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At least 1,567 records · Page 87

Aerosol-Cloud-Meteorology Interaction Airborne Field Investigations: Using Lessons Learned from the US West Coast in the Design of ACTIVATE off the US East Coast

We report on a multi-year set of airborne field campaigns (2005 – 2016) off the California coast to examine aerosols, clouds, and meteorology, and how lessons learned tie into the upcoming NASA Earth Venture Suborbital (EVS-3) campaign: Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) (2019–2023). The largest uncertainty in estimating global anthropogenic radiative forcing is associated with the interactions of aerosol particles with clouds, which stems from the variability of cloud systems and the multiple feedbacks that affect and hamper efforts to ascribe changes in cloud properties to aerosol perturbations. While past campaigns have been limited in flight hours and the ability to fly in and around clouds, efforts sponsored by the Office of Naval Research have resulted in 113 single aircraft flights (> 500 flight hours) in a fixed region with warm marine boundary layer clouds. All flights used nearly the same payload of instruments on a Twin Otter to fly below, in, and above clouds, producing an unprecedented dataset. We provide here (i) an overview of statistics of aerosol, cloud, and meteorological conditions encountered in those campaigns and (ii) quantification of model-relevant metrics associated with aerosol-cloud interactions leveraging the high data volume and statistics. Based on lessons learned from those flights, we describe the pragmatic innovation in sampling strategy (dual aircraft approach with combined in situ and remote sensing) that will be used in ACTIVATE to generate a dataset that can advance scientific understanding and improve physical parameterizations for Earth system and weather forecasting models, and for assessing next-generation remote sensing retrieval algorithms.

54 ENVIRONMENTAL SCIENCES↗

Studying Aerosol, Clouds, and Air Quality in the Coastal Urban Environment of Southeastern Texas

A multi-agency succession of field campaigns was conducted in southeastern Texas during July 2021 through October 2022 to study the complex interactions of aerosols, clouds and air pollution in the coastal urban environment. As part of the Tracking Aerosol Convection interactions Experiment (TRACER), the TRACER- Air Quality (TAQ) campaign the Experiment of Sea Breeze Convection, Aerosols, Precipitation and Environment (ESCAPE) and the Convective Cloud Urban Boundary Layer Experiment (CUBE), a combination of ground-based supersites and mobile laboratories, shipborne measurements and aircraft-based instrumentation were deployed. These diverse platforms collected high-resolution data to characterize the aerosol microphysics and chemistry, cloud and precipitation micro- and macro-physical properties, environmental thermodynamics and air quality-relevant constituents that are being used in follow-on analysis and modeling activities. We present the overall deployment setups, a summary of the campaign conditions and a sampling of early research results related to: (a) aerosol precursors in the urban environment, (b) influences of local meteorology on air pollution, (c) detailed observations of the sea breeze circulation, (d) retrieved supersaturation in convective updrafts, (e) characterizing the convective updraft lifecycle, (f) variability in lightning characteristics of convective storms and (g) urban influences on surface energy fluxes. The work concludes with discussion of future research activities highlighted by the TRACER model-intercomparison project to explore the representation of aerosol-convective interactions in high-resolution simulations.

54 ENVIRONMENTAL SCIENCES↗

Indirect aerosol effect increases CMIP5 models projected Arctic warming

Phase 5 of the Coupled Model Intercomparison Project (CMIP5) climate models’ projections of the 2014–2100 Arctic warming under radiative forcing from representative concentration pathway 4.5 (RCP4.5) vary from 0.9° to 6.7°C. Climate models with or without a full indirect aerosol effect are both equally successful in reproducing the observed (1900–2014) Arctic warming and its trends. However, the 2014–2100 Arctic warming and the warming trends projected by models that include a full indirect aerosol effect (denoted here as AA models) are significantly higher (mean projected Arctic warming is about 1.5°C higher) than those projected by models without a full indirect aerosol effect (denoted here as NAA models). The suggestion is that, within models including full indirect aerosol effects, those projecting stronger future changes are not necessarily distinguishable historically because any stronger past warming may have been partially offset by stronger historical aerosol cooling. In conclusion, the CMIP5 models that include a full indirect aerosol effect follow an inverse radiative forcing to equilibrium climate sensitivity relationship, while models without it do not.

54 ENVIRONMENTAL SCIENCES↗

Impact of Chinese Urbanization and Aerosol Emissions on the East Asian Summer Monsoon

Effects of urbanization and anthropogenic aerosols in China on the East Asian summer monsoon (EASM) are examined using version 5.1 of the Community Atmosphere Model (CAM5.1) by comparing simulations with and without incorporating urban land cover and/or anthropogenic aerosol emissions. Findings show that the increase of urban land cover causes large surface warming and an urban frictional drag, both leading to a northeasterly wind anomaly in the lower troposphere over eastern China (EC). This weakens the southerly winds associated with the EASM and causes a convergence anomaly in southern China (SC) with increased ascent, latent heating, and cloudiness. The enhanced latent heating reinforces surface convergence and upper-level divergence over SC, leading to more northward advection in the upper level into northern China (NC) and descending between 30° and 50°N over East Asia. Cloudiness reduction, adiabatic heating, and warm advection over NC all enhance the urban heating there, together causing anomalous tropospheric warming at those latitudes over East Asia. Anthropogenic aerosols cause widespread cooling at the surface and in the troposphere over EC, which decreases the summer land–ocean thermal contrast, leading to a weakened EASM circulation with reduced moisture transport to NC. This results in wetter and drier conditions over SC and NC, respectively. When both the urbanization and anthropogenic aerosols are included in the model, aerosols’ cooling is partially offset by the urban heating, and their joint effect on the circulation is dominated by the aerosols’ effect with a reduced magnitude. Here, in the combined experiment, surface and tropospheric temperatures are also altered by the decrease (increase) in cloudiness over NC (SC) with most of the cooling confined to SC, which further weakens the EASM circulation.

54 ENVIRONMENTAL SCIENCES↗

Green Ocean Amazon (GoAmazon) 2014/15. Semi-Volatile Thermal Desorption Aerosol Gas Chromatograph (SVTAG) Field Campaign Report

In areas where biogenic emissions are oxidized in the presence of anthropogenic pollutants such as SO2, NOx, and black carbon, it has become increasingly apparent that secondary organic aerosol (SOA) formation from biogenic volatile organic compounds (VOCs) is substantially enhanced. Research is urgently needed to elucidate fundamental processes of natural and anthropogenically influenced VOC oxidation and the contribution of these processes to SOA formation. GoAmazon 2014/15 afforded study of the chemical transformations in the region downwind of Manaus, Brazil, where local biogenic VOC emissions are high, and their chemical oxidation can be studied both inside and outside of the urban plume to differentiate the role of anthropogenic influence on secondary aerosol formation during oxidation of these natural VOC emissions. To understand the connection between primary biogenic VOC emissions and their secondary products that form aerosols, we made time-resolved molecular level measurements by deploying a Semi-Volatile Thermal Desorption Aerosol Gas Chromatograph (SV-TAG) and a sequential filter sampler during two intensive operational periods (IOPs) of the GoAmazon 2014/15 field campaign. The SV-TAG measured semi-volatile organic compounds in both the gas and particle phases and the sequential filter sampler collected aerosols on quartz fiber filters in four-hour increments used for offline analysis. SV-TAG employed novel online derivatization that provided chemical speciation of highly oxygenated or functionalized compounds that comprise a substantial fraction of secondary organic aerosols, yet are poorly characterized. It also provided partitioning of these compounds between the vapor and particle phases at sufficient time resolution to define the importance of competing atmospheric processes. These measurements were supported by offline analysis of the filters using two-dimensional gas chromatography (GC x GC) with high-resolution time-of-flight mass spectrometry (HR-TOF-MS) using both electron impact (EI) and soft vacuum ultraviolet (VUV) ionization with derivatization. Speciated chemical data from SV-TAG and filter measurements were used to elucidate the relative importance of potential oxidation pathways by providing detailed information on the product distribution from atmospheric reactions and the quantification of known tracers for various oxidation pathways. Together, these techniques provided unequivocal molecular identification of a wide range of atmospheric organic compounds spanning the volatile, semi-volatile, and non-volatile phases. This level of chemical characterization provided insight into the chemical and physical processes that control the atmospheric oxidation of biogenic VOC and subsequent formation of SOA.

54 ENVIRONMENTAL SCIENCES↗

Cloud, Aerosol, and Complex Terrain Interactions (CACTI) Preliminary Science Plan

General circulation models and downscaled regional models exhibit persistent biases in deep convective initiation location and timing, cloud top height, stratiform area and precipitation fraction, and anvil coverage. Despite important impacts on the distribution of atmospheric heating, moistening, and momentum, nearly all climate models fail to represent convective organization, while system evolution is not represented at all. Improving representation of convective systems in models requires characterization of their predictability as a function of environmental conditions, and this characterization depends on observing many cases of convective initiation, non-initiation, organization, and non-organization. The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) experiment in the Sierras de Córdoba mountain range of north-central Argentina is designed to improve understanding of cloud life cycle and organization in relation to environmental conditions so that cumulus, microphysics, and aerosol parameterizations in multi-scale models can be improved. The Sierras de Córdoba range has a high frequency of orographic boundary-layer clouds, many reaching congestus depths, many initiating into deep convection, and some organizing into mesoscale systems uniquely observable from a single fixed site. Some systems even grow upscale to become among the deepest, largest, and longest-lived in the world. These systems likely contribute to an observed regional trend of increasing extreme rainfall, and poor prediction of them likely contributes to a warm, dry bias in climate models downstream of the Sierras de Córdoba range in a key agricultural region. Many environmental factors influence the convective lifecycle in this region including orographic, low-level jet, and frontal circulations, surface fluxes, synoptic vertical motions influenced by the Andes, cloud detrainment, and aerosol properties. Local and long-range transport of smoke resulting from biomass burning as well as blowing dust are common in the austral spring, while changes in land surface properties as the wet season progresses impact surface fluxes and boundary layer evolution on daily and seasonal time scales that feed back to cloud and rainfall generation. This range of environmental conditions and cloud properties coupled with a high frequency of events makes this an ideal location for improving our understanding of cloud-environment interactions. The following primary science questions will be addressed through coordinated first ARM Mobile Facility (AMF1), mobile C-band Scanning ARM Precipitation Radar (C-SAPR2), guest instrumentation, and potential ARM Aerial Facility (AAF) Gulfstream-1 (G-1) observations: 1. How are the properties and lifecycles of orographically generated cumulus humulis, mediocris, and congestus clouds affected by environmental kinematics, thermodynamics, aerosols, and surface properties? How do these cloud types alter these environmental conditions? 2. How do environmental kinematics, thermodynamics, and aerosols impact deep convective initiation, upscale growth, and mesoscale organization? How are soil moisture, surface fluxes, and aerosol properties altered by deep convective precipitation events and seasonal accumulation of precipitation? This multi-faceted experiment involves a long term 8.5-month Extended Observing Period (EOP, 15 August, 2018-30 April, 2019) as well as a 6-week Intensive Observation Period (IOP, 1 November-15 December) that will coincide with the international multi-agency RELAMPAGO field campaign.

54 ENVIRONMENTAL SCIENCES↗

Quantifying and Accounting for the Importance of Aerosol Mixing State. Final Report

The objective of this project was to develop a comprehensive framework of modeling and theory to rigorously investigate the impacts of aerosol mixing state on climate-relevant aerosol properties. The project led to several breakthroughs in the development of new methods as well as new science results. The significant accomplishments of this project are as follows: 1. We developed a conceptual framework to quantify mixing state based on rigorous information-theoretic entropy concepts, and used this to quantify climate-relevant aerosol impacts. Our new mixing state index has seen significant adoption by experimentalists and modelers. 2. We developed new numerical algorithms to enable the efficient simulation of particle-resolved aerosol microphysics within 3D atmospheric models, and implemented these in our coupled WRF-PartMC model. This makes WRF-PartMC the world’s most accurate model of aerosol microphysics coupled to atmospheric dynamics, and we performed the first ever 3D regional-scale simulations that fully resolve aerosol mixing state. 3. We integrated our modeling and conceptual framework with observations including ASR field campaigns (CARES) and ASR-supported laboratory campaigns (Boston College BC-3).

58 GEOSCIENCES↗

Size and Time-Resolved Automated Aerosol Sampling Field Campaign Report

To improve the understanding of the impacts of the vertical distribution of aerosol chemical composition on radiative forcing of aerosol, we performed a detailed physicochemical characterization of aerosol particles sampled during ARM deployment of the tethered balloon system at two ARM sites. We used multi-modal microscopy/spectroscopy techniques and advanced mass spectrometry platforms for the analysis of particles. We found variations in size-resolved aerosol composition at different altitudes. We also observed changes in aerosol composition during different seasons. Some of our observations at ARM’s Oliktok Point, Alaska site suggest cloud processing of aerosol while sampling in clouds, below clouds, and above clouds.

54 ENVIRONMENTAL SCIENCES↗

Environmental Persistence of Biological Aerosols in Outdoor and Simulated Environments

The fate of biological aerosols in the atmosphere depends on the unique and dynamic environmental conditions it is exposed to during transport. There exist many processes that can impact the effectiveness of an aerosol release, and its fate in the environment. Aerosol properties may be modified if biological particles that are released into the atmosphere interact with free radicals, volatile organic compounds(VOC), semi-volatile organic compounds, and inorganic gasphase compounds, such as NOx and SOx. Meteorological conditions such as ultraviolet(UV)- light, relative humidity(RH), and temperature have also been shown to affect biological aerosols, with interactions dependent on both the organism and aerosol's chemical make-up. Oxidation or secondary-organic aerosol (SOA) formations on the particle can also lead to changes in surface proteins and extra-cellular nucleic acids that may agent detection technologies, at a different rate than the infectivity of the agents. Once modified, agents may then be transported via many atmospheric processes such as deposition or incorporation into cloud condensation nuclei(CCN). Although these processes are known, it is unclear what the resulting form and potency ofthe bioaerosol may be after alteration by these processes.

54 ENVIRONMENTAL SCIENCES↗

TRACER-VOC: Speciated Volatile Organic Compounds at the Tracking Aerosol Convection Interactions Experiment Field Campaign Report

Formation of secondary organic aerosol (SOA) is responsible for the growth of particles into cloud condensation nuclei (CCN)-relevant sizes and accounts for a substantial fraction of aerosol mass in the troposphere. Despite its wide abundance and importance, capturing SOA in regional and climate models is still challenging due to complex chemical transformations involved in production of SOA. Oxidation products of biogenic hydrocarbons, such as isoprene, monoterpenes, and sesquiterpenes account for the largest fraction of SOA mass over the continents. As such, biogenic SOA is an important source of continental CCN, and has been recently shown to nucleate ice in the deposition mode. To better account for the processes involved in SOA formation in global and regional climate models, we need better measurements of sources and transformations of volatile organic compounds (VOCs), the precursors to SOA formation in the atmosphere. Understanding aerosol-deep convection interactions is an important science driver of the Tracking Aerosol Convection Interactions Experiment (TRACER), requiring a characterization of the critical controls on aerosol properties and processes, and how those properties and processes vary spatially and temporally in the Houston area. In that environment, the atmospheric photo-oxidative chemistry that drives the evolution and transformation of aerosol properties and processes is strongly impacted by the emission of VOCs, which have both anthropogenic (e.g., industrial, urban, transportation, biomass burning) and biogenic (e.g., marine) sources in the region. Understanding (and disentangling) the complex role of VOCs in such a heterogenous region requires high-time-resolution, speciated VOC measurements that are spatially resolved. To meet these measurement requirements, the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s time-of-flight proton transfer reaction-mass spectrometer (ToF-PTR-MS) was deployed during the TRACER intensive operational period (IOP) from June to September, 2022 at the ancillary site (ANC), which was sited to provide a characterization of the rural atmospheric environment in contrast to the main site.

54 ENVIRONMENTAL SCIENCES↗

Testing of Microchannels and Lab-Grown Stress Corrosion Cracks for Quantification of Aerosol Transmission

The formation of a stress corrosion crack (SCC) in the canister wall of a dry cask storage system (DCSS) has been identified as a potential issue for the long-term storage of spent nuclear fuel. The presence of an SCC in a storage system could represent a through-wall flow path from the canister interior to the environment. Modern, vertical DCSSs are of particular interest due to the commercial practice of using higher backfill pressures in the canister, up to approximately 800 kPa, compared to their horizontal counterparts. This pressure differential offers a relatively high driving potential for blowdown of any particulates that might be present in the canister. In this study, the rates of gas flow and aerosol transmission of a spent fuel surrogate through an engineered microchannel with dimensions representative of an SCC were evaluated experimentally using coupled mass flow and aerosol analyzers. The microchannel was formed by mating two gage blocks with a linearly tapering slot orifice nominally 13 μm (0.005 in.) tall on the upstream side and 25 μm (0.0010 in.) tall on the downstream side. The orifice is 12.7 mm (0.500 in.) wide by 8.86 mm (0.349 in.) long (flow length). Surrogate aerosols of cerium oxide, CeO 2 , were seeded and mixed with either helium or air inside a pressurized tank. The aerosol characteristics were measured immediately upstream and downstream of the simulated SCC at elevated and ambient pressures, respectively. These data sets are intended to add to previous testing that characterized SCCs under well-controlled boundary conditions through the inclusion of testing improvements that establish initial conditions in a more consistent way. While the engineered microchannel has dimensions similar to actual SCCs, it does not reproduce the tortuous path the aerosol laden flow would have to traverse for eventual transmission. SCCs can be rapidly grown in a laboratory setting given the right conditions, and initial characterization and clean-flow testing has begun on lab grown crack samples provided to Sandia National Laboratories (SNL). Many such samples are required to produce statistically relevant transmission results, and SNL is developing a procedure to produce samples in welded steel plates. These ongoing testing efforts are focused on understanding the evolution in both size and quantity of a hypothetical release of aerosolized spent fuel particles from failed fuel to the canister interior and ultimately through an SCC.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

PM2.5 Active Aerosol Collection Field Campaign Report

The long-range transport of aerosols can affect local air quality as well as contribute elements and constituents to mountain watersheds that have potentially positive (e.g., nitrate) and negative (e.g., heavy metals) effects to the local ecosystem. Isotopic analysis of aerosols can be a powerful tool for deconvolving the relative contributions of far-distant and local sources to the composition of collected aerosols. Our field campaign involved the week-long collection of PM2.5 (i.e., particulate matter with an aerodynamic diameter of about 2.5 microns) aerosols on filters, which were returned to the laboratories at Lawrence Berkeley National Laboratory (LBNL) for analysis. The sampling sites were located at the Gothic, Colorado Surface Atmosphere Integrated Field Laboratory (SAIL) Atmospheric Radiation Measurement (ARM) and the Mt. Crested Butte, Colorado SAIL ARM sites. The original intention was to measure the lead (Pb) and strontium (Sr) isotopic compositions of the collected aerosols at high precision to provide constraints on source portioning and attribution, as well as analyze the chemical compositions and nitrogen and carbon isotopic compositions. However, severe blank issues arose that prevented the planned isotopic analyses of Sr, Pb, C, and N and severely affected the analyses of the bulk chemical compositions of the collected aerosols, resulting in the failure of the study. The issue is described in Section 2.0.

54 ENVIRONMENTAL SCIENCES↗

Advancing the Understanding of Cloud Microphysical Processes and Aerosol Indirect Effects in High-Latitude Mixed-Phase Clouds by Linking ARM Measurements with Climate Model Simulations (Final Report)

The key objectives of this project were to advance our understanding of cloud microphysical characteristics and aerosol indirect effects on mixed-phase clouds in high latitudes. To improve the representation of ice and mixed-phase clouds in Earth System Models (ESMs), we propose an integrated observation and modeling study of cloud macro- and microphysical properties, including spatial heterogeneities, mass partitioning between ice crystals and supercooled liquid water, effects of ice nucleating particles (INPs), and efficiency of secondary ice production (SIP), etc. Specifically, we took four main approaches in this project: (1) examining macro- and microphysical properties of ice and mixed-phase clouds based on in-situ and ground-based observations from multiple field campaigns funded by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program, including the Mixed-Phase Arctic Cloud Experiment (M-PACE), Indirect and Semi-Direct Aerosol Campaign (ISDAC), Ice Nucleating Particle Sources at Oliktok Point (INPOP), ARM West Antarctic Radiation Experiment (AWARE), Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS), and Macquarie Island Cloud and Radiation Experiment (MICRE); (2) evaluating the DOE Energy Exascale Earth System Model (E3SM) simulations based on observations, particularly for ice and mixed-phase cloud microphysical properties; (3) examining the impacts of INPs on ice and mixed-phase clouds. Specifically, a series of comparisons were conducted using observations over the Arctic, Southern Ocean, and Antarctica, including comparisons between the lower and higher southern latitudes as well as comparisons between the northern and southern hemispheres. In addition, aerosol indirect effects from distinct sources of dust particles were examined; and (4) investigating the impacts of SIP. Ultimately, these results helped to improve cloud microphysics and aerosol-cloud interaction parameterizations in the E3SM model. Overall, the project provided improved understanding regarding various factors, including thermodynamic, dynamic, and aerosol conditions, on the micro- and macrophysical properties of ice and mixed-phase clouds in the high latitudes. Resulting analysis helped to provide an improved physical basis for refining the current cloud microphysics parameterizations related to ice and mixed-phase clouds in E3SM.

54 ENVIRONMENTAL SCIENCES↗

Climatological simulations of ozone and atmospheric aerosols in the Greater Cairo region

An integrated chemistry-climate model (RegCM4-CHEM) simulates present-day climate, ozone and tropospheric aerosols over Egypt with a focus on Greater Cairo (GC) region. The densley populated GC region is known for its severe air quality issues driven by high levels of anthropogenic pollution in conjuction with natural sources such as dust and agricultural burning events. We find that current global emission inventories underestimate key pollutants such as nitrogen oxides and anthropogenic aerosol species. In the GC region, average-ground-based NO2 observations of 40-60 ppb are substantially higher than modeled estimates (5-10 ppb), likely due to model grid resolution, improper boundary layer representation, and poor emissions inventories. Observed ozone concentrations range from 35 ppb (winter) to 80 ppb (summer). The model reproduces the seasonal cycle fairly well, but modeled summer ozone is understimated by approximately 15 ppb and exhibits little interannual variability. For aerosols, springtime dust events dominate the seasonal aerosol cycle. The chemistry-climate model captures the springtime peak aerosol optical depth (AOD) of 0.7-1 but is slightly greater than satellite-derived AOD. Observed AOD decreases in the summer and increases again in the fall due to agricultural burning events in the Nile Delta, yet the model underestimates this fall observed AOD peak, as standard emissions inventories underestimate this burning and the resulting aerosol emissions. Our comparison of modeled gas and particulate phase atmospheric chemistry in the GC region indicates that improved emissions inventories of mobile sources and other anthropogenic activities are needed to improve air quality simulations in this region.

Steiner, A. L.↗

Evaluating the Influence of CAM5 Aerosol Configuration on Simulated Tropical Cyclones in the North Atlantic

This study examines the influence of prescribed and prognostic aerosol model configurations on the formation of tropical cyclones (TCs) in the North Atlantic Ocean in Community Atmosphere Model version 5 (CAM5). The impact of aerosol parameterization is examined by investigating storm track density, genesis density, potential intensity, and genesis potential index. This work shows that both CAM5 configurations simulate reduced storm frequency when compared to observations and that differences in TC climatology between the model configurations can be explained by differences in the large-scale environment. The analysis shows that simulation with the prognostic aerosol parameterization scheme reasonably captures the observed interannual variability in tropical cyclones and aerosols (i.e., dust) in the North Atlantic, while simulation with the prescribed configuration (climatology) is less favorable. The correlation between dust and TCs in observations (i.e., reanalysis and satellite datasets) is shown to be negative, and this relationship was also found for the prognostic aerosol configuration despite an overall decrease in the frequency of TCs. This indicates that, to accurately replicate certain aspects of TC interannual variability, the aerosol configuration within CAM5 needs to account for the appropriate dust variability.

Huff, J. Jacob A. (ORCID:0000000329143817)↗

Predicting the mineral composition of dust aerosols – Part 2: Model evaluation and identification of key processes with observations

A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. In conclusion, the importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Assessment of long-term WRF–CMAQ simulations for understanding direct aerosol effects on radiation "brightening" in the United States

Long-term simulations with the coupled WRF–CMAQ (Weather Research and Forecasting–Community Multi-scale Air Quality) model have been conducted to systematically investigate the changes in anthropogenic emissions of SO 2 and NO x over the past 16 years (1995–2010) across the United States (US), their impacts on anthropogenic aerosol loading over North America, and subsequent impacts on regional radiation budgets. In particular, this study attempts to determine the consequences of the changes in tropospheric aerosol burden arising from substantial reductions in emissions of SO 2 and NO x associated with control measures under the Clean Air Act (CAA) especially on trends in solar radiation. Extensive analyses conducted by Gan et al. (2014a) utilizing observations (e.g., SURFRAD, CASTNET, IMPROVE, and ARM) over the past 16 years (1995–2010) indicate a shortwave (SW) radiation (both all-sky and clear-sky) "brightening" in the US. The relationship of the radiation brightening trend with decreases in the aerosol burden is less apparent in the western US. One of the main reasons for this is that the emission controls under the CAA were aimed primarily at reducing pollutants in areas violating national air quality standards, most of which were located in the eastern US, while the relatively less populated areas in the western US were less polluted at the beginning of this study period. Comparisons of model results with observations of aerosol optical depth (AOD), aerosol concentration, and radiation demonstrate that the coupled WRF–CMAQ model is capable of replicating the trends well even though it tends to underestimate the AOD. In particular, the sulfate concentration predictions were well matched with the observations. The discrepancies found in the clear-sky diffuse SW radiation are likely due to several factors such as the potential increase of ice particles associated with increasing air traffic, the definition of "clear-sky" in the radiation retrieval methodology, and aerosol semi-direct and/or indirect effects which cannot be readily isolated from the observed data.

54 ENVIRONMENTAL SCIENCES↗

Global and regional modeling of clouds and aerosols in the marine boundary layer during VOCALS: the VOCA intercomparison

A diverse collection of models are used to simulate the marine boundary layer in the southeast Pacific region during the period of the October–November 2008 VOCALS REx (VAMOS Ocean Cloud Atmosphere Land Study Regional Experiment) field campaign. Regional models simulate the period continuously in boundary-forced free-running mode, while global forecast models and GCMs (general circulation models) are run in forecast mode. The models are compared to extensive observations along a line at 20° S extending westward from the South American coast. Most of the models simulate cloud and aerosol characteristics and gradients across the region that are recognizably similar to observations, despite the complex interaction of processes involved in the problem, many of which are parameterized or poorly resolved. Some models simulate the regional low cloud cover well, though many models underestimate MBL (marine boundary layer) depth near the coast. Most models qualitatively simulate the observed offshore gradients of SO 2 , sulfate aerosol, CCN (cloud condensation nuclei) concentration in the MBL as well as differences in concentration between the MBL and the free troposphere. Most models also qualitatively capture the decrease in cloud droplet number away from the coast. However, there are large quantitative intermodel differences in both means and gradients of these quantities. Many models are able to represent episodic offshore increases in cloud droplet number and aerosol concentrations associated with periods of offshore flow. Most models underestimate CCN (at 0.1% supersaturation) in the MBL and free troposphere. The GCMs also have difficulty simulating coastal gradients in CCN and cloud droplet number concentration near the coast. The overall performance of the models demonstrates their potential utility in simulating aerosol–cloud interactions in the MBL, though quantitative estimation of aerosol–cloud interactions and aerosol indirect effects of MBL clouds with these models remains uncertain.

54 ENVIRONMENTAL SCIENCES↗