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NASA NTRS2013

Evaluation of Aerosol Mixing State Classes in the GISS Modele-matrix Climate Model Using Single-particle Mass Spectrometry Measurements

Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 micron, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 micron contain large fractions of organic material, internally-mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

climate models↗
NASA NTRS2012

Characterizing the Vertical Profile of Aerosol Particle Extinction and Linear Depolarization over Southeast Asia and the Maritime Continent: The 2007-2009 View from CALIOP

Vertical profiles of 0.532 μm aerosol particle extinction coefficient and linear volume depolarization ratio are described for Southeast Asia and the Maritime Continent. Quality-screened and cloud-cleared Version 3.01 Level 2 NASA Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) 5-km Aerosol Profile datasets are analyzed from 2007 to 2009. Numerical simulations from the U.S. Naval Aerosol Analysis and Predictive System (NAAPS), featuring two-dimensional variational assimilation of NASA Moderate Resolution Imaging Spectroradiometer and Multi-angle Imaging Spectro- Radiometer quality-assured datasets, combined with regional ground-based lidar measurements, are considered for assessing CALIOP retrieval performance, identifying bias, and evaluating regional representativeness. CALIOP retrievals of aerosol particle extinction coefficient and aerosol optical depth (AOD) are high over land and low over open waters relative to NAAPS (0.412/0.312 over land for all data points inclusive, 0.310/0.235 when the per bin average is used and each is treated as single data points; 0.102/0.151 and 0.086/0.124, respectively, over ocean). Regional means, however, are very similar (0.180/0.193 for all data points and 0.155/0.159 when averaged per normalized bin), as the two factors offset one another. The land/ocean offset is investigated, and discrepancies attributed to interpretation of particle composition and a-priori assignment of the extinction-to-backscatter ratio ("lidar ratio") necessary for retrieving the extinction coefficient from CALIOP signals. Over land, NAAPS indicates more dust present than CALIOP algorithms are identifying, indicating a likely assignment of a higher lidar ratio representative of more absorptive particles. NAAPS resolvesmore smoke overwater than identified with CALIOP, indicating likely usage of a lidar ratio characteristic of less absorptive particles to be applied that biases low AOD there. Over open waters except within the Bay of Bengal, aerosol particle scattering is largely capped below 1.5 km MSL, though ground-based lidar measurements at Singapore differ slightly from this finding. Significant aerosol particle presence over land is similarly capped near 3.0 km MSL over most regions. Particle presence at low levels regionally, except over India, is dominated by relatively non-depolarizing particles. Industrial haze, sea salt droplets and fresh smoke are thus most likely present.

linear volume depolarization ratio↗
NASA NTRS2014

Aerosol Remote Sensing in Polar Regions

Multi-year sets of ground-based sun-photometer measurements conducted at 12 Arctic sites and 9 Antarctic sites were examined to determine daily mean values of aerosol optical thickness tau(lambda) at visible and near-infrared wavelengths, from which best-fit values of Ångström's exponent alpha were calculated. Analyzing these data, the monthly mean values of tau(0.50 micrometers) and alpha and the relative frequency histograms of the daily mean values of both parameters were determined for winter-spring and summer-autumn in the Arctic and for austral summer in Antarctica. The Arctic and Antarctic covariance plots of the seasonal median values of alpha versus tau(0.50 micrometers) showed: (i) a considerable increase in tau(0.50 micrometers) for the Arctic aerosol from summer to winter-spring, without marked changes in alpha; and (ii) a marked increase in tau(0.50 micrometer) passing from the Antarctic Plateau to coastal sites, whereas alpha decreased considerably due to the larger fraction of sea-salt aerosol. Good agreement was found when comparing ground-based sun-photometer measurements of tau(lambda) and alpha at Arctic and Antarctic coastal sites with Microtops measurements conducted during numerous AERONET/MAN cruises from 2006 to 2013 in three Arctic Ocean sectors and in coastal and off-shore regions of the Southern Atlantic, Pacific, and Indian Oceans, and the Antarctic Peninsula. Lidar measurements were also examined to characterize vertical profiles of the aerosol backscattering coefficient measured throughout the year at Ny-Ålesund. Satellite-based MODIS, MISR, and AATSR retrievals of tau(lambda) over large parts of the oceanic polar regions during spring and summer were in close agreement with ship-borne and coastal ground-based sun-photometer measurements. An overview of the chemical composition of mode particles is also presented, based on in-situ measurements at Arctic and Antarctic sites. Fourteen log-normal aerosol number size-distributions were defined to represent the average features of nuclei, accumulation and coarse mode particles for Arctic haze, summer background aerosol, Asian dust and boreal forest fire smoke, and for various background austral summer aerosol types at coastal and high-altitude Antarctic sites. The main columnar aerosol optical characteristics were determined for all 14 particle modes, based on in-situ measurements of the scattering and absorption coefficients. Diurnally averaged direct aerosol-induced radiative forcing and efficiency were calculated for a set of multimodal aerosol extinction models, using various Bidirectional Reflectance Distribution Function models over vegetation-covered, oceanic and snow-covered surfaces. These gave a reliable measure of the pronounced effects of aerosols on the radiation balance of the surface-atmosphere system over polar regions.

Sun-photometer measurements↗
NASA NTRS2015

Interannual Variability of Tropospheric Trace Gases and Aerosols: The Role of Biomass Burning Emissions

Fires are responsible for a range of gaseous and aerosol emissions. However, their influence on the interannual variability of atmospheric trace gases and aerosols has not been systematically investigated from a global perspective. We examine biomass burning emissions as a driver of interannual variability of large-scale abundances of short-lived constituents such as carbon monoxide (CO), hydroxyl radicals (OH), ozone and aerosols using the GISS ModelE composition-climate model and a range of observations, with an emphasis on satellite information. Our model captures the observed variability of the constituents examined in most cases, but with substantial underestimates in boreal regions. The strongest interannual variability on a global scale is found for carbon monoxide (10 for its global annual burden), while the lowest is found for tropospheric ozone (10 for its global annual burden). Regionally, aerosol optical depth shows variability that exceeds 50. Areas of strong variability include the tropical land regions and northern high latitudes, while even regions in the northern midlatitudes experience substantial inteannual variability of aerosols. Ozone variability peaks over Equatorial Asia in boreal autumn, partly due to varying biomass burning emissions, and over the western and central Pacific in the rest of the year, mainly due to meteorological fluctuations. We find that biomass burning emissions are almost entirely responsible for global CO interannual variability, and similarly important for OH variability. The same is true for global and regional aerosol variability, especially when not taking into account dust and sea-salt particles. We show that important implications48 can arise from such interannual influences for regional climate and air quality.

aerosols↗
NASA NTRS2016

Exploring Climatology and Long-Term Variations of Aerosols from NASA Reanalysis MERRA-2 with Giovanni

Dust plays important roles in energy cycle and climate variations. The dust deposition is the major source of iron in the open ocean, which is an essential micronutrient for phytoplankton growth and therefore may influence the ocean uptake of atmospheric CO2. Mineral dust can also act as fertilizer for forests over long time periods. Over 35 years of simulated global aerosol products from NASA atmospheric reanalysis, second Modern-Era Retrospective analysis for Research and Applications (MERRA-2) are available from NASA Goddard Earth Science Data and Information Services Center (GES DISC). The MERRA-2 covers the period 1980-present, continuing as an ongoing climate analysis. Aerosol assimilation is included throughout the period, using MODIS, MISR, AERONET, and AVHRR (in the pre-EOS period). The aerosols are assimilated by using MERRA-2 aerosol model, which interact directly with the radiation parameterization, and radiatively coupled with atmospheric model dynamics in the Goddard Earth Observing System Model, Version 5 (GEOS-5). Dust deposition data along with other major aerosol compositions (e.g. black carbon, sea salt, and sulfate, etc.) are simulated as dry and wet deposition, respectively. The hourly and monthly data are available at spatial resolution of 0.5ox0.625o (latitude x longitude). Quick data exploration of climatology and interannual variations of MERRA-2 aerosol can be done through the online visualization and analysis tool, Giovanni. This presentation, using dust deposition as an example, demonstrates a number of MERRA-2 data services at GES DISC. Global distributions of dust depositions, and their seasonal and inter-annual variations are investigated from MERRA-2 monthly aerosol products.

data services↗
NASA NTRS2016

What Controls the Vertical Distribution of Aerosol? Relationships Between Process Sensitivity in HadGEM3-UKCA and Inter-Model Variation from AeroCom Phase II

The vertical profile of aerosol is important for its radiative effects, but weakly constrained by observations on the global scale, and highly variable among different models. To investigate the controlling factors in one particular model, we investigate the effects of individual processes in HadGEM3-UKCA and compare the resulting diversity of aerosol vertical profiles with the inter-model diversity from the AeroCom Phase II control experiment. In this way we show that (in this model at least) the vertical profile is controlled by a relatively small number of processes, although these vary among aerosol components and particle sizes. We also show that sufficiently coarse variations in these processes can produce a similar diversity to that among different models in terms of the global-mean profile and, to a lesser extent, the zonal-mean vertical position. However, there are features of certain models' profiles that cannot be reproduced, suggesting the influence of further structural differences between models. In HadGEM3-UKCA, convective transport is found to be very important in controlling the vertical profile of all aerosol components by mass. In-cloud scavenging is very important for all except mineral dust. Growth by condensation is important for sulfate and carbonaceous aerosol (along with aqueous oxidation for the former and ageing by soluble material for the latter). The vertical extent of biomass-burning emissions into the free troposphere is also important for the profile of carbonaceous aerosol. Boundary-layer mixing plays a dominant role for sea salt and mineral dust, which are emitted only from the surface. Dry deposition and below-cloud scavenging are important for the profile of mineral dust only. In this model, the microphysical processes of nucleation, condensation and coagulation dominate the vertical profile of the smallest particles by number (e.g. total CN >3 nm), while the profiles of larger particles (e.g. CN>100 nm) are controlled by the same processes as the component mass profiles, plus the size distribution of primary emissions. We also show that the processes that affect the AOD-normalised radiative forcing in the model are predominantly those that affect the vertical mass distribution, in particular convective transport, in-cloud scavenging, aqueous oxidation, ageing and the vertical extent of biomass-burning emissions.

dust↗
NASA NTRS2015

Trend Estimates of AERONET-Observed and Model-Simulated AOTs Between 1993 and 2013

Recently, temporal changes in Aerosol Optical Thickness (AOT) have been investigated based on model simulations, satellite and ground-based observations. Most AOT trend studies used monthly or annual arithmetic means that discard details of the generally right-skewed AOT distributions. Potentially, such results can be biased by extreme values (including outliers). This study additionally uses percentiles (i.e., the lowest 5%, 25%, 50%, 75% and 95% of the monthly cumulative distributions fitted to Aerosol Robotic Network (AERONET)-observed and ECHAM/MESSy Atmospheric Chemistry (EMAC)-model simulated AOTs) that are less affected by outliers caused by measurement error, cloud contamination and occasional extreme aerosol events. Since the limited statistical representativeness of monthly percentiles and means can lead to bias, this study adopts the number of observations as a weighting factor, which improves the statistical robustness of trend estimates. By analyzing the aerosol composition of AERONET-observed and EMAC-simulated AOTs in selected regions of interest, we distinguish the dominant aerosol types and investigate the causes of regional AOT trends. The simulated and observed trends are generally consistent with a high correlation coefficient (R = 0.89) and small bias (slope+/-2(sigma) = 0.75 +/- 0.19). A significant decrease in EMAC-decomposed AOTs by water-soluble compounds and black carbon is found over the USA and the EU due to environmental regulation. In particular, a clear reversal in the AERONET AOT trend percentiles is found over the USA, probably related to the AOT diurnal cycle and the frequency of wildfires. In most of the selected regions of interest, EMAC-simulated trends are mainly attributed to the significant changes of the dominant aerosols; e.g., significant decrease in sea salt and water soluble compounds over Central America, increase in dust over Northern Africa and Middle East, and decrease in black carbon and organic carbon over Australia.

AERONET↗
NASA NTRS2016

Oxychlorine Detections on Mars: Implications for Cl Cycling

The Sample Analysis at Mars (SAM) instrument has detected evolved O2 and HCl indicating the presence of perchlorate and/or chlorate (oxychlorine) in all 11 sediments analyzed to date. The hyperarid martian climate is believed to have allowed accumulation of oxychlorine and assumed chloride contents similar to those in hyperarid terrestrial settings. The linear correlation of oxychlorine and chloride of Gale Crater sediments is low (r (sup 2) equals 0.64). Correlations present in hyperarid Antarctica and the Atacama Desert are attributed to unaltered atmospheric source coupled with minimal redox cycling by biological activity. Terrestrial semi-arid to arid settings have low correlations similar to Gale Crater and are attributed to additional inputs of Cl minus from sea salt, dust, and/or proximal playa settings, and possible reduction of oxychlorine phases during wetter periods. While microbiological processes could contribute to low oxychlorine/chloride correlations on Mars, several abiotic mechanisms are more likely, such as changing oxychlorine production rates with time and/or post-depositional geochemical redox processes that altered the Gale Crater oxychlorine and chloride contents.

Sutter, B.↗
NASA NTRS2015

Active and Widespread Halogen Chemistry in the Tropical and Subtropical Free Troposphere

Halogens in the troposphere are increasingly recognized as playing an important role for atmospheric chemistry, and possibly climate. Bromine and iodine react catalytically to destroy ozone (O3), oxidize mercury, and modify oxidative capacity that is relevant for the lifetime of greenhouse gases. Most of the tropospheric O3 and methane (CH4) loss occurs at tropical latitudes. Here we report simultaneous measurements of vertical profiles of bromine oxide (BrO) and iodine oxide (IO) in the tropical and subtropical free troposphere (10degN to 40degS), and show that these halogens are responsible for 34% of the column-integrated loss of tropospheric O3. The observed BrO concentrations increase strongly with altitude (approx.3.4 pptv at 13.5 km), and are 2-4 times higher than predicted in the tropical free troposphere. BrO resembles model predictions more closely in stratospheric air. The largest model low bias is observed in the lower tropical transition layer (TTL) over the tropical eastern Pacific Ocean, and may reflect a missing inorganic bromine source supplying an additional 2.5-6.4 pptv total inorganic bromine (Bry), or model overestimated Bry wet scavenging. Our results highlight the importance of heterogeneous chemistry on ice clouds, and imply an additional Bry source from the debromination of sea salt residue in the lower TTL. The observed levels of bromine oxidize mercury up to 3.5 times faster than models predict, possibly increasing mercury deposition to the ocean. The halogen-catalyzed loss of tropospheric O3 needs to be considered when estimating past and future ozone radiative effects.

Wang, Siyuan↗
NASA NTRS2015

Implementing Marine Organic Aerosols Into the GEOS-Chem Model

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

Aerosols↗
NASA NTRS2016

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

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

aerosols↗
NASA NTRS2016

Variation in Global Chemical Composition of PM2.5: Emerging Results from SPARTAN

The Surface PARTiculate mAtter Network (SPARTAN) is a long-term project that includes characterization of chemical and physical attributes of aerosols from filter samples collected worldwide. This paper discusses the ongoing efforts of SPARTAN to define and quantify major ions and trace metals found in fine particulate matter (PM (sub 2.5). Our methods infer the spatial and temporal variability of PM (sub 2.5) in a cost-effective manner. Gravimetrically weighed filters represent multi-day averages of PM (sub 2.5), with a collocated nephelometer sampling air continuously. SPARTAN instruments are paired with AErosol RObotic NETwork (AERONET) sun photometers to better understand the relationship between ground-level PM (sub 2.5) and columnar aerosol optical depth (AOD). We have examined the chemical composition of PM (sub 2.5) at 12 globally dispersed, densely populated urban locations and a site at Mammoth Cave (US) National Park used as a background comparison. So far, each SPARTAN location has been active between the years 2013 and 2016 over periods of 2-26 months, with an average period of 12 months per site. These sites have collectively gathered over 10 years of quality aerosol data. The major PM (sub 2.5) constituents across all sites (relative contribution plus or minus Standard Deviation) are ammoniated sulfate (20 percent plus or minus 11 percent), crustal material (13.4 percent plus or minus 9.9 percent), equivalent black carbon (11.9 percent plus or minus 8.4 percent), ammonium nitrate (4.7 percent plus or minus 3.0 percent), sea salt (2.3 percent plus or minus 1.6 percent), trace element oxides (1.0 percent plus or minus 1.1 percent), water (7.2 percent plus or minus 3.3 percent) at 35 percent relative humidity, and residual matter (40 percent plus or minus 24 percent). Analysis of filter samples reveals that several PM (sub 2.5) chemical components varied by more than an order of magnitude between sites. Ammoniated sulfate ranges from 1.1 microns per cubic meter (Buenos Aires, Argentina) to 17 microns per cubic meter (Kanpur, India in the dry season). Ammonium nitrate ranged from 0.2 microns per cubic meter (Mammoth Cave, in summer) to 6.8 microns per cubic meter (Kanpur, dry season). Equivalent black carbon ranged from 0.7 microns per cubic meter (Mammoth Cave) to over 8 microns per cubic meter (Dhaka, Bangladesh and Kanpur, India). Comparison of SPARTAN vs. coincident measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network at Mammoth Cave yielded a high degree of consistency for daily PM (sub 2.5) (r squared equals 0.76, slope equals 1.12), daily sulfate (r squared equals 0.86, slope equals 1.03), and mean fractions of all major PM (sub 2.5) components (within 6 percent). Major ions generally agree well with previous studies at the same urban locations (e.g. sulfate fractions agree within 4 percent for 8 out of 11 collocation comparisons). Enhanced anthropogenic dust fractions in large urban areas (e.g. Singapore, Kanpur, Hanoi, and Dhaka) are apparent from high Zn to Al ratios. The expected water contribution to aerosols is calculated via the hygroscopicity parameter kappa (sub v (volume)) for each filter. Mean aggregate values ranged from 0.15 (Ilorin) to 0.28 (Rehovot). The all-site parameter mean is 0.20 plus or minus 0.04. Chemical composition and water retention in each filter measurement allows inference of hourly PM (sub 2.5) at 35 percent relative humidity by merging with nephelometer measurements. These hourly PM (sub 2.5) estimates compare favourably with a beta attenuation monitor (MetOne) at the nearby US embassy in Beijing, with a coefficient of variation r squared equals 0.67 (number equals 3167), compared to r squared equals 0.62 when v (volume) was not considered. SPARTAN continues to provide an open-access database of PM (sub 2.5) compositional filter information and hourly mass collected from a global federation of instruments.

Snider, Graydon↗
NASA NTRS2016

Saharan Dust as a Causal Factor of Significant Cloud Cover Along the Saharan Air Layer in the Atlantic Ocean

The tropical Atlantic is frequently affected by Saharan dust intrusions. Based on MODIS cloud fraction (CF) data during the ten-year study period, we found that these dust intrusions contribute to significant cloud cover along the Saharan Air Layer (SAL). Below the temperature inversion at the SAL's base, the presence of large amounts of settling dust particles, together with marine aerosols, produces meteorological conditions suitable for the formation of shallow stratocumulus clouds. The significant cloud fraction along the SAL together with clouds over the Atlantic Inter-tropical Convergence Zone contributes to the 20% hemispheric CF asymmetry between the tropical North and South Atlantic. This leads to the imbalance in strong solar radiation, which reaches the sea surface between the tropical North and South Atlantic, and, consequently, affects climate formation in the tropical Atlantic. Therefore, despite the fact that, over the global ocean, there is no noticeable hemispheric asymmetry in cloud fraction, over the significant area such as the tropical Atlantic the hemispheric asymmetry in CF takes place. Saharan dust is also the major contributor to hemispheric aerosol asymmetry over the tropical Atlantic. The NASA GEOS-5 model with aerosol data assimilation was used to extend the MERRA reanalysis with five atmospheric aerosol species (desert dust, sulfates, organic carbon, black carbon, and sea-salt). The obtained ten-year (2002 - 2012) MERRA-driven aerosol reanalysis dataset (aka MERRAero) showed that, over the tropical Atlantic, dust and carbonaceous aerosols were distributed asymmetrically relative to the equator, while other aerosol species were distributed more symmetrically.

CF↗
NASA NTRS2015

Evaluation of the Global Aerosol Microphysical ModelE2-TOMAS Model Against Satellite and Ground-Based Observations

The TwO-Moment Aerosol Sectional (TOMAS) microphysics model has been integrated into the state-of-the- art general circulation model, GISS ModelE2. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the ModelE2-TOMAS model is compared to the default aerosol model in ModelE2, which is a one-moment aerosol (OMA) model (i.e. no aerosol microphysics). Overall, the ModelE2- TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement (mostly within a factor of 2) with observations of sulfur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as ModelE2-OMA) cannot capture the observed vertical distribution of sulfur dioxide over the Pacific Ocean, possibly due to overly strong convective transport and over-predicted precipitation. The ModelE2-TOMAS model simulates observed aerosol number concentrations and cloud condensation nuclei concentrations roughly within a factor of 2. Anthropogenic aerosol burdens in ModelE2-OMA differ from ModelE2-TOMAS by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. We observed larger differences for naturally emitted aerosols such as sea salt and mineral dust, as those emission rates are quite different due to different upper size cutoff assumptions.

Lee, Y. H.↗
NASA NTRS2016

Radiative Effect of Springtime Biomass-Burning Aerosols over Northern Indochina During 7-SEAS Baseline 2013 Campaign

The direct aerosol radiative effects of biomass-burning (BB) aerosols over northern Indochina were estimated by using aerosol properties (physical, chemical, and optical) along with the vertical profile measurements from ground-based measurements with integration of an optical and a radiative transfer model during the Seven South East Asian Studies Biomass-Burning Aerosols Stratocumulus Environment: Lifecycles Interactions Experiment (7-SEASBASELInE) conducted in spring 2013. Cluster analysis of backward trajectories showed the air masses arriving at mountainous background site (Doi Ang Khang; 19.93degN, 99.05degE, 1536 m above mean sea level) in northern Indochina, mainly from near-source inland BB activities and being confined in the planetary boundary layer. The PM(sub10) and black carbon (BC)mass were 87 +/- 28 and 7 +/- 2 micrograms m(exp -3), respectively. The aerosol optical depth (AOD (sub 500) was found to be 0.26--1.13 (0.71 +/- 0.24). Finer (fine mode fraction is approximately or equal to 0.95, angstrom-exponent at 440-870 nm is approximately or equal to 1.77) and significantly absorbing aerosols(single scattering albedo is approximately or equal to 0.89, asymmetry-parameter is approximately or equal to 0.67, and absorption AOD 0.1 at 440 nm) dominated over this region. BB aerosols (water soluble and BC) were the main contributor to the aerosol radiative forcing (ARF), while others (water insoluble, sea salt and mineral dust) were negligible mainly due to their low extinction efficiency. BC contributed only 6 to the surface aerosol mass but its contribution to AOD was 12 (2 times higher). The overall mean ARF was 8.0 and -31.4 W m(exp -2) at top-of-atmosphere (TOA) and at the surface (SFC), respectively. Likely, ARF due to BC was +10.7 and -18.1 W m(exp -2) at TOA and SFC, respectively. BC imposed the heating rate of +1.4 K d(exp -1) within the atmosphere and highlighting its pivotal role in modifying the radiation budget. We propose that to upgrade our knowledge on BB aerosol radiative effects in BB source region, the long-term and extensive field measurements are needed.

aerosol optical properties↗
NASA NTRS2017

Reply to Comment on 'Drought Variability in the Eastern Australia and New Zealand Summer Drought Atlas (ANZDA, CE 1500-2012) Modulated by the Interdecadal Pacific Oscillation'

This reply is in response to Vance et al (2017), who expressed concern that their Law Dome summer sea salt record (LDsss; Vance et al 2013) and two Interdecadal Pacific Oscillation (IPO) reconstructions (PLF and DT-median; Vance et al 2015) were not compared properly in our recent study (Palmer et al 2015) describing the eastern Australian and New Zealand summer Drought Atlas (ANZDA) and that this omission mischaracterizes their records.

Palmer, Jonathan G.↗
NASA NTRS2017

AOD Distributions and Trends of Major Aerosol Species over a Selection of the World's Most Populated Cities Based on the 1st Version of NASA's MERRA Aerosol Reanalysis

NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003-2015) and over a selection of 200 of the world's most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don't tend to fluctuate significantly on an annual basis.

Urban air pollution↗
NASA NTRS2017

Aerosols at the Poles: An Aerocom Phase II Multi-Model Evaluation

Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes. The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (seasalt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60 degrees N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70 degrees S) with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (-0.12 W m(exp. -2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments with one of the AeroCom models (GISS modelE) to investigate how regional emissions of BC and sulfate and the lifetime of BC influence the Arctic and Antarctic AOD. A doubling of emissions in eastern Asia results in a 33 percent increase in Arctic AOD of BC. A doubling of the BC lifetime results in a 39 percent increase in Arctic AOD of BC. However, these radical changes still fall within the AeroCom model range.

Sand, Maria↗