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DOE OSTI2022

High temperature and pressure regime soot: Physical, optical and chemical signatures from high explosive detonations

Submicron particles are formed during the detonation and deflagration of carbon-rich energetic materials known as high explosives (HE) that can be lofted and transported long distances in the atmosphere. Particles include refractory species like soot, a.k.a. black carbon (BC), and have impacts to climate and human health at local, regional, and global scales. Here, we contrast detonation soot aerosol physical, optical and chemical properties that are formed more efficiently in terms of emission factors and ratios with traditional combustion sources from biomass burning and fossil fuels. We utilize ambient aerosol techniques for the first time to identify soot from two well-known HE's (1) Comp B-3: 40% trinitrotoluene (TNT) and 60% 1,3,5-trinitro-1,3,5-triazinane (RDX) and (2) PBX 9501: 95% 1,3,5,7-tetranitro-1,3,5,7-tetrazoctane (HMX) with 2.5% Estane and a 2.5% mixture of bis(2,2-dinitropropyl)-acetal (BDNPA) and bis(2,2-dinitropropyl)-formal (BDNPF). Size distributions, optical and chemical properties are presented. Aggregate soot had small mobility diameters (<100 nm) and unique optical and chemical signatures depending on the explosive composite composition, detonation atmosphere (e.g., air, argon) and pressure. Single-scattering albedos (SSA) from 0.3 to 0.8 and absorption Angstrom exponents (AAE) from 0.5 to 2.0 measured across 405–870 nm wavelengths depended on the explosive composite composition and detonation conditions. Comp B-3 detonation soot was similar to other combustion soot sources, whereas PBX 9501 soot had high scattering relative to absorption. Carbonaceous chemical signatures included the presence of fullerenes that were distinct from ambient and laboratory-generated soot surrogates and the detection of trace metals, including aluminum, copper, iron, and zinc.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Evaluation and improvement of the parameterization of aerosol hygroscopicity in global climate models using in-situ surface measurements (Final Report)

Aerosols are tiny particles suspended on the atmosphere that can interact with incoming solar radiation and affect the Earth radiative budget. They do so by scattering and absorbing solar radiation, and these properties vary depending on the aerosol size and chemical composition. Moreover, by taking up water from the surrounding air, hygroscopic aerosol particles will grow in size and change their chemical composition, thus modifying their optical properties (scattering and absorption) and their final impact on radiative forcing calculations. An accurate knowledge of aerosol hygroscopicity is crucial for estimating the net radiative impact of aerosols. We took a three-pronged approach to improve our understanding of aerosol hygroscopicity and how it is implemented in Earth system models. In the first part of our project, we developed a benchmark dataset from existing aerosol hygroscopic growth measurements made by tandem nephelometer humidogram systems. We analyzed, using a standardized methodology, observations from 26 in-situ stations around the globe. Measurement data was collected from multiple data providers, reviewed and harmonized to create a consistent dataset of the scattering enhancement factor due to aerosol water uptake. This dataset is archived in several publicly available databases for use by interested researchers. In the second part of the project, we used the benchmark hygroscopicity dataset to perform a global study on aerosol hygroscopicity and aerosol optical properties. Measurements show a global picture of scattering enhancement with larger values for Arctic and marine sites and lower for urban and desert sites. We assessed the RH dependence of aerosol radiative forcing and showed that the overall effect of aerosol hygroscopicity on DARF is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 compared to dry conditions (RH<40%). Finally, we explored using aerosol single scattering albedo (SSA) and scattering Angstrom exponent (SAE) as possible proxies for aerosol hygroscopicity. SSA showed more promise as a surrogate for the scattering enhancement factor than SAE, but neither was ideal. In the third part of the project we evaluated the output of ten Earth system models (ESMs) against the benchmark hygroscopicity dataset. ESMs utilize various schemes for aerosol hygroscopicity which had not been previously tested against observations on a global scale. We found that ESMs currently overestimate scattering enhancement due to hygroscopic growth. Model parameterizations of hygroscopicity and model chemistry are two main factors driving the observed diversity in hygroscopicity simulations among the models. In addition, our study makes several suggestions for modelers, including improving the parameterizations of organic and sea salt aerosol hygroscopicity. Future hygroscopicity model evaluation experiments should include the model data related to particles size which was not available for our study.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Establishing robust correction schemes for improved and reliable ARM-AOS aerosol optical data products

Aerosol light absorption and scattering of solar radiation play an important role in the earth’s atmosphere in terms of direct and semi-direct radiative forcing. Optical parameters of importance to the US Department of Energy (DOE) climate models include absorption and scattering coefficients, single scattering albedo (SSA), absorption Angstrom exponents (AAE), and the asymmetry parameter (g). These parameters depend on aerosol size, shape and composition (refractive index), and are spectrally sensitive in the shortwave region. Additionally, these parameters have a complex dependency on the emission source, especially for carbonaceous aerosols. The DOE Atmospheric Radiation Measurement (ARM) user facility has deployed aerosol observing systems (AOS) containing several filter-based instruments to measure and constrain aerosol optical properties and related parameters at multiple sites worldwide. For measurement of aerosol light absorption, the AOS includes filter-based instruments (particle soot absorption photometer and tricolor absorption photometer) that infer particle-phase aerosol absorption coefficients at nominal red, green, and blue wavelength bands from the attenuation (ATN) of light passing through a particulate filter on which aerosols are deposited. Measurement of aerosol scattering is done in situ using nephelometers. By combining inferred absorption coefficients from filter-based ATN measurements and in situ scattering coefficients, value-added products (VAPs) such as SSA, AAE, and g are derived.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Direct and semi-direct radiative forcing of biomass-burning aerosols over the southeast Atlantic (SEA) and its sensitivity to absorbing properties: a regional climate modeling study

Simulations are performed for the period 2000-2015 by two different regional climate models, ALADIN and RegCM, to quantify the direct and semi-direct radiative effects of biomass-burning aerosols (BBAs) in the southeast Atlantic (SEA) region. Different simulations have been performed using strongly absorbing BBAs in accordance with recent in situ observations over the SEA. For the July-August-September (JAS) season, the single scattering albedo (SSA) and total aerosol optical depth (AOD) simulated by the ALADIN and RegCM models are consistent with the MACv2 climatology and MERRA-2 and CAMS-RA reanalyses near the biomass-burning emission sources. However, the above-cloud AOD is slightly underestimated compared to satellite (MODIS and POLDER) data during the transport over the SEA. The direct radiative effect exerted at the continental and oceanic surfaces by BBAs is significant in both models and the radiative effects at the top of the atmosphere indicate a remarkable regional contrast over SEA (in all-sky conditions), with a cooling (warming) north (south) of 10°S, which is in agreement with the recent MACv2 climatology. In addition, the two models indicate that BBAs are responsible for an important shortwave radiative heating of ~0.5-1K per day over SEA during JAS with maxima between 2 and 4 km a.m.s.l. (above mean sea level). At these altitudes, BBAs increase air temperature by ~0.2-0.5 K, with the highest values being co-located with low stratocumulus clouds. Vertical changes in air temperature limit the subsidence of air mass over SEA, creating a cyclonic anomaly. The opposite effect is simulated over the continent due to the increase in lower troposphere stability. The BBA semi-direct effect on the lower troposphere circulation is found to be consistent between the two models. Changes in the cloud fraction are moderate in response to the presence of smoke, and the models differ over the Gulf of Guinea. Finally, the results indicate an important sensitivity of the direct and semi-direct effects to the absorbing properties of BBAs. Over the stratocumulus (Sc) region, DRE varies from +0.94 W m -2 (scattering BBAs) to +3.93 W m -2 (most absorbing BBAs).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Aerosols from anthropogenic and biogenic sources and their interactions – modeling aerosol formation, optical properties, and impacts over the central Amazon basin

The Green Ocean Amazon experiment – GoAmazon 2014–2015 – explored the interactions between natural biogenic forest emissions from central Amazonia and urban air pollution from Manaus. Previous GoAmazon 2014–2015 studies showed that nitrogen oxide (NO x = NO + NO 2 ) and sulfur oxide (SO x ) emissions from Manaus strongly interact with biogenic volatile organic compounds (BVOCs), affecting secondary organic aerosol (SOA) formation. In previous studies, ground-based and aircraft measurements provided evidence of SOA formation and strong changes in aerosol composition and properties. Aerosol optical properties also evolve, and their impacts on the Amazonian ecosystem can be significant. As particles age, some processes, such as SOA production, black carbon (BC) deposition, particle growth and the BC lensing effect change the aerosol optical properties, affecting the solar radiation flux at the surface. This study analyzes data and models SOA formation using the Weather Research and Forecasting with Chemistry (WRF-Chem) model to assess the spatial variability in aerosol optical properties as the Manaus plumes interact with the natural atmosphere. The following aerosol optical properties are investigated: single scattering albedo (SSA), asymmetry parameter (g aer ), absorption Ångström exponent (AAE) and scattering Ångström exponent (SAE). These simulations were validated using ground-based measurements at three experimental sites, namely the Amazon Tall Tower Observatory – ATTO (T0a), downtown Manaus (T1), Tiwa Hotel (T2) and Manacapuru (T3), as well as the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) aircraft flights. WRF-Chem simulations were performed over 7 d during March 2014. Results show a mean biogenic SOA (BSOA) mass enrichment of 512 % at the T1 site, 450 % in regions downwind of Manaus, such as the T3 site, and 850 % in areas north of the T3 site in simulations with anthropogenic emissions. The SOA formation is rather fast, with about 80 % of the SOA mass produced in 3–4 h. Comparing the plume from simulations with and without anthropogenic emissions, SSA shows a downwind reduction of approximately 10 %, 11 % and 6 % at the T1, T2 and T3 sites, respectively. Other regions, such as those further downwind of the T3 site, are also affected. The g aer values increased from 0.62 to 0.74 at the T1 site and from 0.67 to 0.72 at the T3 site when anthropogenic emissions are active. During the Manaus plume-aging process, a plume tracking analysis shows an increase in SSA from 0.91 close to Manaus to 0.98 160 km downwind of Manaus as a result of SOA production and BC deposition.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Atmospheric processing and aerosol aging responsible for observed increase in absorptivity of long-range-transported smoke over the southeast Atlantic

Biomass burning aerosol (BBA) from agricultural fires in southern Africa contributes about one-third of the global carbonaceous aerosol load. These particles have strong radiative effects in the southeast Atlantic (SEA), which depend in part on the radiative contrast between the aerosol layer in the free troposphere (FT) and the underlying cloud layer. However, there is large disagreement in model estimates of aerosol-driven climate forcing due to uncertainties in the vertical distribution, optical properties, and life cycle of these particles. This study applies a novel method combining remote sensing observations with regional model outputs to investigate the aging of the BBA and its impact on the optical properties during transatlantic transport from emission sources in Africa to the SEA. Results show distinct variations in extinction Ångström exponent (EAE) and single-scattering albedo (SSA) as aerosols age. Near the source, fresh aerosols are characterized by low mean SSA (0.84) and high EAE (1.85), indicating smaller, highly absorbing particles. By isolating marine contributions from the total column during BBA transport across the SEA, our analysis reveals an initial decrease in BBA absorptivity, with mean FT SSA of 0.87 after 6–7 d, followed by increased absorptivity with mean FT SSA of 0.84 after 10 d, suggesting enhanced absorption due to chemical aging. These findings indicate that BBA becomes more absorbing during extended transport across the SEA, with implications for reducing model uncertainties. Our remote-sensing-based results agree well with previous in situ studies and offer new insights into aerosol–radiation interactions and the energy balance over the SEA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Findings of the African Combustion Aerosol Collaborative Intercomparison Analysis (ACACIA) Pilot Project to Understand the Optical Properties of Biomass Burning Smoke

Africa is a critical source of biomass burning (BB) aerosols, and its importance is increasing. The African Combustion Aerosol Collaborative Intercomparison Analysis (ACACIA) Pilot Project set to optically characterize BB aerosol generated from sub-Saharan African fuels. We used a photoacoustic spectrometer as a reference instrument to determine the multiple-scattering correction factor C λ for an AE33 aethalometer at three wavelengths, which produced weighted mean values of C 370 =3.69, C 470 =5.65, and C 520 =6.39. C λ increased with wavelength and C 370 was statistically independent of the others, suggesting a single C λ is insufficient, especially in BB scenarios. While a dependence of C λ on burning state was not found, C λ was shown to strongly relate to particle single scattering albedo (SSA, ω). When Cλ was plotted against SSA, values slowly rose at low SSA values, followed by a sharp rise around an SSA of ∼ 0.9; indicating a larger correction needed for less absorbing aerosol. A number of functions operating on either SSA or C λ were explored and the best function was -C λ /(1-C λ )=Aω+B. This is an important parametrization of C λ specifically geared towards BB aerosol from African fuels under different aging states, and is of particular importance for future field work in that continent. An Ångström matrix plot shows that African BB aerosol can have values more akin to dust, which demonstrates that these fuels are distinct in their wavelength dependence from more typical BB aerosol. Lastly, we examined the mass extinction and absorbance cross sections for BB aerosol generated for the same fuels with two different tube furnace setups. Not only is this combustion method flexible, it was found to be reproducible between labs.

47 OTHER INSTRUMENTATION↗

NASA NTRS1998

Satellite Estimates of Single Scattering Albedo and Optical Depth of Biomass Burning Carbonaceous Aerosols

Satellite based estimates of aerosol single scattering albedo (ssa), over both land and water surfaces, have been obtained for the first time using measurements of backscattered radiation in the near ultraviolet by the Total Ozone Mapping Spectrometer (TOMS). The retrieval of ssa and aerosol optical depth is based on the strong spectral contrast in the near-UV resulting from the interaction between the particle absorption and scattering (both Rayleigh and Mie) processes. We use the multi-year data set on backscattered radiances by the TOMS family of instruments to analyze the time and space variability of biomass burning generated carbonaceous aerosols. Results of a comparative analysis of satellite derived optical depth and available sunphotometer measurements will also be presented.

Torres, O.↗

NASA NTRS2003

Airborne Measurements of Carbonaceous Aerosols in Southern Africa during the Dry Biomass Burning Season

Particulate matter collected aboard the University of Washington's (UW) Convair-580 research aircrafi over southem Afiica during the dry biomass burning season was analyzed for total carbon (TC), organic carbon (OC), and black carbon (BC) contents using thermal and optical methods. Samples were collected in smoke plumes of burning savanna and in regional haze. A known artifact, produced by the adsorption of organic gases on the quartz filter substrates used to collect the particulate matter samples, comprised a significant portion of the TC collected. Consequently, conclusions derived from the data are greatly dependent on whether or not OC concentrations are corrected for this artifact. For example, the estimated aerosol coalbedo (1 - single scattering albedo (SSA)), which is a measure of aerosol absorption, of the biomass smoke samples is 60% larger using corrected OC concentrations. Thus, the corrected data imply that the biomass smoke is 60% more absorbing than do the uncorrected data. The BC to (corrected) OC mass ratio (BC/OC) of smoke plume samples (0.18 plus or minus 0.06) is lower than that of samples collected in the regional haze (0.25 plus or minus 0.08). The difference may be due to mixing of biomass smoke with background air characterized by a higher BC/OC ratio. A simple source apportionment indicates that biomass smoke contributes about three quarters of the aerosol burden in the regional haze, while other souxes (e.g., fossil fuel burning) contribute the remainder.

Kirchstetter, Thomas W.↗

NASA NTRS2007

Aerosol Radiative Effects on Deep Convective Clouds and Associated Radiative Forcing

The aerosol radiative effects (ARE) on the deep convective clouds are investigated by using a spectral-bin cloud-resolving model (CRM) coupled with a radiation scheme and an explicit land surface model. The sensitivity of cloud properties and the associated radiative forcing to aerosol single-scattering albedo (SSA) are examined. The ARE on cloud properties is pronounced for mid-visible SSA of 0.85. Relative to the case excluding the ARE, cloud fraction and optical depth decrease by about 18% and 20%, respectively. Cloud droplet and ice particle number concentrations, liquid water path (LWP), ice water path (IWP), and droplet size decrease significantly when the ARE is introduced. The ARE causes a surface cooling of about 0.35 K and significantly high heating rates in the lower troposphere (about 0.6K/day higher at 2 km), both of which lead to a more stable atmosphere and hence weaker convection. The weaker convection and the more desiccation of cloud layers explain the less cloudiness, lower cloud optical depth, LWP and IWP, smaller droplet size, and less precipitation. The daytime-mean direct forcing induced by black carbon is about 2.2 W/sq m at the top of atmosphere (TOA) and -17.4 W/sq m at the surface for SSA of 0.85. The semi-direct forcing is positive, about 10 and 11.2 W/sq m at the TOA and surface, respectively. Both the TOA and surface total radiative forcing values are strongly negative for the deep convective clouds, attributed mostly to aerosol indirect forcing. Aerosol direct and semi-direct effects are very sensitive to SSA. Because the positive semi-direct forcing compensates the negative direct forcing at the surface, the surface temperature and heat fluxes decrease less significantly with the increase of aerosol absorption (decreasing SSA). The cloud fraction, optical depth, convective strength, and precipitation decrease with the increase of absorption, resulting from a more stable and dryer atmosphere due to enhanced surface cooling and atmospheric heating.

Fan, J.↗

NASA NTRS2007

Variability of Solar Radiation under Cloud-Free Skies in China: The Role of Aerosols

In this study, we analyzed long-term surface global and diffuse solar radiation, aerosol single scattering albedo (SSA), and relative humidity (RH) from China. Our analysis reveals that much of China experienced significant decreases in global solar radiation (GSR) and increases in diffuse solar radiation under cloud-free skies between the 1960s and 1980s. With RH and aerosol SSA being rather constant during that time period, we suggest that the increasing aerosol loading from emission of pollutants is responsible for the observed reduced GSR and increased diffuse radiation in cloud-free skies. Although pollutant emissions continue to increase after the 1980s, the increment of aerosol SSA since 1980s can partly explain the transition of GSR from a decreasing trend to no apparent trend around that time. Preliminary analysis is also provided on the potential role of RH in affecting the global and diffuse solar radiation reaching the earth surface.

Qian, Yun↗

NASA NTRS2010

MISR Global Aerosol Product Assessment by Comparison with AERONET

A statistical approach is used to assess the quality of the MISR Version 22 (V22) aerosol products. Aerosol Optical Depth (AOD) retrieval results are improved relative to the early post- launch values reported by Kahn et al. [2005a], varying with particle type category. Overall, about 70% to 75% of MISR AOD retrievals fall within 0.05 or 20% AOD of the paired validation data, and about 50% to 55% are within 0.03 or 10% AOD, except at sites where dust, or mixed dust and smoke, are commonly found. Retrieved particle microphysical properties amount to categorical values, such as three groupings in size: "small," "medium," and "large." For particle size, ground-based AERONET sun photometer Angstrom Exponents are used to assess statistically the corresponding MISR values, which are interpreted in terms of retrieved size categories. Coincident Single-Scattering Albedo (SSA) and fraction AOD spherical data are too limited for statistical validation. V22 distinguishes two or three size bins, depending on aerosol type, and about two bins in SSA (absorbing vs. non-absorbing), as well as spherical vs. non-spherical particles, under good retrieval conditions. Particle type sensitivity varies considerably with conditions, and is diminished for mid-visible AOD below about 0.15 or 0.2. Based on these results, specific algorithm upgrades are proposed, and are being investigated by the MISR team for possible implementation in future versions of the product.

Kahn, Ralph A.↗

NASA NTRS2008

Sensitivity of Multiangle Imaging to the Optical and Microphysical Properties of Biomass Burning Aerosols

The treatment of biomass burning (BB) carbonaceous particles in the Multiangle Imaging SpectroRadiometer (MISR) Standard Aerosol Retrieval Algorithm is assessed, and algorithm refinements are suggested, based on a theoretical sensitivity analysis and comparisons with near-coincident AERONET measurements at representative BB sites. Over the natural ranges of BB aerosol microphysical and optical properties observed in past field campaigns, patterns of retrieved Aerosol Optical Depth (AOD), particle size, and single scattering albedo (SSA) are evaluated. On the basis of the theoretical analysis, assuming total column AOD of 0.2, over a dark, uniform surface, MISR can distinguish two to three groups in each of size and SSA, except when the assumed atmospheric particles are significantly absorbing (mid-visible SSA approx.0.84), or of medium sizes (mean radius approx.0.13 pin); sensitivity to absorbing, medium-large size particles increases considerably when the assumed column AOD is raised to 0.5. MISR Research Aerosol Retrievals confirm the theoretical results, based on coincident AERONET inversions under BB-dominated conditions. When BB is externally mixed with dust in the atmosphere, dust optical model and surface reflection uncertainties, along with spatial variability, contribute to differences between the Research Retrievals and AERONET. These results suggest specific refinements to the MISR Standard Aerosol Algorithm complement of component particles and mixtures. They also highlight the importance for satellite aerosol retrievals of surface reflectance characterization, with accuracies that can be difficult to achieve with coupled surface-aerosol algorithms in some higher AOD situations.

Chen, Wei-Ting↗

NASA NTRS2011

Monitoring Aerosols from Space: What We can Say, and What We Can't

Aerosols are understood to play a significant role is the global energy balance, and especially on atmospheric as well as surface energy balances regionally. A combination of direct radiative cooling of the surface, atmospheric warming through diabatic heating, and indirect effects of aerosol on clouds are all thought to contribute to the net aerosol effect, though the magnitudes of each are both highly variable in space and time, and highly uncertain. Passive space-based remote sensing is a key tool for constraining these effects, due to the frequent, global coverage satellites can provide. However, information from such observations about total-column aerosol amount (i.e., aerosol optical depth or AOD), and especially about aerosol type, is limited. The current generation of passive aerosol remote-sensing instruments, including the Multi-angle Imaging SpectroRadiometer (MISR) and the MODerate resolution Imaging Spectroradiometer (MODIS) offer vast improvements over previous instruments, including AOD over water and much of the land surface, fine vs. coarse particle type over ocean from MODIS, and discrimination of about a dozen aerosol types from MISR under good retrieval conditions, based on particle size, shape, and single-scattering albedo (SSA) constraints. This presentation will summarize the capabilities and expected improvements in the currently available aerosol products, in light of required energy budget constraints. Ways of addressing the need for detailed information about particle microphysical properties, especially SSA, unobtainable from MISR or MODIS, will be discussed.

Kahn, Ralph A.↗

NASA NTRS2010

Anthropogenic Air Pollution Observed Near Dust Source Regions in Northwestern China During Springtime 2008

Trace gases and aerosols were measured in Zhangye (39.082degN, 100.276degE, 1460 m a.s. 1.), a rural site near the Gobi deserts in northwestern China during spring 2008. Primary trace gases (CO:265 ppb; SO2:3.4 ppb; NO(*y): 4.2 ppb; hereafter results given as means of hourly data) in the area were lower than in eastern China, but still indicative of marked anthropogenic emissions. Sizable aerosol mass concentration (153 micro-g/cu m) and light scattering (159/Mm at 500 nm) were largely attributable to dust emissions, and aerosol light absorption (10.3/Mm at 500 nm) was dominated by anthropogenic pollution. Distinct diurnal variations in meteorology and pollution were induced by the local valley terrain. Strong daytime northwest valley wind cleaned out pollution and was replaced by southeast mountain wind that allowed pollutants to build up overnight. In the afternoon, aerosols had single scattering albedo (SSA, 500 mn) of 0.95 and were mainly of supermicron particles, presumably dust, while at night smaller particles and SSA of 0.89-0.91 were related to Pollution. The diverse local emission sources were characterized: the CO/SO2, CO/NO(y), NO(y)/SO2 (by moles), and BC/CO (by mass) ratios for small point sources such as factories were 24.6-54.2, 25.8-35.9, 0.79-1.31, and 4.1-6.1 x 10(exp -3), respectively, compared to the corresponding inventory ratios of 43.7-71.9, 23.7-25.7, 1.84-2.79, and 3.4-4.0 x 10(exp -3) for the industrial sector in the area. The mixing between dust and pollution can be ubiquitous in this region. During a dust storm shown as an example, pollutants were observed to mix with dust, causing discernible changes in both SSA and aerosol size distribution. Further interaction between dust and pollutants during transport may modify the properties of dust particles that are critical for their large-scale impact on radiation, clouds, and global biogeochemical cycles.

Li, Can↗

NASA NTRS2010

Biomass Burning Aerosol Absorption Measurements with MODIS Using the Critical Reflectance Method

This research uses the critical reflectance technique, a space-based remote sensing method, to measure the spatial distribution of aerosol absorption properties over land. Choosing two regions dominated by biomass burning aerosols, a series of sensitivity studies were undertaken to analyze the potential limitations of this method for the type of aerosol to be encountered in the selected study areas, and to show that the retrieved results are relatively insensitive to uncertainties in the assumptions used in the retrieval of smoke aerosol. The critical reflectance technique is then applied to Moderate Resolution Imaging Spectrometer (MODIS) data to retrieve the spectral aerosol single scattering albedo (SSA) in South African and South American 35 biomass burning events. The retrieved results were validated with collocated Aerosol Robotic Network (AERONET) retrievals. One standard deviation of mean MODIS retrievals match AERONET products to within 0.03, the magnitude of the AERONET uncertainty. The overlap of the two retrievals increases to 88%, allowing for measurement variance in the MODIS retrievals as well. The ensemble average of MODIS-derived SSA for the Amazon forest station is 0.92 at 670 nm, and 0.84-0.89 for the southern African savanna stations. The critical reflectance technique allows evaluation of the spatial variability of SSA, and shows that SSA in South America exhibits higher spatial variation than in South Africa. The accuracy of the retrieved aerosol SSA from MODIS data indicates that this product can help to better understand 44 how aerosols affect the regional and global climate.

Zhu, Li↗