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Investigating Drivers of Particulate Matter Pollution Over India and the Implications for Radiative Forcing With GEOS-Chem-TOMAS15

Ambient fine particulate matter (PM 2.5 ) concentrations in India frequently exceed 100 μg/m 3 during fall and winter pollution episodes. We use the GEOS-Chem chemical transport model with the TwO-Moment Aerosol Sectional microphysics scheme with 15 size bins (TOMAS15) to assess PM 2.5 composition and impacts on radiation and cloud condensation nuclei (CCN) during pollution episodes as compared to the seasonal (October-December) average. We conduct high resolution (0.25° × 0.3125°) nested-domain simulations over India for short-duration, high-PM2.5 episodes in the fall of 2015 and 2017. The simulations capture the magnitude and spatial patterns of pollution episodes measured by surface monitors (r PM2.5 = 0.69) although aerosol optical depth is underestimated. During the episodes, near-surface organic matter (OM), black carbon (BC), and secondary inorganic aerosol concentrations increase from seasonal averages by up to 36, 7, and 7 μg/m 3 , respectively. Episodic aerosol increases enhance cooling by lowering the top-of-atmosphere clear-sky direct radiative effect (DRE TOA ) during the 2015 episode (−6 W/m 2 ), with a smaller impact during the 2017 episode (−1 W/m 2 ). Differences in DRE TOA reflect larger increases in scattering aerosols in the column during the 2015 episode (+17 mg/m 2 ) than in 2017 (+13 mg/m 2 ), while absorbing aerosol column enhancements are smaller (+3 mg/m2) in both years. Changes in shortwave radiation at the surface (SW sfc ) are spatially similar to DRE TOA and mostly negative during both episodes. CCN enhancements (0.2% supersaturation) during these episodes occur across the western Indo-Gangetic Plain, coincident with higher PM 2.5 concentrations. Changes in DRE TOA , SW sfc , and CCN during high-PM 2.5 episodes may have implications for crops, the hydrologic cycle, and surface temperature.

PM2.5↗

Typical Types and Formation Mechanisms of Haze in an Eastern Asia Megacity, Shanghai

An intensive aerosol and gases campaign was performed at Shanghai in the Yangtze River Delta region over Eastern China from late March to early June 2009. This study provided a complementary picture of typical haze types and the formation mechanisms in megacities over China by using a synergy of ground-based monitoring, satellite and lidar observations. During the whole study period, several extreme low visibility periods were observed with distinct characteristics, and three typical haze types were identified, i.e. secondary inorganic pollution, dust, and biomass burning. Sulfate, nitrate and ammonium accounted for a major part of PM2.5 mass during the secondary inorganic pollution, and the good correlation between SO2/NOx/CO and PM2.5 indicated that coal burning and vehicle emission were the major sources. Large-scale regions with high AOD (aerosol optical depths) and low Angstrom exponent were detected by remote-sensing observation during the dust pollution episode, and this episode corresponded to coarse particles rich in mineral components such as Al and Ca contributing 76.8% to TSP. The relatively low Ca/Al ratio of 0.75 along with the air mass backward trajectory analysis suggested the dust source was from Gobi Desert. Typical tracers for biomass burning from satellite observation (column CO and HCHO) and from ground measurement (CO, particulate K+, OC, and EC) were greatly enhanced during the biomass burning pollution episode. The exclusive linear correlation between CO and PM2.5 corroborated that organic aerosol dominated aerosol chemistry during biomass burning, and the high concentration and enrichment degree of arsenic (As) could be also partly derived from biomass burning. Aerosol optical profile observed by lidar demonstrated that aerosol was mainly constrained below the boundary layer and comprised of spheric aerosol (depolarization ratio <5%) during the secondary inorganic and biomass burning episodes, while thick dust layer distributed at altitudes from near surface to 1.4 km (average depolarization ratio = 0.122+/-0.023) with dust accounting for 44-55% of the total aerosol extinction coefficient during the dust episode. This study portrayed a good picture of the typical haze types and proposed that identification of the complicated emission sources is important for the air quality improvement in megacities in China.

haze↗

Aerosol Concentration, Size, Hygroscopicity and MEE, Globally: What Do We Need to Know and How Can We Know It?

Organizers of the Symposium Clouds, their Properties, and their Climate Feedbacks - What Have We Learned in the Satellite Era, held at Columbia University, NASAGISS June 6-8, 2017 plan to post the presented talks to an online website. http:www.gewex.orgeventclouds-their-properties-and-their-climate-feedbacks-what-have-we-learned-in-the-satellite-era?instance_id293534

Aerosols↗

Regional aerosol chemistry of the Amazon Basin during the dry season

The distribution and chemical composition of the atmospheric aerosol over the Amazon Basin forest were determined during the 1985 July-August dry season, using data on the aerosol chemical constituent concentration collected during the NASA Global Tropospheric Experiment Amazon Boundary Layer Experiment 2A mission. The results of the analyses suggest that there is a remarkable compositional and spatial homogeneity of the atmospheric aerosol on an extensive regional scale. Particulate organic carbon is the dominant component of the atmospheric aerosol, exhibiting an average concentration of about 740 nmol/cu m in the mixed layer and about 220 nmol/cu m in free tropospheric air. Oxalate and SO4(2-) exhibited the greatest enrichment in the mixed layer, while Cl(-) showed essentially no enrichment. The aerosol in the Amazonian atmosphere is essentially acid-base neutral, primarily as a result of incorporation of NH(+), which is presumably derived from NH3 released by the forest ecosystem.

Talbot, R. W.↗

Temporal Variation of Aerosol Properties at a Rural Continental Site and Study of Aerosol Evolution through Growth Law Analysis

Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) onboard the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plains (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May, 2003. During the same period a second SMPS was deployed at a surface station and provided continuous measurements. Combined with trace gas measurements at the SGP site and back-trajectory analysis, the aerosol size distributions provided insights into the sources of aerosols observed at the SGP site. High particle concentrations, observed mostly during daytime, were well correlated with the sulfur dioxide (SO2) mixing ratios, suggesting nucleation involving sulfuric acid is likely the main source of newly formed particles at the SGP. Aerosols within plumes originating from wildfires in Central America were measured at the surface site. Vertically compact aerosol layers, which can be traced back to forest fires in East Asia, were intercepted at altitudes over 3000 meters. Analyses of size dependent particle growth rates for four periods during which high cloud coverage was observed indicate growth dominated by volume controlled reactions. Sulfate accounts for 50% to 72% of the increase in aerosol volume concentration; the rest of the volume concentration increase was likely due to secondary organic species. The growth law analyses and meteorological conditions indicate that the sulfate was produced mainly through aqueous oxidation of SO2 in clouds droplets and hydrated aerosol particles.

Wang, Jian↗

Sources, frequency, and chemical nature of dust events impacting the United States East Coast

This study examines 14 years (2004–2017) of surface aerosol composition data from the EPA IMPROVE network with a focus on the monthly profile, sources, and chemical nature of extreme dust events (>92nd percentile of fine soil concentration each month) impacting ten sites along the United States East Coast ranging in latitude from Florida to Maine. Based on trajectory, remote sensing, and reanalysis data, dust events were categorized into four source categories: African, Asian, Mix (African + Asian), and Other (anything other than African and Asian). The results reveal that extreme dust events account for between 3.3% and 4.6% of total available days depending on the site. March-April-May (MAM) had the most (174) dust events, followed by June-July-August (JJA) with 172, and then by September-October-November (SON) with 160 and December-January-February (DFJ) with 150. There is a variability in the predominant dust sources based on latitude, with African and Other sources more influential from North Carolina to the south, while Asian and Other were most important from New Jersey to the north. The Mix category is consistently the least frequent dust category at all sites. The African dust category was linked to the highest fine soil levels across the entire East Coast relative to other sources regardless of location. JJA is mostly impacted by African dust for sites ranging from Florida to New Jersey, while MAM is dominated by Asian dust for all sites. Mix events occurred mostly between April and October and Other events were most common outside of MAM and JJA seasons. Seven out of ten sites had Other as the most dominant source. Aerosol constituents organic carbon (OC) and elemental carbon (EC) had higher average concentrations in Other events (2.39 ± 0.78 μg m -3 and 0.79 ± 0.81 μg m -3 , respectively) as compared to the other three source categories, suggestive of regional anthropogenic emissions. Moreover, the ratios of elements (Si:Al, K:Fe, Fe:Ca, Al:Ca) contributing to fine soil and PM 2.5 :PM 10 exhibited distinct values depending on the dust source category and the site. This study builds on the growing evidence of the importance of long-range transport of dust in impacting distant regions and how a variety of sources can impact the U.S. East Coast at all times of the year.

Abdulmonam M. Aldhaif↗

Impact of Hydrogen Sulfide on Photochemical Haze Formation in Methane/Nitrogen Atmospheres

The chemistry of trace sulfur gases in planetary organic haze formation is poorly understood, though both are ubiquitous in planetary atmospheres. Here, we perform laboratory studies to explore how the addition of trace amounts of H2S (0.5–5 ppmv) affects organic aerosol produced from ultraviolet photochemistry of CH4 in N2. We analyze the aerosol product composition and size in real time. Inclusion of trace amounts of H2S in the precursor mixture significantly enhances the formation of organic aerosol mass and the particle effective density, both of which increase as a function of initial H2S concentration and in the absence of an additional carbon source. We further present evidence that the addition of trace H2S to the precursor mixtures leads to the formation of organosulfur compounds. Their inclusion in the aerosol-phase contributes to the organic aerosol mass enhancement. Thiyl-alkene chemistry is proposed as a possible organosulfur formation mechanism. In contrast to previous assumptions that sulfur and carbon chemistry occur largely independently of each other, these results suggest a coupling between the two chemistries. This coupling has potential impacts on organic haze and atmospheric sulfur chemistry in planetary atmospheres.

Nathan W Reed↗

Environment Partitioning and Reactivity of Polybrominated Diphenylethers

Polybrominated diphenyl ethers (PBDEs) are an important class of flame retardants. Annual global demand for these compounds was over 67,000 metric tons in 2001. PBDEs have recently been extensively investigated as environmental contaminants because they have been detected in air, sediment, and tissue samples from urban and remote areas. Important issues include quantifying PBDE partitioning in various environmental compartments, and elucidating transformation pathways. The partitioning of PBDE congeners to aerosols was estimated for 16 sites in the United States, Canada, and Mexico. The aerosol particles were PM2.5, the total suspended particle (TSP) concentration varied between 3.0 - 55.4 micro g/cubic meter, and the organic fraction ranged from 11 - 41%; these data are published values for each site. It is estimated that the largest fraction of each PBDE associated with the aerosol particles occurs in Mexico City, and the smallest fraction in Colorado Plateau. Although the organic fraction in Mexico City is about 60% of that observed in the Colorado Plateau, the TSP is larger by a factor of about 18.5, and it is the difference in TSP that strongly influences the fraction of particle-bound PBDE in this case. PBDE partitioning to PM2.5 particles also varies seasonally because of temperature variations. For the less brominated congeners the percentage that is particle-bound is relatively low, regardless of air temperature. In contrast, the heavier congeners exhibit a significant temperature dependence: as the temperature decreases (fall, winter) the percentage of PBDE that is particle-bound increases. The partitioning calculations complement experimental data indicating that decabromodiphenyl ether (DBDE) dissolved in hexane transforms very rapidly when irradiated with solar light. DBDE is the most highly brominated PBDE congener (10 bromine atoms) and occurs in the commercial formulation which is subject to the largest global demand.

Hua, Inez↗

MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

Aerosols↗

Precipitation chemistry in central Amazonia

Rain samples from three sites in central Amazonia were collected over a period of 6 weeks during the 1987 wet season and analyzed for ionic species and dissolved organic carbon. A continuous record of precipitation chemistry and amount was obtained at two of these sites, which were free from local or regional pollution, for a time period of over 1 month. The volume-weighted mean concentrations of most species were found to be about a factor of 5 lower during the wet season compared with previous results from the dry season. Only sodium, potassium, and chloride showed similar concentrations in both seasons. When the seasonal difference in rainfall amount is taken into consideration, the deposition fluxes are only slightly lower for most species during the wet season than during the dry season, again with the exception of chloride, potassium, and sodium. Sodium and chloride are present in the same ratio as in sea salt; rapid advection of air masses of marine origin to the central Amazon Basin during the wet season may be responsible for the observed higher deposition flux of these species. Statistical analysis suggests that sulfate is, to a large extent, of marine (sea salt and biogenic) origin, but that long-range transport of combustion-derived aerosols also makes a significant contribution to sulfate and nitrate levels in Amazonian rain. Organic acid concentrations in rain were responsible for a large fraction of the observed precipitation acidity; their concentration was strongly influenced by gas/liquid interactions.

Andreae, M. O.↗

AWARE: The Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment

The US Department of Energy Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment (AWARE) performed comprehensive meteorological and aerosol measurements, and ground-based atmospheric remote sensing at two Antarctic stations using the most advanced instrumentation available. A suite of cloud research radars, lidars, spectral and broadband radiometers, aerosol chemical and microphysical sampling equipment, and meteorological instrumentation was deployed at McMurdo Station on Ross Island from December 2015 through December 2016. A smaller suite of radiometers and meteorological equipment including radiosondes, optimized for surface energy budget measurement, was deployed on the West Antarctic Ice Sheet between 4 December 2015 and 17 January 2016. AWARE provided Antarctic atmospheric data comparable to several well-instrumented high Arctic sites that have operated for many years and that reveal numerous contrasts with the Arctic in aerosol and cloud microphysical properties. These include persistent differences in liquid cloud occurrence, cloud height and cloud thickness. Antarctic aerosol properties are also quite different from the Arctic in both seasonal cycle and composition, due to the continent’s isolation from lower latitudes by Southern Ocean storm tracks. Antarctic aerosol number and mass concentrations are not only non-negligible but perhaps play a more important role than previously recognized because of the higher sensitivities of clouds at the very low concentrations caused by the large-scale dynamical isolation. Antarctic aerosol chemical composition, particularly organic components, has implications for local cloud microphysics. The AWARE data set, fully available online in the ARM Program data archive, offers numerous case studies for unique and rigorous evaluation of mixed-phase cloud parameterization in climate models.

Atmospheric Radiation Measurement (ARM)↗

Leveraging Scientific Community Knowledge for Air Quality Model Chemistry Parameterizations

Air pollution contributes to adverse health outcomes. Approximately 121 million people in the United States—one third of the population—live where National Ambient Air Quality Standards (NAAQS) are violated. In most cases, the criteria pollutants exceeding standards are ozone (O 3 ) and fine particles (PM 2.5 ). In addition, 188 substances known or suspected to cause cancer or other serious health effects are designated as hazardous air pollutants (HAPs). Essentially, all O 3 and significant portions of PM 2.5 and HAPs are produced in the atmosphere through chemical and physical processes. In the case of PM 2.5 , subcomponents formed primarily from precursor gases—sulfate, nitrate, ammonium, and secondary organic aerosol (SOA)—account for 60% of the U.S. county-level annual mean concentration. In addition, 47% of the cancer risk and 25% of the noncancer risk from HAPs have been attributed to atmospheric chemistry rather than direct emissions. In this article, we introduce the role of chemical mechanisms in air quality models, a new atmospheric science community effort, and needs for further mechanism development.

Havala O.T. Pye↗

Assessment of Natural and Anthropogenic Aerosol Air Pollution In the Middle East Using MERRA-2, CAMS Data Assimilation Products, and High-Resolution WRF-Chem Model Simulations

Modern-Era Retrospective analysis for Research and Applications v.2 (MERRA-2), Copernicus Atmosphere Monitoring Service Operational Analysis (CAMS-OA), and a high-resolution regional Weather Research and Forecasting model coupled with chemistry (WRF-Chem) were used to evaluate natural and anthropogenic particulate matter (PM) air pollution in the Middle East (ME) during 2015–2016. Two Moderate Resolution Imaging Spectrometer (MODIS) retrievals – combined product Deep Blue and Deep Target (MODIS-DB&DT) and Multi-Angle Implementation of Atmospheric Correction (MAIAC) – and Aerosol Robotic Network (AERONET) aerosol optical depth (AOD) observations as well as in situ PM measurements for 2016 were used for validation of the WRF-Chem output and both assimilation products. MERRA-2 and CAMS-OA assimilate AOD observations. WRF-Chem is a free-running model, but dust emission in WRF-Chem is tuned to fit AOD and aerosol volume size distributions obtained from AERONET. MERRA-2 was used to construct WRF-Chem initial and boundary conditions both for meteorology and chemical and aerosol species. SO2 emissions in WRF-Chem are based on the novel OMI-HTAP SO2 emission dataset. The correlation with the AERONET AOD is highest for MERRA-2 (0.72–0.91), MAIAC (0.63–0.96), and CAMSOA (0.65–0.87), followed by MODIS-DB&DT (0.56–0.84) and WRF-Chem (0.43–0.85). However, CAMS-OA has a relatively high positive mean bias with respect to AERONET AOD. The spatial distributions of seasonally averaged AODs from WRF-Chem, assimilation products, and MAIAC are well correlated with MODIS-DB&DT AOD product. MAIAC has the highest correlation (R = 0.8), followed by MERRA-2 (R = 0.66), CAMS-OA (R = 0.65), and WRF-Chem (R = 0.61). WRF-Chem, MERRA-2, and MAIAC underestimate and CAMS-OA overestimates MODIS-DB&DT AOD. The simulated and observed PM concentrations might differ by a factor of 2 because it is more challenging for the model and the assimilation products to reproduce PM concentration measured within the city. Although aerosol fields in WRF-Chem and assimilation products are entirely consistent, WRF-Chem is preferable for analysis of regional air quality over the ME due to its higher spatial resolution and better SO2 emissions. The WRF-Chem’s PM background concentrations exceed the World Health Organization (WHO) guidelines over the entire ME. Mineral dust is the major contributor to PM (≈ 75%–95%) compared to other aerosol types. Near and downwind from the SO2 emission sources, non-dust aerosols (primarily sulfate) contribute up to 30% to PM(sub 2.5). The contribution of sea salt to PM in coastal regions can reach 5%. The contributions of organic matter, black carbon and organic carbon to PM over the Middle East are insignificant. In the major cities over the Arabian Peninsula, the 90th percentile of PM(sub 10) and PM(sub 2.5) (particles with diameters less than 10 and 2.5 μm, respectively) daily mean surface concentrations exceed the corresponding Kingdom of Saudi Arabia air quality limits. The contribution of the non-dust component to PM(sub 2.5) is < 25%, which limits the emission control effect on air quality. The mitigation of the dust effect on air quality requires the development of environment-based approaches like growing tree belts around the cities and enhancing in-city vegetation cover. The WRF-Chem configuration presented in this study could be a prototype of a future air quality forecast system that warns the population against air pollution hazards.

Alexander Ukhov↗

Effective radiative forcing from emissions of reactive gases and aerosols - a multi-model comparison

This paper quantifies the pre-industrial (1850) to present-day (2014) effective radiative forcing (ERF) of anthropogenic emissions of NOX, volatile organic compounds (VOCs; including CO), SO2, NH3, black carbon, organic carbon, and concentrations of methane, N2O and ozone-depleting halocarbons, using CMIP6 models. Concentration and emission changes of reactive species can cause multiple changes in the composition of radiatively active species: tropospheric ozone, stratospheric ozone, stratospheric water vapour, secondary inorganic and organic aerosol, and methane. Where possible we break down the ERFs from each emitted species into the contributions from the composition changes. The ERFs are calculated for each of the models that participated in the AerChemMIP experiments as part of the CMIP6 project, where the relevant model output was available. The 1850 to 2014 multi-model mean ERFs (± standard deviations) are −1.03 ± 0.37 W/sq.m for SO2 emissions, −0.25 ± 0.09 W/sq.m for organic carbon (OC), 0.15 ± 0.17 W/sq.m for black carbon (BC) and −0.07 ± 0.01 W/sq.m for NH3. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W/sq.m. The multi-model means for the reactive well-mixed greenhouse gases (including any effects on ozone and aerosol chemistry) are 0.67 ± 0.17 W/sq.m for methane (CH4), 0.26 ± 0.07 W/sq.m for nitrous oxide (N2O) and 0.12 ± 0.2 W/sq.m for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (NOx), volatile organic compounds and both together (O3) lead to ERFs of 0.14 ± 0.13, 0.09 ± 0.14 and 0.20 ± 0.07 W/sq.m respectively. The differences in ERFs calculated for the different models reflect differences in the complexity of their aerosol and chemistry schemes, especially in the case of methane where tropospheric chemistry captures increased forcing from ozone production.

radiative forcing↗

Semivolatile Particulate Organic Material Southern Africa during SAFARI 2000

During August and September 2000, the University of Washington's Cloud and Aerosol Research Group (CARG) with its Convair-580 research aircraft participated in the Southern African Fire-Atmosphere Research Initiative (SAFARI) 2000 field study in southern Africa. Aboard this aircraft was a Particle Concentrator-Brigham Young University Organic Sampling System (PC-BOSS), which was used to determine semivolatile particulate material with a diffusion denuder sampler. Denuded quartz filters and sorbent beds in series were used to measure nonvolatile and semivolatile materials, respectively. Results obtained with the PC-BOSS are compared to those obtained with conventional quartz-quartz and Teflon-quartz filter pack samplers. Various 10-120 min integrated samples were collected during flights through the h e troposphere, in the atmospheric boundary layer, and in plumes from savanna fires. Significant fine particulate semivolatile organic compounds (SVOC) were found in all samples. The SVOC was not collected by conventional filter pack samplers and therefore would not have been determined in previous studies that used only filter pack samplers. The SVOC averaged 24% of the fine particulate mass in emissions from the fires and 36% of the fine particulate mass in boundary layer samples heavily impacted by aged emissions from savanna fires. Concentrations of fine particulate material in the atmospheric mixed layer heavily impacted by aged savanna frre emissions averaged 130 micrograms per cubic meter. This aerosol was 85% carbonaceous mated.

Eatough, D. J.↗

Description and Evaluation of Brown Carbon Representation in GISS ModelE

Brown carbon (BrC) is an absorbing organic aerosol primarily emitted by the combustion of biomass and biofuel. While field and laboratory studies have shown that BrC exhibits light absorption unique from black carbon (BC) and organic carbon (OC) aerosols, the radiative forcing of BrC is still highly uncertain. We present the implementation of BrC in the One-Moment Aerosol (OMA) module of the GISS ModelE ESM. Primary BrC is emitted from biomass burning with a range of optical properties and is processed through a unique chemical aging scheme. Brown secondary organic aerosols (SOA), formed from several biogenic and anthropogenic precursors, are also represented. Several simulations–with varied emissions, optical properties, and chemistry–have been run to assess the sensitivity of this BrC implementation within ModelE. Initial results show a peak in BrC concentrations near the tropopause, around 200 mb. As BC aerosols do not reach this height in ModelE, this suggests a new source of absorption in the upper troposphere. Organic aerosol representation can be further evaluated through comparison to AERONET retrieval data of BrC mass and optical depth, and total aerosol optical depth.

Brown carbon↗

Going With the Flow: Using a Particle Dispersion Model to Reveal Links Between Ocean Ecosystems and Marine Aerosols

Marine biogenic particle contributions to atmospheric aerosol concentrations are not well understood though they are important for determining cloud optical and cloud nucleating properties. Here we examine the relationship between marine aerosol measurements with satellite and model fields of ocean biology and meteorological variables during the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES). NAAMES consisted of four field campaigns between November 2015 and April 2018 that aligned with the four major phases of the annual phytoplankton bloom cycle. The FLEXPART Lagrangian particle dispersion model is used to connect these variables spatiotemporally to ship-based aerosol. We find that correlations between some aerosol measurements with satellite measured and modelled variables increase with increasing trajectory length. This indicates biological and meteorological processes over the air mass history are influential to measured particle properties. For example, results show organic aerosol mass is driven by biogenic volatile organic compound (VOC) emissions from photosynthesis by phytoplankton stocks during advection into the region. In contrast, primary marine aerosol (PMA) concentrations showed better correlations to variables weighted with shorter air mass residence times, which reflects their localized origin as primary emissions. Evidence also suggest variability in PMA concentrations likely play an important role in VOC emission removal. The removal of VOCs lessen their impact on particle number and mass concentrations. The sensitivity of marine aerosols to the main ecosystem-atmosphere drivers and its dependence on air mass history are to be further discussed.

Kevin J Sanchez↗

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

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.

Menon, Surabi↗