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Modeled and observed properties related to the direct aerosol radiative effect of biomass burning aerosol over the southeastern Atlantic

Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.

54 ENVIRONMENTAL SCIENCES↗

Multiphase Processing of the Water-Soluble and Insoluble Phases of Biomass Burning Organic Aerosol

Biomass burning is one of the most significant sources of organic aerosol in the atmosphere. Biomass burning organic aerosol (BBOA) has been observed to undergo liquid– liquid phase separation (LLPS) to give core–shell morphology with the hydrophobic phase encapsulating the hydrophilic phase, potentially impacting the evolution of light-absorbing components, i.e., brown carbon (BrC), through multiphase processes. Here, we demonstrate how multiphase processing differs between the watersoluble (i.e., hydrophilic) and insoluble (i.e., hydrophobic) phases of BBOA in terms of reactive uptake of ozone in a coated-wall flow tube. Effects of relative humidity (RH) and ultraviolet (UV) irradiation were investigated. Experimental timeseries were used to inform simulations using multilayer kinetic modeling. Among non-irradiated thin films, the uptake coefficient was greatest for the water-soluble phase at 75% RH (3 × 10 –5 , corresponding to a diffusion coefficient of BrC, D BrC , of 3 × 10 –9 cm 2 s –1 ) and least for the same phase at 0% RH (1 × 10 –5 , corresponding to D BrC of 1 × 10 –10 cm 2 s –1 ). The uptake coefficient for the water-insoluble phase fell between these two (about 1.5 × 10 –5 ), regardless of RH, and the corresponding D BrC increased only slightly (8 × 10 –10 cm 2 s –1 at 0% RH to 9 × 10 –10 cm 2 s –1 at 75% RH). The uptake coefficients of both phases at 0% RH decreased significantly after UV irradiation, consistent with a transition from viscous liquid to solid and supported by qualitative microscopy observations. Modeling multiphase ozone oxidation of primary BrC components in the atmosphere demonstrated, first, that LLPS may extend the lifetime of water-soluble BBOA encapsulated by water-insoluble species by a factor of 1.5 at moderate to high RH and, also, that UV irradiation may extend the lifetime of both phases by more than a factor of 2.5.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Semi‐Volatile Organic Partitioning Improves Simulation of Biomass Burning Aerosol Mixing State Evolution

Biomass burning aerosols significantly contribute to atmospheric composition and radiative forcing, with black carbon (BC) mixing states critically influencing optical properties and climate impacts. Recent field observations reveal a systematic three‐phase evolution in BC coating thickness during plume aging: rapid initial growth, quasi‐equilibrium, and gradual coating loss. Current models misrepresent this evolution due to oversimplified treatment of organic aerosol volatility. Here we demonstrate that incorporating semi‐volatile organic partitioning through the MATRIX‐VBS model fundamentally improves simulation accuracy compared to traditional non‐volatile approaches. Evaluation against four field campaigns spanning fresh to aged plumes shows MATRIX‐VBS successfully captures the observed three‐phase pattern, and global application reveals universal three‐phase evolution with substantial regional variations. These advances address critical gaps in aerosol mixing state representation and provide essential improvements for climate model predictions in wildfire‐affected regions.

Gao, Chloe Yuchao [Fudan Univ., Shanghai (China); ↗

Influence of Synoptic-Dynamic Meteorology on the Long-Range Transport of Indochina Biomass Burning Aerosols

Impacts of long-range transported biomass burning aerosols from northern Indochina on regional air quality, atmospheric visibility, and climate effects have been discussed extensively in the literature over the past decade. However, the mechanism between aerosol transport and the low-level jet (LLJ) in synoptic meteorology dynamics (e.g., the frontal system) is still not fully understood. In this study, we present results of aerosol-LLJ interaction based on the National Aeronautics and Space Administration/Modern Era Retrospective-analysis for Research and Application version 2 (NASA/MERRA-2) dataset simultaneous to field campaigns in spring 2013–2015 over Southeast Asia. For linking the atmospheric circulation to aerosol transport, a general meteorological condition favorable for aerosol transport is demonstrated. Biomass burning aerosol accumulation over the source region (i.e., northern Indochina) coincided with weak westerly system over the northern South China Sea, and as the synoptic weather system evolved, the aerosols were transported to downwind regions (i.e., Taiwan and West Pacific) by a cold front and LLJ dynamics. The MERRA-2 reanalysis data show the postcold front accompanied a LLJ stream at approximately 700 hPa (3 km) and accelerated the haze plume transport eastward with a life cycle of approximately 3–5 days, an event that reoccurred multiple times from March to April. Our results indicate that coexistence of LLJ and a South China Sea anticyclone at 700 hPa, which primarily could drive the mechanism behind these transport events. Furthermore, more observational data from Southeast Asia would greatly benefit studies of aerosol-meteorology interactions in the region.

Hsiang-Yu Huang↗

Using OMI Observations to Measure Aerosol Absorption of Biomass Burning Aerosols Above Clouds

The presence of absorbing aerosol layers above clouds is unambiguously detected by the TOMS/OMI UV Aerosol Index (AI) that uses satellite observations at two near-UV channels. A sensitivity study using radiative transfer calculations shows that the AI signal of resulting from the presence of aerosols above clouds is mainly driven by the aerosol absorption optical depth and the optical depth of the underlying cloud. Based on these results, an inversion algorithm has been developed to retrieve the aerosol optical depth (AOD) of aerosol layers above clouds. In this presentation we will discuss the sensitivity analysis, describe the retrieval approach, and present results of applications of the retrieval method to OMI observations over the South Atlantic Ocean. Preliminary error analyses, to be discussed, indicate that the AOD can be underestimated (up to -30%) or overestimated (up to 60%) depending on algorithmic assumptions.

Torres, Omar↗

An Evaluation of Biomass Burning Aerosol Mass, Extinction, and Size Distribution in Geos Using Observations From Camp2EX

Biomass burning aerosol impacts aspects of the atmosphere and Earth system through radiative forcing, serving as cloud condensation nuclei, and air quality. Despite its importance, the representation of biomass burning aerosol is not always accurate in numerical weather prediction and climate models or reanalysis products. Using observations collected as part of the Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) in August through October of 2019, aerosol concentration and optical properties are evaluated within the Goddard Earth Observing System (GEOS) and its underlying aerosol module, GOCART. In the operational configuration, GEOS assimilates aerosol optical depth observations at 550 nm to constrain aerosol fields. Particularly for biomass burning aerosol, without the assimilation of aerosol optical depth, aerosol extinction is underestimated compared to observations collected in the Philippines region during the CAMP2Ex campaign. The assimilation process adds excessive amounts of carbon to account for the underestimated extinction, resulting in positive biases in the mass of black and organic carbon, especially within the boundary layer, relative to in situ observations from the Langley Aerosol Research Group Experiment. Counteracting this, GEOS is deficient in sulphate and nitrate aerosol just above the boundary layer. Aside from aerosol mass, extinction within GEOS is a function of ambient relative humidity and an assumed particle size distribution. The relationship between dry and ambient extinction in GEOS reveals that hygroscopic growth is too aggressive within the model for biomass burning aerosol. An additional concern lies in the assumed particle size distribution for GEOS, which has a mode radius that is too small for organic carbon. Variability in the observed particle size distribution for biomass burning aerosol within a single flight also illuminates the fact that a single assumed particle size distribution is not sufficient and that for a proper representation, a more advanced aerosol module with GEOS may be necessary.

Aerosol Mass↗

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↗

Strong Sensitivity of Simulated Biomass Burning Aerosol Transport and Radiative Effects Over the South Atlantic to Carbonaceous Aerosol Aging and Particle Density

Biomass burning aerosol (BBA) impacts climate through aerosol‐cloud‐radiation interactions, but models disagree on the sign and magnitude of BBA radiative effects. We quantify the sensitivity of BBA radiative effects and transport to three BBA‐relevant processes and properties: parameterized oxidative aging of organic aerosol (OA), a combined change to black carbon (BC) density and the method for calculating aerosol refractive index, and reduction in OA density. We evaluate Unified Model simulations against two aircraft campaigns from summer 2017 over the Southeast Atlantic. The model generally performs well, such that discrepancies between the observational data sets may sometimes limit the precision of the evaluation. Our newly developed aging parameterization reproduces observed OA:BC mass ratios well and allows modeled OA:BC to decrease with smoke age, but increases bias in aerosol extinction and changes the BBA radiative effect little (+0.12 W m -2 ). We calculate aerosol refractive index using either a volume‐weighted component average or the Maxwell‐Garnett (MG) mixing assumption, which represents BC as small inclusions in a host material. Compared to MG mixing, the volume‐weighted average refractive index and reduced BC density increase aerosol absorption, substantially increasing the total BBA radiative effect (+2.66 W m -2 ) and amount of BBA transported across the ocean through BC self‐lofting. Reducing OA density to better match literature values changes the total BBA radiative effect by −1.96 W m -2 . Changes to direct radiative effects exceed changes to cloud radiative effects. Our findings emphasize the sensitivity of aerosol radiative effects and transport to these processes and properties, which we suggest could be improved in climate models.

Southeast Atlantic↗

The Response of the Amazon Ecosystem to the Photosynthetically Active Radiation Fields: Integrating Impacts of Biomass Burning Aerosol and Clouds in the NASA GEOS Earth System Model

The Amazon experiences fires every year, and the resulting biomass burning aerosols, together with cloud particles, influence the penetration of sunlight through the atmosphere, increasing the ratio of diffuse to direct photosynthetically active radiation (PAR) reaching the vegetation canopy and thereby potentially increasing ecosystem productivity. In this study, we use the NASA Goddard Earth Observing System (GEOS) model with coupled aerosol, cloud, radiation, and ecosystem modules to investigate the impact of Amazon biomass burning aerosols on ecosystem productivity, as well as the role of the Amazon’s clouds in tempering this impact. The study focuses on a seven-year period (2010-2016) during which the Amazon experienced a variety of dynamic environments (e.g., La Niña, normal years, and El Niño). The direct radiative impact of biomass burning aerosols on ecosystem productivity—called here the aerosol diffuse radiation fertilization effect —is found to increase Amazonian Gross Primary Production (GPP) by 2.6% via a 3.8% increase in diffuse PAR (DFPAR) despite a 5.4% decrease in direct PAR (DRPAR) on multiyear average during burning seasons. On a monthly basis, this increase in GPP can be as large as 9.9% (occurring in August 2010). Consequently, the net primary production (NPP) in Amazon is increased by 1.5%, or ~92 Tg C a-1– equivalent to ~37% of the average carbon lost due to Amazon fires over the seven years considered. Clouds, however, strongly regulate the effectiveness of the aerosol diffuse radiation fertilization effect. The efficiency of this fertilization effect is the highest in cloud-free conditions and linearly decreases with increasing cloud amount until the cloud fraction reaches ~0.8, at which point the aerosol-influenced light changes from being a stimulator to an inhibitor of plant growth. Nevertheless, interannual changes in the overall strength of the aerosol diffuse radiation fertilization effect are primarily controlled by the large interannual changes in biomass burning aerosols rather than by changes in cloudiness during the studied period.

biomass burning aerosols on ecosystem productivity↗

The response of the Amazon ecosystem to the photosynthetically active radiation fields: integrating impacts of biomass burning aerosol and clouds in the NASA GEOS Earth system model

The Amazon experiences fires every year, and the resulting biomass burning aerosols, together with cloud particles, influence the penetration of sunlight through the atmosphere, increasing the ratio of diffuse to direct photosynthetically active radiation (PAR) reaching the vegetation canopy and thereby potentially increasing ecosystem productivity. In this study, we use the NASA Goddard Earth Observing System (GEOS) model with coupled aerosol, cloud, radiation, and ecosystem modules to investigate the impact of Amazon biomass burning aerosols on ecosystem productivity, as well as the role of the Amazon's clouds in tempering this impact. The study focuses on a 7-year period (2010–2016) during which the Amazon experienced a variety of dynamic environments (e.g., La Niña, normal years, and El Niño). The direct radiative impact of biomass burning aerosols on ecosystem productivity – called here the aerosol diffuse radiation fertilization effect – is found to increase Amazonian gross primary production (GPP) by 2.6 % via a 3.8 % increase in diffuse PAR (DFPAR) despite a 5.4 % decrease in direct PAR (DRPAR) on multiyear average during burning seasons. On a monthly basis, this increase in GPP can be as large as 9.9 % (occurring in August 2010). Consequently, the net primary production (NPP) in the Amazon is increased by 1.5 %, or ~92 Tg C yr -1 – equivalent to ~37 % of the average carbon lost due to Amazon fires over the 7 years considered. Clouds, however, strongly regulate the effectiveness of the aerosol diffuse radiation fertilization effect. The efficiency of this fertilization effect is the highest in cloud-free conditions and linearly decreases with increasing cloud amount until the cloud fraction reaches ~0.8, at which point the aerosol-influenced light changes from being a stimulator to an inhibitor of plant growth. Nevertheless, interannual changes in the overall strength of the aerosol diffuse radiation fertilization effect are primarily controlled by the large interannual changes in biomass burning aerosols rather than by changes in cloudiness during the studied period.

54 ENVIRONMENTAL SCIENCES↗

Impact of biomass burning aerosols on radiation, clouds, and precipitation over the Amazon: relative importance of aerosol–cloud and aerosol–radiation interactions

Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed simulations with a fully coupled meteorology–chemistry model, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). The ARIs of BB aerosols tend to suppress low-level liquid clouds by local warming and increased evaporation and to facilitate the formation of high-level ice clouds by enhancing updrafts and condensation at high altitudes. In contrast, the ACIs of BB aerosol particles tend to enhance the formation and lifetime of low-level liquid clouds by providing more cloud condensation nuclei (CCN) and to suppress the formation of high-level ice clouds by reducing updrafts and condensable water vapor at high altitudes (>8 km). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of –0.2 and 1.5 W m –2 , respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. The dependence of precipitation reduction on BB aerosol loading is greater in a strong convective regime than under weakly convective conditions. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.

54 ENVIRONMENTAL SCIENCES↗

Sources, Transport, and Climate Impacts of Biomass Burning Aerosols

In this presentation, I will first talk about fundamentals of modeling of biomass burning emissions of aerosols, then show the results of GOCART model simulated biomass burning aerosols. I will compare the model results with observations of satellite and ground-based network in terms of total aerosol optical depth, aerosol absorption optical depth, and vertical distributions. Finally the long-range transport of biomass burning aerosols and the climate effects will be addressed. I will also discuss the uncertainties associated with modeling and observations of biomass burning aerosols

Chin, Mian↗

Cloud processing and weeklong ageing affect biomass burning aerosol properties over the south-eastern Atlantic

Abstract Southern Africa produces a third of global biomass burning emissions, which have a long atmospheric lifetime and influence regional radiation balance and climate. Here, we use airmass trajectories to link different aircraft observations to investigate the evolution of biomass-burning aerosols during their westward transport from Southern Africa over the south-eastern Atlantic, where a semi-permanent stratocumulus cloud deck is located. Our results show secondary organic aerosol formation during the initial 3 days of transport, followed by decreases in organic aerosol via photolysis before reaching equilibrium. Aerosol absorption wavelength dependency decreases with ageing, due to an increase in particle size and photochemical bleaching of brown carbon. Cloud processing, including aqueous-phase reaction and scavenging, contributes to the oxidation of organic aerosols, while it strongly reduces large diameter particles and single-scattering albedo of biomass burning aerosols. Together, these processes resulted in a marine boundary layer with fewer yet more oxidized and absorbing aerosols.

54 ENVIRONMENTAL SCIENCES↗

Investigation of the CCN Activity, BC and UVBC Mass Concentrations of Biomass Burning Aerosols during the 2013 BASELInE Campaign

Biomass-burning (BB) aerosols, acting as cloud condensation nuclei (CCN), can influence cloud microphysical and radiative properties. In this study, we present CCN measured near the BB source regions over northern Southeast Asia (Doi Ang Khang, Thailand) and at downwind receptor areas (Lulin Atmospheric Background Station, Taiwan), focusing exclusively on 13-20 March 2013 as part of 2013 spring campaign of the Seven SouthEast Asian Studies (7-SEAS) intensive observation. One of the campaigns objectives is to characterize BB aerosols serving as CCN in SouthEast Asia (SEA). CCN concentrations were measured by a CCN counter at 5 supersaturation (SS) levels: 0.15%, 0.30%, 0.45%, 0.60%, and 0.75%. In addition, PM2.5 and black carbon mass concentrations were analyzed by using a tapered element oscillating microbalance and an aethalometer. It was found the number-size distributions and the characteristics of hygroscopicity (e.g., activation ratio and k) of BB aerosols in SEA have a strong diurnal pattern, and different behaviors of patterns were characterized under two distinct weather systems. The overall average value was low (0.05-0.1) but comparable with previous CCN studies in other BB source regions. Furthermore, a large fraction of UV-absorbing organic material (UVBC) and high Delta-C among BB aerosols were also observed, which suggest the existence of substantial particulate organic matter in fresh BB aerosols. These data provide the most extensive characterization of BB aerosols in SEA until now.

biomass burning aerosol↗

Isolating the effect of biomass burning aerosol emissions on 20th century hydroclimate in South America and Southeast Asia

Abstract Biomass burning is a significant source of aerosol emissions in some regions and has a considerable impact on regional climate. Earth system model simulations indicate that increased biomass burning aerosol emissions contributed to statistically significant decreases in tropical precipitation over the 20th century. In this study, we use the Community Earth System Model version 1 Large Ensemble (CESM1-LENS) experiment to evaluate the mechanisms by which biomass burning aerosol contributed to decreased tropical precipitation, with a focus on South America and Southeast Asia. We analyze the all-but-one forcing simulations in which biomass burning aerosol emissions are held constant while other forcings (e.g., greenhouse gas concentrations) vary throughout the 20th century. This allows us to isolate the influence of biomass burning aerosol on processes that contribute to decreasing precipitation, including cloud microphysics, the radiative effects of absorbing aerosol particles, and alterations in regional circulation. We also show that the 20th century reduction in precipitation identified in the CESM1-LENS historical and biomass burning experiments is consistent across Coupled Model Intercomparison Project Phase 5 models with interactive aerosol schemes and the CESM2 single-forcing experiment. Our results demonstrate that higher concentrations of biomass burning aerosol increases the quantity of cloud condensation nuclei and cloud droplets, limiting cloud droplet size and precipitation formation. Additionally, absorbing aerosols (e.g., black carbon) contribute to a warmer cloud layer, which promotes cloud evaporation, increases atmospheric stability, and alters regional circulation patterns. Corresponding convectively coupled circulation responses, particularly over the tropical Andes, contribute to further reducing the flow of moisture and moisture convergence over tropical land. These results elucidate the processes that affect the water cycle in regions prone to biomass burning and inform our understanding of how future changes in aerosol emissions may impact tropical precipitation over the 21st century.

Environmental Sciences & Ecology↗

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↗

An Overview of Regional Experiments on Biomass Burning Aerosols and Related Pollutants in Southeast Asia: From BASE-ASIA and the Dongsha Experiment to 7-SEAS

By modulating the Earth-atmosphere energy, hydrological and biogeochemical cycles, and affecting regional-to-global weather and climate, biomass burning is recognized as one of the major factors affecting the global carbon cycle. However, few comprehensive and wide-ranging experiments have been conducted to characterize biomass-burning pollutants in Southeast Asia (SEA) or assess their regional impact on meteorology, the hydrological cycle, the radiative budget, or climate change. Recently, BASEASIA (Biomass-burning Aerosols in South-East Asia: Smoke Impact Assessment) and the 7-SEAS (7- South-East Asian Studies) Dongsha Experiment were conducted during the spring seasons of 2006 and 2010 in northern SEA, respectively, to characterize the chemical, physical, and radiative properties of biomass-burning emissions near the source regions, and assess their effects. This paper provides an overview of results from these two campaigns and related studies collected in this special issue, entitled Observation, modeling and impact studies of biomass burning and pollution in the SE Asian Environment. This volume includes 28 papers, which provide a synopsis of the experiments, regional weatherclimate, chemical characterization of biomass-burning aerosols and related pollutants in source and sink regions, the spatial distribution of air toxics (atmospheric mercury and dioxins) in source and remote areas, a characterization of aerosol physical, optical, and radiative properties, as well as modeling and impact studies. These studies, taken together, provide the first relatively complete dataset of aerosol chemistry and physical observations conducted in the sourcesink region in the northern SEA, with particular emphasis on the marine boundary layer and lower free troposphere (LFT). The data, analysis and modeling included in these papers advance our present knowledge of source characterization of biomass-burning pollutants near the source regions as well as the physical and chemical processes along transport pathways. In addition, we raise key questions to be addressed by a coming deployment during springtime 2013 in northern SEA, named 7-SEASBASELInE (Biomass-burning Aerosols Stratocumulus Environment: Lifecycles and Interactions Experiment). This campaign will include a synergistic approach for further exploring many key atmospheric processes (e.g., complex aerosol-cloud interactions) and impacts of biomass burning on the surface-atmosphere energy budgets during the lifecycles of biomass burning emissions.

aerosol/biomass burning↗

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↗