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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth’s radiation budget yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (-7.95° N, -14.36° E) detail how fire source regions (burning conditions and fuel type), transport pathways, and longer-term chemical processing affect the chemical, microphysical, and optical properties of the BBA in the remote MBL between June and September of 2017. Ten individual plume events characterize the seasonal evolution of BBA characteristics. Inefficient burning conditions, determined by the mass ratio of refractory black carbon to above-background carbon monoxide (rBC:ΔCO), enhance organic- and sulfate-rich aerosol concentrations in June–July. In contrast, the heart of the burning season exhibited higher rBC:ΔCO values indicative of efficient burning conditions, correlating with more rBC-enriched BBA. Toward the end of the burning season, a mix of burning conditions results in increased variation of the BBA properties. The BBA transit to Ascension Island was predominantly through slow-moving pathways in the MBL and lower free troposphere (FT), facilitating prolonged chemical transformations through heterogeneous and aqueous phase processes. Heterogeneous oxidation can persist for up to 10 days, resulting in a considerable decrease in organic aerosol (OA) mass. OA to rBC mass ratios (OA:rBC) in the MBL between 2 and 5 contrast to higher values of 5 to 15 observed in the nearby FT. Conversely, early-season aqueous-phase processes primarily contributed to aerosol oxidation and some aerosol production, but not appreciable aerosol removal. These two chemical processes yield more light-absorbing BBA in the MBL than in the FT and explain the notably low scattering albedo at 530 nm (SSA 530 ) values (< 0.80) at Ascension Island. This study establishes a robust correlation between SSA 530 and OA:rBC across both MBL and FT, underscoring the dependency of optical properties on chemical composition. These findings highlight how the interplay between chemical composition and atmospheric processing can be improved in global and regional climate models. Questions remain on the mixing of aerosols with different pathway histories, and on what accounts for the doubling of the mass absorption coefficient in the boundary layer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

Abstract. African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth's radiation budget, yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (7.95° S, 14.36° W) provide insight into how burning conditions, fuel type, transport pathways, and atmospheric processing affect the chemical, microphysical, and optical properties of BBA between June and September 2017. A total of 10 individual plume events characterize the seasonal evolution of the BBA properties. Early-season inefficient fires, determined by low refractory black carbon to above-background carbon monoxide mixing ratios (rBC : ΔCO), led to enhanced concentrations of organic- and sulfate-rich aerosols. Mid-season efficient fires, determined by higher rBC : ΔCO values, led to rBC-enriched BBA. A mix of efficient and inefficient fires later in the season resulted in conflicting BBA properties. Prolonged transport (∼ 10 d) through the MBL and lower free troposphere (FT) facilitated chemical and aqueous-phase processing, which led to a reduction in organic aerosol mass concentrations. This resulted in lower organic aerosol (OA) to rBC (OA : rBC) mass ratios (2–5) in the MBL compared to higher values (5–15) in the nearby FT. These atmospheric and cloud oxidation processes yield more light-absorbing BBA and explain the notably low single-scattering albedo at 530 nm (SSA530) values (< 0.80) observed in the MBL. This study establishes a robust correlation between SSA530 and OA : rBC across the MBL and FT, underscoring the dependency of optical properties on chemical composition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2005

Aerosol properties computed from aircraft-based observations during the ACE- Asia campaign: A case study of lidar ratio closure and aerosol radiative effects - 2

For a vertical profile with three distinct layers (marine boundary, pollution and dust), observed during the ACE-Asia campaign, we carried out a comparison between the modeled lidar ratio vertical profile and that obtained from collocated airborne NASA AATS-14 sunphotometer and shipborne Micro-Pulse Lidar (MPL) measurements. Vertically resolved lidar ratio was calculated from two size distribution vertical profiles - one obtained by inversion of sunphotometer-derived extinction spectra, and one measured in-situ - combined with the same refractive index model based on aerosol chemical composition. The aerosol model implies single scattering albedos of 0.78 - 0.81 and 0.93 - 0.96 at 0.523 microns (the wavelength of the lidar measurements), in the pollution and dust layers, respectively. The lidar ratios calculated from the two size distribution profiles have close values in the dust layer; they are however, significantly lower than the lidar ratios derived from combined lidar and sunphotometer measurements, most probably due to the use of a simple nonspherical model with a single particle shape in our calculations. In the pollution layer, the two size distribution profiles yield generally different lidar ratios. The retrieved size distributions yield a lidar ratio which is in better agreement with that derived from lidar/sunphotometer measurements in this layer, with still large differences at certain altitudes (the largest relative difference was 46%). We explain these differences by non-uniqueness of the result of the size distribution retrieval and lack of information on vertical variability of particle refractive index. Radiative transfer calculations for this profile showed significant atmospheric radiative forcing, which occurred mainly in the pollution layer. We demonstrate that if the extinction profile is known then information on the vertical structure of absorption and asymmetry parameter is not significant for estimating forcing at TOA and the surface, while it is of importance for estimating vertical profiles of radiative forcing and heating rates.

Kuzmanoski, Maja↗
DOE OSTI2021

Sensitivity of Carbonaceous Aerosol Properties to the Implementation of a Dynamic Aging Parameterization in the Regional Climate Model RegCM

Freshly emitted soot is hydrophobic, but condensation of secondary aerosols and coagulation with other particles modify its hygroscopic optical properties. This conversion is referred to as “aerosol aging.” Many climate models represent this aging process with a fixed aging time scale, whereas in reality, it is a dynamic process that depends on environmental conditions. Here, we implement a dynamic aging parameterization scheme in the regional climate model RegCM4 in place of the fixed aging timescale of 1.15 days (~27.6 h) and examine its impact on the aerosol life cycle over the Indian subcontinent. The conversion from hydrophobic to hydrophilic aerosol is usually lower than 27.6 h over the entire landmass and lower than 10 h over the polluted Indo-Gangetic Basin (IGB), with seasonal variability. Due to the implementation of the dynamic aging scheme, the column burden and surface mass concentration of carbonaceous aerosols increase during the drier season (December–February) when washout is negligible. The burden is reduced during the wet season (June–September) due to a more efficient washout except over the IGB, where a reduction in precipitation as a result of radiative feedbacks increases the aerosol concentrations. Over the polluted IGB, surface dimming increases due to the dynamic aging scheme, with the top of the atmosphere forcing remaining mostly unchanged. As a result, atmospheric heating increases by at least 1.2 W/m 2 . Our results suggest that climate models should incorporate dynamic aging for a more realistic representation of aerosol simulations, especially in highly polluted regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1973

Stratospheric aerosol properties and their effects on infrared radiation.

This paper presents a stratospheric aerosol model and infers its effects on terrestrial radiation. Composition of the aerosol is assumed to be concentrated sulfuric acid. An appropriate size distribution has been determined from available size distribution measurements of other investigators. Aerosols composed of concentrated sulfuric acid emit energy in the atmospheric window region of the infrared spectrum, 8-13 microns. Laboratory measurements of optical constant data obtained at room temperature are presented for 75 and 90% aqueous sulfuric acid. Calculations of an aerosol extinction coefficient are then performed by using the above data. Effects of changes in aerosol phase and temperature are discussed but not resolved.

Remsberg, E. E.↗
NASA NTRS1980

Dependence of the spectral surface irradiance on aerosol properties and surface reflectivity

A reduction in global surface irradiance occurs with increasing aerosol loadings when the aerosols are absorbing. For scattering aerosols, a reduction is pronounced for isotropic scattering (characteristic of small particles) but reduction is not as significant for scattering with a high anisotropy of a large forward peak (characteristic of large particles). This distinction between isotropic and anisotropic scattering becomes small or null over highly reflecting terrain; and for reflectivities higher than 0.5 and solar elevation angles close to the zenith, the global irradiance can be slightly higher for isotropic scattering than in the case of an anisotropy of a forward peak. Under such conditions, which can be encountered in reflective infrared bands over dense vegetation or over sandy deserts (close to noon, in low latitudes) the surface irradiance becomes nearly independent of the aerosol optical thickness.

Otterman, J.↗
NASA NTRS2012

Variability and Trends of Aerosol Properties over Kanpur, Northern India using AERONET Data (2001-10)

Natural and anthropogenic aerosols over northern India play an important role in influencing the regional radiation budget, causing climate implications to the overall hydrological cycle of South Asia. In the context of regional climate change and air quality, we discuss aerosol loading variability and trends at Kanpur AERONET station located in the central part of the Indo-Gangetic plains (IGP), during the last decade (2001-10). Ground-based radiometric measurements show an overall increase in column-integrated aerosol optical depth (AOD) on a yearly basis. This upward trend is mainly due to a sustained increase in the seasonal/monthly averaged AOD during the winter (Dec-Feb) and post-monsoon (Oct-Nov) seasons (dominated by anthropogenic emissions). In contrast, a neutral to weak declining trend is observed during late pre-monsoon (Mar-May) and monsoon (Jun-Sep) months, mainly influenced by inter-annual variations of dust outbreaks. A general decrease in coarse-mode aerosols associated with variable dust activity is observed, whereas the statistically significant increasing post-monsoon/winter AOD is reflected in a shift of the columnar size distribution towards relatively larger particles in the accumulation mode. Overall, the present study provides an insight into the pronounced seasonal behavior in aerosol loading trends and, in general, is in agreement with that associating the findings with those recently reported by satellite observations (MODIS and MISR) over northern India. Our results further suggest that anthropogenic emissions (due mainly to fossil-fuel and biomass combustion) over the IGP have continued to increase in the last decade.

AERONET↗
NASA NTRS2005

Evaluation of Aerosol Properties over Ocean from Moderate Resolution Imaging Spectroradiometer (MODIS) during ACE-Asia

The Aerosol Characterization Experiment-Asia (ACE-Asia) was conducted in March-May 2001 in the western North Pacific in order to characterize the complex mix of dust, smoke, urban/industrial pollution, and background marine aerosol that is observed in that region in springtime. The Moderate Resolution Imaging Spectroradiometer (MODIS) provides a large-scale regional view of the aerosol during the ACE-Asia time period. Focusing only on aerosol retrievals over ocean, MODIS data show latitudinal and longitudinal variation in the aerosol characteristics. Typically, aerosol optical depth (tau(sub a)) values at 0.55 micrometers are highest in the 30 deg. - 50 deg. latitude band associated with dust outbreaks. Monthly mean tau(sub a) in this band ranges approx. 0.40-70, although large differences between monthly mean and median values indicate the periodic nature of these dust outbreaks. The size parameters, fine mode fraction (eta), and effective radius (r(sub eff)) vary between monthly mean values of eta = 0.47 and r(sub eff)= 0.75 micrometers in the cleanest regions far offshore to approximately eta = 0.85 and r(sub eff) =.30 micrometers in near-shore regions dominated by biomass burning smoke. The collocated MODIS retrievals with airborne, ship-based, and ground-based radiometers measurements suggest that MODIS retrievals of spectral optical depth fall well within expected error (DELTA tau(sub a) = plus or minus 0.03 plus or minus 0.05 tau(sub a)) except in situations dominated by dust, in which cases MODIS overestimate both the aerosol loading and the aerosol spectral dependence. Such behavior is consistent with issues related to particle nonsphericity. Comparisons of MODIS-derived r(sub eff) with AERONET retrievals at the few occurrences of collocations show MODIS systematically underestimates particle size by 0.2 micrometers. Multiple-year analysis of MODIS aerosol size parameters suggests systematic differences between the year 2001 and the years 2000 and 2002, which are traced to instrumental electronic cross talk. Sensitivity studies show that such calibration errors are negligible in tau(sub a) retrievals but are more pronounced in size parameter retrievals, especially for dust and sea salt.

Chu, D. A.↗
NASA NTRS2015

Aerosol Properties From Combined Oxygen A Band Radiances and Lidar

We have developed a new aerosol retrieval technique based on combing high-resolution A band spectra with lidar profiles. Our goal is the development of a technique to retrieve aerosol absorption, one of the critical parameters affecting the global radiation budget and one which is currently poorly constrained by satellite measurements. Our approach relies on two key factors: 1) the use of high spectral resolution (17,000:1) measurements which resolve the A-band line structure, and 2) the use of co-located lidar profile measurements to constrain the vertical distribution of scatterers in the forward model. The algorithm has been developed to be applied to observations from the CALIPSO and OCO-2 satellites, flying in formation as part of the A-train constellation. We describe the approach and present simulated retrievals to illustrate performance potential.

Winker, Dave↗
DOE OSTI2024

Measurement report: A comparison of ground-level ice-nucleating-particle abundance and aerosol properties during autumn at contrasting marine and terrestrial locations

Abstract. Ice-nucleating particles (INPs) are an essential class of aerosols found worldwide that have far-reaching but poorly quantified climate feedback mechanisms through interaction with clouds and impacts on precipitation. These particles can have highly variable physicochemical properties in the atmosphere, and it is crucial to continuously monitor their long-term concentration relative to total ambient aerosol populations at a wide variety of sites to comprehensively understand aerosol–cloud interactions in the atmosphere. Hence, our study applied an in situ forced expansion cooling device to measure ambient INP concentrations and test its automated continuous measurements at atmospheric observatories, where complementary aerosol instruments are heavily equipped. Using collocated aerosol size, number, and composition measurements from these sites, we analyzed the correlation between sources and abundance of INPs in different environments. Toward this aim, we have measured ground-level INP concentrations at two contrasting sites, one in the Southern Great Plains (SGP) region of the United States with a substantial terrestrially influenced aerosol population and one in the Eastern North Atlantic Ocean (ENA) region with a primarily marine-influenced aerosol population. These measurements examined INPs mainly formed through immersion freezing and were performed at a ≤ 12 min resolution and with a wide range of heterogeneous freezing temperatures (Ts above −31 °C) for at least 45 d at each site. The associated INP data analysis was conducted in a consistent manner. We also explored the additional offline characterization of ambient aerosol particle samples from both locations in comparison to in situ data. From our ENA data, on average, INP abundance ranges from ≈ 1 to ≈ 20 L−1 (−30 °C ≤ T ≤ −20 °C) during October–November 2020. Backward air mass trajectories reveal a strong marine influence at ENA with 75.7 % of air masses originating over the Atlantic Ocean and 96.6 % of air masses traveling over open water, but analysis of particle chemistry suggests an additional INP source besides maritime aerosols (e.g., sea spray aerosols) at ENA. In contrast, 90.8 % of air masses at the SGP location originated from the North American continent, and 96.1 % of the time, these air masses traveled over land. As a result, organic-rich SGP aerosols from terrestrial sources exhibited notably high INP abundance from ≈ 1 to ≈ 100 L−1 (−30 °C ≤ T ≤ −15 °C) during October–November 2019. The probability density function of aerosol surface area-scaled immersion freezing efficiency (ice nucleation active surface site density; ns) was assessed for selected freezing temperatures. While the INP concentrations measured at SGP are higher than those of ENA, the ns(T) values of SGP (≈ 105 to ≈ 107 m−2 for −30 °C ≤ T ≤ −15 °C) are reciprocally lower than ENA for approximately 2 orders of magnitude (≈ 107 to ≈ 109 m−2 for −30 °C ≤ T ≤ −15 °C). The observed difference in ns(T) mainly stems from varied available aerosol surface areas, Saer, from two sites (Saer,SGP > Saer,ENA). INP parameterizations were developed as a function of examined freezing temperatures from SGP and ENA for our study periods.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1998

A Multi-Instrument Approach for Characterizing the Vertical Structure of Aerosol Properties: Case Studies in the Pacific Basin Troposphere

During February/March 1994, a series of aircraft-based aerosol measurements were carried out in the Pacific Basin troposphere using a differential absorption lidar system deployed by NASA Langley, and optical spectrometer probes and a wire-impactor system operated by NASA Ames. A modified Klett inversion algorithm was applied to extract altitude profiles of aerosol backscattering from the IR lidar signal. The algorithm that we have designed for this purpose utilizes the in situ aerosol measurements to normalize the lidar profile at the aircraft altitude and to supply the lidar ratio as a function of height. The lidar-derived aerosol backscattering coefficients were then compared to the backscattering coefficients calculated from the in situ measurements. During several local aircraft descents, we found good agreement between the remote lidar and in situ results for the absolute value of the aerosol backscattering coefficient and its altitude variation only when we allowed for several layers with different aerosol refractive indices. The agreement validates our lidar calibration method and provides an indication of the variation in aerosol refractive index as a function of altitude. Two of the three case studies performed in this paper reveal layers of anthropogenic aerosols transported long distances into the Pacific Basin troposphere. A third case implies the existence of a layer of dustlike aerosol particles in the lower troposphere, most likely of Asian origin.

Redemann, J.↗
NASA NTRS2011

Statistically Optimized Inversion Algorithm for Enhanced Retrieval of Aerosol Properties from Spectral Multi-Angle Polarimetric Satellite Observations

The proposed development is an attempt to enhance aerosol retrieval by emphasizing statistical optimization in inversion of advanced satellite observations. This optimization concept improves retrieval accuracy relying on the knowledge of measurement error distribution. Efficient application of such optimization requires pronounced data redundancy (excess of the measurements number over number of unknowns) that is not common in satellite observations. The POLDER imager on board the PARASOL microsatellite registers spectral polarimetric characteristics of the reflected atmospheric radiation at up to 16 viewing directions over each observed pixel. The completeness of such observations is notably higher than for most currently operating passive satellite aerosol sensors. This provides an opportunity for profound utilization of statistical optimization principles in satellite data inversion. The proposed retrieval scheme is designed as statistically optimized multi-variable fitting of all available angular observations obtained by the POLDER sensor in the window spectral channels where absorption by gas is minimal. The total number of such observations by PARASOL always exceeds a hundred over each pixel and the statistical optimization concept promises to be efficient even if the algorithm retrieves several tens of aerosol parameters. Based on this idea, the proposed algorithm uses a large number of unknowns and is aimed at retrieval of extended set of parameters affecting measured radiation.

Dubovik, O↗
NASA NTRS1992

Upper-atmosphere Aerosols: Properties and Natural Cycles

The middle atmosphere is rich in its variety of particulate matter, which ranges from meteorite debris, to sulfate aerosols, to polar stratospheric ice clouds. Volcanic eruptions strongly perturb the stratospheric sulfate (Junge) layer. High-altitude 'noctilucent' ice clouds condense at the summer mesopause. The properties of these particles, including their composition, sizes, and geographical distribution, are discussed, and their global effects, including chemical, radiative, and climatic roles, are reviewed. Polar stratospheric clouds (PSCs) are composed of water and nitric acid in the form of micron-sized ice crystals. These particles catalyze reactions of chlorine compounds that 'activate' otherwise inert chlorine reservoirs, leading to severe ozone depletions in the southern polar stratosphere during austral spring. PSCs also modify the composition of the polar stratosphere through complex physiocochemical processes, including dehydration and denitrification, and the conversion of reactive nitrogen oxides into nitric acid. If water vapor and nitric acid concentrations are enhanced by high-altitude aircraft activity, the frequency, geographical range, and duration of PSCs might increase accordingly, thus enhancing the destruction of the ozone layer (which would be naturally limited in geographical extent by the same factors that confine the ozone hole to high latitudes in winter). The stratospheric sulfate aerosol layer reflects solar radiation and increases the planetary albedo, thereby cooling the surface and possibly altering the climate. Major volcanic eruptions, which increase the sulfate aerosol burden by a factor of 100 or more, may cause significant global climate anomalies. Sulfate aerosols might also be capable of activating stratospheric chlorine reservoirs on a global scale (unlike PCSs, which represent a localized polar winter phenomenon), although existing evidence suggests relatively minor perturbations in chlorine chemistry. Nevertheless, if atmospheric concentrations of chlorine (associated with anthropogenic use of chlorofluorocarbons) continue to increase by a factor of two or more in future decades, aircraft emissions of sulfur dioxide and water vapor may take on greater significance.

Turco, Richard P.↗