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All sourcesNASA NTRSDOE OSTI
NASA NTRSDate not supplied

Creating Regional and Seasonal Climatologies of Marine and Dusty Marine Aerosol Lidar Ratios using MODIS AOD Constrained Retrievals and GOCART Model Simulations

The CALIPSO aerosol algorithms currently assign one lidar ratio (LR) value globally for each of the seven tropospheric aerosol types. In this study, MODIS total column aerosol optical depths (AODs) are used to constrain collocated CALIOP backscatter profiles in a Fernald inversion that infers aerosol LRs for CALIOP-classified marine and dusty marine aerosols. The GOCART aerosol model is leveraged to estimate the sea salt volume fractions (SSVFs) that are collocated with the CALIOP+MODIS LR retrievals. An inverse empirical relationship is found between the SSVFs and LRs (i.e., smaller SSVFs and larger LRs near coastlines, but the opposite in the remote oceans). This SSVF/LR relationship is applied to create regional and seasonal hybrid (i.e., retrieval & model-assisted) climatological LR maps so as to develop more robust LR selections for marine and dusty marine aerosols in the CALIPSO algorithms. These analyses also provide critical LR information for the next generation of spaceborne elastic backscatter lidars.

Travis D. Toth↗
NASA NTRSDate not supplied

PACE Microphysical Aerosol Properties from Polarimetry (PACE-MAPP)

We present the Plankton, Aerosols, Clouds and Ecosystems Microphysical Aerosol Properties from Polarimetry (PACE-MAPP) polarimetric remote sensing algorithm developed for the newly launched NASA PACE satellite observing system. The objective of PACE-MAPP is to retrieve detailed fine-mode (marine, pollution and smoke) and coarse-mode (sea-salt and dust) aerosol properties over the ocean for a range of light to heavy aerosol loadings using PACE’s polarimetric-imaging capabilities at multiple angles and wavelengths from the ultraviolet (UV) to the near-infrared (NIR). An additional objective for PACE-MAPP is to discriminate aerosols from thin clouds. The PACE-MAPP polarimetric remote sensing retrieval algorithm uses coupled atmosphere-ocean vector radiative transfer, optimal estimation, artificial intelligence and powerful inherent optical property look-up-tables for the Earth’s aerosol, cloud, and hydrosol particles. PACE-MAPP is the only retrieval algorithm designed to invert aerosol/ocean products using both polarimeters onboard PACE. We present results using PACE-MAPP to retrieve aerosol and ocean remote sensing products from measurements by the Hyper-Angular Rainbow Polarimeter #2 (HARP2) and Spectro-polarimeter for Planetary Exploration one (SPEXone) polarimeter instruments onboard PACE.

Snorre Stamnes↗
NASA NTRSDate not supplied

An Overview of Spacecraft Aerosols: Sources, Dynamics, and Knowledge Gaps

NASA has prioritized development of airborne particulate monitoring systems and mitigation strategies for future Lunar, Martian, and deep-space exploration missions. Airborne particles, also called aerosols, can cause human health problems ranging from mild respiratory discomfort to more severe disease. NASA’s suspended cabin particle and Lunar dust concentration requirements are motivated by protecting crew health and comfort during spaceflight, especially as mission durations lengthen and become increasingly ground-independent. Spacecraft cabin aerosols can originate from a variety of sources, including skin flakes, fibers from clothes and other materials, mechanical wear from equipment, and personal care products (e.g., antiperspirant). As NASA plans future expeditions to the Moon and Mars, Lunar and planetary dust compose an additional, under-characterized source for airborne particles. In addition to these known sources, recent studies on ISS cabin aerosols also revealed particles with unknown origins and poorly understood formation mechanisms, including some that may be formed by oxidative and/or heterogeneous chemical processes. The aerosol monitors payload, to be launched February 2025, will focus on understanding these unknown sources and processes, as well as demonstrating novel technologies for particulate monitoring to be infused in future space flight programs. In this presentation, we will present our knowledge of spacecraft cabin aerosols to date, summarizing aerosol measurement experiments from Shuttle through ISS. Cabin aerosol sources, known and unknown, will be summarized, and knowledge gaps for future long-duration space exploration missions will be discussed.

Claire Fortenberry↗
DOE OSTI2017

Multi-year application of WRF-CAM5 over East Asia-Part II: Interannual variability, trend analysis, and aerosol indirect effects

Following a comprehensive evaluation of WRF-CAM5 in Part I, Part II describes analyses of interannual variability, multi-year variation trends, and the direct, indirect, and total effects of anthropogenic aerosols. Here, the interannual variations of chemical column and surface concentrations, and ozone (O 3 )/particulate matter (PM) indicators are strongly correlated to anthropogenic emission changes. Despite model biases, the model captures well the observed interannual variations of temperature at 2-m, cloud fraction, shortwave cloud forcing, downwelling shortwave radiation, cloud droplet number concentration, column O 3 , and column formaldehyde (HCHO) for the whole domain. While the model reproduces the volatile organic compound (VOC)-limited regimes of O 3 chemistry at sites in Hong Kong, Taiwan, Japan, South Korea, and from the Acid Deposition Monitoring Network in East Asia (EANET) and the degree of sulfate neutralization at the EANET sites, it has limited capability in capturing the interannual variations of the ratio of O 3 and nitrogen dioxide (O 3 /NO 2 ) and PM chemical regime indicators, due to uncertainties in the emissions of precursors for O 3 and secondary PM, the model assumption for ammonium bisulfate (NH 4 HSO 4 ) as well as lack of gas/particle partitioning of total ammonia and total nitrate. While the variation trends in multi-year periods in aerosol optical depth and column concentrations of carbon monoxide, sulfur dioxide, and NO 2 are mainly caused by anthropogenic emissions, those of major meteorological and cloud variables partly reflect feedbacks of chemistry to meteorological variables. The impacts of anthropogenic aerosol indirect effects either dominate or play an important role in the aerosol total effects for most cloud and chemical predictions, whereas anthropogenic aerosol direct effects influence most meteorological and radiation variables. The direct, indirect, and total effects of anthropogenic aerosols exhibit a strong interannual variability in 2001, 2006, and 2011.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Near‐Cloud Aerosol Retrieval Using Machine Learning Techniques, and Implied Direct Radiative Effects

Abstract There is a lack of satellite‐based aerosol retrievals in the vicinity of low‐topped clouds, mainly because reflectance from aerosols is overwhelmed by three‐dimensional cloud radiative effects. To account for cloud radiative effects on reflectance observations, we develop a Convolutional Neural Network and retrieve aerosol optical depth (AOD) with 100–500 m horizontal resolution for all cloud‐free regions regardless of their distances to clouds. The retrieval uncertainty is 0.01 + 5%AOD, and the mean bias is approximately −2%. In an application to satellite observations, aerosol hygroscopic growth due to humidification near clouds enhances AOD by 100% in regions within 1 km of cloud edges. The humidification effect leads to an overall 55% increase in the clear‐sky aerosol direct radiative effect. Although this increase is based on a case study, it highlights the importance of aerosol retrievals in near‐cloud regions, and the need to incorporate the humidification effect in radiative forcing estimates.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Development and Evaluation of E3SM‐MOSAIC: Spatial Distributions and Radiative Effects of Nitrate Aerosol

Abstract Nitrate aerosol plays an important role in affecting regional air quality as well as Earth's climate. However, it is not well represented or even neglected in many global climate models. In this study, we couple the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) module with the four‐mode version of the Modal Aerosol Module (MAM4) in DOE's Energy Exascale Earth System Model version 2 (E3SMv2) to simulate nitrate aerosol and its radiative effects. We find that nitrate aerosol simulated by E3SMv2‐MAM4‐MOSAIC is sensitive to the treatment of gaseous HNO 3 transfer to/from interstitial particles related to accommodation coefficients of HNO 3 ( ) on dust and non‐dust particles. We compare three different treatments of HNO 3 transfer: (a) a treatment (MTC_SLOW) that uses a low in the mass transfer coefficient (MTC) calculation; (b) a dust‐weighted MTC treatment (MTC_WGT) that uses a high on non‐dust particles; and (c) a dust‐weighted MTC treatment that also splits coarse mode aerosols into the coarse dust and sea salt sub‐modes in MOSAIC (MTC_SPLC). MTC_WGT and MTC_SPLC increase the global annual mean (2005–2014) nitrate burden from 0.096 (MTC_SLOW) to 0.237 and 0.185 Tg N, respectively, mostly in the coarse mode. MTC_WGT and MTC_SPLC also produce stronger nitrate direct radiative forcing (−0.048 and −0.051 W m −2 , respectively) and indirect forcing (−0.33 and −0.35 W m −2 , respectively) than MTC_SLOW (−0.021 and −0.24 W m −2 ). MTC_WGT and MTC_SPLC improve nitrate surface concentrations over remote oceans based on limited observations and vertical profiles of nitrate concentrations against aircraft measurements below 400 hPa.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Future Anthropogenic Land Use Change Impacts on Carbonaceous Aerosol and Implications for Climate and Air Quality

Future anthropogenic land use change (LUC) may alter atmospheric carbonaceous aerosol (black carbon and organic aerosol) burden by perturbing biogenic and fire emissions. However, there has been little investigation of this effect. We examine the global evolution of future carbonaceous aerosol under the Shared Socioeconomic Pathways projected reforestation and deforestation scenarios using the CESM2 model from present‐day to 2100. Compared to present‐day, the change in future biogenic volatile organic compounds emission follows changes in forest coverage, while fire emissions decrease in both projections, driven by trends in deforestation fires. The associated carbonaceous aerosol burden change produces moderate aerosol direct radiative forcing (−0.021 to +0.034 W/m 2 ) and modest mean reduction in PM 2.5 exposure (−0.11 μg/m 3 to −0.23 μg/m 3 ) in both scenarios. We find that future anthropogenic LUC may be more important in determining atmospheric carbonaceous aerosol burden than direct anthropogenic emissions, highlighting the importance of further constraining the impact of LUC.>

anthropogenic land use change↗
DOE OSTI2021

New Approach Methodology for Assessing Inhalation Risks of a Contact Respiratory Cytotoxicant: Computational Fluid Dynamics-Based Aerosol Dosimetry Modeling for Cross-Species and In Vitro Comparisons

Regulatory agencies are considering alternative approaches to assessing inhalation toxicity that utilizes in vitro studies with human cells and in silico modeling in lieu of additional animal studies. In support of this goal, computational fluid-particle dynamics models were developed to estimate site-specific deposition of inhaled aerosols containing the fungicide, chlorothalonil, in the rat and human for comparisons to prior rat inhalation studies and new human in vitro studies. Under bioassay conditions, the deposition was predicted to be greatest at the front of the rat nose followed by the anterior transitional epithelium and larynx corresponding to regions most sensitive to local contact irritation and cytotoxicity. For humans, simulations of aerosol deposition covering potential occupational or residential exposures (1–50 µm diameter) were conducted using nasal and oral breathing. Aerosols in the 1–5 µm range readily penetrated the deep region of the human lung following both oral and nasal breathing. Under actual use conditions (aerosol formulations >10 µm), the majority of deposited doses were in the upper conducting airways. Beyond the nose or mouth, the greatest deposition in the pharynx, larynx, trachea, and bronchi was predicted for aerosols in the 10–20 µm size range. Only small amounts of aerosols >20 µm penetrated past the pharyngeal region. Using the ICRP clearance model, local retained tissue dose metrics including maximal concentrations and areas under the curve were calculated for each airway region following repeated occupational exposures. These results are directly comparable with benchmark doses from in vitro toxicity studies in human cells leading to estimated human equivalent concentrations that reduce the reliance on animals for risk assessments.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
DOE OSTI2019

Aerosol Direct Radiative and Cloud Adjustment Effects on Surface Climate over Eastern China: Analyses of WRF Model Simulations

The WRF-simulated changes in clouds and climate due to the increased anthropogenic aerosols for the summers of 2002–08 (vs the 1970s) over eastern China were used to offline calculate the radiative forcings associated with aerosol–radiation (AR) and aerosol–cloud–radiation (ACR) interactions, which subsequently facilitated the interpretation of surface temperature changes. During this period, the increases of aerosol optical depth (ΔAOD) averaged over eastern China range from 0.18 in 2004 to 0.26 in 2007 as compared to corresponding cases in the 1970s, and the multiyear means (standard deviations) of AR and ACR forcings at the surface are −6.7 (0.58) and −3.5 (0.63) W m −2 , respectively, indicating the importance of cloud changes in affecting both the aerosol climate forcing and its interannual variation. The simulated mean surface cooling is 0.35°C, dominated by AR and ACR with a positive (cooling) feedback associated with changes in meteorology (~10%), and two negative (warming) feedbacks associated with decreases in latent (~70%) and sensible (~20%) heat fluxes. More detailed spatial characteristics were analyzed using ensemble simulations for the year 2008. Three regions—Jing-Jin-Ji (ΔAOD ~ 0.63), Sichuan basin (ΔAOD ~ 0.31), and middle Yangtze River valley (ΔAOD ~ 0.26)—at different climate regimes were selected to investigate the relative roles of AR and ACR. While the AR forcing is closely related to ΔAOD values, the ACR forcing presents different regional characteristics owing to cloud changes. In addition, the surface heat flux feedbacks are also different between regions. The study thus illustrates that ACR forcing is useful as a diagnostic parameter to unravel the complexity of climate change to aerosol forcing over eastern China.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Impacts of Wildfire Aerosols on Global Energy Budget and Climate: The Role of Climate Feedbacks

Aerosols emitted from wildfires could significantly affect global climate through perturbing global radiation balance. In this study, the Community Earth System Model with prescribed daily fire aerosol emissions is used to investigate fire aerosols’ impacts on global climate with emphasis on the role of climate feedbacks. The total global fire aerosol radiative effect (RE) is estimated to be -0.78 ± 0.29 W m -2 , which is mostly from shortwave RE due to aerosol–cloud interactions (REaci; -0.70 ± 0.20 W m -2 ). The associated global annual-mean surface air temperature (SAT) change ΔT is -0.64 ± 0.16 K with the largest reduction in the Arctic regions where the shortwave REaci is strong. Associated with the cooling, the Arctic sea ice is increased, which acts to reamplify the Arctic cooling through a positive ice-albedo feedback. The fast response (irrelevant to ΔT) tends to decrease surface latent heat flux into atmosphere in the tropics to balance strong atmospheric fire black carbon absorption, which reduces the precipitation in the tropical land regions (southern Africa and South America). The climate feedback processes (associated with ΔT) lead to a significant surface latent heat flux reduction over global ocean areas, which could explain most (~80%) of the global precipitation reduction. The precipitation significantly decreases in deep tropical regions (5°N) but increases in the Southern Hemisphere tropical ocean, which is associated with the southward shift of the intertropical convergence zone and the weakening of Southern Hemisphere Hadley cell. Such changes could partly compensate the interhemispheric temperature asymmetry induced by boreal forest fire aerosol indirect effects, through intensifying the cross-equator atmospheric heat transport.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Evolution of Multispectral Aerosol Absorption Properties in a Biogenically-Influenced Urban Environment during the CARES Campaign

We present the evolution of multispectral optical properties through urban aerosols that have aged and interacted with biogenic emissions, resulting in stronger short wavelength absorption and the formation of moderately brown secondary organic aerosols. Ground-based aerosol measurements were made in June 2010 within the Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area. Data on black carbon (BC) and non-refractory aerosol mass and composition were collected at both sites. In addition, photoacoustic (PA) instruments with integrating nephelometers were used to measure spectral absorption and scattering coefficients for wavelengths ranging from 355 to 870 nm. The daytime absorption Ångström exponent (AAE) indicated a modest wavelength-dependent enhancement of absorption at both sites throughout the study. From 22 to 28 June 2010, secondary organic aerosol mass increased significantly at both sites, which was due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the median BC mass-normalized absorption cross-section (MAC) values for 405 nm and 532 nm at T1 increased by ~23% and ~35%, respectively, compared with the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for the 870 nm wavelength were similar for both sites. Furthermore, these results suggest the formation of moderately brown secondary organic aerosols in biogenically-influenced urban air.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Quantifying aerosol size distributions and their temporal variability in the Southern Great Plains, USA

A quality-controlled, 5-year dataset of aerosol number size distributions (particles with diameters (Dp) from 7 nm through 14 µm) was developed using observations from a scanning mobility particle sizer, aerodynamic particle sizer, and a condensation particle counter at the Department of Energy's Southern Great Plains (SGP) site. This data set was used for two purposes. First, typical characteristics of the aerosol size distribution (number, surface area, and volume) were calculated for the SGP site, both for the entire dataset and on a seasonal basis, and size distribution lognormal fit parameters are provided. While the median size distributions generally had similar shapes (four lognormal modes) in all the seasons, there were some significant differences between seasons. These differences were most significant in the smallest particles(Dp<30 nm) and largest particles (Dp>800 nm).Second, power spectral analysis was conducted on this long-term dataset to determine key temporal cycles of total aerosol concentrations, as well as aerosol concentrations in specified size ranges. The strongest cyclic signal was associated with a diurnal cycle in total aerosol number concentrations that was driven by the number concentrations of the smallest particles(Dp<30 nm). This diurnal cycle in the smallest particles occurred in all seasons in ~50% of the observations,suggesting a persistent influence of new particle formation events on the number concentrations observed at the SGP site. This finding is in contrast with earlier studies that suggest new particle formation is observed primarily in the springtime at this site. The timing of peak concentrations associated with this diurnal cycle was shifted by several hours depending on the season,which was consistent with seasonal differences in insolation and boundary layer processes. Significant diurnal cycles in number concentrations were also found for particles with Dp between 140 and 800 nm, with peak concentrations occurring in the overnight hours, which were primarily associated with both nitrate and organic aerosol cycles. Weaker cyclic signals were observed for longer timescales (days to weeks) and are hypothesized to be related to the timescales of synoptic weather variability. The strongest periodic signals (3.5–5 and 7 d cycles) for these longer timescales varied depending on the season, with no cyclic signals and the lowest variability in the summer.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2013

A Novel Method for Estimating Shortwave Direct Radiative Effect of Above-cloud Aerosols over Ocean Using CALIOP and MODIS Data

This paper describes an efficient and unique method for computing the shortwave direct radiative effect (DRE) of aerosol residing above low-level liquid-phase clouds using CALIOP and MODIS data. It accounts for the overlapping of aerosol and cloud rigorously by utilizing the joint histogram of cloud optical depth and cloud top pressure. Effects of sub-grid scale cloud and aerosol variations on DRE are accounted for. It is computationally efficient through using grid-level cloud and aerosol statistics, instead of pixel-level products, and a pre-computed look-up table in radiative transfer calculations. We verified that for smoke over the southeast Atlantic Ocean the method yields a seasonal mean instantaneous shortwave DRE that generally agrees with more rigorous pixel-level computation within 4%. We have also computed the annual mean instantaneous shortwave DRE of light-absorbing aerosols (i.e., smoke and polluted dust) over global ocean based on 4 yr of CALIOP and MODIS data. We found that the variability of the annual mean shortwave DRE of above-cloud light-absorbing aerosol is mainly driven by the optical depth of the underlying clouds.

CALIOP and MODIS↗
NASA NTRS2023

Reducing Aerosol Forcing Uncertainty by Combining Models With Satellite and Within-The-Atmosphere Observations: A Three-Way Street

Aerosol forcing uncertainty represents the largest climate forcing uncertainty overall. Its magnitude has remained virtually undiminished over the past 20 years despite considerable advances in understanding most of the key contributing elements. Recent work has produced modest increases only in the confidence of the uncertainty estimate itself. This review summarizes the contributions toward reducing the uncertainty in the aerosol forcing of climate made by satellite observations, measurements taken within the atmosphere, as well as modeling and data assimilation. We adopt a more measurement-oriented perspective than most reviews of the subject in assessing the strengths and limitations of each; gaps and possible ways to fill them are considered. Currently planned programs supporting advanced, global-scale satellite and surface-based aerosol, cloud, and precursor gas observations, climate modeling, and intensive field campaigns aimed at characterizing the underlying physical and chemical processes involved, are all essential. But in addition, new efforts are needed: (a) to obtain systematic aircraft in situ measurements capturing the multi-variate probability distribution functions of particle optical, microphysical, and chemical properties (and associated uncertainty estimates), as well as co-variability with meteorology, for the major aerosol airmass types; (b) to conceive, develop, and implement a suborbital (aircraft plus surface-based) program aimed at systematically quantifying the cloud-scale microphysics, cloud optical properties, and cloud-related vertical velocities associated with aerosol-cloud interactions; and (c) to focus much more research on integrating the unique contributions of satellite observations, suborbital measurements, and modeling, to reduce the persistent uncertainty in aerosol climate forcing.

aerosol climate forcing↗
DOE OSTI2021

Modeling Volatility-Based Aerosol Phase State Predictions in the Amazon Rainforest

Organic aerosol (OA) is a complex matrix of various constituents—fresh (primary organic aerosols—POA) and aged via oxidation (secondary organic aerosols—SOA), generated from biogenic, anthropogenic, and biomass burning sources. The viscosity of OA can be critical in influencing new particle formation, reactive uptake processes that impact evaporation-growth kinetics, and the lifetime of particles in the atmosphere. We report this work utilizes a well-defined relationship between volatility and viscosity for pure compounds, which we incorporated within the Weather Research and Forecasting Model coupled to chemistry (WRF-Chem) to simulate the phase state and viscosity of bulk OA during the dry-to-wet transition season (September–October) in the Amazon rainforest during 2014. Our simulations indicate spatial and temporal heterogeneity in aerosol phase state often not captured by global-scale models. We show the strong role of water associated with organic aerosol ($w_s$) as the dominant factor that can be used to quantitatively estimate OA viscosity. Analysis of WRF-Chem simulations across the entire atmospheric column indicates a strong inverse log-linear relationship between $w_s$ and OA viscosity with a correlation coefficient approaching 1, in the background and biomass burning-influenced conditions. At high altitudes where relative humidity (RH) and temperatures are low, our simulations indicate that OA exists in a semisolid-/solid-like phase state, consistent with previous studies. OA hygroscopicity is strongly correlated (ca. –0.8) with OA viscosity at RH ca. 30–50%, but this RH range is found mostly at low OA concentrations and the middle troposphere (ca. 6–10 km altitudes) in our simulated domain. OA hygroscopicity is uncorrelated with viscosity at higher-RH (near surface) and lower-RH (upper troposphere) regimes. At the urban site near surface, where day–night differences in RH are significant, RH is found to drive the phase state. At the background forested site near surface, where day–night RH differences are small, biomass burning-influenced OA is semisolid and a significant OA associated with background conditions is liquid-like. Simulations indicate a long tail of OA viscosity frequency distributions extending in the semisolid/solid regimes over background biogenic-influenced conditions due to the role of low-volatility OA components such as monoterpene oxidation products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

An Atmospheric Aerosol Short Course for Early Career Scientists

The first Department of Energy (DOE) Environmental and Molecular Science Laboratory (EMSL)/Atmospheric Radiation Measurement (ARM) aerosol summer school was held July 15-19, 2019 at the EMSL user facility located at Pacific Northwest National Laboratory. The school set out to provide graduate students and early-career scientists an overview of atmospheric aerosol science and an introduction to the measurement techniques available through the EMSL and ARM user facilities to address current aerosol science issues. Instructors for the course were drawn from scientists from the EMSL (Laskin et al., 2016; China et al., 2018) and ARM facilities (McComiskey and Ferrare, 2016) as well as from the DOE Atmospheric System Research (ASR) program. Student support for the summer school was also jointly provided by EMSL, ARM, and ASR. The school spanned five days with each day covering a particular theme. 25 students from 21 institutions attended morning lectures on aerosol composition, properties, theory, measurements, and modeling. During afternoons, the students explored instruments that collect and analyze aerosol samples at EMSL and PNNL’s Atmospheric Measurements Laboratory. They also tested relevant computer modeling simulations and learned about NWChem, EMSL’s open-source computational chemistry software suite.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2014

Evaluating Clouds, Aerosols, and their Interactions in Three Global Climate Models using COSP and Satellite Observations

Accurately representing aerosol-cloud interactions in global climate models is challenging. As parameterizations evolve, it is important to evaluate their performance with appropriate use of observations. In this work we compare aerosols, clouds, and their interactions in three climate models (AM3, CAM5, ModelE) to MODIS satellite observations. Modeled cloud properties were diagnosed using the CFMIP Observations Simulator Package (COSP). Cloud droplet number concentrations (N) were derived using the same algorithm for both satellite-simulated model values and observations. We find that aerosol optical depth tau simulated by models is similar to observations. For N, AM3 and CAM5 capture the observed spatial pattern of higher values in near-coast versus remote ocean regions, though modeled values in general are higher than observed. In contrast, ModelE simulates lower N in most near-coast versus remote regions. Aerosol- cloud interactions were computed as the sensitivity of N to tau for marine liquid clouds off the coasts of South Africa and Eastern Asia where aerosol pollution varies in time. AM3 and CAM5 are in most cases more sensitive than observations, while the sensitivity for ModelE is statistically insignificant. This widely used sensitivity could be subject to misinterpretation due to the confounding influence of meteorology on both aerosols and clouds. A simple framework for assessing the N – tau sensitivity at constant meteorology illustrates that observed sensitivity can change from positive to statistically insignificant when including the confounding influence of relative humidity. Satellite simulated values of N were compared to standard model output and found to be higher with a bias of 83 cm-3.

aerosols↗
DOE OSTI2017

Multivariate quadrature for representing cloud condensation nuclei activity of aerosol populations

Here, sparse representations of atmospheric aerosols are needed for efficient regional- and global-scale chemical transport models. Here we introduce a new framework for representing aerosol distributions, based on the quadrature method of moments. Given a set of moment constraints, we show how linear programming, combined with an entropy-inspired cost function, can be used to construct optimized quadrature representations of aerosol distributions. The sparse representations derived from this approach accurately reproduce cloud condensation nuclei (CCN) activity for realistically complex distributions simulated by a particleresolved model. Additionally, the linear programming techniques described in this study can be used to bound key aerosol properties, such as the number concentration of CCN. Unlike the commonly used sparse representations, such as modal and sectional schemes, the maximum-entropy approach described here is not constrained to pre-determined size bins or assumed distribution shapes. This study is a first step toward a particle-based aerosol scheme that will track multivariate aerosol distributions with sufficient computational efficiency for large-scale simulations.

54 ENVIRONMENTAL SCIENCES↗