sites: Mineral Characteristics of Cyanide-Treated Mining Waste; Assessment of an Ocean Mixing Parameterization for Climate Studies; Comparative Wind Speed through Doppler Sounding with Pulsed Infrared LIDAR; and Satellite Telemetry and Communications. The CGCR also partners with the New York City Research Initiative (NYCRI) at GISS. The center is supported by NSF ATM-0851932 and the American Recovery and Reinvestment Act of 2009 (ARRA).

Improving organic aerosol treatments in CESM/CAM5: Development, application, and evaluation

NASA Astrophysics Data System (ADS)

Glotfelty, Timothy; He, Jian; Zhang, Yang

2017-06-01

New treatments for organic aerosol (OA) formation have been added to a modified version of the CESM/CAM5 model (CESM-NCSU). These treatments include a volatility basis set treatment for the simulation of primary and secondary organic aerosols (SOAs), a simplified treatment for organic aerosol (OA) formation from glyoxal, and a parameterization representing the impact of new particle formation (NPF) of organic gases and sulfuric acid. With the inclusion of these new treatments, the concentration of oxygenated organic aerosol increases by 0.33 µg m-3 and that of primary organic aerosol (POA) decreases by 0.22 µg m-3 on global average. The decrease in POA leads to a reduction in the OA direct effect, while the increased OOA increases the OA indirect effects. Simulations with the new OA treatments show considerable improvement in simulated SOA, oxygenated organic aerosol (OOA), organic carbon (OC), total carbon (TC), and total organic aerosol (TOA), but degradation in the performance of HOA. In simulations of the current climate period, despite some deviations from observations, CESM-NCSU with the new OA treatments significantly improves the magnitude, spatial pattern, seasonal pattern of OC and TC, as well as, the speciation of TOA between POA and OOA. Sensitivity analysis reveals that the inclusion of the organic NPF treatment impacts the OA indirect effects by enhancing cloud properties. The simulated OA level and its impact on the climate system are most sensitive to choices in the enthalpy of vaporization and wet deposition of SVOCs, indicating that accurate representations of these parameters are critical for accurate OA-climate simulations.

Effects of data assimilation on the global aerosol key optical properties simulations

NASA Astrophysics Data System (ADS)

Yin, Xiaomei; Dai, Tie; Schutgens, Nick A. J.; Goto, Daisuke; Nakajima, Teruyuki; Shi, Guangyu

2016-09-01

We present the one month results of global aerosol optical properties for April 2006, using the Spectral Radiation Transport Model for Aerosol Species (SPRINTARS) coupled with the Non-hydrostatic ICosahedral Atmospheric Model (NICAM), by assimilating Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) with Local Ensemble Transform Kalman Filter (LETKF). The simulated AOD, Ångström Exponent (AE) and single scattering albedo (SSA) are validated by independent Aerosol Robotic Network (AERONET) observations over the global sites. The data assimilation has the strongest positive effect on the AOD simulation and slight positive influences on the AE and SSA simulations. For the time-averaged globally spatial distribution, the data assimilation increases the model skill score (S) of AOD, AE, and SSA from 0.55, 0.92, and 0.75 to 0.79, 0.94, and 0.80, respectively. Over the North Africa (NAF) and Middle East region where the aerosol composition is simple (mainly dust), the simulated AODs are best improved by the data assimilation, indicating the assimilation correctly modifies the wrong dust burdens caused by the uncertainties of the dust emission parameterization. Assimilation also improves the simulation of the temporal variations of the aerosol optical properties over the AERONET sites, with improved S at 60 (62%), 45 (55%) and 11 (50%) of 97, 82 and 22 sites for AOD, AE and SSA. By analyzing AOD and AE at five selected sites with best S improvement, this study further indicates that the assimilation can reproduce short duration events and ratios between fine and coarse aerosols more accurately.

Modeling the Absorbing Aerosol Index

NASA Technical Reports Server (NTRS)

Penner, Joyce; Zhang, Sophia

2003-01-01

We propose a scheme to model the absorbing aerosol index and improve the biomass carbon inventories by optimizing the difference between TOMS aerosol index (AI) and modeled AI with an inverse model. Two absorbing aerosol types are considered, including biomass carbon and mineral dust. A priori biomass carbon source was generated by Liousse et al [1996]. Mineral dust emission is parameterized according to surface wind and soil moisture using the method developed by Ginoux [2000]. In this initial study, the coupled CCM1 and GRANTOUR model was used to determine the aerosol spatial and temporal distribution. With modeled aerosol concentrations and optical properties, we calculate the radiance at the top of the atmosphere at 340 nm and 380 nm with a radiative transfer model. The contrast of radiance at these two wavelengths will be used to calculate AI. Then we compare the modeled AI with TOMS AI. This paper reports our initial modeling for AI and its comparison with TOMS Nimbus 7 AI. For our follow-on project we will model the global AI with aerosol spatial and temporal distribution recomputed from the IMPACT model and DAO GEOS-1 meteorology fields. Then we will build an inverse model, which applies a Bayesian inverse technique to optimize the agreement of between model and observational data. The inverse model will tune the biomass burning source strength to reduce the difference between modelled AI and TOMS AI. Further simulations with a posteriori biomass carbon sources from the inverse model will be carried out. Results will be compared to available observations such as surface concentration and aerosol optical depth.

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.

Improving organic aerosol treatments in CESM/CAM5: Development, application, and evaluation

PubMed Central

Glotfelty, Timothy; He, Jian

2017-01-01

Abstract New treatments for organic aerosol (OA) formation have been added to a modified version of the CESM/CAM5 model (CESM‐NCSU). These treatments include a volatility basis set treatment for the simulation of primary and secondary organic aerosols (SOAs), a simplified treatment for organic aerosol (OA) formation from glyoxal, and a parameterization representing the impact of new particle formation (NPF) of organic gases and sulfuric acid. With the inclusion of these new treatments, the concentration of oxygenated organic aerosol increases by 0.33 µg m−3 and that of primary organic aerosol (POA) decreases by 0.22 µg m−3 on global average. The decrease in POA leads to a reduction in the OA direct effect, while the increased OOA increases the OA indirect effects. Simulations with the new OA treatments show considerable improvement in simulated SOA, oxygenated organic aerosol (OOA), organic carbon (OC), total carbon (TC), and total organic aerosol (TOA), but degradation in the performance of HOA. In simulations of the current climate period, despite some deviations from observations, CESM‐NCSU with the new OA treatments significantly improves the magnitude, spatial pattern, seasonal pattern of OC and TC, as well as, the speciation of TOA between POA and OOA. Sensitivity analysis reveals that the inclusion of the organic NPF treatment impacts the OA indirect effects by enhancing cloud properties. The simulated OA level and its impact on the climate system are most sensitive to choices in the enthalpy of vaporization and wet deposition of SVOCs, indicating that accurate representations of these parameters are critical for accurate OA‐climate simulations. PMID:29104733

Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation

NASA Astrophysics Data System (ADS)

Zheng, Y.; Unger, N.; Hodzic, A.; Emmons, L.; Knote, C.; Tilmes, S.; Lamarque, J.-F.; Yu, P.

2015-12-01

Globally, secondary organic aerosol (SOA) is mostly formed from emissions of biogenic volatile organic compounds (VOCs) by vegetation, but it can be modified by human activities as demonstrated in recent research. Specifically, nitrogen oxides (NOx = NO + NO2) have been shown to play a critical role in the chemical formation of low volatility compounds. We have updated the SOA scheme in the global NCAR (National Center for Atmospheric Research) Community Atmospheric Model version 4 with chemistry (CAM4-chem) by implementing a 4-product volatility basis set (VBS) scheme, including NOx-dependent SOA yields and aging parameterizations. Small differences are found for the no-aging VBS and 2-product schemes; large increases in SOA production and the SOA-to-OA ratio are found for the aging scheme. The predicted organic aerosol amounts capture both the magnitude and distribution of US surface annual mean measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network by 50 %, and the simulated vertical profiles are within a factor of 2 compared to aerosol mass spectrometer (AMS) measurements from 13 aircraft-based field campaigns across different regions and seasons. We then perform sensitivity experiments to examine how the SOA loading responds to a 50 % reduction in anthropogenic nitric oxide (NO) emissions in different regions. We find limited SOA reductions of 0.9-5.6, 6.4-12.0 and 0.9-2.8 % for global, southeast US and Amazon NOx perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to a limited shift in chemical regime, to buffering in chemical pathways (low- and high-NOx pathways, O3 versus NO3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.

Are atmospheric updrafts a key to unlocking climate forcing and sensitivity?

DOE PAGES

Donner, Leo J.; O'Brien, Travis A.; Rieger, Daniel; ...

2016-10-20

Both climate forcing and climate sensitivity persist as stubborn uncertainties limiting the extent to which climate models can provide actionable scientific scenarios for climate change. A key, explicit control on cloud–aerosol interactions, the largest uncertainty in climate forcing, is the vertical velocity of cloud-scale updrafts. Model-based studies of climate sensitivity indicate that convective entrainment, which is closely related to updraft speeds, is an important control on climate sensitivity. Updraft vertical velocities also drive many physical processes essential to numerical weather prediction. Vertical velocities and their role in atmospheric physical processes have been given very limited attention in models for climatemore » and numerical weather prediction. The relevant physical scales range down to tens of meters and are thus frequently sub-grid and require parameterization. Many state-of-science convection parameterizations provide mass fluxes without specifying Vertical velocities and their role in atmospheric physical processes have been given very limited attention in models for climate and numerical weather prediction. The relevant physical scales range down to tens of meters and are thus frequently sub-grid and require parameterization. Many state-of-science convection parameterizations provide mass fluxes without specifying vs in climate models may capture this behavior, but it has not been accounted for when parameterizing cloud and precipitation processes in current models. New observations of convective vertical velocities offer a potentially promising path toward developing process-level cloud models and parameterizations for climate and numerical weather prediction. Taking account of the scale dependence of resolved vertical velocities offers a path to matching cloud-scale physical processes and their driving dynamics more realistically, with a prospect of reduced uncertainty in both climate forcing and sensitivity.« less

Are atmospheric updrafts a key to unlocking climate forcing and sensitivity?

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

Donner, Leo J.; O'Brien, Travis A.; Rieger, Daniel

Both climate forcing and climate sensitivity persist as stubborn uncertainties limiting the extent to which climate models can provide actionable scientific scenarios for climate change. A key, explicit control on cloud–aerosol interactions, the largest uncertainty in climate forcing, is the vertical velocity of cloud-scale updrafts. Model-based studies of climate sensitivity indicate that convective entrainment, which is closely related to updraft speeds, is an important control on climate sensitivity. Updraft vertical velocities also drive many physical processes essential to numerical weather prediction. Vertical velocities and their role in atmospheric physical processes have been given very limited attention in models for climatemore » and numerical weather prediction. The relevant physical scales range down to tens of meters and are thus frequently sub-grid and require parameterization. Many state-of-science convection parameterizations provide mass fluxes without specifying Vertical velocities and their role in atmospheric physical processes have been given very limited attention in models for climate and numerical weather prediction. The relevant physical scales range down to tens of meters and are thus frequently sub-grid and require parameterization. Many state-of-science convection parameterizations provide mass fluxes without specifying vs in climate models may capture this behavior, but it has not been accounted for when parameterizing cloud and precipitation processes in current models. New observations of convective vertical velocities offer a potentially promising path toward developing process-level cloud models and parameterizations for climate and numerical weather prediction. Taking account of the scale dependence of resolved vertical velocities offers a path to matching cloud-scale physical processes and their driving dynamics more realistically, with a prospect of reduced uncertainty in both climate forcing and sensitivity.« less

A Framework for Characterizing how Ice Crystal Size Distributions, Mass-Dimensional and Area-Dimensional Relations Vary with Environmental and Aerosol Properties

NASA Astrophysics Data System (ADS)

McFarquhar, G. M.; Finlon, J.; Um, J.; Nesbitt, S. W.; Borque, P.; Chase, R.; Wu, W.; Morrison, H.; Poellot, M.

2017-12-01

Parameterizations of fall speed-dimension (V-D), mass (m)-D and projected area (A)-D relationships are needed for development of model parameterization and remote sensing retrieval schemes. An approach for deriving such relations is discussed here that improves upon previously developed schemes in the following aspects: 1) surfaces are used to characterize uncertainties in derived coefficients; 2) all derived relations are internally consistent; and 3) multiple bulk measures are used to derive parameter coefficients. In this study, data collected by two-dimensional optical array probes (OAPs) installed on the University of North Dakota Citation aircraft during the Mid-Latitude Continental Convective Clouds Experiment (MC3E) and during the Olympic Mountains Experiment (OLYMPEX) are used in conjunction with data from a Nevzorov total water content (TWC) probe and ground-based radar data at S-band to test a novel approach that determines m-D relationships for a variety of environments. A surface of equally realizable a and b coefficients, where m=aDb, in (a,b) phase space is determined using a technique that minimizes the chi-squared difference between both the TWC and radar reflectivity Z derived from the size distributions measured by the OAPs and those directly measured by a TWC probe and radar, accepting as valid all coefficients within a specified tolerance of the minimum chi-squared difference. Because both A and perimeter P can be directly measured by OAPs, coefficients characterizing these relationships are derived using only one bulk parameter constraint derived from the appropriate images. Because terminal velocity parameterizations depend on both A and m, V-D relations can be derived from these self-consistent relations. Using this approach, changes in parameters associated with varying environmental conditions and varying aerosol amounts and compositions can be isolated from changes associated with statistical noise or measurement errors. The applicability of the derived coefficients for a stochastic framework that employs an observationally-constrained dataset to account for coefficient variability within microphysics parameterization schemes is discussed.

Non-chemistry coupled PM10 modeling in Chiang Mai City, Northern Thailand: A fast operational approach for aerosol forecasts

NASA Astrophysics Data System (ADS)

Macatangay, Ronald; Bagtasa, Gerry; Sonkaew, Thiranan

2017-09-01

The Weather Research and Forecasting (WRF v. 3.7) model was applied to model PM10 data in Chiang Mai city for 10-days during a high haze event utilizing updated land use categories from the Moderate Resolution Imaging Spectroradiometer (MODIS). A higher resolution meteorological lateral boundary condition (from 1 degree to 0.25 degree) was also used from the NCEP GDAS/FNL Global Tropospheric Analyses and Forecast Grid system. A 3-category urban canopy model was also added and the Thompson aerosol-aware microphysics parameterization scheme was used to model the aerosol number concentrations that were later converted to PM10 concentrations. Aerosol number concentration monthly climatology was firstly used as initial and lateral boundary conditions to model PM10 concentrations. These were compared to surface data obtained from two stations of the Pollution Control Department (PCD) of Thailand. The results from the modeled PM10 concentrations could not capture the variability (r = 0.29; 0.27 for each site) and underestimated a high PM10 spike during the period studied. The authors then added satellite data to the aerosol climatology that improved the comparison with observations (r = 0.45; 43). However, both model runs still were not able to capture the high PM10 concentration event. This requires further investigation.

Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) Final Campaign Report

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

Wood, R.

2016-01-01

The extensive coverage of low clouds over the subtropical eastern oceans greatly impacts the current climate. In addition, the response of low clouds to changes in atmospheric greenhouse gases and aerosols is a major source of uncertainty, which thwarts accurate prediction of future climate change. Low clouds are poorly simulated in climate models, partly due to inadequate long-term simultaneous observations of their macrophysical and microphysical structure, radiative effects, and associated aerosol distribution in regions where their impact is greatest. The thickness and extent of subtropical low clouds is dependent on tight couplings between surface fluxes of heat and moisture, radiativemore » cooling, boundary layer turbulence, and precipitation (much of which evaporates before reaching the ocean surface and is closely connected to the abundance of cloud condensation nuclei). These couplings have been documented as a result of past field programs and model studies. However, extensive research is still required to achieve a quantitative understanding sufficient for developing parameterizations, which adequately predict aerosol indirect effects and low cloud response to climate perturbations. This is especially true of the interactions between clouds, aerosol, and precipitation. These processes take place in an ever-changing synoptic environment that can confound interpretation of short time period observations.« less

Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) Science Plan

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

Fast, JD; Berg, LK

Cumulus convection is an important component in the atmospheric radiation budget and hydrologic cycle over the Southern Great Plains and over many regions of the world, particularly during the summertime growing season when intense turbulence induced by surface radiation couples the land surface to clouds. Current convective cloud parameterizations contain uncertainties resulting in part from insufficient coincident data that couples cloud macrophysical and microphysical properties to inhomogeneities in boundary layer and aerosol properties. The Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign is designed to provide a detailed set of measurements that are needed to obtain a moremore » complete understanding of the life cycle of shallow clouds by coupling cloud macrophysical and microphysical properties to land surface properties, ecosystems, and aerosols. HI-SCALE consists of 2, 4-week intensive observational periods, one in the spring and the other in the late summer, to take advantage of different stages and distribution of “greenness” for various types of vegetation in the vicinity of the Atmospheric Radiation and Measurement (ARM) Climate Research Facility’s Southern Great Plains (SGP) site as well as aerosol properties that vary during the growing season. Most of the proposed instrumentation will be deployed on the ARM Aerial Facility (AAF) Gulfstream 1 (G-1) aircraft, including those that measure atmospheric turbulence, cloud water content and drop size distributions, aerosol precursor gases, aerosol chemical composition and size distributions, and cloud condensation nuclei concentrations. Routine ARM aerosol measurements made at the surface will be supplemented with aerosol microphysical properties measurements. The G-1 aircraft will complete transects over the SGP Central Facility at multiple altitudes within the boundary layer, within clouds, and above clouds.« less

Quantification of Semi-Volatile gas-phase Organic Compounds (SVOCs) & Organic Aerosol species and the role of SVOCs in Secondary Organic Aerosol formation

NASA Astrophysics Data System (ADS)

Khan, M. H.; Holzinger, R.

2013-12-01

A Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS) with different sampling systems (multi-stage denuder for gas phase and impact on a collector for aerosol phase) has been deployed in summer 2013 during the Southern Oxidant and Aerosol Study (SOAS) at the SEARCH ground site, Centreville, Alabama for in-situ gas phase and aerosol measurements on an hourly time resolution. A bunch of DB-1 column (0.53 mm x 5.0 μm) is used in the denuder for capturing the bulk of SVOCs and a collection-thermal-desorption (CTD) cell is used for collecting aerosol particles. Several hundreds semivolatile organic compounds (SVOCs) in gas phase and aerosol phases have been detected. The high mass resolution capabilities of ~5000, low detection limit (<0.05 pptv for gas species, <0.01 ng m-3 for aerosol species) and good physical and chemical characterization of SVOCs with the TD-PTR-MS allows constraining both, the quantity and the chemical composition. The SEARCH site was highly impacted by Biogenic Volatile Organic Compounds (BVOCs) and occasionally influenced by anthropogenic pollution. BVOCs and their oxidation products are capable of partitioning into the particle phase, so their simultaneous quantification in both phases has been used to determine the gas/particle-phase partitioning. Our results show the expected diurnal variation based on the changes of air temperature for many species. The results from this study give valuable insights into sources and processing of Secondary Organic Aerosols (SOAs) that can be used to improve parameterization algorithms in regional and global climate models.

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.

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.

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).

Impact of new particle formation on the concentrations of aerosol number and cloud condensation nuclei around Beijing

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

Matsui, H.; Koike, Makoto; Kondo, Yutaka

New particle formation (NPF) is one of the most important processes in controlling the concentrations of aerosol number (condensation nuclei, CN) and cloud condensation nuclei (CCN) in the atmosphere. In this study, we introduced a new aerosol model representation with 20 size bins between 1 nm and 10 {mu}m and activation-type and kinetic nucleation parameterizations into the WRF-chem model (called NPF-explicit WRF-chem). Model calculations were conducted in the Beijing region in China for the periods during the CARE-Beijing 2006 campaign conducted in August and September 2006. Model calculations successfully reproduced the timing of NPF and no-NPF days in the measurementsmore » (21 of 26 days). Model calculations also reproduced the subsequent rapid growth of new particles with a time scale of half a day. These results suggest that once a reasonable nucleation rate at a diameter of 1 nm is given, explicit calculations of condensation and coagulation processes can reproduce the clear contrast between NPF and no-NPF days as well as further growth up to several tens nanometers. With this reasonable representation of the NPF process, we show that NPF contributed 20-30% of CN concentrations (> 10 nm in diameter) in and around Beijing on average. We also show that NPF increases CCN concentrations at higher supersaturations (S > 0.2%), while it decreases them at lower supersaturations (S < 0.1%). This is likely because NPF suppresses the increases in both the size and hygroscopicity of pre-existing particles through the competition of condensable gases between new particles and pre-existing particles. Sensitivity calculations show that a reduction of primary aerosol emissions, such as black carbon (BC), would not necessarily decrease CCN concentrations because of an increase in NPF. Sensitivity calculations also suggest that the reduction ratio of primary aerosol and SO2 emissions will be key in enhancing or damping the BC mitigation effect.« less

Impact of new particle formation on the concentrations of aerosols and cloud condensation nuclei around Beijing

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Takegawa, N.; Wiedensohler, A.; Fast, J. D.; Zaveri, R. A.

2011-10-01

New particle formation (NPF) is one of the most important processes in controlling the concentrations of aerosols (condensation nuclei, CN) and cloud condensation nuclei (CCN) in the atmosphere. In this study, we introduce a new aerosol model representation with 20 size bins between 1 nm and 10 μm and activation-type and kinetic nucleation parameterizations into the WRF-chem model (called NPF-explicit WRF-chem). Model calculations were conducted in the Beijing region in China for the periods during the Campaign of Air Quality Research in Beijing and Surrounding Region 2006 (CARE-Beijing 2006) campaign conducted in August and September 2006. Model calculations successfully reproduced the timing of NPF and no-NPF days in the measurements (21 of 26 days). Model calculations also reproduced the subsequent rapid growth of new particles with a time scale of half a day. These results suggest that once a reasonable nucleation rate at a diameter of 1 nm is given, explicit calculations of condensation and coagulation processes can reproduce the clear contrast between NPF and no-NPF days as well as further growth up to several tens of nanometers. With this reasonable representation of the NPF process, we show that NPF contributed 20%-30% of the CN concentrations (>10 nm in diameter) in and around Beijing on average. We also show that NPF increases CCN concentrations at higher supersaturations (S > 0.2%), while it decreases them at lower supersaturations (S < 0.1%). This is likely because NPF suppresses the increases in both the size and hygroscopicity of preexisting particles through the competition of condensable gases between new particles and preexisting particles. Sensitivity calculations show that a reduction of primary aerosol emissions, such as black carbon (BC), would not necessarily decrease CCN concentrations because of an increase in NPF. Sensitivity calculations also suggest that the reduction ratio of primary aerosol and SO2 emissions will be key in enhancing or damping the BC mitigation effect.

Modeling Secondary Organic Aerosol Formation From Emissions of Combustion Sources

NASA Astrophysics Data System (ADS)

Jathar, Shantanu Hemant

Atmospheric aerosols exert a large influence on the Earth's climate and cause adverse public health effects, reduced visibility and material degradation. Secondary organic aerosol (SOA), defined as the aerosol mass arising from the oxidation products of gas-phase organic species, accounts for a significant fraction of the submicron atmospheric aerosol mass. Yet, there are large uncertainties surrounding the sources, atmospheric evolution and properties of SOA. This thesis combines laboratory experiments, extensive data analysis and global modeling to investigate the contribution of semi-volatile and intermediate volatility organic compounds (SVOC and IVOC) from combustion sources to SOA formation. The goals are to quantify the contribution of these emissions to ambient PM and to evaluate and improve models to simulate its formation. To create a database for model development and evaluation, a series of smog chamber experiments were conducted on evaporated fuel, which served as surrogates for real-world combustion emissions. Diesel formed the most SOA followed by conventional jet fuel / jet fuel derived from natural gas, gasoline and jet fuel derived from coal. The variability in SOA formation from actual combustion emissions can be partially explained by the composition of the fuel. Several models were developed and tested along with existing models using SOA data from smog chamber experiments conducted using evaporated fuel (this work, gasoline, fischertropschs, jet fuel, diesels) and published data on dilute combustion emissions (aircraft, on- and off-road gasoline, on- and off-road diesel, wood burning, biomass burning). For all of the SOA data, existing models under-predicted SOA formation if SVOC/IVOC were not included. For the evaporated fuel experiments, when SVOC/IVOC were included predictions using the existing SOA model were brought to within a factor of two of measurements with minor adjustments to model parameterizations. Further, a volatility-only model suggested that differences in the volatility of the precursors were able to explain most of the variability observed in the SOA formation. For aircraft exhaust, the previous methods to simulate SOA formation from SVOC and IVOC performed poorly. A more physically-realistic modeling framework was developed, which was then used to show that SOA formation from aircraft exhaust was (a) higher for petroleum-based than synthetically derived jet fuel and (b) higher at lower engine loads and vice versa. All of the SOA data from combustion emissions experiments were used to determine source-specific parameterizations to model SOA formation from SVOC, IVOC and other unspeciated emissions. The new parameterizations were used to investigate their influence on the OA budget in the United States. Combustion sources were estimated to emit about 2.61 Tg yr-1 of SVOC, 1VOC and other unspeciated emissions (sixth of the total anthropogenic organic emissions), which are predicted to double SOA production from combustion sources in the United States. The contribution of SVOC and IVOC emissions to global SOA formation was assessed using a global climate model. Simulations were performed using a modified version of GISS GCM 11'. The modified model predicted that SVOC and IVOC contributed to half of the OA mass in the atmosphere. Their inclusion improved OA model-measurement comparisons for absolute concentrations, POA-SOA split and volatility (gas-particle partitioning) globally suggesting that atmospheric models need to incorporate SOA formation from SVOC and IVOC if they are to reasonably predict the abundance and properties of aerosols. This thesis demonstrates that SVOC/IVOC and possibly other unspeciated organics emitted by combustion sources are very important precursors of SOA and potentially large contributors to the atmospheric aerosol mass. Models used for research and policy applications need to represent them to improve model-predictions of aerosols on climate and health outcomes. The improved modeling frameworks developed in this dissertation are suitable for implementation into chemical transport models.

Quantifying sources and sinks of reactive gases in the lower atmosphere using airborne flux observations

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

Wolfe, Glenn; Hanisco, T. F.; Atkinson, H. L.

Atmospheric composition is governed by the interplay of emissions, chemistry, deposition, and transport. Substantial questions surround each of these processes, especially in forested environments with strong biogenic emissions. Utilizing aircraft observations acquired over a forest in the southeast U.S., we calculate eddy covariance fluxes for a suite of reactive gases and apply the synergistic information derived from this analysis to quantify emission and deposition fluxes, oxidant concentrations, aerosol uptake coefficients, and other key parameters. Evaluation of results against state-of-the-science models and parameterizations provides insight into our current understanding of this system and frames future observational priorities. As a near-direct measurementmore » of fundamental process rates, airborne fluxes offer a new tool to improve biogenic and anthropogenic emissions inventories, photochemical mechanisms, and deposition parameterizations.« less

Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

DOE PAGES

Marelle, Louis; Raut, Jean-Christophe; Law, Kathy S.; ...

2017-01-01

In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain–Fritsch +more » Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.« less

Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

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

Marelle, Louis; Raut, Jean-Christophe; Law, Kathy S.

In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain–Fritsch +more » Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.« less

Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

NASA Astrophysics Data System (ADS)

Marelle, Louis; Raut, Jean-Christophe; Law, Kathy S.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Shrivastava, Manish; Thomas, Jennie L.

2017-10-01

In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain-Fritsch + Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.

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

Berkowitz, Carl M.; Berg, Larry K.; Ogren, J. A.

This white paper presents the scientific motivation and preliminary logistical plans for a proposed ASP field campaign to be carried out in the summer of 2007. The primary objective of this campaign is to use the DOE Gulfstream-1 aircraft to make measurements characterizing the chemical, physical and optical properties of aerosols below, within and above large fields of fair weather cumulus and to use the NASA Langley Research Center’s High Spectral Resolution Lidar (HSRL) to make independent measurements of aerosol backscatter and extinction profiles in the vicinity of these fields. Separate from the science questions to be addressed by thesemore » observations will be information to add in the development of a parameterized cumulus scheme capable of including multiple cloud fields within a regional or global scale model. We will also be able to compare and contrast the cloud and aerosol properties within and outside the Oklahoma City plume to study aerosol processes within individual clouds. Preliminary discussions with the Cloud and Land Surface Interaction Campaign (CLASIC) science team have identified overlap between the science questions posed for the CLASIC Intensive Operation Period (IOP) and the proposed ASP campaign, suggesting collaboration would benefit both teams.« less

Study of aerosol direct and indirect effects and auto-conversion processes over the West African monsoon region using a regional climate model

NASA Astrophysics Data System (ADS)

Salah, Zeinab; Shalaby, Ahmed; Steiner, Allison L.; Zakey, Ashraf S.; Gautam, Ritesh; Abdel Wahab, Mohamed M.

2018-02-01

This study assesses the direct and indirect effects of natural and anthropogenic aerosols (e.g., black carbon and sulfate) over West and Central Africa during the West African monsoon (WAM) period (June-July-August). We investigate the impacts of aerosols on the amount of cloudiness, the influences on the precipitation efficiency of clouds, and the associated radiative forcing (direct and indirect). Our study includes the implementation of three new formulations of auto-conversion parameterization [namely, the Beheng (BH), Tripoli and Cotton (TC) and Liu and Daum (R6) schemes] in RegCM4.4.1, besides the default model's auto-conversion scheme (Kessler). Among the new schemes, BH reduces the precipitation wet bias by more than 50% over West Africa and achieves a bias reduction of around 25% over Central Africa. Results from detailed sensitivity experiments suggest a significant path forward in terms of addressing the long-standing issue of the characteristic wet bias in RegCM. In terms of aerosol-induced radiative forcing, the impact of the various schemes is found to vary considerably (ranging from -5 to -25 W m-2).

A CloudSat Perspective of the Atmospheric Water Cycle and Precipitation: Recent Progress and Grand Challenges

NASA Technical Reports Server (NTRS)

Stephens, Graeme L.; Im, Eastwood; Vane, Deborah

2012-01-01

Summary Global - mean precipitation - is controlled by Earth's energy balance and is a quantifiable consequence of the water vapor feedback. Predictability rests on the degree to which the water vapor feedback is predictable. Regional scale - to a significant extent, changes are shaped by atmospheric circulation changes but we do not know the extent to which regional scale changes are predictable. The impacts of changes to atmospheric circulation on regional scale water cycle changes can be dramatic. Process - scale - significant biases to the CHARACTER of precipitation (frequency and intensity) is related to how the precipitation process is parameterized in models. Aerosol - We still do not know the extent to which the water cycle is influenced by aerosol but anecdotal evidence is building. The character of precipitation is affected by the way aerosol influence clouds and thus affects the forcing of the climate system through the albedo effect. Observations - we still have a way to go and need to approach the problem in a more integrated way (tie clouds, aerosol and precipitation together and then link to soil moisture, etc). Globally our capabilities seriously lag behind the science and model development.

Identification of significant precursor gases of secondary organic aerosols from residential wood combustion

PubMed Central

Bruns, Emily A.; El Haddad, Imad; Slowik, Jay G.; Kilic, Dogushan; Klein, Felix; Baltensperger, Urs; Prévôt, André S. H.

2016-01-01

Organic gases undergoing conversion to form secondary organic aerosol (SOA) during atmospheric aging are largely unidentified, particularly in regions influenced by anthropogenic emissions. SOA dominates the atmospheric organic aerosol burden and this knowledge gap contributes to uncertainties in aerosol effects on climate and human health. Here we characterize primary and aged emissions from residential wood combustion using high resolution mass spectrometry to identify SOA precursors. We determine that SOA precursors traditionally included in models account for only ~3–27% of the observed SOA, whereas for the first time we explain ~84–116% of the SOA by inclusion of non-traditional precursors. Although hundreds of organic gases are emitted during wood combustion, SOA is dominated by the aging products of only 22 compounds. In some cases, oxidation products of phenol, naphthalene and benzene alone comprise up to ~80% of the observed SOA. Identifying the main precursors responsible for SOA formation enables improved model parameterizations and SOA mitigation strategies in regions impacted by residential wood combustion, more productive targets for ambient monitoring programs and future laboratories studies, and links between direct emissions and SOA impacts on climate and health in these regions. PMID:27312480

Retrieval of aerosol optical properties using MERIS observations: Algorithm and some first results.

PubMed

Mei, Linlu; Rozanov, Vladimir; Vountas, Marco; Burrows, John P; Levy, Robert C; Lotz, Wolfhardt

2017-08-01

The MEdium Resolution Imaging Spectrometer (MERIS) instrument on board ESA Envisat made measurements from 2002 to 2012. Although MERIS was limited in spectral coverage, accurate Aerosol Optical Thickness (AOT) from MERIS data are retrieved by using appropriate additional information. We introduce a new AOT retrieval algorithm for MERIS over land surfaces, referred to as eXtensible Bremen AErosol Retrieval (XBAER). XBAER is similar to the "dark-target" (DT) retrieval algorithm used for Moderate-resolution Imaging Spectroradiometer (MODIS), in that it uses a lookup table (LUT) to match to satellite-observed reflectance and derive the AOT. Instead of a global parameterization of surface spectral reflectance, XBAER uses a set of spectral coefficients to prescribe surface properties. In this manner, XBAER is not limited to dark surfaces (vegetation) and retrieves AOT over bright surface (desert, semiarid, and urban areas). Preliminary validation of the MERIS-derived AOT and the ground-based Aerosol Robotic Network (AERONET) measurements yield good agreement, the resulting regression equation is y = (0.92 × ± 0.07) + (0.05 ± 0.01) and Pearson correlation coefficient of R = 0.78. Global monthly means of AOT have been compared from XBAER, MODIS and other satellite-derived datasets.

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

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

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

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

Feedbacks between air pollution and weather, part 2: Effects on chemistry

NASA Astrophysics Data System (ADS)

Makar, P. A.; Gong, W.; Hogrefe, C.; Zhang, Y.; Curci, G.; Žabkar, R.; Milbrandt, J.; Im, U.; Balzarini, A.; Baró, R.; Bianconi, R.; Cheung, P.; Forkel, R.; Gravel, S.; Hirtl, M.; Honzak, L.; Hou, A.; Jiménez-Guerrero, P.; Langer, M.; Moran, M. D.; Pabla, B.; Pérez, J. L.; Pirovano, G.; San José, R.; Tuccella, P.; Werhahn, J.; Zhang, J.; Galmarini, S.

2015-08-01

Fully-coupled air-quality models running in ;feedback; and ;no-feedback; configurations were compared against each other and observation network data as part of Phase 2 of the Air Quality Model Evaluation International Initiative. In the ;no-feedback; mode, interactions between meteorology and chemistry through the aerosol direct and indirect effects were disabled, with the models reverting to climatologies of aerosol properties, or a no-aerosol weather simulation, while in the ;feedback; mode, the model-generated aerosols were allowed to modify the models' radiative transfer and/or cloud formation processes. Annual simulations with and without feedbacks were conducted for domains in North America for the years 2006 and 2010, and for Europe for the year 2010. Comparisons against observations via annual statistics show model-to-model variation in performance is greater than the within-model variation associated with feedbacks. However, during the summer and during intense emission events such as the Russian forest fires of 2010, feedbacks have a significant impact on the chemical predictions of the models. The aerosol indirect effect was usually found to dominate feedbacks compared to the direct effect. The impacts of direct and indirect effects were often shown to be in competition, for predictions of ozone, particulate matter and other species. Feedbacks were shown to result in local and regional shifts of ozone-forming chemical regime, between NOx- and VOC-limited environments. Feedbacks were shown to have a substantial influence on biogenic hydrocarbon emissions and concentrations: North American simulations incorporating both feedbacks resulted in summer average isoprene concentration decreases of up to 10%, while European direct effect simulations during the Russian forest fire period resulted in grid average isoprene changes of -5 to +12.5%. The atmospheric transport and chemistry of large emitting sources such as plumes from forest fires and large cities were shown to be strongly impacted by the presence or absence of feedback mechanisms in the model simulations. Summertime model performance for ozone and other gases was improved through the inclusion of indirect effect feedbacks, while performance for particulate matter was degraded, suggesting that current parameterizations for in- and below cloud processes, once the cloud locations become more directly influenced by aerosols, may over- or under-predict the strength of these processes. Process parameterization-level comparisons of fully coupled feedback models are therefore recommended for future work, as well as further studies using these models for the simulations of large scale urban/industrial and/or forest fire plumes.

Global impact of mineral dust on cloud droplet number concentration

NASA Astrophysics Data System (ADS)

Karydis, Vlassis A.; Tsimpidi, Alexandra P.; Bacer, Sara; Pozzer, Andrea; Nenes, Athanasios; Lelieveld, Jos

2017-05-01

The importance of wind-blown mineral dust for cloud droplet formation is studied by considering (i) the adsorption of water on the surface of insoluble particles, (ii) particle coating by soluble material (atmospheric aging) which augments cloud condensation nuclei (CCN) activity, and (iii) the effect of dust on inorganic aerosol concentrations through thermodynamic interactions with mineral cations. The ECHAM5/MESSy Atmospheric Chemistry (EMAC) model is used to simulate the composition of global atmospheric aerosol, while the ISORROPIA-II thermodynamic equilibrium model treats the interactions of K+-Ca2+-Mg2+-NH4+-Na+-SO42--NO3--Cl--H2O aerosol with gas-phase inorganic constituents. Dust is considered a mixture of inert material with reactive minerals and its emissions are calculated online by taking into account the soil particle size distribution and chemical composition of different deserts worldwide. The impact of dust on droplet formation is treated through the unified dust activation parameterization that considers the inherent hydrophilicity from adsorption and acquired hygroscopicity from soluble salts during aging. Our simulations suggest that the presence of dust increases cloud droplet number concentration (CDNC) over major deserts (e.g., up to 20 % over the Sahara and the Taklimakan desert) and decreases CDNC over polluted areas (e.g., up to 10 % over southern Europe and 20 % over northeastern Asia). This leads to a global net decrease in CDNC by 11 %. The adsorption activation of insoluble aerosols and the mineral dust chemistry are shown to be equally important for the cloud droplet formation over the main deserts; for example, these effects increase CDNC by 20 % over the Sahara. Remote from deserts the application of adsorption theory is critically important since the increased water uptake by the large aged dust particles (i.e., due to the added hydrophilicity by the soluble coating) reduce the maximum supersaturation and thus cloud droplet formation from the relatively smaller anthropogenic particles (e.g., CDNC decreases by 10 % over southern Europe and 20 % over northeastern Asia by applying adsorption theory). The global average CDNC decreases by 10 % by considering adsorption activation, while changes are negligible when accounting for the mineral dust chemistry. Sensitivity simulations indicate that CDNC is also sensitive to the mineral dust mass and inherent hydrophilicity, and not to the chemical composition of the emitted dust.

Utilizing NASA Airborne Data to Investigate the Influence of Fuel Type on Biomass Burning Aerosol Properties

NASA Astrophysics Data System (ADS)

Odwuor, A.; Corr, C.; Griffin, R. J.; Pusede, S.; Anderson, B.; Beyersdorf, A. J.; Campuzano Jost, P.; Chen, G.; Day, D. A.; Diskin, G. S.; Jimenez, J. L.; Moore, R.; Nault, B.; Schwarz, J. P.; Shook, M.; Thornhill, K. L., II; Winstead, E.; Armin, W.; Ziemba, L. D.

2017-12-01

Climate models and satellite aerosol classification retrievals rely on well-characterized aerosol optical properties (e.g., scattering and absorption coefficients) that vary with aerosol type. However, generalized parameterizations of aerosol optical properties are weakened by actual variability in aerosol chemical and physical properties that arises from factors independent of aerosol source (e.g., meteorology). This is particularly true for biomass burning (BB) aerosol, which can vary in composition and size depending on burn conditions (e.g., smoldering versus flaming) and fuel. This work investigates the relationships between BB aerosol chemical, physical, and optical properties and fuel. We compare BB aerosol measured in fire plumes associated with distinct fuel types sampled during three NASA airborne research campaigns: boreal forest fires during the Arctic Research of the Troposphere from Aircraft and Satellites (ARCTAS) mission in Saskatchewan, Canada in July 2008; agricultural fires during the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS) over the continental U.S. in August/September 2013; and scrubland fires during the Student Airborne Research Program (SARP) mission in Southern California, U.S. in June 2016. Mean modified combustion efficiency values between 0.9 and 0.92 for the agricultural plumes and between 0.92 and 0.99 for the boreal and scrubland plumes indicate a significant flaming component to these fires. Despite similarities in burn conditions, SSA at 550nm was consistently lower for the agricultural and scrubland fires ( 0.92) compared to the boreal forest ( 0.96). While the ratio of black carbon to organic aerosol (OA) was similar among fires, differences in the OA were noted; f44/f60 ratios derived from Aerosol Mass Spectrometer OA measurements were consistently higher (>5) in scrubland and agricultural fires compared to boreal forest fires (<5). This suggests the amount of oxidized OA relative to fresh BB aerosol in fire plumes under flaming conditions may vary with fuel type and influence plume optical properties. The relationship between size distributions and optical properties is also explored in this work, with particular attention on the role of the coarse mode in aerosol absorption.

Preliminary Results from an Assimilation of Saharan Dust Using TOMS Radiances and the GOCART Model

NASA Technical Reports Server (NTRS)

Weaver, C. J.; daSilva, Arlindo; Ginoux, Paul; Torres, Omar; Einaudi, Franco (Technical Monitor)

2000-01-01

At NASA Goddard we are developing a global aerosol data assimilation system that combines advances in remote sensing and modeling of atmospheric aerosols. The goal is to provide high resolution, 3-D aerosol distributions to the research community. Our first step is to develop a simple assimilation system for Saharan mineral aerosol. The Goddard Chemistry and Aerosol Radiation model (GOCART) provides accurate 3-D mineral aerosol size distributions. Surface mobilization, wet and dry deposition, convective and long-range transport are all driven by assimilated fields from the Goddard Earth Observing System Data Assimilation System, GEOS-DAS. Our version of GOCART transports sizes from .08-10 microns and only simulates Saharan dust. We draw the assimilation to two observables in this study: the TOMS aerosol index (Al) which is directly related to the ratio of the 340 and 380 radiances and the 380 radiance alone. The forward model that simulates the observables requires the aerosol optical thickness, the single scattering albedo and the height of the aerosol layer from the GOCART fields. The forward model also requires a refractive index for the dust. We test three index values to see which best fits the TOMS observables. These are 1) for Saharan dust reported by Patterson, 2) for a mixture of Saharan dust and a highly reflective material (sea salt or sulfate) and 3) for pure illite. The assimilation works best assuming either pure illite or the dust mixture. Our assimilation cycle first determines values of the aerosol index (Al) and the radiance at 380 nm based on the GOCART aerosol fields. Differences between the observed and GOCART model calculated Al and 380 nm radiance are first analyzed horizontally using the Physical-space Statistical Analysis System (PSAS). A quasi-Newton iteration is then performed to produce analyzed 3D aerosol fields according to parameterized background and observation error covariances. We only assimilate observations into the the GOCART model over regions of Africa and the Atlantic where mineral aerosols are dominant and carbonaceous aerosols are minimal.

Modeling the formation and aging of secondary organic aerosols in Los Angeles during CalNex 2010

DOE PAGES

Hayes, P. L.; Carlton, A. G.; Baker, K. R.; ...

2015-05-26

Four different literature parameterizations for the formation and evolution of urban secondary organic aerosol (SOA) frequently used in 3-D models are evaluated using a 0-D box model representing the Los Angeles metropolitan region during the California Research at the Nexus of Air Quality and Climate Change (CalNex) 2010 campaign. We constrain the model predictions with measurements from several platforms and compare predictions with particle- and gas-phase observations from the CalNex Pasadena ground site. That site provides a unique opportunity to study aerosol formation close to anthropogenic emission sources with limited recirculation. The model SOA that formed only from the oxidationmore » of VOCs (V-SOA) is insufficient to explain the observed SOA concentrations, even when using SOA parameterizations with multi-generation oxidation that produce much higher yields than have been observed in chamber experiments, or when increasing yields to their upper limit estimates accounting for recently reported losses of vapors to chamber walls. The Community Multiscale Air Quality (WRF-CMAQ) model (version 5.0.1) provides excellent predictions of secondary inorganic particle species but underestimates the observed SOA mass by a factor of 25 when an older VOC-only parameterization is used, which is consistent with many previous model–measurement comparisons for pre-2007 anthropogenic SOA modules in urban areas. Including SOA from primary semi-volatile and intermediate-volatility organic compounds (P-S/IVOCs) following the parameterizations of Robinson et al. (2007), Grieshop et al. (2009), or Pye and Seinfeld (2010) improves model–measurement agreement for mass concentration. The results from the three parameterizations show large differences (e.g., a factor of 3 in SOA mass) and are not well constrained, underscoring the current uncertainties in this area. Our results strongly suggest that other precursors besides VOCs, such as P-S/IVOCs, are needed to explain the observed SOA concentrations in Pasadena. All the recent parameterizations overpredict urban SOA formation at long photochemical ages (≈ 3 days) compared to observations from multiple sites, which can lead to problems in regional and especially global modeling. However, reducing IVOC emissions by one-half in the model to better match recent IVOC measurements improves SOA predictions at these long photochemical ages. Among the explicitly modeled VOCs, the precursor compounds that contribute the greatest SOA mass are methylbenzenes. Measured polycyclic aromatic hydrocarbons (naphthalenes) contribute 0.7% of the modeled SOA mass. The amounts of SOA mass from diesel vehicles, gasoline vehicles, and cooking emissions are estimated to be 16–27, 35–61, and 19–35%, respectively, depending on the parameterization used, which is consistent with the observed fossil fraction of urban SOA, 71(±3) %. The relative contribution of each source is uncertain by almost a factor of 2 depending on the parameterization used. In-basin biogenic VOCs are predicted to contribute only a few percent to SOA. A regional SOA background of approximately 2.1 μg m −3 is also present due to the long-distance transport of highly aged OA, likely with a substantial contribution from regional biogenic SOA. The percentage of SOA from diesel vehicle emissions is the same, within the estimated uncertainty, as reported in previous work that analyzed the weekly cycles in OA concentrations (Bahreini et al., 2012; Hayes et al., 2013). However, the modeling work presented here suggests a strong anthropogenic source of modern carbon in SOA, due to cooking emissions, which was not accounted for in those previous studies and which is higher on weekends. Lastly, this work adapts a simple two-parameter model to predict SOA concentration and O/C from urban emissions. This model successfully predicts SOA concentration, and the optimal parameter combination is very similar to that found for Mexico City. This approach provides a computationally inexpensive method for predicting urban SOA in global and climate models. We estimate pollution SOA to account for 26 Tg yr −1 of SOA globally, or 17% of global SOA, one-third of which is likely to be non-fossil.« less

Modeling the formation and aging of secondary organic aerosols in Los Angeles during CalNex 2010

NASA Astrophysics Data System (ADS)

Hayes, P. L.; Carlton, A. G.; Baker, K. R.; Ahmadov, R.; Washenfelder, R. A.; Alvarez, S.; Rappengluck, B.; Gilman, J. B.; Kuster, W. C.; de Gouw, J. A.; Zotter, P.; Prevot, A. S. H.; Szidat, S.; Kleindienst, T. E.; Offenberg, J. H.; Ma, P. K.; Jimenez, J. L.

2015-05-01

Four different literature parameterizations for the formation and evolution of urban secondary organic aerosol (SOA) frequently used in 3-D models are evaluated using a 0-D box model representing the Los Angeles metropolitan region during the California Research at the Nexus of Air Quality and Climate Change (CalNex) 2010 campaign. We constrain the model predictions with measurements from several platforms and compare predictions with particle- and gas-phase observations from the CalNex Pasadena ground site. That site provides a unique opportunity to study aerosol formation close to anthropogenic emission sources with limited recirculation. The model SOA that formed only from the oxidation of VOCs (V-SOA) is insufficient to explain the observed SOA concentrations, even when using SOA parameterizations with multi-generation oxidation that produce much higher yields than have been observed in chamber experiments, or when increasing yields to their upper limit estimates accounting for recently reported losses of vapors to chamber walls. The Community Multiscale Air Quality (WRF-CMAQ) model (version 5.0.1) provides excellent predictions of secondary inorganic particle species but underestimates the observed SOA mass by a factor of 25 when an older VOC-only parameterization is used, which is consistent with many previous model-measurement comparisons for pre-2007 anthropogenic SOA modules in urban areas. Including SOA from primary semi-volatile and intermediate-volatility organic compounds (P-S/IVOCs) following the parameterizations of Robinson et al. (2007), Grieshop et al. (2009), or Pye and Seinfeld (2010) improves model-measurement agreement for mass concentration. The results from the three parameterizations show large differences (e.g., a factor of 3 in SOA mass) and are not well constrained, underscoring the current uncertainties in this area. Our results strongly suggest that other precursors besides VOCs, such as P-S/IVOCs, are needed to explain the observed SOA concentrations in Pasadena. All the recent parameterizations overpredict urban SOA formation at long photochemical ages (~ 3 days) compared to observations from multiple sites, which can lead to problems in regional and especially global modeling. However, reducing IVOC emissions by one-half in the model to better match recent IVOC measurements improves SOA predictions at these long photochemical ages. Among the explicitly modeled VOCs, the precursor compounds that contribute the greatest SOA mass are methylbenzenes. Measured polycyclic aromatic hydrocarbons (naphthalenes) contribute 0.7% of the modeled SOA mass. The amounts of SOA mass from diesel vehicles, gasoline vehicles, and cooking emissions are estimated to be 16-27, 35-61, and 19-35%, respectively, depending on the parameterization used, which is consistent with the observed fossil fraction of urban SOA, 71(±3) %. The relative contribution of each source is uncertain by almost a factor of 2 depending on the parameterization used. In-basin biogenic VOCs are predicted to contribute only a few percent to SOA. A regional SOA background of approximately 2.1 μg m-3 is also present due to the long-distance transport of highly aged OA, likely with a substantial contribution from regional biogenic SOA. The percentage of SOA from diesel vehicle emissions is the same, within the estimated uncertainty, as reported in previous work that analyzed the weekly cycles in OA concentrations (Bahreini et al., 2012; Hayes et al., 2013). However, the modeling work presented here suggests a strong anthropogenic source of modern carbon in SOA, due to cooking emissions, which was not accounted for in those previous studies and which is higher on weekends. Lastly, this work adapts a simple two-parameter model to predict SOA concentration and O/C from urban emissions. This model successfully predicts SOA concentration, and the optimal parameter combination is very similar to that found for Mexico City. This approach provides a computationally inexpensive method for predicting urban SOA in global and climate models. We estimate pollution SOA to account for 26 Tg yr-1 of SOA globally, or 17% of global SOA, one-third of which is likely to be non-fossil.

Parameterizing correlations between hydrometeor species in mixed-phase Arctic clouds

NASA Astrophysics Data System (ADS)

Larson, Vincent E.; Nielsen, Brandon J.; Fan, Jiwen; Ovchinnikov, Mikhail

2011-01-01

Mixed-phase Arctic clouds, like other clouds, contain small-scale variability in hydrometeor fields, such as cloud water or snow mixing ratio. This variability may be worth parameterizing in coarse-resolution numerical models. In particular, for modeling multispecies processes such as accretion and aggregation, it would be useful to parameterize subgrid correlations among hydrometeor species. However, one difficulty is that there exist many hydrometeor species and many microphysical processes, leading to complexity and computational expense. Existing lower and upper bounds on linear correlation coefficients are too loose to serve directly as a method to predict subgrid correlations. Therefore, this paper proposes an alternative method that begins with the spherical parameterization framework of Pinheiro and Bates (1996), which expresses the correlation matrix in terms of its Cholesky factorization. The values of the elements of the Cholesky matrix are populated here using a "cSigma" parameterization that we introduce based on the aforementioned bounds on correlations. The method has three advantages: (1) the computational expense is tolerable; (2) the correlations are, by construction, guaranteed to be consistent with each other; and (3) the methodology is fairly general and hence may be applicable to other problems. The method is tested noninteractively using simulations of three Arctic mixed-phase cloud cases from two field experiments: the Indirect and Semi-Direct Aerosol Campaign and the Mixed-Phase Arctic Cloud Experiment. Benchmark simulations are performed using a large-eddy simulation (LES) model that includes a bin microphysical scheme. The correlations estimated by the new method satisfactorily approximate the correlations produced by the LES.

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

Donner, Leo J.; O'Brien, Travis A.; Rieger, Daniel

Both climate forcing and climate sensitivity persist as stubborn uncertainties limiting the extent to which climate models can provide actionable scientific scenarios for climate change. A key, explicit control on cloud-aerosol interactions, the largest uncertainty in climate forcing, is the vertical velocity of cloud-scale updrafts. Model-based studies of climate sensitivity indicate that convective entrainment, which is closely related to updraft speeds, is an important control on climate sensitivity. Updraft vertical velocities also drive many physical processes essential to numerical weather prediction. Vertical velocities and their role in atmospheric physical processes have been given very limited attention in models for climatemore » and numerical weather prediction. The relevant physical scales range down to tens of meters and are thus frequently sub-grid and require parameterization. Many state-of-science convection parameterizations provide mass fluxes without specifying vertical velocities, and parameterizations which do provide vertical velocities have been subject to limited evaluation against what have until recently been scant observations. Atmospheric observations imply that the distribution of vertical velocities depends on the areas over which the vertical velocities are averaged. Distributions of vertical velocities in climate models may capture this behavior, but it has not been accounted for when parameterizing cloud and precipitation processes in current models. New observations of convective vertical velocities offer a potentially promising path toward developing process-level cloud models and parameterizations for climate and numerical weather prediction. Taking account of scale-dependence of resolved vertical velocities offers a path to matching cloud-scale physical processes and their driving dynamics more realistically, with a prospect of reduced uncertainty in both climate forcing and sensitivity.« less

Evaluation and Windspeed Dependence of MODIS Aerosol Retrievals Over Open Ocean

NASA Technical Reports Server (NTRS)

Kleidman, Richard G.; Smirnov, Alexander; Levy, Robert C.; Mattoo, Shana; Tanre, Didier

2011-01-01

The Maritime Aerosol Network (MAN) data set provides high quality ground-truth to validate the MODIS aerosol product over open ocean. Prior validation of the ocean aerosol product has been limited to coastal and island sites. Comparing MODIS Collection 5 ocean aerosol retrieval products with collocated MAN measurements from ships shows that MODIS is meeting the pre-launch uncertainty estimates for aerosol optical depth (AOD) with 64% and 67% of retrievals at 550 nm, and 74% and 78% of retrievals at 870 nm, falling within expected uncertainty for Terra and Aqua, respectively. Angstrom Exponent comparisons show a high correlation between MODIS retrievals and shipboard measurements (R= 0.85 Terra, 0.83 Aqua), although the MODIS aerosol algorithm tends to underestimate particle size for large particles and overestimate size for small particles, as seen in earlier Collections. Prior analysis noted an offset between Terra and Aqua ocean AOD, without concluding which sensor was more accurate. The simple linear regression reported here, is consistent with other anecdotal evidence that Aqua agreement with AERONET is marginally better. However we cannot claim based on the current study that the better Aqua comparison is statistically significant. Systematic increase of error as a function of wind speed is noted in both Terra and Aqua retrievals. This wind speed dependency enters the retrieval when winds deviate from the 6 m/s value assumed in the rough ocean surface and white cap parameterizations. Wind speed dependency in the results can be mitigated by using auxiliary NCEP wind speed information in the retrieval process.

Aerosol optical properties measurements by a CAPS single scattering albedo monitor: Comparisons between summer and winter in Beijing, China

NASA Astrophysics Data System (ADS)

Han, Tingting; Xu, Weiqi; Li, Jie; Freedman, Andrew; Zhao, Jian; Wang, Qingqing; Chen, Chen; Zhang, Yingjie; Wang, Zifa; Fu, Pingqing; Liu, Xingang; Sun, Yele

2017-02-01

Aerosol optical properties were measured in Beijing in summer and winter using a state-of-the-art cavity attenuated phase shift single scattering albedo monitor (CAPS PMssa) along with aerosol composition measurements by aerosol mass spectrometers and aethalometers. The SSA directly measured by the CAPS PMssa showed overall agreements with those derived from colocated measurements. However, substantial differences were observed during periods with low SSA values in both summer and winter, suggesting that interpretation of low SSA values needs to be cautious. The average (±σ) extinction coefficient (bext) and absorption coefficient (bap) were 336 (±343) Mm-1 and 44 (±41) Mm-1, respectively, during wintertime, which were approximately twice those observed in summer, while the average SSA was relatively similar, 0.86 (±0.06) and 0.85 (±0.04) in summer and winter, respectively. Further analysis showed that the variations in SSA can be approximately parameterized as a function of mass fraction of secondary particulate matter (fSPM), which is SSA = 0.74 + 0.19 × fSPM (fSPM > 0.3, r2 = 0.85). The contributions of aerosol species to extinction coefficients during the two seasons were also estimated. Our results showed that the light extinction was dominantly contributed by ammonium sulfate (30%) and secondary organic aerosol (22%) in summer, while organic aerosol was the largest contributor (51%) in winter. Consistently, SPM played the major role in visibility degradation in both seasons by contributing 70% of the total extinction.

Exploring Climatology and Long-Term Variations of Aerosols from NASA Reanalysis MERRA-2 with Giovanni

NASA Technical Reports Server (NTRS)

Shen, Suhung; Ostrenga, Dana; Vollmer, Bruce; Li, Zhanqing

2016-01-01

Dust plays important roles in energy cycle and climate variations. The dust deposition is the major source of iron in the open ocean, which is an essential micronutrient for phytoplankton growth and therefore may influence the ocean uptake of atmospheric CO2. Mineral dust can also act as fertilizer for forests over long time periods. Over 35 years of simulated global aerosol products from NASA atmospheric reanalysis, second Modern-Era Retrospective analysis for Research and Applications (MERRA-2) are available from NASA Goddard Earth Science Data and Information Services Center (GES DISC). The MERRA-2 covers the period 1980-present, continuing as an ongoing climate analysis. Aerosol assimilation is included throughout the period, using MODIS, MISR, AERONET, and AVHRR (in the pre-EOS period). The aerosols are assimilated by using MERRA-2 aerosol model, which interact directly with the radiation parameterization, and radiatively coupled with atmospheric model dynamics in the Goddard Earth Observing System Model, Version 5 (GEOS-5). Dust deposition data along with other major aerosol compositions (e.g. black carbon, sea salt, and sulfate, etc.) are simulated as dry and wet deposition, respectively. The hourly and monthly data are available at spatial resolution of 0.5ox0.625o (latitude x longitude). Quick data exploration of climatology and interannual variations of MERRA-2 aerosol can be done through the online visualization and analysis tool, Giovanni. This presentation, using dust deposition as an example, demonstrates a number of MERRA-2 data services at GES DISC. Global distributions of dust depositions, and their seasonal and inter-annual variations are investigated from MERRA-2 monthly aerosol products.

Application of Spectral Analysis Techniques in the Intercomparison of Aerosol Data: Part III. Using Combined PCA to Compare Spatiotemporal Variability of MODIS, MISR and OMI Aerosol Optical Depth

NASA Technical Reports Server (NTRS)

Li, Jing; Carlson, Barbara E.; Lacis, Andrew A.

2014-01-01

Satellite measurements of global aerosol properties are very useful in constraining aerosol parameterization in climate models. The reliability of different data sets in representing global and regional aerosol variability becomes an essential question. In this study, we present the results of a comparison using combined principal component analysis (CPCA), applied to monthly mean, mapped (Level 3) aerosol optical depth (AOD) product from Moderate Resolution Imaging Spectroradiometer (MODIS), Multiangle Imaging Spectroradiometer (MISR), and Ozone Monitoring Instrument (OMI). This technique effectively finds the common space-time variability in the multiple data sets by decomposing the combined AOD field. The results suggest that all of the sensors capture the globally important aerosol regimes, including dust, biomass burning, pollution, and mixed aerosol types. Nonetheless, differences are also noted. Specifically, compared with MISR and OMI, MODIS variability is significantly higher over South America, India, and the Sahel. MODIS deep blue AOD has a lower seasonal variability in North Africa, accompanied by a decreasing trend that is not found in either MISR or OMI AOD data. The narrow swath of MISR results in an underestimation of dust variability over the Taklamakan Desert. The MISR AOD data also exhibit overall lower variability in South America and the Sahel. OMI does not capture the Russian wild fire in 2010 nor the phase shift in biomass burning over East South America compared to Central South America, likely due to cloud contamination and the OMI row anomaly. OMI also indicates a much stronger (boreal) winter peak in South Africa compared with MODIS and MISR.

Spatial heterogeneities in aerosol size distribution over Bay of Bengal during Winter-ICARB Experiment

NASA Astrophysics Data System (ADS)

Sinha, P. R.; Manchanda, R. K.; Kaskaoutis, D. G.; Sreenivasan, S.; Krishna Moorthy, K.; Suresh Babu, S.

2011-09-01

This work examines the aerosol physical properties and size distribution measured in the Marine Atmospheric Boundary Layer (MABL) over entire Bay of Bengal (BoB) and Northern Indian Ocean (NIO) during the Winter Integrated Campaign on Aerosols, Gases and Radiation Budget (W-ICARB). The measurements were taken using the GRIMM optical particle counter from 27th December 2008 to 30th January 2009. The results show large spatial heterogeneities regarding both the total aerosol number concentrations ( N T) and the size distributions over BoB, which in turn indicates the variations in the source strength or advection from different regions. The aerosol number size distribution seems to be bi-modal in the 72% of the cases and can also be parameterized by uni-modal or by a combination of power-law and uni-modal distributions for the rest of the cases. The mode radius for accumulation and coarse-mode particles ranges from ˜0.1-0.2 μm and ˜0.6-0.8 μm, respectively. In the northern BoB and along the Indian coast, the aerosols are mainly of sub-micron size with effective radius ( Reff) ranging between 0.25 and 0.3 μm highlighting the strong anthropogenic influence, while in the open oceanic areas they are much higher (0.4-0.6 μm). It was also found that the sea-surface wind plays a considerable role in the super-micron number concentration, Reff and mode radius for coarse-mode aerosols. Using the relation between N T and columnar AOD from Terra and Aqua-MODIS we found that the majority of the aerosols are within the lower MABL, while in some areas vertical heterogeneities also exist.

Green Ocean Amazon 2014/15 Manaus Pollution Study Field Campaign Report

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

Keutsch, Frank N.

This work was part of the larger Green Ocean Amazon 2014/15 (GOAmazon 2014/15) experiment, which extended through the wet and dry seasons from January 2014 through December 2015 and which took place around the urban region of Manaus, Brazil in central Amazonia. This work was conducted as part of this experiment at the main U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility ground research site “T3” circa 100 km west of Manaus during two intensive operational periods, “IOP1” and “IOP2” (February 1 to March 31, 2014, and August 15 to October 15, 2014, respectively). Funding formore » this work was provided by the National Science Foundation AGS 1321987/1628491. The GoAmazon experiment was designed to enable the study of how aerosols and surface fluxes influence cloud cycles under clean conditions, as well as how aerosol and cloud life cycles, including cloud-aerosol-precipitation interactions, are influenced by pollutant outflow from a tropical megacity. These observations provide a data set vital to constrain tropical rain forest model parameterizations for organic aerosols, cloud and convection schemes, and terrestrial vegetation components and how these are perturbed by pollution. Research objectives specific to this work and the T3 ground site included studies of how outflow of pollution from Manaus modulated the photochemically driven conversion of emitted precursors to aerosol precursors and aerosol.« less

Parameterization of Cirrus Cloud Vertical Profiles and Geometrical Thickness Using CALIPSO and CloudSat Data

NASA Astrophysics Data System (ADS)

Khatri, P.; Iwabuchi, H.; Saito, M.

2017-12-01

High-level cirrus clouds, which normally occur over more than 20% of the globe, are known to have profound impacts on energy budget and climate change. The scientific knowledge regarding the vertical structure of such high-level cirrus clouds and their geometrical thickness are relatively poorer compared to low-level water clouds. Knowledge regarding cloud vertical structure is especially important in passive remote sensing of cloud properties using infrared channels or channels strongly influenced by gaseous absorption when clouds are geometrically thick and optically thin. Such information is also very useful for validating cloud resolving numerical models. This study analyzes global scale data of ice clouds identified by Cloud profiling Radar (CPR) onboard CloudSat and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard CALIPSO to parameterize (i) vertical profiles of ice water content (IWC), cloud-particle effective radius (CER), and ice-particle number concentration for varying ice water path (IWP) values and (ii) the relation of cloud geometrical thickness (CGT) with IWP and CER for varying cloud top temperature (CTT) values. It is found that the maxima in IWC and CER profile shifts towards cloud base with the increase of IWP. Similarly, if the cloud properties remain same, CGT shows an increasing trend with the decrease of CTT. The implementation of such cloud vertical inhomogeneity parameterization in the forward model used in the Integrated Cloud Analysis System ICAS (Iwabuchi et al., 2016) generally shows increase of brightness temperatures in infrared channels compared to vertically homogeneous cloud assumption. The cloud vertical inhomogeneity is found to bring noticeable changes in retrieved cloud properties. Retrieved CER and cloud top height become larger for optically thick cloud. We will show results of comparison of cloud properties retrieved from infrared measurements and active remote sensing.

Assessing the role of "bottom-up" emissions and simplified chemical mechanisms in reconciling CESM2.0 with TOGA observations from the ORCAS and ATom-2 campaigns

NASA Astrophysics Data System (ADS)

Asher, E.; Emmons, L. K.; Kinnison, D. E.; Tilmes, S.; Hills, A. J.; Hornbrook, R. S.; Stephens, B. B.; Apel, E. C.

2017-12-01

Surface albedo and precipitation over the Southern Ocean are sensitive to parameterizations of aerosol formation and cloud dynamics in global climate models. Observations of precursor gases for natural aerosols can help constrain the uncertainty in these parameterizations, if used in conjunction with an appropriately simplified chemical mechanism. We implement current oceanic "bottom-up" emission climatologies of dimethyl sulfide (DMS) and isoprene in CESM2.0 (Lana et al. 2016; Archer et al. 2009) and compare modeled constituents from two separate chemical mechanisms with data obtained from the Trace Organic Gas Analyzer (TOGA) on the O2/N2 Ratios and CO2 Airborne Study in the Southern Ocean (ORCAS) and the Atmospheric Tomography Mission 2 (ATom-2). We use ORCAS measurements of DMS, isoprene, methyl vinyl ketone (MVK) and methacrolein (MACR) from over 10 flights in Jan. - Feb. 2016 as a training dataset to improve "bottom-up" emissions. Thereafter, we evaluate the scaled "top-down" emissions in CESM with TOGA data obtained from the Atmospheric Tomography Mission (ATom-2) in Feb. 2017. Recent laboratory studies at NCAR confirm that TOGA surpasses proton transfer reaction mass spectrometry (PTR-MS) and commercial gas chromatography (GC) instruments with respect to accurate measurements of oxygenated VOCs in low nitrogen oxide (NO) environments, such as MVK and MACR.

Advancing Heliophysics Student Research and Public Outreach in an Urban Environment

NASA Astrophysics Data System (ADS)

Johnson, L. P.; Ng, C.; Marchese, P.; Austin, S. A.; Frost, J.; Cheung, T. K.; Tremberger, G.; Robbins, I.; Paglione, T.; Damas, C.; Steiner, J. C.; Rudolph, E.; Carlson, B. E.; Lewis, E.; Cline, T. D.; Zalava-Gutierrez, R.; Howard, A.; Morris, P. A.; Reiff, P. H.; Scalzo, F.; Chow, Y.; Stewart, A.; Zamor, P.; Brathwaite, K.; Barley, R.; Tulsee, T.

2012-12-01

During 2012, City University of New York (CUNY) and NASA Goddard Space Fight Center (GSFC) Heliophysics Research and Education Consortium centered on faculty and undergraduate research, as well as public outreach. Research areas spanned Heliophysics from solar surface to Earth's magnetosphere/ionosphere, microsatellite development for ionospheric experiments and climate change investigations. The Summer 2012 research teams were located at CUNY campuses and GSFC. Fourteen undergraduate students participated; four are female and eleven are underrepresented minorities. Topics included: Analyzing the Links Between Aurora Borealis, Magnetic Reconnection, and Substorms; Solar Energy Upsurge in 2012-Jun Active Region 1520 with 2010-Jun Active Region 1108 Calibration; Solar Limb Active Region 1515 Analysis and Coronal Heating; Testing Solar Energetic Particle Origin Through COMPTEL Small X-Ray Line Flares; Investigation of Sunspot Regions connection to Coronal Mass Ejections and Solar Flares; A Study of the Stratospheric Aerosols on Jupiter Using Hubble Space Telescope Data; An Integration and Testing Methodology for a Nanosatellite; Software Architecture for Autonomous Control; Combining Passive Polarimetric Remote Sensing and Advanced Measurements of Lidar Intensive Variables in Vertically Resolved Aerosol Retrievals; Tropospheric Ozone Investigations in New York City; The Effects of the Arctic, North Atlantic and El Niño-Southern Oscillation on Climate in the New York Metropolitan Area; Fluctuation Analysis of Magnetic Tornadoes Simulation Model; Ocean Mixing Models Parameterization for Climate Studies; and Analyses of Colloidal Leachate Recovered from Field- and Laboratory-Experiments on Bio-reacted Mining Waste. Public outreach activities included Space Weather workshops, for high school teachers and undergraduate students, conducted by GSFC Space Weather Action Center scientist and a week of CUNY-wide activities for Sun-Earth Day conducted by CUNY faculty and external university partners. The project is supported by NASA awards NNX10AE72G and NNX09AL77G.

First Evaluation of the CCAM Aerosol Simulation over Africa: Implications for Regional Climate Modeling

NASA Astrophysics Data System (ADS)

Horowitz, H.; Garland, R. M.; Thatcher, M. J.; Naidoo, M.; van der Merwe, J.; Landman, W.; Engelbrecht, F.

2015-12-01

An accurate representation of African aerosols in climate models is needed to understand the regional and global radiative forcing and climate impacts of aerosols, at present and under future climate change. However, aerosol simulations in regional climate models for Africa have not been well-tested. Africa contains the largest single source of biomass-burning smoke aerosols and dust globally. Although aerosols are short-lived relative to greenhouse gases, black carbon in particular is estimated to be second only to carbon dioxide in contributing to warming on a global scale. Moreover, Saharan dust is exported great distances over the Atlantic Ocean, affecting nutrient transport to regions like the Amazon rainforest, which can further impact climate. Biomass burning aerosols are also exported from Africa, westward from Angola over the Atlantic Ocean and off the southeastern coast of South Africa to the Indian Ocean. Here, we perform the first extensive quantitative evaluation of the Conformal-Cubic Atmospheric Model (CCAM) aerosol simulation against monitored data, focusing on aerosol optical depth (AOD) observations over Africa. We analyze historical regional simulations for 1999 - 2012 from CCAM consistent with the experimental design of CORDEX at 50 km global horizontal resolution, through the dynamical downscaling of ERA-Interim data reanalysis data, with the CMIP5 emissions inventory (RCP8.5 scenario). CCAM has a prognostic aerosol scheme for organic carbon, black carbon, sulfate, and dust, and non-prognostic sea salt. The CCAM AOD at 550nm was compared to AOD (observed at 440nm, adjusted to 550nm with the Ångström exponent) from long-term AERONET stations across Africa. Sites strongly impacted by dust and biomass burning and with long continuous records were prioritized. In general, the model captures the monthly trends of the AERONET data. This presentation provides a basis for understanding how well aerosol particles are represented over Africa in regional climate modeling and the potential impact on climate predictions, and is the first large scale climate model-measurement verification of aerosols over Africa that we are aware of. CCAM is widely used for regional climate modeling applications, and we also discuss further improvements to the aerosol parameterizations based on our results.

How Models Simulate the Radiative Effect in the Transition Zone of the Aerosol-Cloud Continuum

NASA Astrophysics Data System (ADS)

Calbo Angrill, J.; González, J. A.; Long, C. N.; McComiskey, A. C.

2017-12-01

Several studies have pointed towards dealing with clouds and aerosols as two manifestations of what is essentially the same physical phenomenon: a suspension of tiny particles in the air. Although the two extreme cases (i.e., pure aerosol and well-defined cloud) are easily distinguished, and obviously produce different radiative effects, there are many situations in the transition (or "twilight") zone. In a recent paper [Calbó et al., Atmos. Res. 2017, j.atmosres.2017.06.010], the authors of the current communication estimated that about 10% of time there might be a suspension of particles in the air that is difficult to distinguish as either cloud or aerosol. Radiative transfer models, however, simulate the effect of clouds and aerosols with different modules, routines, or parameterizations. In this study, we apply a sensitivity analysis approach to assess the ability of two radiative transfer models (SBDART and RRTM) in simulating the radiative effect of a suspension of particles with characteristics in the boundary between cloud and aerosol. We simulate this kind of suspension either in "cloud mode" or in "aerosol mode" and setting different values of optical depth, droplet size, water path, aerosol type, cloud height, etc. Irradiances both for solar and infrared bands are studied, both at ground level and at the top of the atmosphere, and all analyses are repeated for different solar zenith angles. We obtain that (a) water clouds and ice clouds have similar radiative effects if they have the same optical depth; (b) the spread of effects regarding different aerosol type/aerosol characteristics is remarkable; (c) radiative effects of an aerosol layer and of a cloud layer are different, even if they have similar optical depth; (d) for a given effect on the diffuse component, the effect on the direct component is usually greater (more extinction of direct beam) by aerosols than by clouds; (e) radiative transfer models are somewhat limited when simulating the effects of a suspension of particles in the transition zone, as the approach to this zone as an aerosol or as a cloud produces different results.

Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

NASA Technical Reports Server (NTRS)

da Silva, Arlindo

2010-01-01

A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of assimilating AOD retrievals from MODIS (on both Aqua and TERRA satellites) from AERONET for validation. The impact on the GEOS-5 Aerosol Forecasting will be fully documented.

Evaluating the Assumptions of Surface Reflectance and Aerosol Type Selection Within the MODIS Aerosol Retrieval Over Land: The Problem of Dust Type Selection

NASA Technical Reports Server (NTRS)

Mielonen, T.; Levy, R. C.; Aaltonen, V.; Komppula, M.; de Leeuw, G.; Huttunen, J.; Lihavainen, H.; Kolmonen, P.; Lehtinen, K. E. J.; Arola, A.

2011-01-01

Aerosol Optical Depth (AOD) and Angstrom exponent (AE) values derived with the MODIS retrieval algorithm over land (Collection 5) are compared with ground based sun photometer measurements at eleven sites spanning the globe. Although, in general, total AOD compares well at these sites (R2 values generally over 0.8), there are cases (from 2 to 67% of the measurements depending on the site) where MODIS clearly retrieves the wrong spectral dependence, and hence, an unrealistic AE value. Some of these poor AE retrievals are due to the aerosol signal being too small (total AOD<0.3) but in other cases the AOD should have been high enough to derive accurate AE. However, in these cases, MODIS indicates AE values close to 0.6 and zero fine model weighting (FMW), i.e. dust model provides the best fitting to the MODIS observed reflectance. Yet, according to evidence from the collocated sun photometer measurements and back-trajectory analyses, there should be no dust present. This indicates that the assumptions about aerosol model and surface properties made by the MODIS algorithm may have been incorrect. Here we focus on problems related to parameterization of the land-surface optical properties in the algorithm, in particular the relationship between the surface reflectance at 660 and 2130 nm.

Evaluate transport processes in MERRA driven chemical transport models using updated 222Rn emission inventories and global observations

NASA Astrophysics Data System (ADS)

Zhang, B.; Liu, H.; Crawford, J. H.; Fairlie, T. D.; Chen, G.; Chambers, S. D.; Kang, C. H.; Williams, A. G.; Zhang, K.; Considine, D. B.; Payer Sulprizio, M.; Yantosca, R.

2015-12-01

Convective and synoptic processes play a major role in determining the transport and distribution of trace gases and aerosols in the troposphere. The representation of these processes in global models (at ~100-1000 km horizontal resolution) is challenging, because convection is a sub-grid process and needs to be parameterized, while synoptic processes are close to the grid scale. Depending on the parameterization schemes used in climate models, the role of convection in transporting trace gases and aerosols may vary from model to model. 222Rn is a chemically inert and radioactive gas constantly emitted from soil and has a half-life (3.8 days) comparable to synoptic timescale, which makes it an effective tracer for convective and synoptic transport. In this study, we evaluate the convective and synoptic transport in two chemical transport models (GMI and GEOS-Chem), both driven by the NASA's MERRA reanalysis. Considering the uncertainties in 222Rn emissions, we incorporate two more recent scenarios with regionally varying 222Rn emissions into GEOS-Chem/MERRA and compare the simulation results with those using the relatively uniform 222Rn emissions in the standard model. We evaluate the global distribution and seasonality of 222Rn concentrations simulated by the two models against an extended collection of 222Rn observations from 1970s to 2010s. The intercomparison will improve our understanding of the spatial variability in global 222Rn emissions, including the suspected excessive 222Rn emissions in East Asia, and provide useful feedbacks on 222Rn emission models. We will assess 222Rn vertical distributions at different latitudes in the models using observations at surface sites and in the upper troposphere and lower stratosphere. Results will be compared with previous models driven by other meteorological fields (e.g., fvGCM and GEOS4). Since the decay of 222Rn is the source of 210Pb, a useful radionuclide tracer attached to submicron aerosols, improved understanding of emissions and transport of 222Rn will provide insights into the transport, distribution, and wet deposition of 210Pb aerosols.

Parameterization retrieval of trace gas volume mixing ratios from Airborne MAX-DOAS

NASA Astrophysics Data System (ADS)

Dix, Barbara; Koenig, Theodore K.; Volkamer, Rainer

2016-11-01

We present a parameterization retrieval of volume mixing ratios (VMRs) from differential slant column density (dSCD) measurements by Airborne Multi-AXis Differential Optical Absorption Spectroscopy (AMAX-DOAS). The method makes use of the fact that horizontally recorded limb spectra (elevation angle 0°) are strongly sensitive to the atmospheric layer at instrument altitude. These limb spectra are analyzed using reference spectra that largely cancel out column contributions from above and below the instrument, so that the resulting limb dSCDs, i.e., the column integrated concentration with respect to a reference spectrum, are almost exclusively sensitive to the atmospheric layers around instrument altitude. The conversion of limb dSCDs into VMRs is then realized by calculating box air mass factors (Box-AMFs) for a Rayleigh atmosphere and applying a scaling factor constrained by O4 dSCDs to account for aerosol extinction. An iterative VMR retrieval scheme corrects for trace gas profile shape effects. Benefits of this method are (1) a fast conversion that only requires the computation of Box-AMFs in a Rayleigh atmosphere; (2) neither local aerosol extinction nor the slant column density in the DOAS reference (SCDref) needs to be known; and (3) VMRs can be retrieved for every measurement point along a flight track, thus increasing statistics and adding flexibility to capture concentration gradients. Sensitivity studies are performed for bromine monoxide (BrO), iodine monoxide (IO) and nitrogen dioxide (NO2), using (1) simulated dSCD data for different trace gas and aerosol profiles and (2) field measurements from the Tropical Ocean tRoposphere Exchange of Reactive halogen species and Oxygenated VOC (TORERO) field experiment. For simulated data in a Rayleigh atmosphere, the agreement between the VMR from the parameterization method (VMRpara) and the true VMR (VMRtrue) is excellent for all trace gases. Offsets, slopes and R2 values for the linear fit of VMRpara over VMRtrue are, respectively (0.008 ± 0.001) pptv, 0.988 ± 0.001, 0.987 for BrO; (-0.0066 ± 0.0001) pptv, 1.0021 ± 0.0003, 0.9979 for IO; (-0.17 ± 0.03) pptv, 1.0036 ± 0.0001, 0.9997 for NO2. The agreement for atmospheres with aerosol shows comparable R2 values to the Rayleigh case, but slopes deviate a bit more from one: (0.093 ± 0.002) pptv, 0.933 ± 0.002, 0.907 for BrO; (0.0021 ± 0.0004) pptv, 0.887 ± 0.001, 0.973 for IO; (8.5 ± 0.1) pptv, 0.8302 ± 0.0006, 0.9923 for NO2. VMRpara from field data are further compared with optimal estimation retrievals (VMROE). Least orthogonal distance fit of the data give the following equations: BrOpara = (0.1 ± 0.2) pptv + (0.95 ± 0.14) × BrOOE; IOpara = (0.01 ± 0.02) pptv + (1.00 ± 0.12) × IOOE; NO2para = (3.9 ± 2.5) pptv + (0.87 ± 0.15) × NO2OE. Overall, we conclude that the parameterization retrieval is accurate with an uncertainty of 20 % for IO, 30 % for BrO and NO2, but not better than 0.05 pptv IO, 0.5 pptv BrO and 10 pptv NO2. The retrieval is applicable over a wide range of atmospheric conditions and measurement geometries and not limited to the interpretation of vertical profile measurements in the remote troposphere.

Evaluation of atmospheric aerosol and tropospheric ozone effects on global terrestrial ecosystem carbon dynamics

NASA Astrophysics Data System (ADS)

Chen, Min

The increasing human activities have produced large amounts of air pollutants ejected into the atmosphere, in which atmospheric aerosols and tropospheric ozone are considered to be especially important because of their negative impacts on human health and their impacts on global climate through either their direct radiative effect or indirect effect on land-atmosphere CO2 exchange. This dissertation dedicates to quantifying and evaluating the aerosol and tropospheric ozone effects on global terrestrial ecosystem dynamics using a modeling approach. An ecosystem model, the integrated Terrestrial Ecosystem Model (iTem), is developed to simulate biophysical and biogeochemical processes in terrestrial ecosystems. A two-broad-band atmospheric radiative transfer model together with the Moderate-Resolution Imaging Spectroradiometer (MODIS) measured atmospheric parameters are used to well estimate global downward solar radiation and the direct and diffuse components in comparison with observations. The atmospheric radiative transfer modeling framework were used to quantify the aerosol direct radiative effect, showing that aerosol loadings cause 18.7 and 12.8 W m -2 decrease of direct-beam Photosynthetic Active Radiation (PAR) and Near Infrared Radiation (NIR) respectively, and 5.2 and 4.4 W m -2 increase of diffuse PAR and NIR, respectively, leading to a total 21.9 W m-2 decrease of total downward solar radiation over the global land surface during the period of 2003-2010. The results also suggested that the aerosol effect may be overwhelmed by clouds because of the stronger extinction and scattering ability of clouds. Applications of the iTem with solar radiation data and with or without considering the aerosol loadings shows that aerosol loading enhances the terrestrial productions [Gross Primary Production (GPP), Net Primary Production (NPP) and Net Ecosystem Production (NEP)] and carbon emissions through plant respiration (RA) in global terrestrial ecosystems over the period of 2003-2010. Ecosystem heterotrophic respiration (RH) was negatively affected by the aerosol loading. These results support previous conclusions of the advantage of aerosol light scattering effect on plant productions in other studies but suggest there is strong spatial variation. This study finds indirect aerosol effects on terrestrial ecosystem carbon dynamics through affecting plant phenology, thermal and hydrological environments. All these evidences suggested that the aerosol direct radiative effect on global terrestrial ecosystem carbon dynamics should be considered to better understand the global carbon cycle and climate change. An ozone sub-model is developed in this dissertation and fully coupled with iTem. The coupled model, named iTemO3 considers the processes of ozone stomatal deposition, plant defense to ozone influx, ozone damage and plant repairing mechanism. By using a global atmospheric chemical transport model (GACTM) estimated ground-level ozone concentration data, the model estimated global annual stomatal ozone deposition is 234.0 Tg O3 yr-1 and indicates which regions have high ozone damage risk. Different plant functional types, sunlit and shaded leaves are shown to have different responses to ozone. The model predictions suggest that ozone has caused considerable change on global terrestrial ecosystem carbon storage and carbon exchanges over the study period 2004-2008. The study suggests that uncertainty of the key parameters in iTemO3 could result in large errors in model predictions. Thus more experimental data for better model parameterization is highly needed.

Water Quality Monitoring for Lake Constance with a Physically Based Algorithm for MERIS Data.

PubMed

Odermatt, Daniel; Heege, Thomas; Nieke, Jens; Kneubühler, Mathias; Itten, Klaus

2008-08-05

A physically based algorithm is used for automatic processing of MERIS level 1B full resolution data. The algorithm is originally used with input variables for optimization with different sensors (i.e. channel recalibration and weighting), aquatic regions (i.e. specific inherent optical properties) or atmospheric conditions (i.e. aerosol models). For operational use, however, a lake-specific parameterization is required, representing an approximation of the spatio-temporal variation in atmospheric and hydrooptic conditions, and accounting for sensor properties. The algorithm performs atmospheric correction with a LUT for at-sensor radiance, and a downhill simplex inversion of chl-a, sm and y from subsurface irradiance reflectance. These outputs are enhanced by a selective filter, which makes use of the retrieval residuals. Regular chl-a sampling measurements by the Lake's protection authority coinciding with MERIS acquisitions were used for parameterization, training and validation.

Submicron aerosol organic functional groups, ions, and water content at the Centreville SEARCH site (Alabama), during SOAS campaign

NASA Astrophysics Data System (ADS)

Ruggeri, G.; Ergin, G.; Modini, R. L.; Takahama, S.

2013-12-01

The SOAS campaign was conducted from June 1 to July 15 of 2013 in order to understand the relationship between biogenic and anthropogenic emissions in the South East US1,2. In this study, the organic and inorganic composition of submicron aerosol in the Centreville SEARCH site was measured by Fourier Transform Infrared Spectroscopy (FTIR) and the Ambient Ion Monitor (AIM; URG Corporation), whereas the aerosol water content was measured with a Dry Ambient Aerosol Size Spectrometer (DAASS)3. Organic functional group analysis was performed on PM1 aerosol selected by cyclone and collected on teflon filters with a time resolution of 4-12 hours, using one inlet heated to 50 °C and the other operated either at ambient temperature or 70 °C 4. The AIM measured both condensed and gas phase composition with a time resolution of 1 hour, providing partitioning behavior of inorganic species such as NH3/NH4+, HNO3/NO3-. These measurements collectively permit calculation of pure-component vapor pressures of candidate organic compounds and activity coefficients of interacting components in the condensed phase, using models such as SIMPOL.15, E-AIM6, and AIOMFAC7. From these results, the water content of the aerosol is predicted, and a comparison between modeled and measured partitioning of inorganic compounds and water vapor are discussed, in addition to organic aerosol volatility prediction based on functional group analysis. [1]- Goldstein, A.H., et al., Biogenic carbon and anthropogenic pollutants combine to form a cooling haze over the southeastern United States. Proceedings of the National Academy of Sciences of the United States of America, 2009. 106(22), 8835-8840. [2]- Carlton, A.G., Turpin, B.J., 2013. Particle partitioning potential of organic compounds is highest in the Eastern US and driven by anthropogenic water. Atmospheric Chemistry and Physics Discussions 13, 12743-12770. [3]- Khlystov, A., Stanier, C.O., Takahama, S., Pandis, S.N., 2005. Water content of ambient aerosol during the Pittsburgh Air Quality Study. Journal of Geophysical Research: Atmospheres 110, n/a-n/a. [4]- Takahama, S., Johnson, A., Russell, L.M., 2013. Quantification of Carboxylic and Carbonyl Functional Groups in Organic Aerosol Infrared Absorbance Spectra. Aerosol Science and Technology 47, 310-325. [5]- Pankow, J.F., Asher, W.E., 2008. SIMPOL.1: a simple group contribution method for predicting vapor pressures and enthalpies of vaporization of multifunctional organic compounds. Atmos. Chem. Phys. 8, 2773-2796. [6]- Clegg, S.L., Brimblecombe, P., Wexler, A.S., 1998. Thermodynamic Model of the System H+-NH4+-SO42--NO3--H2O at Tropospheric Temperatures. J. Phys. Chem. A 102, 2137-2154. [7]- Zuend, A., Marcolli, C., Booth, A.M., Lienhard, D.M., Soonsin, V., Krieger, U.K., Topping, D.O., McFiggans, G., Peter, T., Seinfeld, J.H., 2011. New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups. Atmos. Chem. Phys. 11, 9155-9206.

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.

An accurate method to measure alpha-emitting natural radionuclides in atmospheric filters: Application in two NORM industries

NASA Astrophysics Data System (ADS)

Lozano, R. L.; Bolívar, J. P.; San Miguel, E. G.; García-Tenorio, R.; Gázquez, M. J.

2011-12-01

In this work, an accurate method for the measurement of natural alpha-emitting radionuclides from aerosols collected in air filters is presented and discussed in detail. The knowledge of the levels of several natural alpha-emitting radionuclides (238U, 234U, 232Th, 230Th, 228Th, 226Ra and 210Po) in atmospheric aerosols is essential not only for a better understanding of the several atmospheric processes and changes, but also for a proper evaluation of the potential doses, which can inadvertently be received by the population via inhalation. The proposed method takes into account the presence of intrinsic amounts of these radionuclides in the matrices of the quartz filters used, as well as the possible variation in the humidity of the filters throughout the collection process. In both cases, the corrections necessary in order to redress these levels have been evaluated and parameterized. Furthermore, a detailed study has been performed into the optimisation of the volume of air to be sampled in order to increase the accuracy in the determination of the radionuclides. The method as a whole has been applied for the determination of the activity concentrations of U- and Th-isotopes in aerosols collected at two NORM (Naturally Occurring Radioactive Material) industries located in the southwest of Spain. Based on the levels found, a conservative estimation has been performed to yield the additional committed effective doses to which the workers are potentially susceptible due to inhalation of anthropogenic material present in the environment of these two NORM industries.

Can Aerosol Direct Radiative Effects Account for Analysis Increments of Temperature in the Tropical Atlantic?

NASA Technical Reports Server (NTRS)

da Silva, Arlindo M.; Alpert, Pinhas

2016-01-01

In the late 1990's, prior to the launch of the Terra satellite, atmospheric general circulation models (GCMs) did not include aerosol processes because aerosols were not properly monitored on a global scale and their spatial distributions were not known well enough for their incorporation in operational GCMs. At the time of the first GEOS Reanalysis (Schubert et al. 1993), long time series of analysis increments (the corrections to the atmospheric state by all available meteorological observations) became readily available, enabling detailed analysis of the GEOS-1 errors on a global scale. Such analysis revealed that temperature biases were particularly pronounced in the Tropical Atlantic region, with patterns depicting a remarkable similarity to dust plumes emanating from the African continent as evidenced by TOMS aerosol index maps. Yoram Kaufman was instrumental encouraging us to pursue this issue further, resulting in the study reported in Alpert et al. (1998) where we attempted to assess aerosol forcing by studying the errors of a the GEOS-1 GCM without aerosol physics within a data assimilation system. Based on this analysis, Alpert et al. (1998) put forward that dust aerosols are an important source of inaccuracies in numerical weather-prediction models in the Tropical Atlantic region, although a direct verification of this hypothesis was not possible back then. Nearly 20 years later, numerical prediction models have increased in resolution and complexity of physical parameterizations, including the representation of aerosols and their interactions with the circulation. Moreover, with the advent of NASA's EOS program and subsequent satellites, atmospheric aerosols are now monitored globally on a routine basis, and their assimilation in global models are becoming well established. In this talk we will reexamine the Alpert et al. (1998) hypothesis using the most recent version of the GEOS-5 Data Assimilation System with assimilation of aerosols. We will explicitly calculate the impact of aerosols on the temperature analysis increments in the tropical Atlantic and assess the extent to which inclusion of atmospheric aerosols have reduced these increments.

Direct and semidirect aerosol effects of southern African biomass burning aerosol

NASA Astrophysics Data System (ADS)

Sakaeda, Naoko; Wood, Robert; Rasch, Philip J.

2011-06-01

Direct and semidirect radiative effects of biomass burning aerosols from southern African fires during July-October are investigated using 20 year runs of the Community Atmospheric Model (CAM) coupled to a slab ocean model. Aerosol optical depth is constrained using observations in clear skies from Moderate Resolution Imaging Spectroradiometer (MODIS) and for aerosol layers above clouds from Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). Over the ocean, where the aerosol layers are primarily located above cloud, negative top of atmosphere (TOA) semidirect radiative effects associated with increased low cloud cover dominate over a weaker positive all-sky direct radiative effect (DRE). In contrast, over the land where the aerosols are often below or within cloud layers, reductions in cloud liquid water path (LWP) lead to a positive semidirect radiative effect that dominates over a near-zero DRE. Over the ocean, the cloud response can be understood as a response to increased lower tropospheric stability (LTS) which is caused both by radiative heating in overlying layers and surface cooling in response to direct aerosol forcing. The marine cloud changes are robust to changes in the cloud parameterization (removal of the hard-wired dependence of clouds on LTS), suggesting that they are physically realistic. Over land, decreased LWP is consistent with weaker convection driven by increased static stability. Over the entire region the overall TOA radiative effect from the biomass burning aerosols is almost zero due to opposing effects over the land and ocean. However, the surface forcing is strongly negative, which leads to a reduction in precipitation and also a reduction in sensible heat flux. The former is primarily realized through reductions in convective precipitation on both the southern and northern flanks of the convective precipitation region spanning the equatorial rain forest and the Intertropical Convergence Zone (ITCZ) in the southern Sahel. The changes are consistent with the low-level aerosol-forced cooling pattern. The results highlight the importance of semidirect radiative effects and precipitation responses for determining the climatic effects of aerosols in the African region.

Testing cloud microphysics parameterizations in NCAR CAM5 with ISDAC and M-PACE observations

NASA Astrophysics Data System (ADS)

Liu, Xiaohong; Xie, Shaocheng; Boyle, James; Klein, Stephen A.; Shi, Xiangjun; Wang, Zhien; Lin, Wuyin; Ghan, Steven J.; Earle, Michael; Liu, Peter S. K.; Zelenyuk, Alla

2011-01-01

Arctic clouds simulated by the National Center for Atmospheric Research (NCAR) Community Atmospheric Model version 5 (CAM5) are evaluated with observations from the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Indirect and Semi-Direct Aerosol Campaign (ISDAC) and Mixed-Phase Arctic Cloud Experiment (M-PACE), which were conducted at its North Slope of Alaska site in April 2008 and October 2004, respectively. Model forecasts for the Arctic spring and fall seasons performed under the Cloud-Associated Parameterizations Testbed framework generally reproduce the spatial distributions of cloud fraction for single-layer boundary-layer mixed-phase stratocumulus and multilayer or deep frontal clouds. However, for low-level stratocumulus, the model significantly underestimates the observed cloud liquid water content in both seasons. As a result, CAM5 significantly underestimates the surface downward longwave radiative fluxes by 20-40 W m-2. Introducing a new ice nucleation parameterization slightly improves the model performance for low-level mixed-phase clouds by increasing cloud liquid water content through the reduction of the conversion rate from cloud liquid to ice by the Wegener-Bergeron-Findeisen process. The CAM5 single-column model testing shows that changing the instantaneous freezing temperature of rain to form snow from -5°C to -40°C causes a large increase in modeled cloud liquid water content through the slowing down of cloud liquid and rain-related processes (e.g., autoconversion of cloud liquid to rain). The underestimation of aerosol concentrations in CAM5 in the Arctic also plays an important role in the low bias of cloud liquid water in the single-layer mixed-phase clouds. In addition, numerical issues related to the coupling of model physics and time stepping in CAM5 are responsible for the model biases and will be explored in future studies.

Parameterizing correlations between hydrometeor species in mixed-phase Arctic clouds

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

Larson, Vincent E.; Nielsen, Brandon J.; Fan, Jiwen

2011-08-16

Mixed-phase Arctic clouds, like other clouds, contain small-scale variability in hydrometeor fields, such as cloud water or snow mixing ratio. This variability may be worth parameterizing in coarse-resolution numerical models. In particular, for modeling processes such as accretion and aggregation, it would be useful to parameterize subgrid correlations among hydrometeor species. However, one difficulty is that there exist many hydrometeor species and many microphysical processes, leading to complexity and computational expense.Existing lower and upper bounds (inequalities) on linear correlation coefficients provide useful guidance, but these bounds are too loose to serve directly as a method to predict subgrid correlations. Therefore,more » this paper proposes an alternative method that is based on a blend of theory and empiricism. The method begins with the spherical parameterization framework of Pinheiro and Bates (1996), which expresses the correlation matrix in terms of its Cholesky factorization. The values of the elements of the Cholesky matrix are parameterized here using a cosine row-wise formula that is inspired by the aforementioned bounds on correlations. The method has three advantages: 1) the computational expense is tolerable; 2) the correlations are, by construction, guaranteed to be consistent with each other; and 3) the methodology is fairly general and hence may be applicable to other problems. The method is tested non-interactively using simulations of three Arctic mixed-phase cloud cases from two different field experiments: the Indirect and Semi-Direct Aerosol Campaign (ISDAC) and the Mixed-Phase Arctic Cloud Experiment (M-PACE). Benchmark simulations are performed using a large-eddy simulation (LES) model that includes a bin microphysical scheme. The correlations estimated by the new method satisfactorily approximate the correlations produced by the LES.« less

Impact of Snow Grain Shape and Internal Mixing with Black Carbon Aerosol on Snow Optical Properties for use in Climate Models

NASA Astrophysics Data System (ADS)

He, C.; Liou, K. N.; Takano, Y.; Yang, P.; Li, Q.; Chen, F.

2017-12-01

A set of parameterizations is developed for spectral single-scattering properties of clean and black carbon (BC)-contaminated snow based on geometric-optic surface-wave (GOS) computations, which explicitly resolves BC-snow internal mixing and various snow grain shapes. GOS calculations show that, compared with nonspherical grains, volume-equivalent snow spheres show up to 20% larger asymmetry factors and hence stronger forward scattering, particularly at wavelengths <1 mm. In contrast, snow grain sizes have a rather small impact on the asymmetry factor at wavelengths <1 mm, whereas size effects are important at longer wavelengths. The snow asymmetry factor is parameterized as a function of effective size, aspect ratio, and shape factor, and shows excellent agreement with GOS calculations. According to GOS calculations, the single-scattering coalbedo of pure snow is predominantly affected by grain sizes, rather than grain shapes, with higher values for larger grains. The snow single-scattering coalbedo is parameterized in terms of the effective size that combines shape and size effects, with an accuracy of >99%. Based on GOS calculations, BC-snow internal mixing enhances the snow single-scattering coalbedo at wavelengths <1 mm, but it does not alter the snow asymmetry factor. The BC-induced enhancement ratio of snow single-scattering coalbedo, independent of snow grain size and shape, is parameterized as a function of BC concentration with an accuracy of >99%. Overall, in addition to snow grain size, both BC-snow internal mixing and snow grain shape play critical roles in quantifying BC effects on snow optical properties. The present parameterizations can be conveniently applied to snow, land surface, and climate models including snowpack radiative transfer processes.

Assessment of two physical parameterization schemes for desert dust emissions in an atmospheric chemistry general circulation model

NASA Astrophysics Data System (ADS)

Astitha, M.; Abdel Kader, M.; Pozzer, A.; Lelieveld, J.

2012-04-01

Atmospheric particulate matter and more specific desert dust has been the topic of numerous research studies in the past due to the wide range of impacts in the environment and climate and the uncertainty of characterizing and quantifying these impacts in a global scale. In this work we present two physical parameterizations of the desert dust production that have been incorporated in the atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy2.41 Atmospheric Chemistry). The scope of this work is to assess the impact of the two physical parameterizations in the global distribution of desert dust and highlight the advantages and disadvantages of using either technique. The dust concentration and deposition has been evaluated using the AEROCOM dust dataset for the year 2000 and data from the MODIS and MISR satellites as well as sun-photometer data from the AERONET network was used to compare the modelled aerosol optical depth with observations. The implementation of the two parameterizations and the simulations using relatively high spatial resolution (T106~1.1deg) has highlighted the large spatial heterogeneity of the dust emission sources as well as the importance of the input parameters (soil size and texture, vegetation, surface wind speed). Also, sensitivity simulations with the nudging option using reanalysis data from ECMWF and without nudging have showed remarkable differences for some areas. Both parameterizations have revealed the difficulty of simulating all arid regions with the same assumptions and mechanisms. Depending on the arid region, each emission scheme performs more or less satisfactorily which leads to the necessity of treating each desert differently. Even though this is a quite different task to accomplish in a global model, some recommendations are given and ideas for future improvements.

Are Atmospheric Updrafts a Key to Unlocking Climate Forcing and Sensitivity?

DOE PAGES

Donner, Leo J.; O'Brien, Travis A.; Rieger, Daniel; ...

2016-06-08

Both climate forcing and climate sensitivity persist as stubborn uncertainties limiting the extent to which climate models can provide actionable scientific scenarios for climate change. A key, explicit control on cloud-aerosol interactions, the largest uncertainty in climate forcing, is the vertical velocity of cloud-scale updrafts. Model-based studies of climate sensitivity indicate that convective entrainment, which is closely related to updraft speeds, is an important control on climate sensitivity. Updraft vertical velocities also drive many physical processes essential to numerical weather prediction. Vertical velocities and their role in atmospheric physical processes have been given very limited attention in models for climatemore » and numerical weather prediction. The relevant physical scales range down to tens of meters and are thus frequently sub-grid and require parameterization. Many state-of-science convection parameterizations provide mass fluxes without specifying vertical velocities, and parameterizations which do provide vertical velocities have been subject to limited evaluation against what have until recently been scant observations. Atmospheric observations imply that the distribution of vertical velocities depends on the areas over which the vertical velocities are averaged. Distributions of vertical velocities in climate models may capture this behavior, but it has not been accounted for when parameterizing cloud and precipitation processes in current models. New observations of convective vertical velocities offer a potentially promising path toward developing process-level cloud models and parameterizations for climate and numerical weather prediction. Taking account of scale-dependence of resolved vertical velocities offers a path to matching cloud-scale physical processes and their driving dynamics more realistically, with a prospect of reduced uncertainty in both climate forcing and sensitivity.« less

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.

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.

Planetary Boundary Layer from AERI and MPL

DOE Data Explorer

Sawyer, Virginia

2014-02-13

The distribution and transport of aerosol emitted to the lower troposphere is governed by the height of the planetary boundary layer (PBL), which limits the dilution of pollutants and influences boundary-layer convection. Because radiative heating and cooling of the surface strongly affect the PBL top height, it follows diurnal and seasonal cycles and may vary by hundreds of meters over a 24-hour period. The cap the PBL imposes on low-level aerosol transport makes aerosol concentration an effective proxy for PBL height: the top of the PBL is marked by a rapid transition from polluted, well-mixed boundary-layer air to the cleaner, more stratified free troposphere. Micropulse lidar (MPL) can provide much higher temporal resolution than radiosonde and better vertical resolution than infrared spectrometer (AERI), but PBL heights from all three instruments at the ARM SGP site are compared to one another for validation. If there is agreement among them, the higher-resolution remote sensing-derived PBL heights can accurately fill in the gaps left by the low frequency of radiosonde launches, and thus improve model parameterizations and our understanding of boundary-layer processes.

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

Assessment of simulated aerosol effective radiative forcings in the terrestrial spectrum

NASA Astrophysics Data System (ADS)

Heyn, Irene; Block, Karoline; Mülmenstädt, Johannes; Gryspeerdt, Edward; Kühne, Philipp; Salzmann, Marc; Quaas, Johannes

2017-01-01

In its fifth assessment report (AR5), the Intergovernmental Panel on Climate Change provides a best estimate of the effective radiative forcing (ERF) due to anthropogenic aerosol at -0.9 W m-2. This value is considerably weaker than the estimate of -1.2 W m-2 in AR4. A part of the difference can be explained by an offset of +0.2 W m-2 which AR5 added to all published estimates that only considered the solar spectrum, in order to account for adjustments in the terrestrial spectrum. We find that, in the CMIP5 multimodel median, the ERF in the terrestrial spectrum is small, unless microphysical effects on ice- and mixed-phase clouds are parameterized. In the latter case it is large but accompanied by a very strong ERF in the solar spectrum. The total adjustments can be separated into microphysical adjustments (aerosol "effects") and thermodynamic adjustments. Using a kernel technique, we quantify the latter and find that the rapid thermodynamic adjustments of water vapor and temperature profiles are small. Observation-based constraints on these model results are urgently needed.

Effects of atmospheric dynamics and aerosols on the fraction of supercooled water clouds

NASA Astrophysics Data System (ADS)

Li, Jiming; Lv, Qiaoyi; Zhang, Min; Wang, Tianhe; Kawamoto, Kazuaki; Chen, Siyu; Zhang, Beidou

2017-02-01

Based on 8 years of (January 2008-December 2015) cloud phase information from the GCM-Oriented Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) Cloud Product (GOCCP), aerosol products from CALIPSO and meteorological parameters from the ERA-Interim products, the present study investigates the effects of atmospheric dynamics on the supercooled liquid cloud fraction (SCF) during nighttime under different aerosol loadings at global scale to better understand the conditions of supercooled liquid water gradually transforming to ice phase. Statistical results indicate that aerosols' effect on nucleation cannot fully explain all SCF changes, especially in those regions where aerosols' effect on nucleation is not a first-order influence (e.g., due to low ice nuclei aerosol frequency). By performing the temporal and spatial correlations between SCFs and different meteorological factors, this study presents specifically the relationship between SCF and different meteorological parameters under different aerosol loadings on a global scale. We find that the SCFs almost decrease with increasing of aerosol loading, and the SCF variation is closely related to the meteorological parameters but their temporal relationship is not stable and varies with the different regions, seasons and isotherm levels. Obviously negative temporal correlations between SCFs versus vertical velocity and relative humidity indicate that the higher vertical velocity and relative humidity the smaller SCFs. However, the patterns of temporal correlation for lower-tropospheric static stability, skin temperature and horizontal wind are relatively more complex than those of vertical velocity and humidity. For example, their close correlations are predominantly located in middle and high latitudes and vary with latitude or surface type. Although these statistical correlations have not been used to establish a certain causal relationship, our results may provide a unique point of view on the phase change of mixed-phase cloud and have potential implications for further improving the parameterization of the cloud phase and determining the climate feedbacks.

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

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

WRF-Chem Model Simulations of Arizona Dust Storms

NASA Astrophysics Data System (ADS)

Mohebbi, A.; Chang, H. I.; Hondula, D.

2017-12-01

The online Weather Research and Forecasting model with coupled chemistry module (WRF-Chem) is applied to simulate the transport, deposition and emission of the dust aerosols in an intense dust outbreak event that took place on July 5th, 2011 over Arizona. Goddard Chemistry Aerosol Radiation and Transport (GOCART), Air Force Weather Agency (AFWA), and University of Cologne (UoC) parameterization schemes for dust emission were evaluated. The model was found to simulate well the synoptic meteorological conditions also widely documented in previous studies. The chemistry module performance in reproducing the atmospheric desert dust load was evaluated using the horizontal field of the Aerosol Optical Depth (AOD) from Moderate Resolution Imaging Spectro (MODIS) radiometer Terra/Aqua and Aerosol Robotic Network (AERONET) satellites employing standard Dark Target (DT) and Deep Blue (DB) algorithms. To assess the temporal variability of the dust storm, Particulate Matter mass concentration data (PM10 and PM2.5) from Arizona Department of Environmental Quality (AZDEQ) ground-based air quality stations were used. The promising performance of WRF-Chem indicate that the model is capable of simulating the right timing and loading of a dust event in the planetary-boundary-layer (PBL) which can be used to forecast approaching severe dust events and to communicate an effective early warning.

Missing ozone-induced potential aerosol formation in a suburban deciduous forest

NASA Astrophysics Data System (ADS)

Nakayama, T.; Kuruma, Y.; Matsumi, Y.; Morino, Y.; Sato, K.; Tsurumaru, H.; Ramasamy, S.; Sakamoto, Y.; Kato, S.; Miyazaki, Y.; Mochizuki, T.; Kawamura, K.; Sadanaga, Y.; Nakashima, Y.; Matsuda, K.; Kajii, Y.

2017-12-01

As a new approach to investigating formation processes of secondary organic aerosol (SOA) in the atmosphere, ozone-induced potential aerosol formation was measured in summer at a suburban forest site surrounded by deciduous trees, near Tokyo, Japan. After passage through a reactor containing high concentrations of ozone, increases in total particle volume (average of 1.4 × 109 nm3/cm3, which corresponds to 17% that of pre-existing particles) were observed, especially during daytime. The observed aerosol formations were compared with the results of box model simulations using simultaneously measured concentrations of gaseous and particulate species. According to the model, the relative contributions of isoprene, monoterpene, and aromatic hydrocarbon oxidation to SOA formation in the reactor were 24, 21, and 55%, respectively. However, the model could explain, on average, only ∼40% of the observed particle formation, and large discrepancies between the observations and model were found, especially around noon and in the afternoon when the concentrations of isoprene and oxygenated volatile organic compounds were high. The results suggest a significant contribution of missing (unaccounted-for) SOA formation processes from identified and/or unidentified volatile organic compounds, especially those emitted during daytime. Further efforts should be made to explore and parameterize this missing SOA formation to assist in the improvement of atmospheric chemistry and climate models.

Vertical distributions of fluorescent aerosol over the Eastern U.S.

NASA Astrophysics Data System (ADS)

Perring, A. E.; Robinson, E. S.; Schwarz, J. P.; Gao, R. S.

2016-12-01

The prevalence of bioaerosol in the atmosphere is relevant to atmospheric chemistry, microbial ecology and climate. These particles can act as effective cloud condensation nuclei (CCN) and ice nuclei (IN), representing a potential feedback between vegetation and precipitation. As bioaerosol frequently account for a substantial fraction of coarse mode aerosol in the boundary layer, they may have significant impacts on mixed-phase and/or cirrus cloud formation and climate. Very few measurements are available, however, to constrain loadings of bioaerosol in the free troposphere. Here we present vertical profiles of fluorescent aerosol concentration as a proxy for bioaerosol. The data were obtained over the eastern U.S. during the summer of 2016 using a Wide Band Integrated Bioaerosol Sensor (WIBS) installed aboard a NOAA Twin Otter research aircraft. The airspeed and inlet configuration were chosen to permit efficient sampling of aerosol with diameters of up to 10 μm. Vertical profiles extend from 1000 to 17,500 feet AGL, spanning a temperature range relevant to ice formation. 100 hours of data cover a latitude range from 30N to 46N and target a variety of potential bioaerosol source regions including forests, croplands, the Gulf of Mexico, and Lake Michigan. Observed vertical profiles are compared to expected loadings based on current model parameterizations and implications are discussed.

Chemical transport model simulations of organic aerosol in ...

EPA Pesticide Factsheets

Gasoline- and diesel-fueled engines are ubiquitous sources of air pollution in urban environments. They emit both primary particulate matter and precursor gases that react to form secondary particulate matter in the atmosphere. In this work, we updated the organic aerosol module and organic emissions inventory of a three-dimensional chemical transport model, the Community Multiscale Air Quality Model (CMAQ), using recent, experimentally derived inputs and parameterizations for mobile sources. The updated model included a revised volatile organic compound (VOC) speciation for mobile sources and secondary organic aerosol (SOA) formation from unspeciated intermediate volatility organic compounds (IVOCs). The updated model was used to simulate air quality in southern California during May and June 2010, when the California Research at the Nexus of Air Quality and Climate Change (CalNex) study was conducted. Compared to the Traditional version of CMAQ, which is commonly used for regulatory applications, the updated model did not significantly alter the predicted organic aerosol (OA) mass concentrations but did substantially improve predictions of OA sources and composition (e.g., POA–SOA split), as well as ambient IVOC concentrations. The updated model, despite substantial differences in emissions and chemistry, performed similar to a recently released research version of CMAQ (Woody et al., 2016) that did not include the updated VOC and IVOC emissions and SOA data

Identifying Aerosol Type/Mixture from Aerosol Absorption Properties Using AERONET

NASA Technical Reports Server (NTRS)

Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Dickerson, R. R.; Thompson, A. M.; Slutsker, I.; Li, Z.; Tripathi, S. N.; Singh, R. P.;

Simulating Aerosol Size Distribution and Mass Concentration with Simultaneous Nucleation, Condensation/Coagulation, and Deposition with the GRAPES-CUACE

NASA Astrophysics Data System (ADS)

Zhou, Chunhong; Shen, Xiaojing; Liu, Zirui; Zhang, Yangmei; Xin, Jinyuan

2018-04-01

A coupled aerosol-cloud model is essential for investigating the formation of haze and fog and the interaction of aerosols with clouds and precipitation. One of the key tasks of such a model is to produce correct mass and number size distributions of aerosols. In this paper, a parameterization scheme for aerosol size distribution in initial emission, which took into account the measured mass and number size distributions of aerosols, was developed in the GRAPES-CUACE [Global/Regional Assimilation and PrEdiction System-China Meteorological Administration (CMA) Unified Atmospheric Chemistry Environment model]—an online chemical weather forecast system that contains microphysical processes and emission, transport, and chemical conversion of sectional multi-component aerosols. In addition, the competitive mechanism between nucleation and condensation for secondary aerosol formation was improved, and the dry deposition was also modified to be in consistent with the real depositing length. Based on the above improvements, the GRAPES-CUACE simulations were verified against observational data during 1-31 January 2013, when a series of heavy regional haze-fog events occurred in eastern China. The results show that the aerosol number size distribution from the improved experiment was much closer to the observation, whereas in the old experiment the number concentration was higher in the nucleation mode and lower in the accumulation mode. Meanwhile, the errors in aerosol number size distribution as diagnosed by its sectional mass size distribution were also reduced. Moreover, simulations of organic carbon, sulfate, and other aerosol components were improved and the overestimation as well as underestimation of PM2.5 concentration in eastern China was significantly reduced, leading to increased correlation coefficient between simulated and observed PM2.5 by more than 70%. In the remote areas where bad simulation results were produced previously, the correlation coefficient grew from 0.35 to 0.61, and the mean mass concentration went up from 43% to 87.5% of the observed value. Thus, the simulation of particulate matters in these areas has been improved considerably.

MACv2-SP: a parameterization of anthropogenic aerosol optical properties and an associated Twomey effect for use in CMIP6

NASA Astrophysics Data System (ADS)

Stevens, Bjorn; Fiedler, Stephanie; Kinne, Stefan; Peters, Karsten; Rast, Sebastian; Müsse, Jobst; Smith, Steven J.; Mauritsen, Thorsten

2017-02-01

A simple plume implementation of the second version (v2) of the Max Planck Institute Aerosol Climatology, MACv2-SP, is described. MACv2-SP provides a prescription of anthropogenic aerosol optical properties and an associated Twomey effect. It was created to provide a harmonized description of post-1850 anthropogenic aerosol radiative forcing for climate modeling studies. MACv2-SP has been designed to be easy to implement, change and use, and thereby enable studies exploring the climatic effects of different patterns of aerosol radiative forcing, including a Twomey effect. MACv2-SP is formulated in terms of nine spatial plumes associated with different major anthropogenic source regions. The shape of the plumes is fit to the Max Planck Institute Aerosol Climatology, version 2, whose present-day (2005) distribution is anchored by surface-based observations. Two types of plumes are considered: one predominantly associated with biomass burning, the other with industrial emissions. These differ in the prescription of their annual cycle and in their optical properties, thereby implicitly accounting for different contributions of absorbing aerosol to the different plumes. A Twomey effect for each plume is prescribed as a change in the host model's background cloud-droplet population density using relationships derived from satellite data. Year-to-year variations in the amplitude of the plumes over the historical period (1850-2016) are derived by scaling the plumes with associated national emission sources of SO2 and NH3. Experiments using MACv2-SP are performed with the Max Planck Institute Earth System Model. The globally and annually averaged instantaneous and effective aerosol radiative forcings are estimated to be -0.6 and -0.5 W m-2, respectively. Forcing from aerosol-cloud interactions (the Twomey effect) offsets the reduction of clear-sky forcing by clouds, so that the net effect of clouds on the aerosol forcing is small; hence, the clear-sky forcing, which is more readily measurable, provides a good estimate of the total aerosol forcing.

Characterization of 3D Cirrus Cloud and Radiation Fields Using ARS/AIRS/MODIS data and its Application to Climate Model

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

Liou, Kuo-Nan; Ou, S. C.; Gu, Y.

During the report period, we have made the following research accomplishments. First, we performed analysis for a number of MODIS scenes comprising of heavy dust events and ice clouds, covering regions of frequent dust outbreaks in East Asia, Middle East, and West Africa, as well as areas associated with long-range dust transports over the Equatorial Tropical Atlantic Ocean. These scenes contain both dust/aerosols and clouds. We collected suitable aerosol/ice-cloud data, correlated ice cloud and aerosol parameters by means of statistical analysis, and interpreted resulting correlation trends based on the physical principles governing cloud microphysics. Aerosol and cloud optical depths andmore » cloud effective particle size inferred from MODIS for selected domains were analyzed from which the parameters including dust aerosol number concentration, ice cloud water path, and ice particle number concentration were subsequently derived. We illustrated that the Twomey (solar albedo) effect can be statistically quantified based on the slope of best-fit straight lines in the correlation study. Analysis of aerosol and cloud retrieval products revealed that for all cases, the region with a larger dust aerosol optical depth is always characterized by a smaller cloud particle size, consistent with the Twomey hypothesis for aerosol-cloud interactions. Second, we developed mean correlation curves with uncertainties associated with small ice-crystal concentration observations for the mean effective ice crystal size (De) and ice water content (IWC) by dividing the atmosphere into three characteristic regions: Tropics cirrus, Midlatitude cirrus, including a temperature classification to improve correlation, and Arctic ice clouds. We illustrated that De has a high correlation with IWC based on theoretical consideration and analysis of thousands of observed ice crystal data obtained from a number of ARM-DOE field campaigns and other experiments. The correlation has the form: ln(De) = a + b ln(IWC) + c ((ln(IWC))2, where a, b, and c are fitting coefficients and are functions of three regions. We demonstrated that this correlation can be effectively incorporated in GCMs and climate models that predict IWC - a significant advance in ice microphysics parameterization for interactive cloud-radiation analysis and feedback. Substantial July mean differences are shown in the OLR (W/m2) and precipitation (mm/day) patterns between UCLA GCM simulations based on Des determined from the De-IWC correlations and the control run using a fixed ice crystal size. Third, in order to improve the computation of spectral radiative transfer processes in the WRF model, we developed a consistent and efficient radiation scheme that can better resolve the spectral bands, determine the cloud optical properties, and provide more reliable and accurate radiative heating fields. In the newly developed radiation module, we have implemented in WRF a modified and improved version referred to as the Fu-Liou-Gu scheme, which includes a combination of delta-four-stream and delta-two-stream approximations for solar and IR flux calculations, respectively. This combination has been proven to be computationally efficient and at the same time to produce a high degree of accuracy. The incorporation of nongray gaseous absorption in multiple scattering atmospheres was based on the correlated k-distribution method. The solar and IR spectra are divided into 6 and 12 bands, respectively, according to the location of absorption bands of H2O, CO2, O3, CH4, N2O, and CFCs. We further included absorption by the water vapor continuum and a number of minor absorbers in the solar spectrum leading to an additional absorption of solar flux in a clear atmosphere on the order of 1-3 W/m2. Additionally, we incorporated the ice microphysics parameterization that includes an interactive mean effective ice crystal size in association with radiation parameterizations. The Fu-Liou-Gu scheme is an ideal tool for the simulation of radiative transfer and ice microphysics within the domain of WRF. It is particularly useful for studying direct and indirect aerosol radiative effects associated with ice cloud formation. The newly implemented radiation module has been demonstrated to work well in WRF and can be effectively used for studies related to cirrus cloud formation and evolution as well as aerosol-cloud-radiation interactions. With the newly implemented radiation scheme, the simulations of cloud cover and ice water path have been improved for cirrus clouds, with a more consistent comparison with the corresponding MODIS observations, especially for optically thin cirrus with an improvement of about 20% in the simulated mean ice water path.« less

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.

Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation

DOE PAGES

Zheng, Y.; Unger, N.; Hodzic, A.; ...

2015-12-08

Globally, secondary organic aerosol (SOA) is mostly formed from emissions of biogenic volatile organic compounds (VOCs) by vegetation, but it can be modified by human activities as demonstrated in recent research. Specifically, nitrogen oxides (NO x = NO + NO 2) have been shown to play a critical role in the chemical formation of low volatility compounds. We have updated the SOA scheme in the global NCAR (National Center for Atmospheric Research) Community Atmospheric Model version 4 with chemistry (CAM4-chem) by implementing a 4-product volatility basis set (VBS) scheme, including NO x-dependent SOA yields and aging parameterizations. Small differences aremore » found for the no-aging VBS and 2-product schemes; large increases in SOA production and the SOA-to-OA ratio are found for the aging scheme. The predicted organic aerosol amounts capture both the magnitude and distribution of US surface annual mean measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network by 50 %, and the simulated vertical profiles are within a factor of 2 compared to aerosol mass spectrometer (AMS) measurements from 13 aircraft-based field campaigns across different regions and seasons. We then perform sensitivity experiments to examine how the SOA loading responds to a 50 % reduction in anthropogenic nitric oxide (NO) emissions in different regions. We find limited SOA reductions of 0.9–5.6, 6.4–12.0 and 0.9–2.8 % for global, southeast US and Amazon NO x perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NO x can be largely attributed to a limited shift in chemical regime, to buffering in chemical pathways (low- and high-NO x pathways, O 3 versus NO 3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.« less

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.

Estimating surface visibility at Hong Kong from ground-based LIDAR, sun photometer and operational MODIS products.

PubMed

Shahzad, Muhammad I; Nichol, Janet E; Wang, Jun; Campbell, James R; Chan, Pak W

2013-09-01

Hong Kong's surface visibility has decreased in recent years due to air pollution from rapid social and economic development in the region. In addition to deteriorating health standards, reduced visibility disrupts routine civil and public operations, most notably transportation and aviation. Regional estimates of visibility solved operationally using available ground and satellite-based estimates of aerosol optical properties and vertical distribution may prove more effective than standard reliance on a few existing surface visibility monitoring stations. Previous studies have demonstrated that such satellite measurements correlate well with near-surface optical properties, despite these sensors do not consider range-resolved information and indirect parameterizations necessary to solve relevant parameters. By expanding such analysis to include vertically resolved aerosol profile information from an autonomous ground-based lidar instrument, this work develops six models for automated assessment of surface visibility. Regional visibility is estimated using co-incident ground-based lidar, sun photometer visibility meter and MODerate-resolution maging Spectroradiometer (MODIS) aerosol optical depth data sets. Using a 355 nm extinction coefficient profile solved from the lidar MODIS AOD (aerosol optical depth) is scaled down to the surface to generate a regional composite depiction of surface visibility. These results demonstrate the potential for applying passive satellite depictions of broad-scale aerosol optical properties together with a ground-based surface lidar and zenith-viewing sun photometer for improving quantitative assessments of visibility in a city such as Hong Kong.

Numerical investigation of the coagulation mixing between dust and hygroscopic aerosol particles and its impacts

NASA Astrophysics Data System (ADS)

Tsai, I.-Chun; Chen, Jen-Ping; Lin, Yi-Chiu; Chung-Kuang Chou, Charles; Chen, Wei-Nai

2015-05-01

A statistical-numerical aerosol parameterization was incorporated into the Community Multiscale Air Quality modeling system to study the coagulation mixing process focusing on a dust storm event that occurred over East Asia. Simulation results show that the coagulation mixing process tends to decrease aerosol mass, surface area, and number concentrations over the dust source areas. Over the downwind oceanic areas, aerosol concentrations generally increased due to enhanced sedimentation as particles became larger upon coagulation. The mixture process can reduce the overall single-scattering albedo by up to 10% as a result of enhanced core with shell absorption by dust and reduction in the number of scattering particles. The enhanced dry deposition speed also altered the vertical distribution. In addition, the ability of aerosol particles to serve as cloud condensation nuclei (CCN) increased from around 107 m-3 to above 109 m-3 over downwind areas because a large amount of mineral dust particles became effective CCN with solute coating, except over the highly polluted areas where multiple collections of hygroscopic particles by dust in effect reduced CCN number. This CCN effect is much stronger for coagulation mixing than by the uptake of sulfuric acid gas on dust, although the nitric acid gas uptake was not investigated. The ability of dust particles to serve as ice nuclei may decrease or increase at low or high subzero temperatures, respectively, due to the switching from deposition nucleation to immersion freezing or haze freezing.

Modeling aerosol surface chemistry and gas-particle interaction kinetics with K2-SURF: PAH oxidation

NASA Astrophysics Data System (ADS)

Shiraiwa, M.; Garland, R.; Pöschl, U.

2009-04-01

Atmospheric aerosols are ubiquitous in the atmosphere. They have the ability to impact cloud properties, radiative balance and provide surfaces for heterogeneous reactions. The uptake of gaseous species on aerosol surfaces impacts both the aerosol particles and the atmospheric budget of trace gases. These subsequent changes to the aerosol can in turn impact the aerosol chemical and physical properties. However, this uptake, as well as the impact on the aerosol, is not fully understood. This uncertainty is due not only to limited measurement data, but also a dearth of comprehensive and applicable modeling formalizations used for the analysis, interpretation and description of these heterogeneous processes. Without a common model framework, comparing and extrapolating experimental data is difficult. In this study, a novel kinetic surface model (K2-SURF) [Ammann & Pöschl, 2007; Pöschl et al., 2007] was used to describe the oxidation of a variety of polycyclic aromatic hydrocarbons (PAHs). Integrated into this consistent and universally applicable kinetic and thermodynamic process model are the concepts, terminologies and mathematical formalizations essential to the description of atmospherically relevant physicochemical processes involving organic and mixed organic-inorganic aerosols. Within this process model framework, a detailed master mechanism, simplified mechanism and parameterizations of atmospheric aerosol chemistry are being developed and integrated in analogy to existing mechanisms and parameterizations of atmospheric gas-phase chemistry. One of the key aspects to this model is the defining of a clear distinction between various layers of the particle and surrounding gas phase. The processes occurring at each layer can be fully described using known fluxes and kinetic parameters. Using this system there is a clear separation of gas phase, gas-surface and surface bulk transport and reactions. The partitioning of compounds can be calculated using the flux values between the layers. By describing these layers unambiguously, the interactions of all species in the system can be appropriately modeled. In describing the oxidation of PAHs, the focus was on the interactions between the sorption layer and quasi-static surface layer. The results from a variety of published experimental studies [Pöschl et al., 2001; Kahan et al., 2006; Kwamena et al., 2004, 2006, 2007; Mmereki and Donaldson, 2003; Mmereki et al., 2004; Dubowski et al., 2004; Donaldson et al., 2005; Segal-Rosenheimer and Dubowski, 2007] were analyzed and compared utilizing K2-SURF. The heterogeneous reaction of PAH and O3 are found to follow a Langmuir-Hinshelwood mechanism, in which ozone first absorbs to the surface and then reacts with PAH. The Langmuir equilibrium constants and second-order-rate coefficients of surface reaction were estimated. In PAH/O3/solid substrate system, they showed similar reaction rate (×10), but large difference (×1000) in adsorption. The mean residence time and adsorption enthalpy were estimated for O3 at the surface of substrates, suggesting the chemisorption of O3 molecules or O atoms, respectively. Initial uptake coefficients of O3 under different conditions were also investigated. The observed dependence on gas-phase O3 concentration was well explained with K2-SURF model in five-order range. In addition, competitive adsorption of other gas phase species (NO2, H2O) was well described by the model. Possible mechanism of PAH degradation system and atmospheric implications are discussed.

Harmful and favourable ultraviolet conditions for human health over Northern Eurasia

NASA Astrophysics Data System (ADS)

Chubarova, Nataly; Zhdanova, Ekaterina

2014-05-01

We provide the analysis of the spatial and temporal distribution of ultraviolet (UV) radiation over Northern Eurasia taking into account for both its detrimental (erythema and eye-damage effects) and favourable (vitamin D synthesis) influence on human health. The UV effects on six different skin types are considered in order to cover the variety of skin types of European and Asian inhabitants. To better quantifying the vitamin D irradiance threshold we accounted for an open body fraction S as a function of effective air temperature. The spatial and temporal distribution of UV resources was estimated by radiative transfer (RT) modeling (8 stream DISORT RT code) with 1x 1 degree grid and monthly resolution. For this purpose special datasets of main input geophysical parameters (total ozone content, aerosol characteristics, surface UV albedo, UV cloud modification factor) have been created over the territory of Northern Eurasia, which can be of separate interest for the different multidisciplinary scientific applications over the PEEX domain. The new approaches were used to retrieve aerosol and cloud transmittance from different satellite and re-analysis datasets for calculating the solar UV irradiance at ground. Using model simulations and some experimental data we provide the altitude parameterization for different types of biologically active irradiance in mountainous area taking into account not only for the effects of molecular scattering but for the altitude dependence of aerosol parameters and surface albedo. Based on the new classification of UV resources (Chubarova, Zhdanova, 2013) we show that the distribution of harmful (UV deficiency and UV excess) and favorable UV conditions is regulated by various geophysical parameters (mainly, total ozone, cloudiness and open body fraction) and can significantly deviate from latitudinal dependence. The interactive tool for providing simulations of biologically active irradiance and its attribution to the different classes of UV resources is demonstrated. Reference: Natalia Chubarova, Yekaterina Zhdanova. Ultraviolet resources over Northern Eurasia, Photochemistry and Photobiology, Elsevier, 127, 2013, p. 38-51

NOAA's National Air Quality Prediction and Development of Aerosol and Atmospheric Composition Prediction Components for NGGPS

NASA Astrophysics Data System (ADS)

Stajner, I.; McQueen, J.; Lee, P.; Stein, A. F.; Wilczak, J. M.; Upadhayay, S.; daSilva, A.; Lu, C. H.; Grell, G. A.; Pierce, R. B.

2017-12-01

NOAA's operational air quality predictions of ozone, fine particulate matter (PM2.5) and wildfire smoke over the United States and airborne dust over the contiguous 48 states are distributed at http://airquality.weather.gov. The National Air Quality Forecast Capability (NAQFC) providing these predictions was updated in June 2017. Ozone and PM2.5 predictions are now produced using the system linking the Community Multiscale Air Quality model (CMAQ) version 5.0.2 with meteorological inputs from the North American Mesoscale Forecast System (NAM) version 4. Predictions of PM2.5 include intermittent dust emissions and wildfire emissions from an updated version of BlueSky system. For the latter, the CMAQ system is initialized by rerunning it over the previous 24 hours to include wildfire emissions at the time when they were observed from the satellites. Post processing to reduce the bias in PM2.5 prediction was updated using the Kalman filter analog (KFAN) technique. Dust related aerosol species at the CMAQ domain lateral boundaries now come from the NEMS Global Aerosol Component (NGAC) v2 predictions. Further development of NAQFC includes testing of CMAQ predictions to 72 hours, Canadian fire emissions data from Environment and Climate Change Canada (ECCC) and the KFAN technique to reduce bias in ozone predictions. NOAA is developing the Next Generation Global Predictions System (NGGPS) with an aerosol and gaseous atmospheric composition component to improve and integrate aerosol and ozone predictions and evaluate their impacts on physics, data assimilation and weather prediction. Efforts are underway to improve cloud microphysics, investigate aerosol effects and include representations of atmospheric composition of varying complexity into NGGPS: from the operational ozone parameterization, GOCART aerosols, with simplified ozone chemistry, to CMAQ chemistry with aerosol modules. We will present progress on community building, planning and development of NGGPS.

In situ measurements of the photochemical formation rates and optical properties of organic aerosols in CH4/CO2 mixtures.

NASA Astrophysics Data System (ADS)

Adamkovics, M.; Boering, K. A.

2003-12-01

The presence of photochemically-generated hazes has a significant impact on radiative transfer in planetary atmospheres. While the rates of particle formation have been inferred from photochemical or microphysical models constrained to match observations, these rates have not been determined experimentally. Thus, the fundamental kinetics of particle formation are not known and remain highly parameterized in planetary atmospheric models. We have developed instrumentation for measuring the formation rates and optical properties of organic aerosols produced by irradiating mixtures of precursor gases via in situ optical (633nm) scattering and online quadrupole mass spectrometry (1-200 amu). Results for the generation of particulate hydrocarbons from the irradiation of pure, gas-phase CH4 as well as CH4/CO2 mixtures with vacuum ultraviolet (120-160nm) light, along with simultaneous measurements of the evolution of higher gas-phase hydrocarbons will be presented.

The Impact of Different Complexity on Numerical Weather Predictions within the Coupled Global Online Modeling System

NASA Astrophysics Data System (ADS)

Zhang, L.; Grell, G. A.; McKeen, S. A.; Ahmadov, R.

2017-12-01

The global Flow-following finite-volume Icosahedra Model (FIM), which was developed in the Global Systems Division of NOAA/ESRL and the Finite-volume cubed-sphere dynamical core (FV3) developed by GFDL, have been coupled online with aerosol and gas-phase chemistry schemes (FIM-Chem and FV3-Chem). Within the aerosol and chemistry modules, the models handle wet and dry deposition, chemical reactions, aerosol direct and semi-direct effect, anthropogenic emissions, biogenic emissions, biomass burning, dust and sea-salt emissions. They are able to provide chemical weather predictions at various spatial resolutions and with different levels of complexity. FIM-Chem is also able to quantify the impact of aerosol on numerical weather predictions (NWP). Currently, three different chemical schemes have been coupled with the FIM model. The simplest aerosol modules are from the GOCART model with its simplified parameterization of sulfur/sulfate chemistry. The photochemical gas-phase mechanism RACM was included to determine the impact of additional complexity on the aerosol and gas simulations. We have also implemented a more sophisticated aerosol scheme that includes secondary organic aerosols (SOA) based on the VBS approach. The model performance has been evaluated by comparing with the ATom-1 observations. FIM-Chem is able to reproduce many observed aerosol and gas features very well. A five-day NWP on 120 km horizontal resolution using FIM-Chem has been done for the end of July, 2016 to quantify the impact of the three different chemical schemes on weather forecasts. Compared to a meteorological run that excludes the model chemical schemes, and is driven only by background AODs from the GFS model, the 5-day forecast results shows significant impact on weather predictions when including the prognostic aerosol schemes. This includes convective precipitation, surface temperature, and 700 hPa air temperature. We also use FIM-Chem to investigate the 2012 South American Biomass Burning Analysis (SAMBBA) campaign period to determine whether more complex chemistry provides benefits for global numerical weather prediction.

MACv2-SP: a parameterization of anthropogenic aerosol optical properties and an associated Twomey effect for use in CMIP6

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

Stevens, Bjorn; Fiedler, Stephanie; Kinne, Stefan

A simple plume implementation of the second version (v2) of the Max Planck Institute Aerosol Climatology, MACv2-SP, is described. MACv2-SP provides a prescription of anthropogenic aerosol optical properties and an associated Twomey effect. It was created to provide a harmonized description of post-1850 anthropogenic aerosol radiative forcing for climate modeling studies. MACv2-SP has been designed to be easy to implement, change and use, and thereby enable studies exploring the climatic effects of different patterns of aerosol radiative forcing, including a Twomey effect. MACv2-SP is formulated in terms of nine spatial plumes associated with different major anthropogenic source regions. The shapemore » of the plumes is fit to the Max Planck Institute Aerosol Climatology, version 2, whose present-day (2005) distribution is anchored by surface-based observations. Two types of plumes are considered: one predominantly associated with biomass burning, the other with industrial emissions. These differ in the prescription of their annual cycle and in their optical properties, thereby implicitly accounting for different contributions of absorbing aerosol to the different plumes. A Twomey effect for each plume is prescribed as a change in the host model's background cloud-droplet population density using relationships derived from satellite data. Year-to-year variations in the amplitude of the plumes over the historical period (1850–2016) are derived by scaling the plumes with associated national emission sources of SO 2 and NH 3. Experiments using MACv2-SP are performed with the Max Planck Institute Earth System Model. The globally and annually averaged instantaneous and effective aerosol radiative forcings are estimated to be -0.6 and -0.5 W m -2, respectively. Forcing from aerosol–cloud interactions (the Twomey effect) offsets the reduction of clear-sky forcing by clouds, so that the net effect of clouds on the aerosol forcing is small; hence, the clear-sky forcing, which is more readily measurable, provides a good estimate of the total aerosol forcing.« less

Implementing a warm cloud microphysics parameterization for convective clouds in NCAR CESM

NASA Astrophysics Data System (ADS)

Shiu, C.; Chen, Y.; Chen, W.; Li, J. F.; Tsai, I.; Chen, J.; Hsu, H.

2013-12-01

Most of cumulus convection schemes use simple empirical approaches to convert cloud liquid mass to rain water or cloud ice to snow e.g. using a constant autoconversion rate and dividing cloud liquid mass into cloud water and ice as function of air temperature (e.g. Zhang and McFarlane scheme in NCAR CAM model). There are few studies trying to use cloud microphysical schemes to better simulate such precipitation processes in the convective schemes of global models (e.g. Lohmann [2008] and Song, Zhang, and Li [2012]). A two-moment warm cloud parameterization (i.e. Chen and Liu [2004]) is implemented into the deep convection scheme of CAM5.2 of CESM model for treatment of conversion of cloud liquid water to rain water. Short-term AMIP type global simulations are conducted to evaluate the possible impacts from the modification of this physical parameterization. Simulated results are further compared to observational results from AMWG diagnostic package and CloudSAT data sets. Several sensitivity tests regarding to changes in cloud top droplet concentration (here as a rough testing for aerosol indirect effects) and changes in detrained cloud size of convective cloud ice are also carried out to understand their possible impacts on the cloud and precipitation simulations.

Sensitivity analysis with the regional climate model COSMO-CLM over the CORDEX-MENA domain

NASA Astrophysics Data System (ADS)

Bucchignani, E.; Cattaneo, L.; Panitz, H.-J.; Mercogliano, P.

2016-02-01

The results of a sensitivity work based on ERA-Interim driven COSMO-CLM simulations over the Middle East-North Africa (CORDEX-MENA) domain are presented. All simulations were performed at 0.44° spatial resolution. The purpose of this study was to ascertain model performances with respect to changes in physical and tuning parameters which are mainly related to surface, convection, radiation and cloud parameterizations. Evaluation was performed for the whole CORDEX-MENA region and six sub-regions, comparing a set of 26 COSMO-CLM runs against a combination of available ground observations, satellite products and reanalysis data to assess temperature, precipitation, cloud cover and mean sea level pressure. The model proved to be very sensitive to changes in physical parameters. The optimized configuration allows COSMO-CLM to improve the simulated main climate features of this area. Its main characteristics consist in the new parameterization of albedo, based on Moderate Resolution Imaging Spectroradiometer data, and the new parameterization of aerosol, based on NASA-GISS AOD distributions. When applying this configuration, Mean Absolute Error values for the considered variables are as follows: about 1.2 °C for temperature, about 15 mm/month for precipitation, about 9 % for total cloud cover, and about 0.6 hPa for mean sea level pressure.

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

NASA Astrophysics Data System (ADS)

Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; Zhou, Shan; Zhang, Xiaolu; Cappa, Christopher D.; Seco, Roger; Kim, Saewung; Zhang, Qi

2016-05-01

The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno-Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 µg m-3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C = 0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O / C = 0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C = 0.33; BBOA2: 20 % of total OA, O / C = 0.60) most likely associated with residential space heating from wood combustion, and semivolatile oxygenated OA (SV-OOA; 16 % of total OA, O / C = 0.63) and low-volatility oxygenated OA (LV-OOA; 24 % of total OA, O / C = 0.90) formed via chemical reactions in the atmosphere. Large differences in aerosol chemistry at Fresno were observed between the current campaign (winter 2013) and a previous campaign in winter 2010, most notably that PM1 concentrations were nearly 3 times higher in 2013 than in 2010. These variations were attributed to differences in the meteorological conditions, which influenced primary emissions and secondary aerosol formation. In particular, COA and BBOA concentrations were greater in 2013 than 2010, where colder temperatures in 2013 likely resulted in increased biomass burning activities. The influence from a nighttime formed residual layer that mixed down in the morning was found to be much more intense in 2013 than 2010, leading to sharp increases in ground-level concentrations of secondary aerosol species including nitrate, sulfate, and OOA, in the morning between 08:00 and 12:00 PST. This is an indication that nighttime chemical reactions may have played a more important role in 2013. As solar radiation was stronger in 2013 the higher nitrate and OOA concentrations in 2013 could also be partly due to greater photochemical production of secondary aerosol species. The greater solar radiation and larger range in temperature in 2013 also likely led to both SV-OOA and LV-OOA being observed in 2013 whereas only a single OOA factor was identified in 2010.

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

NASA Astrophysics Data System (ADS)

Young, D. E.; Kim, H.; Parworth, C.; Zhou, S.; Zhang, X.; Cappa, C. D.; Seco, R.; Kim, S.; Zhang, Q.

2015-12-01

The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models.

Response of different regional online coupled models to aerosol-radiation interactions

NASA Astrophysics Data System (ADS)

Forkel, Renate; Balzarini, Alessandra; Brunner, Dominik; Baró, Rocio; Curci, Gabriele; Hirtl, Marcus; Honzak, Luka; Jiménez-Guerrero, Pedro; Jorba, Oriol; Pérez, Juan L.; Pirovano, Guido; San José, Roberto; Schröder, Wolfram; Tuccella, Paolo; Werhahn, Johannes; Wolke, Ralf; Žabkar, Rahela

2016-04-01

The importance of aerosol-meteorology interactions and their representation in online coupled regional atmospheric chemistry-meteorology models was investigated in COST Action ES1004 (EuMetChem, http://eumetchem.info/). Case study results from different models (COSMO-Muscat, COSMO-ART, and different configurations of WRF-Chem), which were applied for Europe as a coordinated exercise for the year 2010, are analyzed with respect to inter-model variability and the response of the different models to direct and indirect aerosol-radiation interactions. The main focus was on two episodes - the Russian heat wave and wildfires episode in July/August 2010 and a period in October 2010 with enhanced cloud cover and rain and including an of Saharan dust transport to Europe. Looking at physical plausibility the decrease in downward solar radiation and daytime temperature due to the direct aerosol effect is robust for all model configurations. The same holds for the pronounced decrease in cloud water content and increase in solar radiation for cloudy conditions and very low aerosol concentrations that was found for WRF-Chem when aerosol cloud interactions were considered. However, when the differences were tested for statistical significance no significant differences in mean solar radiation and mean temperature between the baseline case and the simulations including the direct and indirect effect from simulated aerosol concentrations were found over Europe for the October episode. Also for the fire episode differences between mean temperature and radiation from the simulations with and without the direct aerosol effect were not significant for the major part of the modelling domain. Only for the region with high fire emissions in Russia, the differences in mean solar radiation and temperature due to the direct effect were found to be significant during the second half of the fire episode - however only for a significance level of 0.1. The few observational data indicate that the inclusion of aerosol radiative effects improves simulated temperatures in this area. In summary, the direct aerosol effect leads to lower temperatures and PBL heights for all seasons whereas the impact of the aerosol indirect effect on temperature and pollutant concentrations over Northern Europe was found to depend strongly on the season. It cannot be generalized whether the inclusion of aerosol radiative effects and aerosol cloud interactions based on simulated aerosol concentrations does improve the simulation results. Furthermore, assumptions how aerosol optical properties are calculated, i.e. on the aerosol's mixing state have a strong effect on simulated aerosol optical depth and the aerosol effect on incoming solar radiation and temperature. The inter-model variation of the response of different online coupled models suggests that further work comparing the methodologies and parameterizations used to represent the direct and indirect aerosol effect in these models is still necessary.

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

Matsui, H.; Koike, Makoto; Takegawa, Nobuyuki

The new particle formation (NPF)-explicit version of the WRF-chem model, which we developed recently, can calculate the growth and sink of nucleated clusters explicitly with 20 aerosol size bins from 1 nm to 10 μm. In this study, the model is used to understand spatial and temporal variations of the frequency of NPF events and the concentrations of aerosols (condensation nuclei, CN) and cloud condensation nuclei (CCN) within the boundary layer in East Asia in spring 2009. Model simulations show distinct north-south contrast in the frequency and mechanism of NPF in East Asia. NPF mostly occurred over limited periods andmore » regions between 30° and 45°N, such as northeast China, Korea, and Japan, including regions around active volcanoes (Miyakejima and Sakurajima). At these latitudes, NPF was considerably suppressed by high concentrations of preexisting particles under stagnant air conditions associated with high-pressure systems, while nucleation occurred more extensively on most days during the simulation period. Conversely, neither nucleation nor NPF occurred frequently south of 30°N because of lower SO2 emissions and H2SO4 concentrations. The period-averaged NPF frequency was 3 times higher at latitudes of 30° - 45°N than at latitudes of 20° - 30°N. The north-south contrast of NPF frequency is validated by surface measurements in outflow regions in East Asia. The period- and domain-averaged contribution of secondary particles is estimated to be 44% for CN (> 10 nm) and 26% for CCN at a supersaturation of 1.0% in our simulation, though the contribution is highly sensitive to the magnitudes and size distributions of primary aerosol emissions and the coefficients in the nucleation parameterizations.« less

Influence of Humidity on the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

NASA Technical Reports Server (NTRS)

Gasso, B. S.; Hegg, D. A.; Covert, D. S.; Collins, D.; Noone, K.; Oestroem, E.; Schmid, B.; Russell, P. B.; Livingston, J. M.; Durkee, P. A.;

Long term measurements of the estimated hygroscopic enhancement of aerosol optical properties

NASA Astrophysics Data System (ADS)

Hervo, Maxime; Sellegri, Karine; Pichon, Jean Marc; Roger, Jean Claude; Laj, Paolo

2015-04-01

Water vapour has a major impact on aerosol optical properties, thus on the Radiative Forcing for aerosol-radiation interaction (RFari). However there is few studies measuring this impact over a large period. Optical properties of aerosols were measured at the GAW Puy de Dôme station (1465m) over a seven year period (2006-2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010-2011). The analysis of the spatial and temporal variability of the dry optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the planetary boundary layer height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type and the season. At 90% humidity, the scattering factor enhancement (fsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH= 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type. To our knowledge, these results are one of the first presenting the impact of water vapour on the aerosol optical properties for a long period, and the first for a site at the border between the planetary boundary layer and the free troposphere. Acknowledgements. The authors would like to acknowledge the OPGC and its staff and INSU/CNRS for their contribution to establishing and maintaining the PdD measurement site. This work was performed in the frame of the european EUSAAR (R113-CT-2006-026140) and EUCAARI (0136833-2) and the french ORAURE SOERE.

A parallel direct numerical simulation of dust particles in a turbulent flow

NASA Astrophysics Data System (ADS)

Nguyen, H. V.; Yokota, R.; Stenchikov, G.; Kocurek, G.

2012-04-01

Due to their effects on radiation transport, aerosols play an important role in the global climate. Mineral dust aerosol is a predominant natural aerosol in the desert and semi-desert regions of the Middle East and North Africa (MENA). The Arabian Peninsula is one of the three predominant source regions on the planet "exporting" dust to almost the entire world. Mineral dust aerosols make up about 50% of the tropospheric aerosol mass and therefore produces a significant impact on the Earth's climate and the atmospheric environment, especially in the MENA region that is characterized by frequent dust storms and large aerosol generation. Understanding the mechanisms of dust emission, transport and deposition is therefore essential for correctly representing dust in numerical climate prediction. In this study we present results of numerical simulations of dust particles in a turbulent flow to study the interaction between dust and the atmosphere. Homogenous and passive dust particles in the boundary layers are entrained and advected under the influence of a turbulent flow. Currently no interactions between particles are included. Turbulence is resolved through direct numerical simulation using a parallel incompressible Navier-Stokes flow solver. Model output provides information on particle trajectories, turbulent transport of dust and effects of gravity on dust motion, which will be used to compare with the wind tunnel experiments at University of Texas at Austin. Results of testing of parallel efficiency and scalability is provided. Future versions of the model will include air-particle momentum exchanges, varying particle sizes and saltation effect. The results will be used for interpreting wind tunnel and field experiments and for improvement of dust generation parameterizations in meteorological models.

Simulation of a severe convective storm using a numerical model with explicitly incorporated aerosols

NASA Astrophysics Data System (ADS)

Lompar, Miloš; Ćurić, Mladjen; Romanic, Djordje

2017-09-01

Despite an important role the aerosols play in all stages of cloud lifecycle, their representation in numerical weather prediction models is often rather crude. This paper investigates the effects the explicit versus implicit inclusion of aerosols in a microphysics parameterization scheme in Weather Research and Forecasting (WRF) - Advanced Research WRF (WRF-ARW) model has on cloud dynamics and microphysics. The testbed selected for this study is a severe mesoscale convective system with supercells that struck west and central parts of Serbia in the afternoon of July 21, 2014. Numerical products of two model runs, i.e. one with aerosols explicitly (WRF-AE) included and another with aerosols implicitly (WRF-AI) assumed, are compared against precipitation measurements from surface network of rain gauges, as well as against radar and satellite observations. The WRF-AE model accurately captured the transportation of dust from the north Africa over the Mediterranean and to the Balkan region. On smaller scales, both models displaced the locations of clouds situated above west and central Serbia towards southeast and under-predicted the maximum values of composite radar reflectivity. Similar to satellite images, WRF-AE shows the mesoscale convective system as a merged cluster of cumulonimbus clouds. Both models over-predicted the precipitation amounts; WRF-AE over-predictions are particularly pronounced in the zones of light rain, while WRF-AI gave larger outliers. Unlike WRF-AI, the WRF-AE approach enables the modelling of time evolution and influx of aerosols into the cloud which could be of practical importance in weather forecasting and weather modification. Several likely causes for discrepancies between models and observations are discussed and prospects for further research in this field are outlined.

The DRAGON scale concept and results for remote sensing of aerosol properties

NASA Astrophysics Data System (ADS)

Holben, B. N.; Eck, T. F.; Schafer, J.; Giles, D. M.; Kim, J.; Sano, I.; Mukai, S.; Kim, Y. J.; Reid, J. S.; Pickering, K. E.; Crawford, J. H.; Smirnov, A.; Sinyuk, A.; Slutsker, I.; Sorokin, M.; Rodriguez, J.; Liew, S.; Trevino, N.; Lim, H.; Lefer, B. L.; Nadkarni, R.; Macke, A.; Kinne, S. A.; Anderson, B. E.; Russell, P. B.; Maring, H. B.; Welton, E. J.; da Silva, A.; Toon, O. B.; Redemann, J.

2013-12-01

Aerosol processes occur at microscales but are typically observed and reported at continental to global scales. Often observable aerosol processes that have significant anthropogenic impact occur on spatial scales of tens to a few hundred km, representative of convective cloud processing, urban/megacity sources, anthropogenic burning and natural wildfires, dry lakebed dust sources etc. Historically remote sensing of aerosols has relied on relatively coarse temporal and spatial resolution satellite observations or high temporal resolution point observations from ground-based monitoring sites from networks such as AERONET, SKYNET, MPLNET and many other surface observation platforms. Airborne remote and in situ observations combined with assimilation models were/are to be the mesoscale link between the ground- and space-based RS scales. However clearly the in situ and ground-based RS characterizations of aerosols require a convergence of thought, parameterization and actual scale measurements in order to advance this goal. This has been served by periodic multidisciplinary field campaigns yet only recently has a concerted effort been made to establish these ground-based networks in an effort to capture the mesoscale processes through measurement programs such as DISCOVER AQ and NASA AERONET's effort to foster such measurements and analysis through the Distributed Regional Aerosol Gridded Observation Networks (DRAGON), short term meso-networks, with partners in Asia and Europe and N. America. This talk will review the historical need for such networks and discuss some of the results and in some cases unexpected findings from the eight DRAGON campaigns conducted the last several years. Emphasis will be placed on the most recent DISCOVER AQ campaign conducted in Houston TX and the synergism with a regional to global network plan through the SEAC4RS US campaign.

Characterizing the Asian Tropopause Aerosol Layer using in situ balloon measurements: the BATAL campaigns of 2014-2017

NASA Astrophysics Data System (ADS)

Fairlie, T. D.; Vernier, J. P.; Deshler, T.; Pandit, A. K.; Ratnam, M. V.; Gadhavi, H. S.; Liu, H.; Natarajan, M.; Jayaraman, A.; Kumar, S.; Singh, A. K.; Stenchikov, G. L.; Wienhold, F.; Vignelles, D.; Bedka, K. M.; Avery, M. A.

2017-12-01

We present in situ balloon observations of the Asian Tropopause Aerosol Layer (ATAL), a summertime accumulation of aerosols in the upper troposphere and lower stratosphere (UTLS), associated with Asian Summer Monsoon (ASM). The ATAL was first revealed by CALIPSO satellite data, and has been linked with deep convection of boundary layer pollution into the UTLS. The ATAL has potential implications for regional cloud properties, radiative transfer, and chemical processes in the UTLS. The "Balloon measurements of the Asian Tropopause Aerosol Layer (BATAL)" field campaigns to India and Saudi Arabia in were designed to characterize the physical and optical properties of the ATAL, to explore its composition, and its relationship with clouds in the UTLS. We launched 55 balloon flights from 4 locations, in summers 2014-2016. We return to India to make more balloon flights in summer 2017. Balloon payloads range from 500g to 50 kg, making measurements of meteorological parameters, ozone, water vapor, aerosol optical properties, concentration, volatility, and composition in the UTLS region. This project represents the most important effort to date to study UTLS aerosols during the ASM, given few in situ observations. We complement the in situ data presented with 3-d chemical transport simulations, designed to further explore the ATAL's chemical composition, the sensitivity of such to scavenging in parameterized deep convection, and the relative contribution of regional vs. rest-of-the-world pollution sources. The BATAL project has been a successful partnership between institutes in the US, India, Saudi Arabia, and Europe, and continues for the next 3-4 years, sponsored by the NASA Upper Atmosphere Research program. This partnership may provide a foundation for potential high-altitude airborne measurement studies during the ASM in the future.

Trace Gas/Aerosol Interactions and GMI Modeling Support

NASA Technical Reports Server (NTRS)

Penner, Joyce E.; Liu, Xiaohong; Das, Bigyani; Bergmann, Dan; Rodriquez, Jose M.; Strahan, Susan; Wang, Minghuai; Feng, Yan

2005-01-01

Current global aerosol models use different physical and chemical schemes and parameters, different meteorological fields, and often different emission sources. Since the physical and chemical parameterization schemes are often tuned to obtain results that are consistent with observations, it is difficult to assess the true uncertainty due to meteorology alone. Under the framework of the NASA global modeling initiative (GMI), the differences and uncertainties in aerosol simulations (for sulfate, organic carbon, black carbon, dust and sea salt) solely due to different meteorological fields are analyzed and quantified. Three meteorological datasets available from the NASA DAO GCM, the GISS-II' GCM, and the NASA finite volume GCM (FVGCM) are used to drive the same aerosol model. The global sulfate and mineral dust burdens with FVGCM fields are 40% and 20% less than those with DAO and GISS fields, respectively due to its heavier rainfall. Meanwhile, the sea salt burden predicted with FVGCM fields is 56% and 43% higher than those with DAO and GISS, respectively, due to its stronger convection especially over the Southern Hemispheric Ocean. Sulfate concentrations at the surface in the Northern Hemisphere extratropics and in the middle to upper troposphere differ by more than a factor of 3 between the three meteorological datasets. The agreement between model calculated and observed aerosol concentrations in the industrial regions (e.g., North America and Europe) is quite similar for all three meteorological datasets. Away from the source regions, however, the comparisons with observations differ greatly for DAO, FVGCM and GISS, and the performance of the model using different datasets varies largely depending on sites and species. Global annual average aerosol optical depth at 550 nm is 0.120-0.131 for the three meteorological datasets.

Regional aerosol trends over the North Atlantic Ocean since 2002: identifying and attributing using satellite, surface, and model datasets

NASA Astrophysics Data System (ADS)

Jongeward, A.; Li, Z.

2017-12-01

Aerosols from natural and anthropogenic sources can influence atmospheric variability and alter Earth's radiative balance through direct and indirect processes. Recently, policies targeting anthropogenic species (e.g. the Clean Air Act) have seen success in improving air quality. The anthropogenic contributions to the total aerosol loading and its spatiotemporal pattern/trend are anticipated to be altered. In this work the aerosol loading and trend over the North Atlantic Ocean since 2002 are examined, a period of significant change due to anthropogenic emissions control measures within the U.S. Monthly mean data from satellite (MODIS), ground (AERONET, IMPROVE), and model (GOCART, MERRA) sources are employed. Two annual trends in aerosol optical depth (AOD) observed by MODIS are present: a -0.020 decade-1 trend in the mid-latitudes and a 0.015 decade-1 trend in the sub-tropics. Trends in GOCART species AOD reveal anthropogenic (natural) species as the likely driver of the mid-latitude (sub-tropical) trend. AERONET AOD trends confirm negative AOD trends at three upwind sites in the Eastern U.S. and IMPROVE particulate matter (PM) observations identifies the role of decreasing ammonium sulfate in the overall PM decrease. Meanwhile, an increasing AOD trend seen during summertime in the eastern sub-tropics is associated with dust aerosol from North Africa. A dust parameterization from Kaufman et al. (2005) allows for changes in the flux transport across the sub-tropics to be calculated and analyzed. Using MERRA reanalysis fields, it is hypothesized that amplified warming and increases in baroclinic instability over the Saharan desert may lead to increased dust mobilization and export from North Africa to the sub-tropical Atlantic. This study provides updated analysis through 2016.

Modeling the formation and aging of secondary organic aerosols during CalNex 2010

NASA Astrophysics Data System (ADS)

Hayes, P. L.; Ortega, A. M.; Ahmadov, R.; McKeen, S. A.; Washenfelder, R. A.; Alvarez, S.; Rappenglueck, B.; Holloway, J. S.; Gilman, J. B.; Kuster, W. C.; De Gouw, J. A.; Zotter, P.; Prevot, A. S.; Kleindienst, T. E.; Offenberg, J. H.; Jimenez, J. L.

2012-12-01

Several traditional and recently proposed models are applied to predict the concentrations and properties of secondary organic aerosols (SOA) and organic gases at the Pasadena ground site during the CalNex campaign. The models are constrained with and compared against results from available observations. The CalNex campaign and specifically the Pasadena ground site featured a large and sophisticated suite of aerosol and gas phase instrumentation, and thus, it provides a unique opportunity to test SOA models under conditions of strong urban emissions at a range of low photochemical ages. The oxidation of volatile organic compounds (VOCs) using an updated traditional model cannot explain the observed ambient SOA, and under-predicts the measurements by a factor of ~40. Similarly, after accounting for the multi-generation oxidation of VOCs using a volatility basis set (VBS) approach as described by Tsimpidi et al. (2010), SOA is still under-predicted by a factor of ~8. For SOA formed from VOCs (V-SOA) the dominant precursors are aromatics (xylenes, toluene, and trimethylbenzenes). The model SOA formed from the oxidation of primary semivolatile and intermediate volatility organic compounds (P-S/IVOCs, producing SI-SOA) is also predicted using the parameterizations of Robinson et al. (2007) and Grieshop et al. (2009), and the properties of V-SOA + SI-SOA are compared against the measured O:C and volatility. We also compare the results of the different models against fossil/non-fossil carbon measurements as well as tracers of different SOA precursors. Potential Aerosol Mass (PAM) measurements of the SOA forming potential of the Pasadena air masses are also compared against that predicted by the models. The PAM analysis allows for model/measurement comparisons of SOA properties over a range of photochemical ages spanning almost two weeks. Using the V-SOA model, at low photochemical ages (< 1 day) the modeled PAM V-SOA is less than the measured PAM SOA, similar to the ambient results. In contrast, at high photochemical ages (i.e., more than about three days) the modeled PAM V-SOA is substantially greater than that measured, which is likely due fragmentation reactions that are not included in that model. We derive a parameterization of the measured PAM SOA as a function of the input photochemical age and the PAM photochemical age that serves as a comparison with other SOA models.

Performance Analysis of Transposition Models Simulating Solar Radiation on Inclined Surfaces: Preprint

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

Xie, Yu; Sengupta, Manajit

2016-06-01

Transposition models are widely used in the solar energy industry to simulate solar radiation on inclined photovoltaic (PV) panels. These transposition models have been developed using various assumptions about the distribution of the diffuse radiation, and most of the parameterizations in these models have been developed using hourly ground data sets. Numerous studies have compared the performance of transposition models, but this paper aims to understand the quantitative uncertainty in the state-of-the-art transposition models and the sources leading to the uncertainty using high-resolution ground measurements in the plane of array. Our results suggest that the amount of aerosol optical depthmore » can affect the accuracy of isotropic models. The choice of empirical coefficients and the use of decomposition models can both result in uncertainty in the output from the transposition models. It is expected that the results of this study will ultimately lead to improvements of the parameterizations as well as the development of improved physical models.« less

Active Subspaces of Airfoil Shape Parameterizations

NASA Astrophysics Data System (ADS)

Grey, Zachary J.; Constantine, Paul G.

2018-05-01

Design and optimization benefit from understanding the dependence of a quantity of interest (e.g., a design objective or constraint function) on the design variables. A low-dimensional active subspace, when present, identifies important directions in the space of design variables; perturbing a design along the active subspace associated with a particular quantity of interest changes that quantity more, on average, than perturbing the design orthogonally to the active subspace. This low-dimensional structure provides insights that characterize the dependence of quantities of interest on design variables. Airfoil design in a transonic flow field with a parameterized geometry is a popular test problem for design methodologies. We examine two particular airfoil shape parameterizations, PARSEC and CST, and study the active subspaces present in two common design quantities of interest, transonic lift and drag coefficients, under each shape parameterization. We mathematically relate the two parameterizations with a common polynomial series. The active subspaces enable low-dimensional approximations of lift and drag that relate to physical airfoil properties. In particular, we obtain and interpret a two-dimensional approximation of both transonic lift and drag, and we show how these approximation inform a multi-objective design problem.

Transition from Gaseous Compounds to Aerosols in Titan's Atmosphere

NASA Technical Reports Server (NTRS)

Lebonnois, Sebastien; Bakes, E. L. O.; McKay, Christopher P.; DeVincenzi, Donald (Technical Monitor)

2002-01-01

We investigate the chemical transition of simple molecules like C2H2 and HCN into aerosol particles in the context of Titan's atmosphere. Experiments that synthesize analogs (tholins) for these aerosols can help understand and constrain these polymerization mechanisms. Using information available from these experiments, we suggest chemical pathways that can link simple molecules to macromolecules, that will be the precursors to aerosol particles: polymers of acetylene and cyanoacetylene, polycyclic aromatics (PAHs), polymers of HCN and other nitriles, and polynes. Although our goal here is not to build a detailed kinetic model for this transition, we propose parameterizations to estimate the production rates of these macromolecules, their C/N and C/H ratios, and the loss of parent molecules (C2H2, HCN, HC3N and other nitriles, C6H6) from the gas phase to the haze. We use a 1-dimensional photochemical model of Titan's atmosphere to estimate the formation rate of precursors macromolecules. We find a production zone slightly lower than 200 km altitude with a total production rate of 4 x 10(exp -14) g/ sq cm s and a C/N approx. = 4. These results are compared with experimental data, and to microphysical models requirements. The Cassini/Huygens mission will bring a detailed picture of the haze distribution and properties, that will be a great challenge for our understanding of those chemical processes.

Deterministic chaos in atmospheric radon dynamics

NASA Astrophysics Data System (ADS)

Cuculeanu, Vasile; Lupu, Alexandru

2001-08-01

The correlation dimension and Lyapunov exponents have been calculated for two time series of atmospheric radon daughter concentrations obtained from four daily measurements during the period 1993-1996. A number of about 6000 activity concentration values of 222Rn and 220Rn daughters have been used. The measuring method is based on aerosol collection on filters. In order to determine the filter activity, a low background gross beta measuring device with Geiger-Müller counter tubes in anticoincidence was used. The small noninteger value of the correlation dimension (≃2.2) and the existence of a positive Lyapunov exponent prove that deterministic chaos is present in the time series of atmospheric 220Rn daughters. This shows that a simple diffusion equation with a parameterized turbulent diffusion coefficient is insufficient for describing the dynamics in the near-ground layer where turbulence is not fully developed and coherent structures dominate. The analysis of 222Rn series confirms that the dynamics of the boundary layer cannot be described by a system of ordinary differential equations with a low number of independent variables.

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.

A new temperature and humidity dependent surface site density approach for deposition ice nucleation

NASA Astrophysics Data System (ADS)

Steinke, I.; Hoose, C.; Möhler, O.; Connolly, P.; Leisner, T.

2014-07-01

Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol surface area concentration. Additionally, a contact angle parameterization according to classical nucleation theory was fitted to the experimental data in order to relate the ice nucleation efficiencies to contact angle distributions. From this study it can be concluded that the INAS density formulation is a very useful tool to decribe the temperature and humidity dependent ice nucleation efficiency of ATD particles. Deposition nucleation on ATD particles can be described by a temperature and relative humidity dependent INAS density function ns(T, Sice) with ns(xtherm) = 1.88 × 105 \\centerdot exp(0.2659 \\centerdot xtherm) [m-2] (1) where the thermodynamic variable xtherm is defined as xtherm = -(T - 273.2) + (Sice-1) × 100 (2) with Sice>1 and within a temperature range between 226 and 250 K. For lower temperatures, xtherm deviates from a linear behavior with temperature and relative humidity over ice. Two different approaches for describing the time dependence of deposition nucleation initiated by ATD particles are proposed. Box model estimates suggest that the time dependent contribution is only relevant for small cooling rates and low number fractions of ice-active particles.

Broadband optical properties of biomass burning aerosol and identification of brown carbon chromophores

NASA Astrophysics Data System (ADS)

Rudich, Y.; Bluvshtein, N.; Lin, P.; Flores, J. M.; Segey, L.; Tas, E.; Snider, G.; Weagle, C. L. M.; Brown, S. S.; Laskin, J.; Laskin, A.

2017-12-01

Accurate modeling of the radiative effects of smoke aerosols requires wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass burning aerosols from 300 to 650 nm wavelengths during a regional nighttime bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about two orders of magnitude, changing the single scattering albedo from a background level of 0.95 to 0.7. In addition, PM2.5 filter samples were collected for detailed chemical analysis of the water soluble organics that contribute to light absorption. Nitroaromatic compounds were identified as major organic species responsible for the 50-80% of the total visible light absorption (> 400 nm). Typical chromophores include 4-nitrocatechol, 4-nitrophenol, nitro-syringol and nitro-guaiacol; oxidation-nitration products of methoxyphenols, and known products of lignin pyrolysis. Our results suggests that night time chemistry of nitrogen oxides with particles may play a significant role in atmospheric transformations of brown carbon.

The response of a simulated mesoscale convective system to increased aerosol pollution: Part I: Precipitation intensity, distribution, and efficiency

NASA Astrophysics Data System (ADS)

Clavner, Michal; Cotton, William R.; van den Heever, Susan C.; Saleeby, Stephen M.; Pierce, Jeffery R.

2018-01-01

Mesoscale Convective Systems (MCSs) are important contributors to rainfall in the High Plains of the United States and elsewhere in the world. It is therefore of interest to understand how different aerosols serving as cloud condensation nuclei (CCN) may impact the total amount, rates and spatial distribution of precipitation produced by MCSs. In this study, different aerosol concentrations and their effects on precipitation produced by an MCS are examined by simulating the 8 May 2009 "Super-Derecho" MCS using the Regional Atmospheric Modeling System (RAMS), a cloud-resolving model (CRM) with sophisticated aerosol and microphysical parameterizations. Three simulations were conducted that differed only in the initial concentration, spatial distribution, and chemical composition of aerosols. Aerosol fields were derived from the output of GEOS-Chem, a 3D chemical transport numerical model. Results from the RAMS simulations show that the total domain precipitation was not significantly affected by variations in aerosol concentrations, however, the pollution aerosols altered the precipitation characteristics. The more polluted simulations exhibited higher precipitation rates, higher bulk precipitation efficiency, a larger area with heavier precipitation, and a smaller area with lighter precipitation. These differences arose as a result of aerosols enhancing precipitation in the convective region of the MCS while suppressing precipitation from the MCS's stratiform-anvil. In the convective region, several processes likely contributed to an increase of precipitation. First, owing to the very humid environment of this storm, the enhanced amount of cloud water available to be collected overwhelmed the reduction in precipitation efficiency associated with the aerosol-induced production of smaller droplets which led to a net increase in the conversion of cloud droplets to precipitation. Second, higher aerosol concentrations led to invigoration of convective updrafts which enhanced precipitation in accordance to the convective invigoration hypothesis. The reduction in stratiform precipitation in the more polluted simulations was found to be attributed to the presence of greater aerosol number concentrations that reduced both collision-coalescence and riming. Analysis of back trajeocty flow showed that the air feeding the stratiform-anvil originated within the free troposphere, by mesoscale ascent. Therefore, increased aerosol pollution at higher elevations impacted the stratiform precipitation formation within the simulated MCS. As a consequence, the more polluted simulations produced the smallest precipitation from the MCS stratiform-anvil region. In Part II the impact of aerosols on the severe winds produced by this storm is examined.

Aerosol direct radiative effects over the northwest Atlantic, northwest Pacific, and North Indian Oceans: estimates based on in-situ chemical and optical measurements and chemical transport modeling

NASA Astrophysics Data System (ADS)

Bates, T. S.; Anderson, T. L.; Baynard, T.; Bond, T.; Boucher, O.; Carmichael, G.; Clarke, A.; Erlick, C.; Guo, H.; Horowitz, L.; Howell, S.; Kulkarni, S.; Maring, H.; McComiskey, A.; Middlebrook, A.; Noone, K.; O'Dowd, C. D.; Ogren, J.; Penner, J.; Quinn, P. K.; Ravishankara, A. R.; Savoie, D. L.; Schwartz, S. E.; Shinozuka, Y.; Tang, Y.; Weber, R. J.; Wu, Y.

2006-05-01

The largest uncertainty in the radiative forcing of climate change over the industrial era is that due to aerosols, a substantial fraction of which is the uncertainty associated with scattering and absorption of shortwave (solar) radiation by anthropogenic aerosols in cloud-free conditions (IPCC, 2001). Quantifying and reducing the uncertainty in aerosol influences on climate is critical to understanding climate change over the industrial period and to improving predictions of future climate change for assumed emission scenarios. Measurements of aerosol properties during major field campaigns in several regions of the globe during the past decade are contributing to an enhanced understanding of atmospheric aerosols and their effects on light scattering and climate. The present study, which focuses on three regions downwind of major urban/population centers (North Indian Ocean (NIO) during INDOEX, the Northwest Pacific Ocean (NWP) during ACE-Asia, and the Northwest Atlantic Ocean (NWA) during ICARTT), incorporates understanding gained from field observations of aerosol distributions and properties into calculations of perturbations in radiative fluxes due to these aerosols. This study evaluates the current state of observations and of two chemical transport models (STEM and MOZART). Measurements of burdens, extinction optical depth (AOD), and direct radiative effect of aerosols (DRE - change in radiative flux due to total aerosols) are used as measurement-model check points to assess uncertainties. In-situ measured and remotely sensed aerosol properties for each region (mixing state, mass scattering efficiency, single scattering albedo, and angular scattering properties and their dependences on relative humidity) are used as input parameters to two radiative transfer models (GFDL and University of Michigan) to constrain estimates of aerosol radiative effects, with uncertainties in each step propagated through the analysis. Constraining the radiative transfer calculations by observational inputs increases the clear-sky, 24-h averaged AOD (34±8%), top of atmosphere (TOA) DRE (32±12%), and TOA direct climate forcing of aerosols (DCF - change in radiative flux due to anthropogenic aerosols) (37±7%) relative to values obtained with "a priori" parameterizations of aerosol loadings and properties (GFDL RTM). The resulting constrained clear-sky TOA DCF is -3.3±0.47, -14±2.6, -6.4±2.1 Wm-2 for the NIO, NWP, and NWA, respectively. With the use of constrained quantities (extensive and intensive parameters) the calculated uncertainty in DCF was 25% less than the "structural uncertainties" used in the IPCC-2001 global estimates of direct aerosol climate forcing. Such comparisons with observations and resultant reductions in uncertainties are essential for improving and developing confidence in climate model calculations incorporating aerosol forcing.

Application of remote sensing techniques to study aerosol water vapour uptake in a real atmosphere

NASA Astrophysics Data System (ADS)

Fernández, A. J.; Molero, F.; Becerril-Valle, M.; Coz, E.; Salvador, P.; Artíñano, B.; Pujadas, M.

2018-04-01

In this work, a study of several observations of aerosol water uptake in a real (non-controlled) atmosphere, registered by remote sensing techniques, are presented. In particular, three events were identified within the Atmospheric Boundary Layer (ABL) and other two events were detected in the free troposphere (beyond the top of the ABL). Then, aerosol optical properties were measured at different relative humidity (RH) conditions by means of a multi-wavelength (MW) Raman lidar located at CIEMAT (Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas, Research Centre for Energy, Environment and Technology) facilities in Madrid (Spain). Additionally, aerosol optical and microphysical properties provided by automatic sun and sky scanning spectral radiometers (CIMEL CE-318) and a meteorological analysis complement the study. However, a detailed analysis only could be carried out for the cases observed within the ABL since well-mixed atmospheric layers are required to properly characterize these processes. This characterization of aerosol water uptake is based on the curve described by the backscatter coefficient at 532 nm as a function of RH which allows deriving the enhancement factor. Thus, the Hänel parameterization is utilized, and the results obtained are in the range of values reported in previous studies, which shows the suitability of this approach to study such hygroscopic processes. Furthermore, the anti-correlated pattern observed on backscatter-related Ångström exponent (532/355 nm) and RH indicates plausible signs of aerosol hygroscopic growth. According to the meteorological analysis performed, we attribute such hygroscopic behaviour to marine aerosols which are advected from the Atlantic Ocean to the low troposphere in Madrid. We have also observed an interesting response of aerosols to RH at certain levels which it is suggested to be due to a hysteresis process. The events registered in the free troposphere, which deal with volcano and wild fire plumes transported at higher altitudes, indicate that these processes can take place in the free troposphere, where the climate relevance can be rather different considering the role of aerosol as cloud condensation nuclei.

Configuration and Assessment of the GISS ModelE2 Contributions to the CMIP5 Archive

NASA Technical Reports Server (NTRS)

Schmidt, Gavin A.; Kelley, Max; Nazarenko, Larissa; Ruedy, Reto; Russell, Gary L.; Aleinov, Igor; Bauer, Mike; Bauer, Susanne E.; Bhat, Maharaj K.; Bleck, Rainer;

An improved hindcast approach for evaluation and diagnosis of physical processes in global climate models

DOE PAGES

Ma, H. -Y.; Chuang, C. C.; Klein, S. A.; ...

2015-11-06

Here, we present an improved procedure of generating initial conditions (ICs) for climate model hindcast experiments with specified sea surface temperature and sea ice. The motivation is to minimize errors in the ICs and lead to a better evaluation of atmospheric parameterizations' performance in the hindcast mode. We apply state variables (horizontal velocities, temperature and specific humidity) from the operational analysis/reanalysis for the atmospheric initial states. Without a data assimilation system, we apply a two-step process to obtain other necessary variables to initialize both the atmospheric (e.g., aerosols and clouds) and land models (e.g., soil moisture). First, we nudge onlymore » the model horizontal velocities towards operational analysis/reanalysis values, given a 6-hour relaxation time scale, to obtain all necessary variables. Compared to the original strategy in which horizontal velocities, temperature and specific humidity are nudged, the revised approach produces a better representation of initial aerosols and cloud fields which are more consistent and closer to observations and model's preferred climatology. Second, we obtain land ICs from an offline land model simulation forced with observed precipitation, winds, and surface fluxes. This approach produces more realistic soil moisture in the land ICs. With this refined procedure, the simulated precipitation, clouds, radiation, and surface air temperature over land are improved in the Day 2 mean hindcasts. Following this procedure, we propose a “Core” integration suite which provides an easily repeatable test allowing model developers to rapidly assess the impacts of various parameterization changes on the fidelity of modelled cloud-associated processes relative to observations.« less

An improved hindcast approach for evaluation and diagnosis of physical processes in global climate models

NASA Astrophysics Data System (ADS)

Ma, H.-Y.; Chuang, C. C.; Klein, S. A.; Lo, M.-H.; Zhang, Y.; Xie, S.; Zheng, X.; Ma, P.-L.; Zhang, Y.; Phillips, T. J.

2015-12-01

We present an improved procedure of generating initial conditions (ICs) for climate model hindcast experiments with specified sea surface temperature and sea ice. The motivation is to minimize errors in the ICs and lead to a better evaluation of atmospheric parameterizations' performance in the hindcast mode. We apply state variables (horizontal velocities, temperature, and specific humidity) from the operational analysis/reanalysis for the atmospheric initial states. Without a data assimilation system, we apply a two-step process to obtain other necessary variables to initialize both the atmospheric (e.g., aerosols and clouds) and land models (e.g., soil moisture). First, we nudge only the model horizontal velocities toward operational analysis/reanalysis values, given a 6 h relaxation time scale, to obtain all necessary variables. Compared to the original strategy in which horizontal velocities, temperature, and specific humidity are nudged, the revised approach produces a better representation of initial aerosols and cloud fields which are more consistent and closer to observations and model's preferred climatology. Second, we obtain land ICs from an off-line land model simulation forced with observed precipitation, winds, and surface fluxes. This approach produces more realistic soil moisture in the land ICs. With this refined procedure, the simulated precipitation, clouds, radiation, and surface air temperature over land are improved in the Day 2 mean hindcasts. Following this procedure, we propose a "Core" integration suite which provides an easily repeatable test allowing model developers to rapidly assess the impacts of various parameterization changes on the fidelity of modeled cloud-associated processes relative to observations.

Long-term observations of cloud condensation nuclei in the Amazon rain forest

NASA Astrophysics Data System (ADS)

Pöhlker, Mira L.; Pöhlker, Christopher; Ditas, Florian; Klimach, Thomas; Hrabe de Angelis, Isabella; Brito, Joel; Carbone, Samara; Cheng, Yafang; Martin, Scot T.; Moran-Zuloaga, Daniel; Rose, Diana; Saturno, Jorge; Su, Hang; Thalman, Ryan; Walter, David; Wang, Jian; Barbosa, Henrique; Artaxo, Paulo; Andreae, Meinrat O.; Pöschl, Ulrich

2017-04-01

Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in the central Amazon Basin over a full seasonal cycle (Mar 2014 - Feb 2015). The measurements provide a climatology of CCN properties characteristic of a remote central Amazonian rain forest site [1,2]. The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), higher values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol. The hygroscopicity parameter, κ, exhibits remarkably little temporal variability: no pronounced diurnal cycles, only weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes. For modelling purposes, we compare different approaches of predicting CCN number concentration and present a novel parameterization, which allows accurate CCN predictions based on a small set of input data. In addition, we analyzed the CCN short-term variability in relation to air mass changes as well as aerosol emission and transformation processes. The CCN short term variability is presented for selected case studies, which analyze particularly interesting and characteristic events/conditions in the Amazon region. References: [1] Andreae, M. O., et al. (2015), Atmos. Chem. Phys., 15, 10723-10776. [2] Pöhlker, M. L.., et al. (2016), Atmos. Chem. Phys., 16, 15709-15740.

Acidity of Aerosols during Winter Heavy Haze Events in Beijing and Gucheng, China

NASA Astrophysics Data System (ADS)

Chi, Xiyuan; He, Pengzhen; Jiang, Zhuang; Yu, Xiawei; Yue, Fange; Wang, Longquan; Li, Bokun; Kang, Hui; Liu, Cheng; Xie, Zhouqing

2018-02-01

We investigated the acidity and concentrations of water-soluble ions in PM2.5 aerosol samples collected from an urban site in Beijing and a rural site in Gucheng, Hebei Province from November 2016 to January 2017 to gain an insight into the formation of secondary inorganic species. The average SO4 2-, NO3 -, and NH4 + concentrations were 8.3, 12.5, and 14.1 μg m-3, respectively, at the urban site and 14.0, 14.2, and 24.2 μg m-3, respectively, at the rural site. The nitrogen and sulfur oxidation ratios in urban Beijing were correlated with relative humidity (with correlation coefficient r = 0.79 and 0.67, respectively) and the aerosol loadings. Based on a parameterization model, we found that the rate constant of the heterogeneous reactions for SO2 on polluted days was about 10 times higher than that on clear days, suggesting that the heterogeneous reactions in the aerosol water played an essential role in haze events. The ISORROPIA II model was used to predict the aerosol pH, which had a mean (range) of 5.0 (4.9-5.2) and 5.3 (4.6-6.3) at the urban and rural site, respectively. Under the conditions with this predicted pH value, oxidation by dissolved NO2 and the hydrolysis of N2O5 may be the major heterogeneous reactions forming SO4 2- and NO3 - in haze. We also analyzed the sensitivity of the aerosol pH to changes in the concentrations of SO4 2-, NO3 -, and NH4 + under haze conditions. The aerosol pH was more sensitive to the SO4 2- and NH4 + concentrations with opposing trends, than to the NO3 - concentrations. The sensitivity of the pH was relatively weak overall, which was attributed to the buffering effect of NH3 partitioning.

Aerosol direct radiative effects over the northwest Atlantic, northwest Pacific, and North Indian Oceans: estimates based on in-situ chemical and optical measurements and chemical transport modeling

NASA Astrophysics Data System (ADS)

Bates, T. S.; Anderson, T. L.; Baynard, T.; Bond, T.; Boucher, O.; Carmichael, G.; Clarke, A.; Erlick, C.; Guo, H.; Horowitz, L.; Howell, S.; Kulkarni, S.; Maring, H.; McComiskey, A.; Middlebrook, A.; Noone, K.; O'Dowd, C. D.; Ogren, J.; Penner, J.; Quinn, P. K.; Ravishankara, A. R.; Savoie, D. L.; Schwartz, S. E.; Shinozuka, Y.; Tang, Y.; Weber, R. J.; Wu, Y.

2006-01-01

The largest uncertainty in the radiative forcing of climate change over the industrial era is that due to aerosols, a substantial fraction of which is the uncertainty associated with scattering and absorption of shortwave (solar) radiation by anthropogenic aerosols in cloud-free conditions (IPCC, 2001). Quantifying and reducing the uncertainty in aerosol influences on climate is critical to understanding climate change over the industrial period and to improving predictions of future climate change for assumed emission scenarios. Measurements of aerosol properties during major field campaigns in several regions of the globe during the past decade are contributing to an enhanced understanding of atmospheric aerosols and their effects on light scattering and climate. The present study, which focuses on three regions downwind of major urban/population centers (North Indian Ocean (NIO) during INDOEX, the Northwest Pacific Ocean (NWP) during ACE-Asia, and the Northwest Atlantic Ocean (NWA) during ICARTT), incorporates understanding gained from field observations of aerosol distributions and properties into calculations of perturbations in radiative fluxes due to these aerosols. This study evaluates the current state of observations and of two chemical transport models (STEM and MOZART). Measurements of burdens, extinction optical depth (AOD), and direct radiative effect of aerosols (DRE - change in radiative flux due to total aerosols) are used as measurement-model check points to assess uncertainties. In-situ measured and remotely sensed aerosol properties for each region (mixing state, mass scattering efficiency, single scattering albedo, and angular scattering properties and their dependences on relative humidity) are used as input parameters to two radiative transfer models (GFDL and University of Michigan) to constrain estimates of aerosol radiative effects, with uncertainties in each step propagated through the analysis. Constraining the radiative transfer calculations by observational inputs increases the clear-sky, 24-h averaged AOD (34±8%), top of atmosphere (TOA) DRE (32±12%), and TOA direct climate forcing of aerosols (DCF - change in radiative flux due to anthropogenic aerosols) (37±7%) relative to values obtained with "a priori" parameterizations of aerosol loadings and properties (GFDL RTM). The resulting constrained TOA DCF is -3.3±0.47, -14±2.6, -6.4±2.1 Wm-2 for the NIO, NWP, and NWA, respectively. Constraining the radiative transfer calculations by observational inputs reduces the uncertainty range in the DCF in these regions relative to global IPCC (2001) estimates by a factor of approximately 2. Such comparisons with observations and resultant reductions in uncertainties are essential for improving and developing confidence in climate model calculations incorporating aerosol forcing.

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.

Parameterized isoprene and monoterpene emissions from the boreal forest floor: Implementation into a 1D chemistry-transport model and investigation of the influence on atmospheric chemistry

NASA Astrophysics Data System (ADS)

Mogensen, Ditte; Aaltonen, Hermanni; Aalto, Juho; Bäck, Jaana; Kieloaho, Antti-Jussi; Gierens, Rosa; Smolander, Sampo; Kulmala, Markku; Boy, Michael

2015-04-01

Volatile organic compounds (VOCs) are emitted from the biosphere and can work as precursor gases for aerosol particles that can affect the climate (e.g. Makkonen et al., ACP, 2012). VOC emissions from needles and leaves have gained the most attention, however other parts of the ecosystem also have the ability to emit a vast amount of VOCs. This, often neglected, source can be important e.g. at periods where leaves are absent. Both sources and drivers related to forest floor emission of VOCs are currently limited. It is thought that the sources are mainly due to degradation of organic matter (Isidorov and Jdanova, Chemosphere, 2002), living roots (Asensio et al., Soil Biol. Biochem., 2008) and ground vegetation. The drivers are biotic (e.g. microbes) and abiotic (e.g. temperature and moisture). However, the relative importance of the sources and the drivers individually are currently poorly understood. Further, the relative importance of these factors is highly dependent on the tree species occupying the area of interest. The emission of isoprene and monoterpenes where measured from the boreal forest floor at the SMEAR II station in Southern Finland (Hari and Kulmala, Boreal Env. Res., 2005) during the snow-free period in 2010-2012. We used a dynamic method with 3 automated chambers analyzed by Proton Transfer Reaction - Mass Spectrometer (Aaltonen et al., Plant Soil, 2013). Using this data, we have developed empirical parameterizations for the emission of isoprene and monoterpenes from the forest floor. These parameterizations depends on abiotic factors, however, since the parameterizations are based on field measurements, biotic features are captured. Further, we have used the 1D chemistry-transport model SOSAA (Boy et al., ACP, 2011) to test the seasonal relative importance of inclusion of these parameterizations of the forest floor compared to the canopy crown emissions, on the atmospheric reactivity throughout the canopy.

Apparatus for rapid measurement of aerosol bulk chemical composition

DOEpatents

Lee, Yin-Nan E.; Weber, Rodney J.

2003-01-01

An apparatus and method for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution are provided. The apparatus includes a modified particle size magnifier for producing activated aerosol particles and a collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical methods. The method provided for on-line measurement of chemical composition of aerosol particles includes exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

Apparatus for rapid measurement of aerosol bulk chemical composition

DOEpatents

Lee, Yin-Nan E.; Weber, Rodney J.; Orsini, Douglas

2006-04-18

An apparatus for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution is provided. The apparatus includes an enhanced particle size magnifier for producing activated aerosol particles and an enhanced collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical means. Methods for on-line measurement of chemical composition of aerosol particles are also provided, the method including exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; and flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

Aerosols and lightning activity: The effect of vertical profile and aerosol type

NASA Astrophysics Data System (ADS)

Proestakis, E.; Kazadzis, S.; Lagouvardos, K.; Kotroni, V.; Amiridis, V.; Marinou, E.; Price, C.; Kazantzidis, A.

2016-12-01

The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite has been utilized for the first time in a study regarding lightning activity modulation due to aerosols. Lightning activity observations, obtained by the ZEUS long range Lightning Detection Network, European Centre for Medium range Weather Forecasts (ECMWF) Convective Available Potential Energy (CAPE) data and Cloud Fraction (CF) retrieved by MODIS on board Aqua satellite have been combined with CALIPSO CALIOP data over the Mediterranean basin and for the period March to November, from 2007 to 2014. The results indicate that lightning activity is enhanced during days characterized by higher Aerosol Optical Depth (AOD) values, compared to days with no lightning. This study contributes to existing studies on the link between lightning activity and aerosols, which have been based just on columnar AOD satellite retrievals, by performing a deeper analysis into the effect of aerosol profiles and aerosol types. Correlation coefficients of R = 0.73 between the CALIPSO AOD and the number of lightning strikes detected by ZEUS and of R = 0.93 between ECMWF CAPE and lightning activity are obtained. The analysis of extinction coefficient values at 532 nm indicates that at an altitudinal range exists, between 1.1 km and 2.9 km, where the values for extinction coefficient of lightning-active and non-lightning-active cases are statistically significantly different. Finally, based on the CALIPSO aerosol subtype classification, we have investigated the aerosol conditions of lightning-active and non-lightning-active cases. According to the results polluted dust aerosols are more frequently observed during non-lightning-active days, while dust and smoke aerosols are more abundant in the atmosphere during the lightning-active days.

Parameterization retrieval of trace gas volume mixing ratios from Airborne MAX-DOAS

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

Dix, Barbara; Koenig, Theodore K.; Volkamer, Rainer

We present a parameterization retrieval of volume mixing ratios (VMRs) from differential slant column density (dSCD) measurements by Airborne Multi-AXis Differential Optical Absorption Spectroscopy (AMAX-DOAS). The method makes use of the fact that horizontally recorded limb spectra (elevation angle 0°) are strongly sensitive to the atmospheric layer at instrument altitude. These limb spectra are analyzed using reference spectra that largely cancel out column contributions from above and below the instrument, so that the resulting limb dSCDs, i.e., the column integrated concentration with respect to a reference spectrum, are almost exclusively sensitive to the atmospheric layers around instrument altitude. The conversionmore » of limb dSCDs into VMRs is then realized by calculating box air mass factors (Box-AMFs) for a Rayleigh atmosphere and applying a scaling factor constrained by O 4 dSCDs to account for aerosol extinction. An iterative VMR retrieval scheme corrects for trace gas profile shape effects. Benefits of this method are (1) a fast conversion that only requires the computation of Box-AMFs in a Rayleigh atmosphere; (2) neither local aerosol extinction nor the slant column density in the DOAS reference (SCD ref) needs to be known; and (3) VMRs can be retrieved for every measurement point along a flight track, thus increasing statistics and adding flexibility to capture concentration gradients. Sensitivity studies are performed for bromine monoxide (BrO), iodine monoxide (IO) and nitrogen dioxide (NO 2), using (1) simulated dSCD data for different trace gas and aerosol profiles and (2) field measurements from the Tropical Ocean tRoposphere Exchange of Reactive halogen species and Oxygenated VOC (TORERO) field experiment. For simulated data in a Rayleigh atmosphere, the agreement between the VMR from the parameterization method (VMR para) and the true VMR (VMR true) is excellent for all trace gases. Offsets, slopes and R 2 values for the linear fit of VMR para over VMR true are, respectively (0.008 ± 0.001) pptv, 0.988 ± 0.001, 0.987 for BrO; (-0.0066 ± 0.0001) pptv, 1.0021 ± 0.0003, 0.9979 for IO; (-0.17 ± 0.03) pptv, 1.0036 ± 0.0001, 0.9997 for NO 2. The agreement for atmospheres with aerosol shows comparable R 2 values to the Rayleigh case, but slopes deviate a bit more from one: (0.093 ± 0.002) pptv, 0.933 ± 0.002, 0.907 for BrO; (0.0021 ± 0.0004) pptv, 0.887 ± 0.001, 0.973 for IO; (8.5 ± 0.1) pptv, 0.8302 ± 0.0006, 0.9923 for NO 2. VMR para from field data are further compared with optimal estimation retrievals (VMR OE). Least orthogonal distance fit of the data give the following equations: BrO para = (0.1 ± 0.2) pptv + (0.95 ± 0.14) × BrO OE; IO para = (0.01 ± 0.02) pptv + (1.00 ± 0.12) × IO OE; NO 2para = (3.9 ± 2.5) pptv + (0.87 ± 0.15) × NO 2OE. Overall, we conclude that the parameterization retrieval is accurate with an uncertainty of 20 % for IO, 30 % for BrO and NO 2, but not better than 0.05 pptv IO, 0.5 pptv BrO and 10 pptv NO 2. Finally, the retrieval is applicable over a wide range of atmospheric conditions and measurement geometries and not limited to the interpretation of vertical profile measurements in the remote troposphere.« less

Parameterization retrieval of trace gas volume mixing ratios from Airborne MAX-DOAS

DOE PAGES

Dix, Barbara; Koenig, Theodore K.; Volkamer, Rainer

2016-11-28

We present a parameterization retrieval of volume mixing ratios (VMRs) from differential slant column density (dSCD) measurements by Airborne Multi-AXis Differential Optical Absorption Spectroscopy (AMAX-DOAS). The method makes use of the fact that horizontally recorded limb spectra (elevation angle 0°) are strongly sensitive to the atmospheric layer at instrument altitude. These limb spectra are analyzed using reference spectra that largely cancel out column contributions from above and below the instrument, so that the resulting limb dSCDs, i.e., the column integrated concentration with respect to a reference spectrum, are almost exclusively sensitive to the atmospheric layers around instrument altitude. The conversionmore » of limb dSCDs into VMRs is then realized by calculating box air mass factors (Box-AMFs) for a Rayleigh atmosphere and applying a scaling factor constrained by O 4 dSCDs to account for aerosol extinction. An iterative VMR retrieval scheme corrects for trace gas profile shape effects. Benefits of this method are (1) a fast conversion that only requires the computation of Box-AMFs in a Rayleigh atmosphere; (2) neither local aerosol extinction nor the slant column density in the DOAS reference (SCD ref) needs to be known; and (3) VMRs can be retrieved for every measurement point along a flight track, thus increasing statistics and adding flexibility to capture concentration gradients. Sensitivity studies are performed for bromine monoxide (BrO), iodine monoxide (IO) and nitrogen dioxide (NO 2), using (1) simulated dSCD data for different trace gas and aerosol profiles and (2) field measurements from the Tropical Ocean tRoposphere Exchange of Reactive halogen species and Oxygenated VOC (TORERO) field experiment. For simulated data in a Rayleigh atmosphere, the agreement between the VMR from the parameterization method (VMR para) and the true VMR (VMR true) is excellent for all trace gases. Offsets, slopes and R 2 values for the linear fit of VMR para over VMR true are, respectively (0.008 ± 0.001) pptv, 0.988 ± 0.001, 0.987 for BrO; (-0.0066 ± 0.0001) pptv, 1.0021 ± 0.0003, 0.9979 for IO; (-0.17 ± 0.03) pptv, 1.0036 ± 0.0001, 0.9997 for NO 2. The agreement for atmospheres with aerosol shows comparable R 2 values to the Rayleigh case, but slopes deviate a bit more from one: (0.093 ± 0.002) pptv, 0.933 ± 0.002, 0.907 for BrO; (0.0021 ± 0.0004) pptv, 0.887 ± 0.001, 0.973 for IO; (8.5 ± 0.1) pptv, 0.8302 ± 0.0006, 0.9923 for NO 2. VMR para from field data are further compared with optimal estimation retrievals (VMR OE). Least orthogonal distance fit of the data give the following equations: BrO para = (0.1 ± 0.2) pptv + (0.95 ± 0.14) × BrO OE; IO para = (0.01 ± 0.02) pptv + (1.00 ± 0.12) × IO OE; NO 2para = (3.9 ± 2.5) pptv + (0.87 ± 0.15) × NO 2OE. Overall, we conclude that the parameterization retrieval is accurate with an uncertainty of 20 % for IO, 30 % for BrO and NO 2, but not better than 0.05 pptv IO, 0.5 pptv BrO and 10 pptv NO 2. Finally, the retrieval is applicable over a wide range of atmospheric conditions and measurement geometries and not limited to the interpretation of vertical profile measurements in the remote troposphere.« less

Influence of Humidity On the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

NASA Technical Reports Server (NTRS)

Gasso, S.; Hegg, D. A.; Covert, D. S.; Collins, D.; Noone, K. J.; Oestroem, E.; Schmid, B.; Russell, P. B.; Livingston, J. M.; Durkee, P. A.

2000-01-01

Aerosol scattering coefficients (sigma(sub sp)) have been measured over the ocean at different relative humidities (RH) as a function of altitude in the region surrounding the Canary Islands during the Second Aerosol Characterization Experiment (ACE-2) in June and July 1997. The data were collected by the University of Washington passive humidigraph (UWPH) mounted on the Pelican research aircraft. Concurrently, particle size distributions, absorption coefficients and aerosol optical depth were measured throughout 17 flights. A parameterization of sigma(sub sp) as a function of RH was utilized to assess the impact of aerosol hydration on the upwelling radiance (normalized to the solar constant and cosine of zenith angle). The top of the atmosphere radiance signal was simulated at wavelengths corresponding to visible and near-infrared bands of the EOS (Earth Observing System) AM-1 (Terra) detectors, MODIS (Moderate Resolution Imaging Spectroradiometer) and MISR (Multi-angle Imaging Spectroradiometer). The UWPH measured sigma(sub sp) at two RHs, one below and the other above ambient conditions. Ambient sigma(sub sp) was obtained by interpolation of these two measurements. The data were stratified in terms of three types of aerosols: Saharan dust, clean marine (marine boundary layer background) and polluted marine aerosols (i.e., two- or one-day old polluted aerosols advected from Europe). An empirical relation for the dependence of sigma(sub sp) on RH, defined by sigma(sub sp)(RH) = k.(1 - RH/100)(sup gamma), was used with the hygroscopic exponent gamma derived from the data. The following gamma values were obtained for the 3 aerosol types: gamma(dust) = 0.23 +/- 0.05, gamma(clean marine) = 0.69 +/- 0.06 and gamma(polluted marine) = 0.57 +/- 0.06. Based on the measured gammas, the above equation was utilized to derive aerosol models with different hygroscopicities. The satellite simulation signal code 6S was used to compute the upwelling radiance corresponding to each of those aerosol models at several ambient humidities. For the prelaunch estimated precision of the sensors and the assumed viewing geometry of the instrument, the simulations suggest that the spectral and angular dependence of the reflectance measured by MISR is not sufficient to distinguish aerosol models with various different combinations of values for dry composition, gamma and ambient RH. A similar behavior is observed for MODIS at visible wavelengths. However, the 2100 nm band of MODIS appears to be able to differentiate between at least same aerosol models with different aerosol hygroscopicity given the MODIS calibration error requirements. This result suggests the possibility of retrieval of aerosol hygroscopicity by MODIS.

Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning

DOE PAGES

Murphy, Benjamin N.; Woody, Matthew C.; Jimenez, Jose L.; ...

2017-09-20

Mounting evidence from field and laboratory observations coupled with atmospheric model analyses shows that primary combustion emissions of organic compounds dynamically partition between the vapor and particulate phases, especially as near-source emissions dilute and cool to ambient conditions. The most recent version of the Community Multiscale Air Quality model version 5.2 (CMAQv5.2) accounts for the semivolatile partitioning and gas-phase aging of these primary organic aerosol (POA) compounds consistent with experimentally derived parameterizations. We also include a new surrogate species, potential secondary organic aerosol from combustion emissions (pcSOA), which provides a representation of the secondary organic aerosol (SOA) from anthropogenic combustionmore » sources that could be missing from current chemical transport model predictions. The reasons for this missing mass likely include the following: (1) unspeciated semivolatile and intermediate volatility organic compound (SVOC and IVOC, respectively) emissions missing from current inventories, (2) multigenerational aging of organic vapor products from known SOA precursors (e.g., toluene, alkanes), (3) underestimation of SOA yields due to vapor wall losses in smog chamber experiments, and (4) reversible organic compounds–water interactions and/or aqueous-phase processing of known organic vapor emissions. CMAQ predicts the spatially averaged contribution of pcSOA to OA surface concentrations in the continental United States to be 38.6 and 23.6 % in the 2011 winter and summer, respectively. Whereas many past modeling studies focused on a particular measurement campaign, season, location, or model configuration, we endeavor to evaluate the model and important uncertain parameters with a comprehensive set of United States-based model runs using multiple horizontal scales (4 and 12 km), gas-phase chemical mechanisms, and seasons and years. The model with representation of semivolatile POA improves predictions of hourly OA observations over the traditional nonvolatile model at sites during field campaigns in southern California (CalNex, May–June 2010), northern California (CARES, June 2010), the southeast US (SOAS, June 2013; SEARCH, January and July, 2011). Model improvements manifest better correlations (e.g., the correlation coefficient at Pasadena at night increases from 0.38 to 0.62) and reductions in underprediction during the photochemically active afternoon period (e.g., bias at Pasadena from -5.62 to -2.42 µg m -3). Daily averaged predictions of observations at routine-monitoring networks from simulations over the continental US (CONUS) in 2011 show modest improvement during winter, with mean biases reducing from 1.14 to 0.73 µg m -3, but less change in the summer when the decreases from POA evaporation were similar to the magnitude of added SOA mass. Because the model-performance improvement realized by including the relatively simple pcSOA approach is similar to that of more-complicated parameterizations of OA formation and aging, we recommend caution when applying these more-complicated approaches as they currently rely on numerous uncertain parameters. The pcSOA parameters optimized for performance at the southern and northern California sites lead to higher OA formation than is observed in the CONUS evaluation. This may be due to any of the following: variations in real pcSOA in different regions or time periods, too-high concentrations of other OA sources in the model that are important over the larger domain, or other model issues such as loss processes. This discrepancy is likely regionally and temporally dependent and driven by interferences from factors like varying emissions and chemical regimes.« less

Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning

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

Murphy, Benjamin N.; Woody, Matthew C.; Jimenez, Jose L.

Mounting evidence from field and laboratory observations coupled with atmospheric model analyses shows that primary combustion emissions of organic compounds dynamically partition between the vapor and particulate phases, especially as near-source emissions dilute and cool to ambient conditions. The most recent version of the Community Multiscale Air Quality model version 5.2 (CMAQv5.2) accounts for the semivolatile partitioning and gas-phase aging of these primary organic aerosol (POA) compounds consistent with experimentally derived parameterizations. We also include a new surrogate species, potential secondary organic aerosol from combustion emissions (pcSOA), which provides a representation of the secondary organic aerosol (SOA) from anthropogenic combustionmore » sources that could be missing from current chemical transport model predictions. The reasons for this missing mass likely include the following: (1) unspeciated semivolatile and intermediate volatility organic compound (SVOC and IVOC, respectively) emissions missing from current inventories, (2) multigenerational aging of organic vapor products from known SOA precursors (e.g., toluene, alkanes), (3) underestimation of SOA yields due to vapor wall losses in smog chamber experiments, and (4) reversible organic compounds–water interactions and/or aqueous-phase processing of known organic vapor emissions. CMAQ predicts the spatially averaged contribution of pcSOA to OA surface concentrations in the continental United States to be 38.6 and 23.6 % in the 2011 winter and summer, respectively. Whereas many past modeling studies focused on a particular measurement campaign, season, location, or model configuration, we endeavor to evaluate the model and important uncertain parameters with a comprehensive set of United States-based model runs using multiple horizontal scales (4 and 12 km), gas-phase chemical mechanisms, and seasons and years. The model with representation of semivolatile POA improves predictions of hourly OA observations over the traditional nonvolatile model at sites during field campaigns in southern California (CalNex, May–June 2010), northern California (CARES, June 2010), the southeast US (SOAS, June 2013; SEARCH, January and July, 2011). Model improvements manifest better correlations (e.g., the correlation coefficient at Pasadena at night increases from 0.38 to 0.62) and reductions in underprediction during the photochemically active afternoon period (e.g., bias at Pasadena from -5.62 to -2.42 µg m -3). Daily averaged predictions of observations at routine-monitoring networks from simulations over the continental US (CONUS) in 2011 show modest improvement during winter, with mean biases reducing from 1.14 to 0.73 µg m -3, but less change in the summer when the decreases from POA evaporation were similar to the magnitude of added SOA mass. Because the model-performance improvement realized by including the relatively simple pcSOA approach is similar to that of more-complicated parameterizations of OA formation and aging, we recommend caution when applying these more-complicated approaches as they currently rely on numerous uncertain parameters. The pcSOA parameters optimized for performance at the southern and northern California sites lead to higher OA formation than is observed in the CONUS evaluation. This may be due to any of the following: variations in real pcSOA in different regions or time periods, too-high concentrations of other OA sources in the model that are important over the larger domain, or other model issues such as loss processes. This discrepancy is likely regionally and temporally dependent and driven by interferences from factors like varying emissions and chemical regimes.« less

Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning

NASA Astrophysics Data System (ADS)

Murphy, Benjamin N.; Woody, Matthew C.; Jimenez, Jose L.; Carlton, Ann Marie G.; Hayes, Patrick L.; Liu, Shang; Ng, Nga L.; Russell, Lynn M.; Setyan, Ari; Xu, Lu; Young, Jeff; Zaveri, Rahul A.; Zhang, Qi; Pye, Havala O. T.

2017-09-01

Mounting evidence from field and laboratory observations coupled with atmospheric model analyses shows that primary combustion emissions of organic compounds dynamically partition between the vapor and particulate phases, especially as near-source emissions dilute and cool to ambient conditions. The most recent version of the Community Multiscale Air Quality model version 5.2 (CMAQv5.2) accounts for the semivolatile partitioning and gas-phase aging of these primary organic aerosol (POA) compounds consistent with experimentally derived parameterizations. We also include a new surrogate species, potential secondary organic aerosol from combustion emissions (pcSOA), which provides a representation of the secondary organic aerosol (SOA) from anthropogenic combustion sources that could be missing from current chemical transport model predictions. The reasons for this missing mass likely include the following: (1) unspeciated semivolatile and intermediate volatility organic compound (SVOC and IVOC, respectively) emissions missing from current inventories, (2) multigenerational aging of organic vapor products from known SOA precursors (e.g., toluene, alkanes), (3) underestimation of SOA yields due to vapor wall losses in smog chamber experiments, and (4) reversible organic compounds-water interactions and/or aqueous-phase processing of known organic vapor emissions. CMAQ predicts the spatially averaged contribution of pcSOA to OA surface concentrations in the continental United States to be 38.6 and 23.6 % in the 2011 winter and summer, respectively. Whereas many past modeling studies focused on a particular measurement campaign, season, location, or model configuration, we endeavor to evaluate the model and important uncertain parameters with a comprehensive set of United States-based model runs using multiple horizontal scales (4 and 12 km), gas-phase chemical mechanisms, and seasons and years. The model with representation of semivolatile POA improves predictions of hourly OA observations over the traditional nonvolatile model at sites during field campaigns in southern California (CalNex, May-June 2010), northern California (CARES, June 2010), the southeast US (SOAS, June 2013; SEARCH, January and July, 2011). Model improvements manifest better correlations (e.g., the correlation coefficient at Pasadena at night increases from 0.38 to 0.62) and reductions in underprediction during the photochemically active afternoon period (e.g., bias at Pasadena from -5.62 to -2.42 µg m-3). Daily averaged predictions of observations at routine-monitoring networks from simulations over the continental US (CONUS) in 2011 show modest improvement during winter, with mean biases reducing from 1.14 to 0.73 µg m-3, but less change in the summer when the decreases from POA evaporation were similar to the magnitude of added SOA mass. Because the model-performance improvement realized by including the relatively simple pcSOA approach is similar to that of more-complicated parameterizations of OA formation and aging, we recommend caution when applying these more-complicated approaches as they currently rely on numerous uncertain parameters. The pcSOA parameters optimized for performance at the southern and northern California sites lead to higher OA formation than is observed in the CONUS evaluation. This may be due to any of the following: variations in real pcSOA in different regions or time periods, too-high concentrations of other OA sources in the model that are important over the larger domain, or other model issues such as loss processes. This discrepancy is likely regionally and temporally dependent and driven by interferences from factors like varying emissions and chemical regimes.

Hygroscopic Growth and Activation of Particles containing Algea-Exudate

NASA Astrophysics Data System (ADS)

Wex, Heike; Fuentes, Elena; Tsagkogeorgas, Georgios; Voigtländer, Jens; Clauss, Tina; Kiselev, Alexei; Green, David; Coe, Hugh; McFiggans, Gordon; Stratmann, Frank

2010-05-01

A large amount of the Earth is covered by oceans, which provide a constant source of marine aerosol particles, produced due to bubble bursting processes that depend on wind speed (O'Dowd and de Leeuw, 2007). In general, marine particles can be assumed to play an important role for the Earth atmosphere on a global scale, due to their abundance and due to their effect on clouds. E.g. marine stratus and stratocumulus clouds contribute about 30% to 40% to the Earth's albedo (Randall et al., 1984). The activation of aerosol particles to cloud droplets depends on the hygroscopic properties of the particles, which, in turn, depend on their chemical composition. For marine particles, is has been and still is discussed what the effects of organic substances being present in the particles might be. These substances originate from marine biota where they enrich at the ocean surface. To mimic marine aerosol particles, algae-exudates of different algae species were mixed with artificial sea-water. These samples were used in the laboratory to produce particles via a bubble bursting process (Fuentes et al., 2009). The hygroscopic growth and activation of the (size selected) particles was measured, using LACIS (Leipzig Aerosol Cloud Interaction Simulator, Stratmann et al., 2004) and the DMT-CCNc (Cloud Condensation Nucleus counter from Droplet Measurement Technologies, Roberts and Nenes, 2005). The hygroscopic growth was measured twice, 3 and 10 seconds after humidification, and no difference in the grown size was detected, i.e. no kinetic effect was observed for the examined time range. From LACIS and CCNc measurements, the hygroscopicity was deduced through determination of the amount of ions being effective in the particle / droplet solution (Rho(ion), Wex et al., 2007). A concentration dependent non-ideal behaviour was found for particles produced from an artificial sea-water sample that contained only inorganic salts, as can be expected (see e.g. Niedermeier et al., 2008). For particles containing also algae-exudate, however, the concentration dependent non-ideal behaviour was quenched, resulting in a quasi ideal solution behavior. Such solutions could be described by a single-parameter representation for all water-vapour saturations at which measurements had been done (from 0.8 up to supersaturation). References: Fuentes, E., H. Coe, D. Green, G. De Leeuw, and G. McFiggans (2009), Laboratory-generated primary marine aerosol via bubble-bursting and atomization, Aerosol Meas. Tech. Discuss., 2, 2281-2320. O'Dowd, C. D., and G. de Leeuw (2007), Marine aerosol production: A review of the current knowledge, Phil. Trans. R. Soc. A, 365(1856), 1753-1774, doi:1710.1098/rsta.2007.2043. Niedermeier, D., H. Wex, J. Voigtländer, F. Stratmann, E. Brüggemann, A. Kiselev, H. Henk, and J. Heintzenberg (2008), LACIS-measurements and parameterization of sea-salt particle hygroscopic growth and activation, Atmos. Chem. Phys., 8, 579-590. Randall, D. A., Coakley, J. A., Fairall, C. W., Kropfli, R. A., and Lenschow, D. H. (1984) Outlook for research on subtropical marine stratiform clouds, Bull. Am. Meteor. Soc., 65, 1290-1301, 1984. Roberts, G., and A. Nenes (2005), A continuous-flow streamwise thermal-gradient CCN chamber for atmospheric measurements, Aerosol Sci. Technol., 39, 206-221. 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. Wex, H., T. Hennig, I. Salma, R. Ocskay, A. Kiselev, S. Henning, A. Massling, A. Wiedensohler, and F. Stratmann (2007), Hygroscopic growth and measured and modeled critical super-saturations of an atmospheric HULIS sample, Geophys. Res. Lett., 34(L02818), doi:10.1029/2006GL028260.

Black Carbon Concentration from Worldwide Aerosol Robotic Network (AERONET) Measurements

NASA Technical Reports Server (NTRS)

Schuster, Gregory L.; Dubovik, Oleg; Holben, Brent N.; Clothiaux, Eugene E.

2006-01-01

The carbon emissions inventories used to initialize transport models and general circulation models are highly parameterized, and created on the basis of multiple sparse datasets (such as fuel use inventories and emission factors). The resulting inventories are uncertain by at least a factor of 2, and this uncertainty is carried forward to the model output. [Bond et al., 1998, Bond et al., 2004, Cooke et al., 1999, Streets et al., 2001] Worldwide black carbon concentration measurements are needed to assess the efficacy of the carbon emissions inventory and transport model output on a continuous basis.

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.

Enviro-HIRLAM/ HARMONIE Studies in ECMWF HPC EnviroAerosols Project

NASA Astrophysics Data System (ADS)

Hansen Sass, Bent; Mahura, Alexander; Nuterman, Roman; Baklanov, Alexander; Palamarchuk, Julia; Ivanov, Serguei; Pagh Nielsen, Kristian; Penenko, Alexey; Edvardsson, Nellie; Stysiak, Aleksander Andrzej; Bostanbekov, Kairat; Amstrup, Bjarne; Yang, Xiaohua; Ruban, Igor; Bergen Jensen, Marina; Penenko, Vladimir; Nurseitov, Daniyar; Zakarin, Edige

2017-04-01

The EnviroAerosols on ECMWF HPC project (2015-2017) "Enviro-HIRLAM/ HARMONIE model research and development for online integrated meteorology-chemistry-aerosols feedbacks and interactions in weather and atmospheric composition forecasting" is aimed at analysis of importance of the meteorology-chemistry/aerosols interactions and to provide a way for development of efficient techniques for on-line coupling of numerical weather prediction and atmospheric chemical transport via process-oriented parameterizations and feedback algorithms, which will improve both the numerical weather prediction and atmospheric composition forecasts. Two main application areas of the on-line integrated modelling are considered: (i) improved numerical weather prediction with short-term feedbacks of aerosols and chemistry on formation and development of meteorological variables, and (ii) improved atmospheric composition forecasting with on-line integrated meteorological forecast and two-way feedbacks between aerosols/chemistry and meteorology. During 2015-2016 several research projects were realized. At first, the study on "On-line Meteorology-Chemistry/Aerosols Modelling and Integration for Risk Assessment: Case Studies" focused on assessment of scenarios with accidental and continuous emissions of sulphur dioxide for case studies for Atyrau (Kazakhstan) near the northern part of the Caspian Sea and metallurgical enterprises on the Kola Peninsula (Russia), with GIS integration of modelling results into the RANDOM (Risk Assessment of Nature Detriment due to Oil spill Migration) system. At second, the studies on "The sensitivity of precipitation simulations to the soot aerosol presence" & "The precipitation forecast sensitivity to data assimilation on a very high resolution domain" focused on sensitivity and changes in precipitation life-cycle under black carbon polluted conditions over Scandinavia. At third, studies on "Aerosol effects over China investigated with a high resolution convection permitting weather model" & "Meteorological and chemical urban scale modelling for Shanghai metropolitan area" with focus on aerosol effects and influence of urban areas in China at regional-subregional-urban scales. At fourth, study on "Direct variational data assimilation algorithm for atmospheric chemistry data with transport and transformation model" with focus on testing chemical data assimilation algorithm of in situ concentration measurements on real data scenario. At firth, study on "Aerosol influence on High Resolution NWP HARMONIE Operational Forecasts" with focus on impact of sea salt aerosols on numerical weather prediction during low precipitation events. And finally, study on "Impact of regional afforestation on climatic conditions in metropolitan areas: case study of Copenhagen" with focus on impact of forest and land-cover change on formation and development of temperature regimes in the Copenhagen metropolitan area of Denmark. Selected results and findings will be presented and discussed.

60 years of UK visibility measurements: impact of meteorology and atmospheric pollutants on visibility

NASA Astrophysics Data System (ADS)

Singh, Ajit; Bloss, William J.; Pope, Francis D.

2017-02-01

Reduced visibility is an indicator of poor air quality. Moreover, degradation in visibility can be hazardous to human safety; for example, low visibility can lead to road, rail, sea and air accidents. In this paper, we explore the combined influence of atmospheric aerosol particle and gas characteristics, and meteorology, on long-term visibility. We use visibility data from eight meteorological stations, situated in the UK, which have been running since the 1950s. The site locations include urban, rural and marine environments. Most stations show a long-term trend of increasing visibility, which is indicative of reductions in air pollution, especially in urban areas. Additionally, the visibility at all sites shows a very clear dependence on relative humidity, indicating the importance of aerosol hygroscopicity on the ability of aerosol particles to scatter radiation. The dependence of visibility on other meteorological parameters, such as wind speed and wind direction, is also investigated. Most stations show long-term increases in temperature which can be ascribed to climate change, land-use changes (e.g. urban heat island effects) or a combination of both; the observed effect is greatest in urban areas. The impact of this temperature change upon local relative humidity is discussed. To explain the long-term visibility trends and their dependence on meteorological conditions, the measured data were fitted to a newly developed light-extinction model to generate predictions of historic aerosol and gas scattering and absorbing properties. In general, an excellent fit was achieved between measured and modelled visibility for all eight sites. The model incorporates parameterizations of aerosol hygroscopicity, particle concentration, particle scattering, and particle and gas absorption. This new model should be applicable and is easily transferrable to other data sets worldwide. Hence, historical visibility data can be used to assess trends in aerosol particle properties. This approach may help constrain global model simulations which attempt to generate aerosol fields for time periods when observational data are scarce or non-existent. Both the measured visibility and the modelled aerosol properties reported in this paper highlight the success of the UK's Clean Air Act, which was passed in 1956, in cleaning the atmosphere of visibility-reducing pollutants.

GoAmazon 2014/15. SRI-PTR-ToFMS Field Campaign Report

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

Guenther, A.

Our science team, including Dr. Alex Guenther (previously at Pacific Northwest National Laboratory (PNNL) and now at the University of California, Irvine) Dr. Saewung Kim and Dr. Roger Seco, and Dr. Jim Smith (previously at NCAR and now at UC Irvine), deployed a selected reagent ion – proton transfer reaction – time-of-flight mass spectrometer (SRI-PTR-TOFMS) to the T3 site during the GoAmazon study. One of the major uncertainties in climate model simulations is the effects of aerosols on radiative forcing, and a better understanding of the factors controlling aerosol distributions and life cycle is urgently needed. Aerosols contribute directly tomore » the Earth’s radiation balance by scattering or absorbing light as a function of their physical properties and indirectly through particle-cloud interactions that lead to cloud formation and the modification of cloud properties. On a global scale, the dominant source of organic aerosol is biogenic volatile organic compounds (BVOC) emitted from terrestrial ecosystems. These organic aerosols are a major part of the total mass of all airborne particles and are currently not sufficiently represented in climate models. To incorporate quantitatively the effects of BVOCs and their oxidation products on biogenic organic aerosol (BOA) requires parameterization of their production in terrestrial ecosystems and their atmospheric transformations. This project was designed to reduce the gaps in our understanding of how these processes control BVOCs and BOAs, and their impact on climate. This was accomplished by wet and dry season measurements at the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Climate Research Facility T3 site along with a comprehensive suite of complementary measurements. The specific goals were to 1) measure and mechanistically understand the factors affecting aerosol distributions over a tropical rain forest, especially the effects of anthropogenic pollution as a perturbation to the natural state, and 2) develop and implement an upscaling analysis from this new data set and knowledge of aerosol distributions to prognosticate possible climatic impacts of present-day urban pollution and possibly greater pollution in the future.« less

Top-down and Bottom-up aerosol-cloud-closure: towards understanding sources of unvertainty in deriving cloud radiative flux

NASA Astrophysics Data System (ADS)

Sanchez, K.; Roberts, G.; Calmer, R.; Nicoll, K.; Hashimshoni, E.; Rosenfeld, D.; Ovadnevaite, J.; Preissler, J.; Ceburnis, D.; O'Dowd, C. D. D.; Russell, L. M.

2017-12-01

Top-down and bottom-up aerosol-cloud shortwave radiative flux closures were conducted at the Mace Head atmospheric research station in Galway, Ireland in August 2015. Instrument platforms include ground-based, unmanned aerial vehicles (UAV), and satellite measurements of aerosols, clouds and meteorological variables. The ground-based and airborne measurements of aerosol size distributions and cloud condensation nuclei (CCN) concentration were used to initiate a 1D microphysical aerosol-cloud parcel model (ACPM). UAVs were equipped for a specific science mission, with an optical particle counter for aerosol distribution profiles, a cloud sensor to measure cloud extinction, or a 5-hole probe for 3D wind vectors. These are the first UAV measurements at Mace Head. ACPM simulations are compared to in-situ cloud extinction measurements from UAVs to quantify closure in terms of cloud shortwave radiative flux. Two out of seven cases exhibit sub-adiabatic vertical temperature profiles within the cloud, which suggests that entrainment processes affect cloud microphysical properties and lead to an overestimate of simulated cloud shortwave radiative flux. Including an entrainment parameterization and explicitly calculating the entrainment fraction in the ACPM simulations both improved cloud-top radiative closure. Entrainment reduced the difference between simulated and observation-derived cloud-top shortwave radiative flux (δRF) by between 25 W m-2 and 60 W m-2. After accounting for entrainment, satellite-derived cloud droplet number concentrations (CDNC) were within 30% of simulated CDNC. In cases with a well-mixed boundary layer, δRF is no greater than 20 W m-2 after accounting for cloud-top entrainment, and up to 50 W m-2 when entrainment is not taken into account. In cases with a decoupled boundary layer, cloud microphysical properties are inconsistent with ground-based aerosol measurements, as expected, and δRF is as high as 88 W m-2, even high (> 30 W m-2) after accounting for cloud-top entrainment. This work demonstrates the need to take in-situ measurements of aerosol properties for cases where the boundary layer is decoupled as well as consider cloud-top entrainment to accurately model stratocumulus cloud radiative flux.

Top-down and Bottom-up aerosol-cloud-closure: towards understanding sources of unvertainty in deriving cloud radiative flux

NASA Astrophysics Data System (ADS)

Sanchez, K.; Roberts, G.; Calmer, R.; Nicoll, K.; Hashimshoni, E.; Rosenfeld, D.; Ovadnevaite, J.; Preissler, J.; Ceburnis, D.; O'Dowd, C. D. D.; Russell, L. M.

2016-12-01

Top-down and bottom-up aerosol-cloud shortwave radiative flux closures were conducted at the Mace Head atmospheric research station in Galway, Ireland in August 2015. Instrument platforms include ground-based, unmanned aerial vehicles (UAV), and satellite measurements of aerosols, clouds and meteorological variables. The ground-based and airborne measurements of aerosol size distributions and cloud condensation nuclei (CCN) concentration were used to initiate a 1D microphysical aerosol-cloud parcel model (ACPM). UAVs were equipped for a specific science mission, with an optical particle counter for aerosol distribution profiles, a cloud sensor to measure cloud extinction, or a 5-hole probe for 3D wind vectors. These are the first UAV measurements at Mace Head. ACPM simulations are compared to in-situ cloud extinction measurements from UAVs to quantify closure in terms of cloud shortwave radiative flux. Two out of seven cases exhibit sub-adiabatic vertical temperature profiles within the cloud, which suggests that entrainment processes affect cloud microphysical properties and lead to an overestimate of simulated cloud shortwave radiative flux. Including an entrainment parameterization and explicitly calculating the entrainment fraction in the ACPM simulations both improved cloud-top radiative closure. Entrainment reduced the difference between simulated and observation-derived cloud-top shortwave radiative flux (δRF) by between 25 W m-2 and 60 W m-2. After accounting for entrainment, satellite-derived cloud droplet number concentrations (CDNC) were within 30% of simulated CDNC. In cases with a well-mixed boundary layer, δRF is no greater than 20 W m-2 after accounting for cloud-top entrainment, and up to 50 W m-2 when entrainment is not taken into account. In cases with a decoupled boundary layer, cloud microphysical properties are inconsistent with ground-based aerosol measurements, as expected, and δRF is as high as 88 W m-2, even high (> 30 W m-2) after accounting for cloud-top entrainment. This work demonstrates the need to take in-situ measurements of aerosol properties for cases where the boundary layer is decoupled as well as consider cloud-top entrainment to accurately model stratocumulus cloud radiative flux.

Hygroscopic growth study in the framework of EARLINET during the SLOPE I campaign: synergy of remote sensing and in situ instrumentation

NASA Astrophysics Data System (ADS)

Esteban Bedoya-Velásquez, Andrés; Navas-Guzmán, Francisco; José Granados-Muñoz, María; Titos, Gloria; Román, Roberto; Andrés Casquero-Vera, Juan; Ortiz-Amezcua, Pablo; Benavent-Oltra, Jose Antonio; de Arruda Moreira, Gregori; Montilla-Rosero, Elena; Hoyos, Carlos David; Artiñano, Begoña; Coz, Esther; José Olmo-Reyes, Francisco; Alados-Arboledas, Lucas; Guerrero-Rascado, Juan Luis

2018-05-01

This study focuses on the analysis of aerosol hygroscopic growth during the Sierra Nevada Lidar AerOsol Profiling Experiment (SLOPE I) campaign by using the synergy of active and passive remote sensors at the ACTRIS Granada station and in situ instrumentation at a mountain station (Sierra Nevada, SNS). To this end, a methodology based on simultaneous measurements of aerosol profiles from an EARLINET multi-wavelength Raman lidar (RL) and relative humidity (RH) profiles obtained from a multi-instrumental approach is used. This approach is based on the combination of calibrated water vapor mixing ratio (r) profiles from RL and continuous temperature profiles from a microwave radiometer (MWR) for obtaining RH profiles with a reasonable vertical and temporal resolution. This methodology is validated against the traditional one that uses RH from co-located radiosounding (RS) measurements, obtaining differences in the hygroscopic growth parameter (γ) lower than 5 % between the methodology based on RS and the one presented here. Additionally, during the SLOPE I campaign the remote sensing methodology used for aerosol hygroscopic growth studies has been checked against Mie calculations of aerosol hygroscopic growth using in situ measurements of particle number size distribution and submicron chemical composition measured at SNS. The hygroscopic case observed during SLOPE I showed an increase in the particle backscatter coefficient at 355 and 532 nm with relative humidity (RH ranged between 78 and 98 %), but also a decrease in the backscatter-related Ångström exponent (AE) and particle linear depolarization ratio (PLDR), indicating that the particles became larger and more spherical due to hygroscopic processes. Vertical and horizontal wind analysis is performed by means of a co-located Doppler lidar system, in order to evaluate the horizontal and vertical dynamics of the air masses. Finally, the Hänel parameterization is applied to experimental data for both stations, and we found good agreement on γ measured with remote sensing (γ532 = 0.48 ± 0.01 and γ355 = 0.40 ± 0.01) with respect to the values calculated using Mie theory (γ532 = 0.53 ± 0.02 and γ355 = 0.45 ± 0.02), with relative differences between measurements and simulations lower than 9 % at 532 nm and 11 % at 355 nm.

Updating Sea Spray Aerosol Emissions in the Community Multiscale Air Quality Model

NASA Astrophysics Data System (ADS)

Gantt, B.; Bash, J. O.; Kelly, J.

2014-12-01

Sea spray aerosols (SSA) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. In this study, the Community Multiscale Air Quality (CMAQ) model is updated to enhance fine mode SSA emissions, include sea surface temperature (SST) dependency, and revise surf zone emissions. Based on evaluation with several regional and national observational datasets in the continental U.S., the updated emissions generally improve surface concentrations predictions of primary aerosols composed of sea-salt and secondary aerosols affected by sea-salt chemistry in coastal and near-coastal sites. Specifically, the updated emissions lead to better predictions of the magnitude and coastal-to-inland gradient of sodium, chloride, and nitrate concentrations at Bay Regional Atmospheric Chemistry Experiment (BRACE) sites near Tampa, FL. Including SST-dependency to the SSA emission parameterization leads to increased sodium concentrations in the southeast U.S. and decreased concentrations along the Pacific coast and northeastern U.S., bringing predictions into closer agreement with observations at most Interagency Monitoring of Protected Visual Environments (IMPROVE) and Chemical Speciation Network (CSN) sites. Model comparison with California Research at the Nexus of Air Quality and Climate Change (CalNex) observations will also be discussed, with particular focus on the South Coast Air Basin where clean marine air mixes with anthropogenic pollution in a complex environment. These SSA emission updates enable more realistic simulation of chemical processes in coastal environments, both in clean marine air masses and mixtures of clean marine and polluted conditions.

Stereoscopic Retrieval of Smoke Plume Heights and Motion from Space-Based Multi-Angle Imaging, Using the MISR INteractive eXplorer(MINX)

NASA Technical Reports Server (NTRS)

Nelson, David L.; Kahn, Ralph A.

2014-01-01

Airborne particles desert dust, wildfire smoke, volcanic effluent, urban pollution affect Earth's climate as well as air quality and health. They are found in the atmosphere all over the planet, but vary immensely in amount and properties with season and location. Most aerosol particles are injected into the near-surface boundary layer, but some, especially wildfire smoke, desert dust and volcanic ash, can be injected higher into the atmosphere, where they can stay aloft longer, travel farther, produce larger climate effects, and possibly affect human and ecosystem health far downwind. So monitoring aerosol injection height globally can make important contributions to climate science and air quality studies. The Multi-angle Imaging Spectro-Radiometer (MISR) is a space borne instrument designed to study Earths clouds, aerosols, and surface. Since late February 2000 it has been retrieving aerosol particle amount and properties, as well as cloud height and wind data, globally, about once per week. The MINX visualization and analysis tool complements the operational MISR data products, enabling users to retrieve heights and winds locally for detailed studies of smoke plumes, at higher spatial resolution and with greater precision than the operational product and other space-based, passive remote sensing techniques. MINX software is being used to provide plume height statistics for climatological studies as well as to investigate the dynamics of individual plumes, and to provide parameterizations for climate modeling.

Resolving Size Distribution of Black Carbon Internally Mixed With Snow: Impact on Snow Optical Properties and Albedo

NASA Astrophysics Data System (ADS)

He, Cenlin; Liou, Kuo-Nan; Takano, Yoshi

2018-03-01

We develop a stochastic aerosol-snow albedo model that explicitly resolves size distribution of aerosols internally mixed with various snow grains. We use the model to quantify black carbon (BC) size effects on snow albedo and optical properties for BC-snow internal mixing. Results show that BC-induced snow single-scattering coalbedo enhancement and albedo reduction decrease by a factor of 2-3 with increasing BC effective radii from 0.05 to 0.25 μm, while polydisperse BC results in up to 40% smaller visible single-scattering coalbedo enhancement and albedo reduction compared to monodisperse BC with equivalent effective radii. We further develop parameterizations for BC size effects for application to climate models. Compared with a realistic polydisperse assumption and observed shifts to larger BC sizes in snow, respectively, assuming monodisperse BC and typical atmospheric BC effective radii could lead to overestimates of 24% and 40% in BC-snow albedo forcing averaged over different BC and snow conditions.

UV-B measurements in India

NASA Astrophysics Data System (ADS)

Prasad, B. S. N.; Gayathri, H. B.; Muralikrishnan, N.

1992-01-01

Global UV-B flux (sum of direct and diffuse radiations) data at four wavelengths 280, 290, 300 and 310 nm are recorded at several locations in India as part of Indian Middle Atmosphere Programme (IMAP). The stations have been selected considering distinct geographic features and possible influence of atmospheric aerosols and particulates on the ground reaching UV-B flux. Mysore (12.6°N, 76.6°E) has been selected as a continental station largely free from any industrial pollution and large scale bio-mass burning. An examination of the ground reaching UV-B flux at Mysore shows a marked dirunal and seasonal asymmetry. This can be attributed to the seasonally varying atmospheric aerosols and particulates which influence the scattering of UV-B radiation. The available parameterization models are used to reproduce the experimental UV-B irradiance by varying the input parameters to the model. These results on the dirunal and seasonal variation of global UV-B flux from experiment and models are discussed in this paper.

Modelling ice microphysics of mixed-phase clouds

NASA Astrophysics Data System (ADS)

Ahola, J.; Raatikainen, T.; Tonttila, J.; Romakkaniemi, S.; Kokkola, H.; Korhonen, H.

2017-12-01

The low-level Arctic mixed-phase clouds have a significant role for the Arctic climate due to their ability to absorb and reflect radiation. Since the climate change is amplified in polar areas, it is vital to apprehend the mixed-phase cloud processes. From a modelling point of view, this requires a high spatiotemporal resolution to capture turbulence and the relevant microphysical processes, which has shown to be difficult.In order to solve this problem about modelling mixed-phase clouds, a new ice microphysics description has been developed. The recently published large-eddy simulation cloud model UCLALES-SALSA offers a good base for a feasible solution (Tonttila et al., Geosci. Mod. Dev., 10:169-188, 2017). The model includes aerosol-cloud interactions described with a sectional SALSA module (Kokkola et al., Atmos. Chem. Phys., 8, 2469-2483, 2008), which represents a good compromise between detail and computational expense.Newly, the SALSA module has been upgraded to include also ice microphysics. The dynamical part of the model is based on well-known UCLA-LES model (Stevens et al., J. Atmos. Sci., 56, 3963-3984, 1999) which can be used to study cloud dynamics on a fine grid.The microphysical description of ice is sectional and the included processes consist of formation, growth and removal of ice and snow particles. Ice cloud particles are formed by parameterized homo- or heterogeneous nucleation. The growth mechanisms of ice particles and snow include coagulation and condensation of water vapor. Autoconversion from cloud ice particles to snow is parameterized. The removal of ice particles and snow happens by sedimentation and melting.The implementation of ice microphysics is tested by initializing the cloud simulation with atmospheric observations from the Indirect and Semi-Direct Aerosol Campaign (ISDAC). The results are compared to the model results shown in the paper of Ovchinnikov et al. (J. Adv. Model. Earth Syst., 6, 223-248, 2014) and they show a good match. One of the advantages of UCLALES-SALSA is that it can be used to quantify the effect of aerosol scavenging on cloud properties in a precise way.

Optimal Aerosol Parameterization for Remote Sensing Retrievals

NASA Technical Reports Server (NTRS)

Newchurch, Michael J.

2004-01-01

We have developed a new algorithm for the retrieval of aerosol and gases from SAGE It1 solar transmission measurements. This algorithm improves upon the NASA operational algorithm in several key aspects, including solving the problem non-linearly and incorporating a new methodology for separating the contribution of aerosols and gases. In order to extract aerosol information we have built a huge database of aerosol models for both stratospheric and tropospheric aerosols, and polar stratospheric cloud particles. This set of models allows us to calculate a vast range of possible extinction spectra for aerosols. and from these, derive a set of eigenvectors which then provide the basis set used in our inversion algorithm. Our aerosol algorithm and retrievals are described in several articles (listed in References Section) published under this grant. In particular they allow us to analyze the spectral properties of aerosols and PSCs and ultimately derive their microphysical properties. We have found some considerable differences between our spectra and the ones derived from the SAGE III operational algorithm. These are interesting as they provide an independent check on the validity of published aerosol data and, in particular, on their associated uncertainties. In order to understand these differences, we are assembling independent aerosol data from other sources with which to make comparisons. We have carried out extensive comparisons of our ozone retrievals with both SAGE III and independent lidar, ozonesonde, and satellite measurements (Polyakov et al., 2004). These show very good agreement throughout the stratosphere and help to quantify differences which can be attributed to natural variation in ozone versus that produced by algorithmic differences. In the mid - upper stratosphere, agreement with independent data was generally within 5 - 20%. but in the lower stratosphere the differences were considerably larger. We believe that a large proportion of this discrepancy in the lower stratosphere is attributable to natural variation, and is also seen in comparisons between lidar and ozonesonde measurements. NO2 profiles obtained with our algorithm were compared to those obtained through the SAGE III operational algorithm and exhibited differences of 20 - 40%. Our retrieved profiles agree with the HALOE NO2 measurements significantly better than those of the operational retrieval. In other work (described below), we are extending our aerosol retrievals into the infrared regime and plan to perform retrievals from combined uv-visible-infrared spectra. This work will allow us to use the spectra to derive the size and composition of aerosols, and we plan to employ our algorithms in the analysis of PSC spectra. We are presently also developing a limb-scattering algorithm to retrieve aerosol data from limb measurements of solar scattered radiation.

Observations and Measurements of Dust Transport from the Patagonia Desert into the South Atlantic Ocean in 2004 and 2005

NASA Astrophysics Data System (ADS)

Gasso, S.; Gaiero, D. M.; Villoslada, B.; Liske, E.

2005-12-01

The largest continental landmass south of the 40-degree parallel and potentially one of the largest sources of dust into the Southern Ocean (SO) is the Patagonia desert. Most of the estimates of dust outflow and deposition from this region into the South Atlantic Ocean are based on model simulations. However, there are very few measurements available that can corroborate these estimates. Satellite assessments of dust activity offer conflicting views. For example, monthly time series of satellite-derived (e.g. AVHRR and MODIS) aerosol optical depth (AOD) indicate that dust activity is minimal. However, a study with the TOMS Aerosol Index (Prospero et al., 2002) showed that the frequency of dust events is in the range of 7-14 days/month during the years 1978 through 1993. In addition, surface visibility observations along the Patagonian coast confirm that ocean-going dust events do occur during the summer and spring months. These discrepancies indicate fundamental uncertainties regarding the frequency and extent of dust activity in Patagonia. Given that the SO is the largest high-chlorophyll, low-nutrient area in the world and that the flux of nutrient-rich dust has the potential to modify biological activity with possible climatic consequences, it is of interest to have a better understanding of how often and intense are dust events in the Patagonia region. We surveyed the reports of dust activity from surface weather stations in the Patagonia region during the period June, 2004 to April, 2005. These observations were compared with simultaneous MODIS true color pictures and the corresponding aerosol retrievals. In addition, measurements of vertical and horizontal dust flux were collected by dust samplers at four sites along the coast. The horizontal flux measurements were compared with the same estimates derived from MODIS. According to the true color pictures and confirmed by the surface visibility observations, we recorded at least 16 ocean-going dust events. The scale of the events varied from small (single dust plumes along the coast) to large (dust front extending ~600 km). Most of the large events occurred during the late summer. Due to the presence of sun glint, cloud obstruction, or coastal sediments, the MODIS automatic aerosol algorithm did not derive AODs in many instances and, as result, many events were not recorded in the MODIS monthly database. Dust sources are numerous and dust plumes outflow at any place along the coastline (> 1000 km) including some very active sources as far south as in the Tierra del Fuego Island (54S). The main sources identified are coastal saltbeds, inland deflation hollows and receding shores of large lakes. Although some of major emitting points have been included as sources in dust models, there are some notable exceptions, for example most of the coastal sources. We note, in addition, that the scale and diversity of the different sources pose significant challenges with respect to parameterization in global models of dust dispersion.

Modeling and Evaluation of the Global Sea-Salt Aerosol Distribution: Sensitivity to Emission Schemes and Resolution Effects at Coastal/Orographic Sites

NASA Technical Reports Server (NTRS)

Spada, M.; Jorba, O.; Perez Garcia-Pando, C.; Janjic, Z.; Baldasano, J. M.

2013-01-01

One of the major sources of uncertainty in model estimates of the global sea-salt aerosol distribution is the emission parameterization. We evaluate a new sea-salt aerosol life cycle module coupled to the online multi-scale chemical transport model NMMB/BSC-CTM. We compare 5 year global simulations using five state-of-the-art sea-salt open-ocean emission schemes with monthly averaged coarse aerosol optical depth (AOD) from selected AERONET sun photometers, surface concentration measurements from the University of Miami's Ocean Aerosol Network, and measurements from two NOAA/PMEL cruises (AEROINDOEX and ACE1). Model results are highly sensitive to the introduction of sea-surface-temperature (SST)-dependent emissions and to the accounting of spume particles production. Emission ranges from 3888 teragrams per year to 8114 teragrams per year, lifetime varies between 7.3 hours and 11.3 hours, and the average column mass load is between 5.0 teragrams and 7.2 teragrams. Coarse AOD is reproduced with an overall correlation of around 0.5 and with normalized biases ranging from +8.8 percent to +38.8 percent. Surface concentration is simulated with normalized biases ranging from minus 9.5 percent to plus 28 percent and the overall correlation is around 0.5. Our results indicate that SST-dependent emission schemes improve the overall model performance in reproducing surface concentrations. On the other hand, they lead to an overestimation of the coarse AOD at tropical latitudes, although it may be affected by uncertainties in the comparison due to the use of all-sky model AOD, the treatment of water uptake, deposition and optical properties in the model and/or an inaccurate size distribution at emission.

Dispersion of aerosol particles in the atmosphere: Fukushima

NASA Astrophysics Data System (ADS)

Haszpra, Tímea; Lagzi, István; Tél, Tamás

2013-04-01

Investigation of dispersion and deposition of aerosol particles in the atmosphere is an essential issue, because they have an effect on the biosphere and atmosphere. Moreover, aerosol particles have different transport properties and chemical and physical transformations in the atmosphere compared to gas phase air pollutants. The motion of a particle is described by a set of ordinary differential equations. The large-scale dynamics in the horizontal direction can be described by the equations of passive scalar advection, but in the vertical direction a well-defined terminal velocity should be taken into account as a term added to the vertical wind component. In the planetary boundary layer turbulent diffusion has an important role in the particle dispersion, which is taken into account by adding stochastic terms to the deterministic equations above. Wet deposition is also an essential process in the lower levels of the atmosphere, however, its precise parameterization is a challenge. For the simulations the wind field and other necessary data were taken from the ECMWF ERA-Interim database. In the case of the Fukushima Daiichi nuclear disaster (March-April 2011) radioactive aerosol particles were also released in the planetary boundary layer. Simulations (included the continuous and varying emission from the nuclear power plant) will be presented for the period of 14-23 March. Results show that wet deposition also has to be taken into consideration in the lower levels of the atmosphere. Furthermore, dynamical system characteristics are evaluated for the aerosol particle dynamics. The escape rate of particles was estimated both with and without turbulent diffusion, and in both cases when there was no wet deposition and also when wet deposition was taken into consideration.

Sensitivity of biogenic volatile organic compounds to land surface parameterizations and vegetation distributions in California

NASA Astrophysics Data System (ADS)

Zhao, Chun; Huang, Maoyi; Fast, Jerome D.; Berg, Larry K.; Qian, Yun; Guenther, Alex; Gu, Dasa; Shrivastava, Manish; Liu, Ying; Walters, Stacy; Pfister, Gabriele; Jin, Jiming; Shilling, John E.; Warneke, Carsten

2016-05-01

Current climate models still have large uncertainties in estimating biogenic trace gases, which can significantly affect atmospheric chemistry and secondary aerosol formation that ultimately influences air quality and aerosol radiative forcing. These uncertainties result from many factors, including uncertainties in land surface processes and specification of vegetation types, both of which can affect the simulated near-surface fluxes of biogenic volatile organic compounds (BVOCs). In this study, the latest version of Model of Emissions of Gases and Aerosols from Nature (MEGAN v2.1) is coupled within the land surface scheme CLM4 (Community Land Model version 4.0) in the Weather Research and Forecasting model with chemistry (WRF-Chem). In this implementation, MEGAN v2.1 shares a consistent vegetation map with CLM4 for estimating BVOC emissions. This is unlike MEGAN v2.0 in the public version of WRF-Chem that uses a stand-alone vegetation map that differs from what is used by land surface schemes. This improved modeling framework is used to investigate the impact of two land surface schemes, CLM4 and Noah, on BVOCs and examine the sensitivity of BVOCs to vegetation distributions in California. The measurements collected during the Carbonaceous Aerosol and Radiative Effects Study (CARES) and the California Nexus of Air Quality and Climate Experiment (CalNex) conducted in June of 2010 provided an opportunity to evaluate the simulated BVOCs. Sensitivity experiments show that land surface schemes do influence the simulated BVOCs, but the impact is much smaller than that of vegetation distributions. This study indicates that more effort is needed to obtain the most appropriate and accurate land cover data sets for climate and air quality models in terms of simulating BVOCs, oxidant chemistry and, consequently, secondary organic aerosol formation.

Spatial Variability of CCN Sized Aerosol Particles

NASA Astrophysics Data System (ADS)

Asmi, A.; Väänänen, R.

2014-12-01

The computational limitations restrict the grid size used in GCM models, and for many cloud types they are too large when compared to the scale of the cloud formation processes. Several parameterizations for e.g. convective cloud formation exist, but information on spatial subgrid variation of the cloud condensation nuclei (CCNs) sized aerosol concentration is not known. We quantify this variation as a function of the spatial scale by using datasets from airborne aerosol measurement campaigns around the world including EUCAARI LONGREX, ATAR, INCA, INDOEX, CLAIRE, PEGASOS and several regional airborne campaigns in Finland. The typical shapes of the distributions are analyzed. When possible, we use information obtained by CCN counters. In some other cases, we use particle size distribution measured by for example SMPS to get approximated CCN concentration. Other instruments used include optical particle counters or condensational particle counters. When using the GCM models, the CCN concentration used for each the grid-box is often considered to be either flat, or as an arithmetic mean of the concentration inside the grid-box. However, the aircraft data shows that the concentration values are often lognormal distributed. This, combined with the subgrid variations in the land use and atmospheric properties, might cause that the aerosol-cloud interactions calculated by using mean values to vary significantly from the true effects both temporary and spatially. This, in turn, can cause non-linear bias into the GCMs. We calculate the CCN aerosol concentration distribution as a function of different spatial scales. The measurements allow us to study the variation of these distributions within from hundreds of meters up to hundreds of kilometers. This is used to quantify the potential error when mean values are used in GCMs.

Assessing the influence of NOx concentrations and relative humidity on secondary organic aerosol yields from α-pinene photo-oxidation through smog chamber experiments and modelling calculations

NASA Astrophysics Data System (ADS)

Stirnweis, Lisa; Marcolli, Claudia; Dommen, Josef; Barmet, Peter; Frege, Carla; Platt, Stephen M.; Bruns, Emily A.; Krapf, Manuel; Slowik, Jay G.; Wolf, Robert; Prévôt, Andre S. H.; Baltensperger, Urs; El-Haddad, Imad

2017-04-01

Secondary organic aerosol (SOA) yields from the photo-oxidation of α-pinene were investigated in smog chamber (SC) experiments at low (23-29 %) and high (60-69 %) relative humidity (RH), various NOx / VOC ratios (0.04-3.8) and with different aerosol seed chemical compositions (acidic to neutralized sulfate-containing or hydrophobic organic). A combination of a scanning mobility particle sizer and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer was used to determine SOA mass concentration and chemical composition. We used a Monte Carlo approach to parameterize smog chamber SOA yields as a function of the condensed phase absorptive mass, which includes the sum of OA and the corresponding bound liquid water content. High RH increased SOA yields by up to 6 times (1.5-6.4) compared to low RH. The yields at low NOx / VOC ratios were in general higher compared to yields at high NOx / VOC ratios. This NOx dependence follows the same trend as seen in previous studies for α-pinene SOA. A novel approach of data evaluation using volatility distributions derived from experimental data served as the basis for thermodynamic phase partitioning calculations of model mixtures in this study. These calculations predict liquid-liquid phase separation into organic-rich and electrolyte phases. At low NOx conditions, equilibrium partitioning between the gas and liquid phases can explain most of the increase in SOA yields observed at high RH, when in addition to the α-pinene photo-oxidation products described in the literature, fragmentation products are added to the model mixtures. This increase is driven by both the increase in the absorptive mass and the solution non-ideality described by the compounds' activity coefficients. In contrast, at high NOx, equilibrium partitioning alone could not explain the strong increase in the yields with RH. This suggests that other processes, e.g. reactive uptake of semi-volatile species into the liquid phase, may occur and be enhanced at higher RH, especially for compounds formed under high NOx conditions, e.g. carbonyls.

A new temperature- and humidity-dependent surface site density approach for deposition ice nucleation

NASA Astrophysics Data System (ADS)

Steinke, I.; Hoose, C.; Möhler, O.; Connolly, P.; Leisner, T.

2015-04-01

Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol surface area concentration. Additionally, a contact angle parameterization according to classical nucleation theory was fitted to the experimental data in order to relate the ice nucleation efficiencies to contact angle distributions. From this study it can be concluded that the INAS density formulation is a very useful tool to describe the temperature- and humidity-dependent ice nucleation efficiency of ATD particles. Deposition nucleation on ATD particles can be described by a temperature- and relative-humidity-dependent INAS density function ns(T, Sice) with ns(xtherm) = 1.88 ×105 · exp(0.2659 · xtherm) [m-2] , (1) where the temperature- and saturation-dependent function xtherm is defined as xtherm = -(T-273.2)+(Sice-1) ×100, (2) with the saturation ratio with respect to ice Sice >1 and within a temperature range between 226 and 250 K. For lower temperatures, xtherm deviates from a linear behavior with temperature and relative humidity over ice. Also, two different approaches for describing the time dependence of deposition nucleation initiated by ATD particles are proposed. Box model estimates suggest that the time-dependent contribution is only relevant for small cooling rates and low number fractions of ice-active particles.

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

NASA Astrophysics Data System (ADS)

Hummel, Matthias; Egill Kristjansson, Jon

2016-04-01

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

Oligomer formation in the troposphere: from experimental knowledge to 3-D modeling

NASA Astrophysics Data System (ADS)

Lemaire, V.; Coll, I.; Couvidat, F.; Mouchel-Vallon, C.; Seigneur, C.; Siour, G.

2015-10-01

The organic fraction of atmospheric aerosols has proven to be a critical element of air quality and climate issues. However, its composition and the aging processes it undergoes remain insufficiently understood. This work builds on laboratory knowledge to simulate the formation of oligomers from biogenic secondary organic aerosol (BSOA) in the troposphere at the continental scale. We compare the results of two different modeling approaches, a 1st-order kinetic process and a pH-dependent parameterization, both implemented in the CHIMERE air quality model (AQM), to simulate the spatial and temporal distribution of oligomerized SOA over western Europe. Our results show that there is a strong dependence of the results on the selected modeling approach: while the irreversible kinetic process leads to the oligomerization of about 50 % of the total BSOA mass, the pH-dependent approach shows a broader range of impacts, with a strong dependency on environmental parameters (pH and nature of aerosol) and the possibility for the process to be reversible. In parallel, we investigated the sensitivity of each modeling approach to the representation of SOA precursor solubility (Henry's law constant values). Finally, the pros and cons of each approach for the representation of SOA aging are discussed and recommendations are provided to improve current representations of oligomer formation in AQMs.

CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: seasonal and diel variations and impact of anthropogenic emissions

NASA Astrophysics Data System (ADS)

Thalman, Ryan; de Sá, Suzane S.; Palm, Brett B.; Barbosa, Henrique M. J.; Pöhlker, Mira L.; Lizabeth Alexander, M.; Brito, Joel; Carbone, Samara; Castillo, Paulo; Day, Douglas A.; Kuang, Chongai; Manzi, Antonio; Ng, Nga Lee; Sedlacek, Arthur J., III; Souza, Rodrigo; Springston, Stephen; Watson, Thomas; Pöhlker, Christopher; Pöschl, Ulrich; Andreae, Meinrat O.; Artaxo, Paulo; Jimenez, Jose L.; Martin, Scot T.; Wang, Jian

2017-10-01

During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60 km downwind of the city of Manaus, Brazil, in central Amazonia for 1 year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κCCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg) was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely due to an increase in sulfate volume fraction. During both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ˜ 0. 15 is consistent with the largely uniform and high O : C value (˜ 0. 8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O : C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O : C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF (positive matrix factorization) analysis of AMS (aerosol mass spectrometry) spectra, were estimated through multivariable linear regression. For the SOA factors, the variation of the κ value with O : C agrees well with the linear relationship reported from earlier laboratory studies of SOA hygroscopicity. On the other hand, the variation in O : C of ambient aerosol organics is largely driven by the variation in the volume fractions of POA and SOA factors, which have very different O : C values. As POA factors have hygroscopicity values well below the linear relationship between SOA hygroscopicity and O : C, mixtures with different POA and SOA fractions exhibit a steeper slope for the increase in κorg with O : C, as observed during this and earlier field studies. This finding helps better understand and reconcile the differences in the relationships between κorg and O : C observed in laboratory and field studies, therefore providing a basis for improved parameterization in global models, especially in a tropical context.

Parameterization of dust emissions in the global atmospheric chemistry-climate model EMAC: impact of nudging and soil properties

NASA Astrophysics Data System (ADS)

Astitha, M.; Lelieveld, J.; Abdel Kader, M.; Pozzer, A.; de Meij, A.

2012-11-01

Airborne desert dust influences radiative transfer, atmospheric chemistry and dynamics, as well as nutrient transport and deposition. It directly and indirectly affects climate on regional and global scales. Two versions of a parameterization scheme to compute desert dust emissions are incorporated into the atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy2.41 Atmospheric Chemistry). One uses a globally uniform soil particle size distribution, whereas the other explicitly accounts for different soil textures worldwide. We have tested these two versions and investigated the sensitivity to input parameters, using remote sensing data from the Aerosol Robotic Network (AERONET) and dust concentrations and deposition measurements from the AeroCom dust benchmark database (and others). The two versions are shown to produce similar atmospheric dust loads in the N-African region, while they deviate in the Asian, Middle Eastern and S-American regions. The dust outflow from Africa over the Atlantic Ocean is accurately simulated by both schemes, in magnitude, location and seasonality. Approximately 70% of the modelled annual deposition data and 70-75% of the modelled monthly aerosol optical depth (AOD) in the Atlantic Ocean stations lay in the range 0.5 to 2 times the observations for all simulations. The two versions have similar performance, even though the total annual source differs by ~50%, which underscores the importance of transport and deposition processes (being the same for both versions). Even though the explicit soil particle size distribution is considered more realistic, the simpler scheme appears to perform better in several locations. This paper discusses the differences between the two versions of the dust emission scheme, focusing on their limitations and strengths in describing the global dust cycle and suggests possible future improvements.

A global lightning parameterization based on statistical relationships among environmental factors, aerosols, and convective clouds in the TRMM climatology

NASA Astrophysics Data System (ADS)

Stolz, Douglas C.; Rutledge, Steven A.; Pierce, Jeffrey R.; van den Heever, Susan C.

2017-07-01

The objective of this study is to determine the relative contributions of normalized convective available potential energy (NCAPE), cloud condensation nuclei (CCN) concentrations, warm cloud depth (WCD), vertical wind shear (SHEAR), and environmental relative humidity (RH) to the variability of lightning and radar reflectivity within convective features (CFs) observed by the Tropical Rainfall Measuring Mission (TRMM) satellite. Our approach incorporates multidimensional binned representations of observations of CFs and modeled thermodynamics, kinematics, and CCN as inputs to develop approximations for total lightning density (TLD) and the average height of 30 dBZ radar reflectivity (AVGHT30). The results suggest that TLD and AVGHT30 increase with increasing NCAPE, increasing CCN, decreasing WCD, increasing SHEAR, and decreasing RH. Multiple-linear approximations for lightning and radar quantities using the aforementioned predictors account for significant portions of the variance in the binned data set (R2 ≈ 0.69-0.81). The standardized weights attributed to CCN, NCAPE, and WCD are largest, the standardized weight of RH varies relative to other predictors, while the standardized weight for SHEAR is comparatively small. We investigate these statistical relationships for collections of CFs within various geographic areas and compare the aerosol (CCN) and thermodynamic (NCAPE and WCD) contributions to variations in the CF population in a partial sensitivity analysis based on multiple-linear regression approximations computed herein. A global lightning parameterization is developed; the average difference between predicted and observed TLD decreases from +21.6 to +11.6% when using a hybrid approach to combine separate approximations over continents and oceans, thus highlighting the need for regionally targeted investigations in the future.

Implications of Low Volatility SOA and Gas-Phase Fragmentation Reactions on SOA Loadings and their Spatial and Temporal Evolution in the Atmosphere

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

Shrivastava, ManishKumar B.; Zelenyuk, Alla; Imre, Dan

2013-04-27

Recent laboratory and field measurements by a number of groups show that secondary organic aerosol (SOA) evaporates orders of magnitude slower than traditional models assume. In addition, chemical transport models using volatility basis set (VBS) SOA schemes neglect gas-phase fragmentation reactions, which are known to be extremely important. In this work, we present modeling studies to investigate the implications of non-evaporating SOA and gas-phase fragmentation reactions. Using the 3-D chemical transport model, WRF-Chem, we show that previous parameterizations, which neglect fragmentation during multi-generational gas-phase chemistry of semi-volatile/inter-mediate volatility organics ("aging SIVOC"), significantly over-predict SOA as compared to aircraft measurements downwindmore » of Mexico City. In sharp contrast, the revised models, which include gas-phase fragmentation, show much better agreement with measurements downwind of Mexico City. We also demonstrate complex differences in spatial SOA distributions when we transform SOA to non-volatile secondary organic aerosol (NVSOA) to account for experimental observations. Using a simple box model, we show that for same amount of SOA precursors, earlier models that do not employ multi-generation gas-phase chemistry of precursors ("non-aging SIVOC"), produce orders of magnitude lower SOA than "aging SIVOC" parameterizations both with and without fragmentation. In addition, traditional absorptive partitioning models predict almost complete SOA evaporation at farther downwind locations for both "non-aging SIVOC" and "aging SIVOC" with fragmentation. In contrast, in our revised approach, SOA transformed to NVSOA implies significantly higher background concentrations as it remains in particle phase even under highly dilute conditions. This work has significant implications on understanding the role of multi-generational chemistry and NVSOA formation on SOA evolution in the atmosphere.« less

Parameterization of cloud glaciation by atmospheric dust

NASA Astrophysics Data System (ADS)

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

2016-04-01

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

Global Performance of a Fast Parameterization Scheme for Estimating Surface Solar Radiation from MODIS data

NASA Astrophysics Data System (ADS)

Tang, W.; Yang, K.; Sun, Z.; Qin, J.; Niu, X.

2016-12-01

A fast parameterization scheme named SUNFLUX is used in this study to estimate instantaneous surface solar radiation (SSR) based on products from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor onboard both Terra and Aqua platforms. The scheme mainly takes into account the absorption and scattering processes due to clouds, aerosols and gas in the atmosphere. The estimated instantaneous SSR is evaluated against surface observations obtained from seven stations of the Surface Radiation Budget Network (SURFRAD), four stations in the North China Plain (NCP) and 40 stations of the Baseline Surface Radiation Network (BSRN). The statistical results for evaluation against these three datasets show that the relative root-mean-square error (RMSE) values of SUNFLUX are less than 15%, 16% and 17%, respectively. Daily SSR is derived through temporal upscaling from the MODIS-based instantaneous SSR estimates, and is validated against surface observations. The relative RMSE values for daily SSR estimates are about 16% at the seven SURFRAD stations, four NCP stations, 40 BSRN stations and 90 China Meteorological Administration (CMA) radiation stations.

New Particle Formation (NPF) within the volcanic plume of Piton de la Fournaise at Maïdo observatory (21.1° S 55.4° E), on La Réunion Island.

NASA Astrophysics Data System (ADS)

Foucart, Brice; Sellegri, Karine; Tulet, Pierre

2017-04-01

Volcanic emissions can have a significant effect on the environment, and may impact climate through the injection of gases and aerosols in the upper troposphere where they have a long residence time and an impact on clouds formation [Makkonen et al., 2012]. The Piton de La Fournaise volcano on La Réunion Island erupted four times in 2015 [Peltier et al., 2016] and volcanic particles were ejected in the atmosphere both as primary particles rapidly deposited due to their large size and secondary particles mainly derived from oxidation of sulphur dioxide. In this study, we focus on this secondary process of forming new aerosol particles (NPF). Sulphuric acid (H2SO4), resulting from SO2 oxidation in the presence of light, is known to be the major precursor to nucleation events [kulmala et al., 2004 and Kerminen et al., 2010]. During the April 2007 eruption of Piton de la Fournaise, Tulet and Villeneuve [2010] estimated by OMI and CALIOP space sensors analysis a total SO2 release of 230 kt, among of which 60 kt that have been transformed into H2SO4 supposing NPF processes. However, the nucleation phenomenon has rarely been directly observed in volcanic environments [Kulmala et al., 2004] except for Mauna Loa volcano on Hawaii [Weber et al., 1995] and for Eyjafjallajokull plume caught at the Puy de Dôme station [Boulon et al., 2011]. Within the STRAP project (Synergie Trans-disciplinaire pour Répondre aux Aléas de Panache Volcanique), a multidisciplinary tracking of a volcanic gas and aerosol plume that has been conducted by Tulet et al. [2016] through a strong collaboration between volcanologists and meteorologists. Part of the measurements were performed at Maïdo observatory (21.1° S 55.4° E) which is located at 40 km from the volcano but which has been reached several times by the volcanic plume, each time accompanied by a NPF event. A statistical analysis of the influence of the plume presence on the NPF frequency, intensity and new particles growth rates is performed over a one year observation period. Then, focusing on the NPF events and according to Kuang et al. [2007], we developed a parameterization of the nucleation rate as a function of a proxy of sulphuric acid within the volcanic plume which can be used in meteorological meso-scale models. Keywords: aerosols, nucleation, volcanic plume, parameterization

Evolution of aerosol downwind of a major highway

NASA Astrophysics Data System (ADS)

Liggio, J.; Staebler, R. M.; Brook, J.; Li, S.; Vlasenko, A. L.; Sjostedt, S. J.; Gordon, M.; Makar, P.; Mihele, C.; Evans, G. J.; Jeong, C.; Wentzell, J. J.; Lu, G.; Lee, P.

2010-12-01

Primary aerosol from traffic emissions can have a considerable impact local and regional scale air quality. In order to assess the effect of these emissions and of future emissions scenarios, air quality models are required which utilize emissions representative of real world conditions. Often, the emissions processing systems which provide emissions input for the air quality models rely on laboratory testing of individual vehicles under non-ambient conditions. However, on the sub-grid scale particle evolution may lead to changes in the primary emitted size distribution and gas-particle partitioning that are not properly considered when the emissions are ‘instantly mixed’ within the grid volume. The affect of this modeling convention on model results is not well understood. In particular, changes in organic gas/particle partitioning may result in particle evaporation or condensation onto pre-existing aerosol. The result is a change in the particle distribution and/or an increase in the organic mass available for subsequent gas-phase oxidation. These effects may be missing from air-quality models, and a careful analysis of field data is necessary to quantify their impact. A study of the sub-grid evolution of aerosols (FEVER; Fast Evolution of Vehicle Emissions from Roadways) was conducted in the Toronto area in the summer of 2010. The study included mobile measurements of particle size distributions with a Fast mobility particle sizer (FMPS), aerosol composition with an Aerodyne aerosol mass spectrometer (AMS), black carbon (SP2, PA, LII), VOCs (PTR-MS) and other trace gases. The mobile laboratory was used to measure the concentration gradient of the emissions at perpendicular distances from the highway as well as the physical and chemical evolution of the aerosol. Stationary sites at perpendicular distances and upwind from the highway also monitored the particle size distribution. In addition, sonic anemometers mounted on the mobile lab provided measurements of turbulent dispersion as a function of distance from the highway, and a traffic camera was used to determine traffic density, composition and speed. These measurements differ from previous studies in that turbulence is measured under realistic conditions and hence the relationship of the aerosol evolution to atmospheric stability and mixing will also be quantified. Preliminary results suggest that aerosol size and composition does change on the sub-grid scale, and sub-grid scale parameterizations of turbulence and particle chemistry should be included in models to accurately represent these effects.

New particle dependant parameterizations of heterogeneous freezing processes.

NASA Astrophysics Data System (ADS)

Diehl, Karoline; Mitra, Subir K.

2014-05-01

For detailed investigations of cloud microphysical processes an adiabatic air parcel model with entrainment is used. It represents a spectral bin model which explicitly solves the microphysical equations. The initiation of the ice phase is parameterized and describes the effects of different types of ice nuclei (mineral dust, soot, biological particles) in immersion, contact, and deposition modes. As part of the research group INUIT (Ice Nuclei research UnIT), existing parameterizations have been modified for the present studies and new parameterizations have been developed mainly on the basis of the outcome of INUIT experiments. Deposition freezing in the model is dependant on the presence of dry particles and on ice supersaturation. The description of contact freezing combines the collision kernel of dry particles with the fraction of frozen drops as function of temperature and particle size. A new parameterization of immersion freezing has been coupled to the mass of insoluble particles contained in the drops using measured numbers of ice active sites per unit mass. Sensitivity studies have been performed with a convective temperature and dew point profile and with two dry aerosol particle number size distributions. Single and coupled freezing processes are studied with different types of ice nuclei (e.g., bacteria, illite, kaolinite, feldspar). The strength of convection is varied so that the simulated cloud reaches different levels of temperature. As a parameter to evaluate the results the ice water fraction is selected which is defined as the relation of the ice water content to the total water content. Ice water fractions between 0.1 and 0.9 represent mixed-phase clouds, larger than 0.9 ice clouds. The results indicate the sensitive parameters for the formation of mixed-phase and ice clouds are: 1. broad particle number size distribution with high number of small particles, 2. temperatures below -25°C, 3. specific mineral dust particles as ice nuclei such as illite or montmorillonite. Coupled cases of deposition and contact freezing show that they are hardly in competition because of differences in the preferred particle sizes. In the contact mode, small particles are less efficient for collisions as well as less efficient as ice nuclei so that these are available for deposition freezing. On the other hand, immersion freezing is the dominant process when it is coupled with deposition freezing. As it is initiated earlier the formed ice particles consume water vapor for growing. The competition of combined contact and immersion freezing leads to lower ice water contents because more ice particles are formed via the immersion mode. In general, ice clouds and mixed-phase clouds with high ice water fractions are not directly the result of primary ice formation but of secondary ice formation and growth of ice particles at the expense of liquid drops.

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: Results from DISCOVER-AQ California

DOE PAGES

Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; ...

2016-05-02

The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno–Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) andmore » an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM 1) concentration was 31.0 µg m −3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C  =  0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O / C  =  0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C  =  0.33; BBOA2: 20 % of total OA, O / C  =  0.60) most likely associated with residential space heating from wood combustion, and semivolatile oxygenated OA (SV-OOA; 16 % of total OA, O / C  =  0.63) and low-volatility oxygenated OA (LV-OOA; 24 % of total OA, O / C  =  0.90) formed via chemical reactions in the atmosphere. Large differences in aerosol chemistry at Fresno were observed between the current campaign (winter 2013) and a previous campaign in winter 2010, most notably that PM 1 concentrations were nearly 3 times higher in 2013 than in 2010. These variations were attributed to differences in the meteorological conditions, which influenced primary emissions and secondary aerosol formation. In particular, COA and BBOA concentrations were greater in 2013 than 2010, where colder temperatures in 2013 likely resulted in increased biomass burning activities. The influence from a nighttime formed residual layer that mixed down in the morning was found to be much more intense in 2013 than 2010, leading to sharp increases in ground-level concentrations of secondary aerosol species including nitrate, sulfate, and OOA, in the morning between 08:00 and 12:00 PST. This is an indication that nighttime chemical reactions may have played a more important role in 2013. As solar radiation was stronger in 2013 the higher nitrate and OOA concentrations in 2013 could also be partly due to greater photochemical production of secondary aerosol species. The greater solar radiation and larger range in temperature in 2013 also likely led to both SV-OOA and LV-OOA being observed in 2013 whereas only a single OOA factor was identified in 2010.« less

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modeling of complete high time-resolution aerosol mass spectra

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-08-01

Receptor modeling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's Canadian Regional and Urban Investigation System for Environmental Research (CRUISER) mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach compared to the more common method of analyzing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulfate- and oxygenated organic aerosol-containing factor (Sulfate-OA); an ammonium nitrate- and oxygenated organic aerosol-containing factor (Nitrate-OA); an ammonium chloride-containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analyzing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case the Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability to understand better the chemical nature of atypical factors from high-resolution mass spectra. Second, utilizing PMF to extract factors containing inorganic species allowed for the determination of the extent of neutralization, which could have implications for aerosol parameterization. Third, subtler differences in organic aerosol components were resolved through the incorporation of inorganic mass into the PMF matrix. The additional temporal features provided by the inorganic aerosol components allowed for the resolution of more types of oxygenated organic aerosol than could be reliably resolved from PMF of organics alone. Comparison of findings from the PMFFull MS and PMFOrg MS methods showed that for the Windsor airshed, the PMFFull MS method enabled additional conclusions to be drawn in terms of aerosol sources and chemical processes. While performing PMFOrg MS can provide important distinctions between types of organic aerosol, it is shown that including inorganic species in the PMF analysis can permit further apportionment of organics for unit mass resolution AMS mass spectra.

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-02-01

Receptor modelling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's CRUISER mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach was compared to the more common method of analysing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulphate and oxygenated organic aerosol containing factor (Sulphate-OA); an ammonium nitrate and oxygenated organic aerosol containing factor (Nitrate-OA); an ammonium chloride containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analysing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case, an Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability to better understand the chemical nature of atypical factors from high resolution mass spectra. Second, utilizing PMF to extract factors containing inorganic species allowed for the determination of extent of neutralization, which could have implications for aerosol parameterization. Third, subtler differences in organic aerosol components were resolved through the incorporation of inorganic mass into the PMF matrix. The additional temporal features provided by the inorganic aerosol components allowed for the resolution of more types of oxygenated organic aerosol than could be reliably resolved from PMF of organics alone. Comparison of findings from the PMFFull MS and PMFOrg MS methods showed that for the Windsor airshed, the PMFFull MS method enabled additional conclusions to be drawn in terms of aerosol sources and chemical processes. While performing PMFOrg MS can provide important distinctions between types of organic aerosol, it is shown that including inorganic species in the PMF analysis can permit further apportionment of organics for unit mass resolution AMS mass spectra.

Aerosol Activation Properties within and above Mixing Layer in the North China Plain

NASA Astrophysics Data System (ADS)

Deng, Z.; Ran, L.

2013-12-01

Aerosol particles, serving as cloud condensation nuclei (CCN), may modify the properties of clouds and have an impact on climate. The vertical distribution of aerosols and their activation properties is critical to quantify the effect of aerosols on clouds. An intensive field campaign, Vertical Observations of trace Gases and Aerosols in the North China Plain (VOGA-NCP 2013), was conducted in the North China Plain during the late July and early August 2013 to measure the vertical profiles of atmospheric components in this polluted region and estimate their effects on atmospheric environment and climate. Aerosols were measured with in-situ instruments and Lidar. Particularly, the aerosols were collected at 1000 m height with a 1 m3 bag sampler attached to a tethered balloon, and subsequently measured with combined scanning mobility particle sizer (SMPS) and CCN counter. Comparisons of size-resolved activation ratios at ground level and 1000 m height showed that aerosols in upper atmosphere were not only less concentrated, but also less CCN-active than those at the surface. The difference in aerosol properties between upper atmosphere and the ground indicates that the analysis of impacts of aerosols on cloud might be misleading in heavily polluted region based on the relationship of cloud properties and surface aerosols or column without considering the vertical distribution of aerosol activation abilities.

Parameterization of planetary wave breaking in the middle atmosphere

NASA Technical Reports Server (NTRS)

Garcia, Rolando R.

1991-01-01

A parameterization of planetary wave breaking in the middle atmosphere has been developed and tested in a numerical model which includes governing equations for a single wave and the zonal-mean state. The parameterization is based on the assumption that wave breaking represents a steady-state equilibrium between the flux of wave activity and its dissipation by nonlinear processes, and that the latter can be represented as linear damping of the primary wave. With this and the additional assumption that the effect of breaking is to prevent further amplitude growth, the required dissipation rate is readily obtained from the steady-state equation for wave activity; diffusivity coefficients then follow from the dissipation rate. The assumptions made in the derivation are equivalent to those commonly used in parameterizations for gravity wave breaking, but the formulation in terms of wave activity helps highlight the central role of the wave group velocity in determining the dissipation rate. Comparison of model results with nonlinear calculations of wave breaking and with diagnostic determinations of stratospheric diffusion coefficients reveals remarkably good agreement, and suggests that the parameterization could be useful for simulating inexpensively, but realistically, the effects of planetary wave transport.

Analysis of the Diurnal Variation of the Global Electric Circuit Obtained From Different Numerical Models

NASA Astrophysics Data System (ADS)

Jánský, Jaroslav; Lucas, Greg M.; Kalb, Christina; Bayona, Victor; Peterson, Michael J.; Deierling, Wiebke; Flyer, Natasha; Pasko, Victor P.

2017-12-01

This work analyzes different current source and conductivity parameterizations and their influence on the diurnal variation of the global electric circuit (GEC). The diurnal variations of the current source parameterizations obtained using electric field and conductivity measurements from plane overflights combined with global Tropical Rainfall Measuring Mission satellite data give generally good agreement with measured diurnal variation of the electric field at Vostok, Antarctica, where reference experimental measurements are performed. An approach employing 85 GHz passive microwave observations to infer currents within the GEC is compared and shows the best agreement in amplitude and phase with experimental measurements. To study the conductivity influence, GEC models solving the continuity equation in 3-D are used to calculate atmospheric resistance using yearly averaged conductivity obtained from the global circulation model Community Earth System Model (CESM). Then, using current source parameterization combining mean currents and global counts of electrified clouds, if the exponential conductivity is substituted by the conductivity from CESM, the peak to peak diurnal variation of the ionospheric potential of the GEC decreases from 24% to 20%. The main reason for the change is the presence of clouds while effects of 222Rn ionization, aerosols, and topography are less pronounced. The simulated peak to peak diurnal variation of the electric field at Vostok is increased from 15% to 18% from the diurnal variation of the global current in the GEC if conductivity from CESM is used.

A 3D parameterization of iron atmospheric deposition to the global ocean

NASA Astrophysics Data System (ADS)

Myriokefalitakis, Stelios; Krol, Maarten C.; van Noije, Twan P. C.; Le Sager, Philippe

2017-04-01

Atmospheric deposition of trace constituents, both of natural and anthropogenic origin, can act as a nutrient source into the open ocean and affect marine ecosystem functioning and subsequently the exchange of CO2 between the atmosphere and the global ocean. Dust is known as a major source of nutrients to the global ocean, but only a fraction of these nutrients is released in soluble form that can be assimilated by the ecosystems. Iron (Fe) is a key micronutrient that significantly modulates gross primary production in High-Nutrient-Low-Chlorophyll (HNLC) oceans, where macronutrients like nitrate are abundant but primary production is limited by Fe scarcity. The global atmospheric Fe cycle is here parameterized in the state-of-the-art global Earth System Model EC-Earth. The model takes into account the primary emissions of both insoluble and soluble Fe, associated with dusts and combustion processes. The impact of atmospheric acidity on mineral solubility is parameterized based on updated experimental and theoretical findings, and model results are evaluated against available observations. The link between the soluble Fe atmospheric deposition and anthropogenic sources is also investigated. Overall, the response of the chemical composition of nutrient containing aerosols to atmospheric composition changes is demonstrated and quantified. This work has been financed by the Marie-Curie H2020-MSCA-IF-2015 grant (ID 705652) ODEON (Online DEposition over OceaNs: Modeling the effect of air pollution on ocean bio-geochemistry in an Earth System Model).

Airborne observations of bioaerosol over the Southeast United States using a Wideband Integrated Bioaerosol Sensor

NASA Astrophysics Data System (ADS)

Ziemba, Luke D.; Beyersdorf, Andreas J.; Chen, Gao; Corr, Chelsea A.; Crumeyrolle, Suzanne N.; Diskin, Glenn; Hudgins, Charlie; Martin, Robert; Mikoviny, Tomas; Moore, Richard; Shook, Michael; Thornhill, K. Lee; Winstead, Edward L.; Wisthaler, Armin; Anderson, Bruce E.

2016-07-01

Biological aerosols represent a diverse subset of particulate matter that is emitted directly to the atmosphere in the form of (but not limited to) bacteria, fungal spores, pollens, viruses, and plant debris. These particles can have local air quality implications, but potentially play a larger climate role by acting as efficient ice nucleating particles (INPs) and cloud condensation nuclei. We have deployed a Wideband Integrated Bioaerosol Sensor on the NASA DC-8 aircraft to (1) quantify boundary layer (BL) variability of fluorescent biological aerosol particle (FBAP) concentrations in the Southeast United States (SEUS), (2) link this variability explicitly to land cover heterogeneity in the region, and (3) examine the vertical profile of bioaerosols in the context of convective vertical redistribution. Flight-averaged FBAP concentrations ranged between 0.1 and 0.43 scm-3 (cm-3 at standard temperature and pressure) with relatively homogeneous concentrations throughout the region; croplands showed the highest concentrations in the BL (0.37 scm-3), and lowest concentrations were associated with evergreen forests (0.24 scm-3). Observed FBAP concentrations are in generally good agreement with model parameterized emission rates for bacteria, and discrepancies are likely the result of fungal spore contributions. Shallow convection in the region is shown to be a relatively efficient lofting mechanism as the vertical transport efficiency of FBAP is at least equal to black carbon aerosol, suggesting that ground-level FBAP survives transport into the free troposphere to be available for INP activation. Comparison of the fraction of coarse-mode particles that were biological (fFBAP) suggested that the SEUS (fFBAP = 8.5%) was a much stronger source of bioaerosols than long-range transport during a Saharan Air Layer (SAL) dust event (fFBAP = 0.17%) or summertime marine emissions in the Gulf of Mexico (fFBAP = 0.73%).

Aerosol indirect effects -- general circulation model intercomparison and evaluation with satellite data

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

Quaas, Johannes; Ming, Yi; Menon, Surabi

2009-04-10

Aerosol indirect effects continue to constitute one of the most important uncertainties for anthropogenic climate perturbations. Within the international AEROCOM initiative, the representation of aerosol-cloud-radiation interactions in ten different general circulation models (GCMs) is evaluated using three satellite datasets. The focus is on stratiform liquid water clouds since most GCMs do not include ice nucleation effects, and none of the model explicitly parameterizes aerosol effects on convective clouds. We compute statistical relationships between aerosol optical depth (Ta) and various cloud and radiation quantities in a manner that is consistent between the models and the satellite data. It is found thatmore » the model-simulated influence of aerosols on cloud droplet number concentration (Nd) compares relatively well to the satellite data at least over the ocean. The relationship between Ta and liquid water path is simulated much too strongly by the models. It is shown that this is partly related to the representation of the second aerosol indirect effect in terms of autoconversion. A positive relationship between total cloud fraction (fcld) and Ta as found in the satellite data is simulated by the majority of the models, albeit less strongly than that in the satellite data in most of them. In a discussion of the hypotheses proposed in the literature to explain the satellite-derived strong fcld - Ta relationship, our results indicate that none can be identified as unique explanation. Relationships similar to the ones found in satellite data between Ta and cloud top temperature or outgoing long-wave radiation (OLR) are simulated by only a few GCMs. The GCMs that simulate a negative OLR - Ta relationship show a strong positive correlation between Ta and fcld The short-wave total aerosol radiative forcing as simulated by the GCMs is strongly influenced by the simulated anthropogenic fraction of Ta, and parameterisation assumptions such as a lower bound on Nd. Nevertheless, the strengths of the statistical relationships are good predictors for the aerosol forcings in the models. An estimate of the total short-wave aerosol forcing inferred from the combination of these predictors for the modelled forcings with the satellite-derived statistical relationships yields a global annual mean value of -1.5+-0.5 Wm-2. An alternative estimate obtained by scaling the simulated clear- and cloudy-sky forcings with estimates of anthropogenic Ta and satellite-retrieved Nd - Ta regression slopes, respectively, yields a global annual mean clear-sky (aerosol direct effect) estimate of -0.4+-0.2 Wm-2 and a cloudy-sky (aerosol indirect effect) estimate of -0.7+-0.5 Wm-2, with a total estimate of -1.2+-0.4 Wm-2.« less

Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

NASA Astrophysics Data System (ADS)

Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.

2015-09-01

We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 × 25 km2 resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the southeast US. OA is simulated successfully with a simple parameterization, assuming irreversible uptake of low-volatility products of hydrocarbon oxidation. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 25 % in the cloud convective layer at 1.5-3 km, and 15 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-]) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by OA. This would explain the long-term decline of ammonium aerosol in the southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 8-28 % (consistently biased low). The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines are due to shutdowns in both biogenic emissions and UV-driven photochemistry. Surface PM2.5 shows far less summer-to-winter decrease than AOD and we attribute this in part to the offsetting effect of weaker boundary layer ventilation. The SEAC4RS aircraft data demonstrate that AODs measured from space are consistent with surface PM2.5. This implies that satellites can be used reliably to infer surface PM2.5 over monthly timescales if a good CTM representation of the aerosol vertical profile is available.