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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Fine Ash-Bearing Particles as a Major Aerosol Component in Biomass Burning Smoke

Biomass burning (BB) events are occurring globally with increasing frequency, and their emissions are having more impacts on human health and climate. Large ash particles are recognized as a BB product with major influences on soil and water environments. However, fine-ash particles, which have diameters smaller than several microns and characteristic morphologies and compositions (mainly Ca and Mg carbonates), have not yet been explicitly considered as a major BB aerosol component either in field observations or climate models. This study measured BB aerosol samples using transmission electron microscopy (TEM) and ion chromatography during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. We show that significant amounts of fine ash-bearing particles are transported >100 km from their fire sources. Our environmental chamber experiments suggest that they can act as cloud condensation and ice nuclei. We also found considerable amounts of fine ash-bearing particles in the TEM samples collected during previous campaigns (Biomass Burning Observation Project and Megacity Initiative: Local and Global Research Observations). These ash particles are commonly mixed with organic matter and make up ~8% and 5% of BB smoke by number and mass, respectively, in samples collected during the FIREX-AQ campaign. The measured ash-mass concentrations are approximately five times and six times greater than those of BB black carbon and potassium, respectively, scaling to an estimated global emission of 11.6 Tg yr -1 with a range of 8.8–16.3 Tg yr -1 . Better characterization and constraints on these fine ash-bearing particles will improve BB aerosol measurements and strengthen assessments of BB impacts on human health and climate.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRSDate not supplied

Identifying Chemical and Optical Smoke Signatures in Suborbital Observations to Improve Model Projections

Biomass Burning (BB) fires are expected to occur more frequently in the future due to climate change, the build‐up of fuels due to fire suppression, and the expansion of the wildland‐urban interface [Schoennagel et al., 2017; Shivdenko & Schepaschenko, 2013; Stevens et al., 2014; Turner et al., 2019; Yue et al., 2015; Tilman et al., 2001]. Accurate knowledge of the abundance, distribution, and optical properties of absorbing aerosols such as BB smoke is essential to understanding regional and global aerosol radiative effects [Boucher et al., 2013]. It is recognized that differing fuel types (e.g., rice straw, ponderosa pine), combustion modes (i.e., flaming, smoldering or both) and temperature/ moisture content produce smoke with differing optical characteristics (e.g., aerosol light scattering and absorption) and component mixing ratios [e.g., BC, OC and inorganic species such as sulfate, potassium, chloride; Streets et al. 2003; Reid et al., 2005a, b; Janhäll et al., 2010; Sayer et al., 2014]. However, climate models often ascribe a fixed set of emission factors [i.e., amount of particulate for a given species released in the atmosphere per unit dry fuel burned; Darmenov and Dasilva, 2013] and optical properties [Hess et al., 1998] to all BB aerosol plumes, inherently limiting accurate representation of the global and regional heterogeneity of BB. The overarching goal of the proposed work is to improve the microphysical and optical representation of different types of Biomass Burning in Chemistry Transport Models. Our strategy is to capitalize on multiple airborne campaigns (e.g., ARCTAS, SEAC4RS, ORACLES, FIREX-AQ), which sampled different types of BB plumes at different aging stages. Models, when improved and combined with satellite, airborne, and ground observations will help address many aerosol science objectives from the NASA Decadal survey [National Academies of Sciences, Engineering, and Medicine. 2018].

Meloe Shenandoah F Kacenelenbogen↗
NASA NTRS2022

Satellite-Based Evaluation of AeroCom Model Bias in Biomass Burning Regions

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by −93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

biomass burning aerosols↗
DOE OSTI2022

Satellite-based evaluation of AeroCom model bias in biomass burning regions

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by –93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Undersizing of aged African biomass burning aerosol by an ultra-high-sensitivity aerosol spectrometer

The ultra-high-sensitivity aerosol spectrometer (UHSAS) differs from most other optical particle spectrometers by using a high-power infrared (IR) laser to detect small particles and reduce the sizing ambiguity due to the non-monotonicity of scattering with particle size. During the NASA ORACLES project (ObseRvations of Aerosols above CLouds and their intEractionS) over the southeast Atlantic Ocean, the UHSAS clearly undersized particles in the biomass burning plume extending from southern Africa. Since the horizontal and vertical extent of the plume was vast, the NASA P-3B research aircraft often flew through a fairly uniform biomass burning plume for periods exceeding 30 min, sufficient time to explore the details of the UHSAS response by selecting single particle sizes with a differential mobility analyzer (DMA) and passing them to the UHSAS. This was essentially an in-flight calibration of the UHSAS using the particles of interest. Two modes of responses appeared. Most particles were undersized by moderate amounts, ranging from not at all for 70 nm aerosols to 15 % for 280 nm particles. Mie scattering calculations show that composition-dependent refractive index of the particles cannot explain the pattern. Heating of brown carbon or tarballs in the beam causing evaporation and shrinking of the particles is the most plausible explanation, though mis-sizing due to non-sphericity cannot be ruled out. A small fraction (10 %–30 %) of the particles were undersized by 25 % to 35 %. Those were apparently the particles containing refractory black carbon. Laboratory calibrations confirm that black carbon is drastically undersized by the UHSAS, because particles heat to their vaporization point and shrink. A simple empirical correction equation was implemented that dramatically improves agreement with DMA distributions between 100 and 500 nm. It raised the median particle diameter by 18 nm, from 163 to 181 nm, during the August 2017 deployment and by smaller amounts during deployments with less intense pollution. Calculated scattering from UHSAS size distributions increased by about 130 %, dramatically improving agreement with scattering measured by nephelometers. The correction is only valid in polluted instances; clean marine boundary layer and free troposphere aerosols behaved more like the calibration spheres. We were unable to directly test the correction between 500 and 1000 nm, though aerodynamic particle sizer (APS) data appear to show that the correction is poor at the largest diameters, which is no surprise as the composition of those particles is likely to be quite different than that of the accumulation mode. This adds to the evidence that UHSAS data must be treated cautiously whenever the aerosol may absorb infrared light. Similar corrections may be required whenever brown carbon aerosol is present.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2021

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth’s biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~ 350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~ 100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

Jens Redemann↗
DOE OSTI2021

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June-October), aerosol particles reaching 3-5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2003

The Study of Biomass Emissions for Defining Radiative Forcing of Climate

Accurate quantification of the amounts of trace gases and particulate matter emitted from vegetation fires and other sources of biomass burning (agricultural waste and biofuels) on a regional and global basis is required by a number of users, including scientists studying a wide range of atmospheric processes, national governments who are required to report greenhouse gas emissions, and those interested in quantifying the sources of air pollution that affect human health at regional scales. Over the past decade, improvements in the ability to detect and map fires using a number of different satellite systems have been achieved, largely through efforts coordinated through working groups organized by the IGBP Data and Information System and Global Observation of Forest Cover (GOFC) projects. In addition, significant advances and improvement in or understanding of the emissions factors for biomass burning in different biomes has resulted through efforts by the Biomass Burning Experiment (BIBEX) organized through the International Global Atmospheric Chemistry project. A number of satellite-based fire data products have been generated, and a number of new products will shortly be available. These new data products will provide the basis for estimating emissions from biomass burning on a global basis. However, a number of issues remain concerning the availability of other data sets needed to generate these estimates. Recognizing these issues, the GOFC-Fire Satellite Validation Workshop (held in Lisbon, Portugal on 9-11 July 2001), recommended that a workshop focusing on Improving Global Estimates of Atmospheric Emissions from Biomass Burning be organized. This workshop was held from 17- 19 July 2002 on the campus of the University of Maryland, College Park, Maryland. This workshop served as the annual meeting of the GOFC/GOLD-Fire Program. The overall goals of the meeting were to review the information products generated from satellite imagery and other sources that are currently available for developing emission estimates from biomass burning, evaluate areas where improved or additional products would be beneficial, and recommend products for use by the atmospheric science community.

Penner, Joyce↗
DOE OSTI2016

Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS) Field Campaign Report

Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS), a National Aeronautics and Space Administration (NASA) field campaign, was based out of Ellington Field in Houston, Texas, during August and September 2013. The study focused on pollution emissions and the evolution of gases and aerosols in deep convective outflow, and the influences and feedbacks of aerosol particles from anthropogenic pollution and biomass burning on meteorology, clouds, and climate. The project required three aircraft to accomplish these goals. The NASA DC-8 provided observations from near the surface to 12 km, while the NASA ER-2 provided high-altitude observations reaching into the lower stratosphere as well as important remote-sensing observations connecting satellites with observations from lower-flying aircraft and surface sites. The SPEC, Inc. Learjet obtained aerosol and cloud microphysical measurement in convective clouds and convective outflow.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2004

Heterogeneous Chemistry Involving Methanol in Tropospheric Clouds

In this report we analyze airborne measurements to suggest that methanol in biomass burning smoke is lost heterogeneously in clouds. When a smoke plume intersected a cumulus cloud during the SAFARI 2000 field project, the observed methanol gas phase concentration rapidly declined. Current understanding of gas and aqueous phase chemistry cannot explain the loss of methanol documented by these measurements. Two plausible heterogeneous reactions are proposed to explain the observed simultaneous loss and production of methanol and formaldehyde, respectively. If the rapid heterogeneous processing of methanol, seen in a cloud impacted by smoke, occurs in more pristine clouds, it could affect the oxidizing capacity of the troposphere on a global scale.

Tabazadeh, A.↗
NASA NTRS2017

Historic Global Biomass Burning Emissions for CMIP6 (BB4CMIP) Based on Merging Satellite Observations with Proxies and Fire Models (1750-2015)

Fires have influenced atmospheric composition and climate since the rise of vascular plants, and satellite data has shown the overall global extent of fires. Our knowledge of historic fire emissions has progressively improved over the past decades due mostly to the development of new proxies and the improvement of fire models. Currently there is a suite of proxies including sedimentary charcoal records, measurements of fire-emitted trace gases and black carbon stored in ice and firn, and visibility observations. These proxies provide opportunities to extrapolate emissions estimates based on satellite data starting in 1997, but each proxy has strengths and weaknesses regarding, for example, the spatial and temporal extents over which they are representative. We developed a new historic biomass burning emissions dataset starting in 1750 that merges the satellite record with several existing proxies, and uses the average of six models from the Fire Model Intercomparison Project (FireMIP) protocol to estimate emissions when the available proxies had limited coverage. According to our approach, global biomass burning emissions were relatively constant with 10-year averages varying between 1.8 and 2.3 petagrams of carbon per year. Carbon emissions increased only slightly over the full time period and peaked during the 1990's after which they decreased gradually. There is substantial uncertainty in these estimates and patterns varied depending on choices regarding data representation, especially on regional scales. The observed pattern in fire carbon emissions is for a large part driven by African fires, which accounted for 58 percent of global fire carbon emissions. African fire emissions declined since about 1950 due to conversion of savanna to cropland, and this decrease is partially compensated for by increasing emissions in deforestation zones of South America and Asia. These global fire emissions estimates are mostly suited for global analyses and will be used in the Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations.

Biomass burning; Satellite observations; computer ↗
NASA NTRS2002

Visions of our Planet's Atmosphere, Land & Oceans

The NASA/NOAA Electronic Theater presents Earth science observations and visualizations in a historical perspective. Fly in from outer space to South Africa, Cape Town and Johannesburg using NASA Terra MODIS data, Landsat data and 1m IKONOS "Spy Satellite" data. Zoom in to any place South Africa using Earth Viewer 3D from Keyhole Inc. and Landsat data at 30 m resolution. Go back to the early weather satellite images from the 1960s and see them contrasted with the latest US and international global satellite weather movies including hurricanes & "tornadoes". See the latest visualizations of spectacular images from NASA/NOAA remote sensing missions like Terra, GOES, TRMM, SeaWiFS, Landsat 7 including 1 - min GOES rapid scan image sequences of Nov 9th 2001 Midwest tornadic thunderstorms and have them explained. See how High-Definition Television (HDTV) is revolutionizing the way we present science to the public. See dust storms and flooding in Africa and smoke plumes from fires in Mexico. See visualizations featured on the covers of Newsweek, TIME, National Geographic, Popular Science & on National & International Network TV. New computer software tools allow us to roam & zoom through massive global images e.g. Landsat tours of the US, and Africa, showing desert and mountain geology as well as seasonal changes in vegetation. See animations of the north and south polar ice packs and with icebergs on the coasts of Greenland and off the coast of Antarctica. Spectacular new visualizations of the global land, atmosphere & oceans are shown. Listen to the pulse of our planet. See how land vegetation, ocean plankton, clouds and temperatures respond to the sun & seasons. See vortexes and currents in the global oceans that bring up the nutrients to feed tiny algae and draw the fish, whales and fisherman. See the how the ocean blooms in response to these currents and El Nino/La Nina climate changes. See the city lights, fishing fleets, gas flares and biomass burning of the Earth at night observed by the "night-vision" DMSP military satellite. The presentation will be made using the latest HDTV and video projection technology that is now done from a laptop computer through an entirely digital path.

Hasler, Arthur F.↗
NASA NTRS2016

In-Situ and Remotely-Sensed Observations of Biomass Burning Aerosols at Doi Ang Khang, Thailand During 7-SEAS BASELInE 2015

The spring 2015 deployment of a suite of instrumentation at Doi Ang Khang (DAK) in northwestern Thailand enabled the characterization of air masses containing smoke aerosols from burning predominantly in Myanmar. Aerosol Robotic Network (AERONET) Sun photometer data were used to validate Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 6 "Deep Blue" aerosol optical depth (AOD) retrievals; MODIS Terra and Aqua provided results of similar quality, with correlation coefficients of 0.93-0.94 and similar agreement within expected uncertainties to global-average performance. Scattering and absorption measurements were used to compare surface and total column aerosol single scatter albedo (SSA); while the two were well-correlated, and showed consistent positive relationships with moisture (increasing SSA through the season as surface relative humidity and total columnar water vapor increased), in situ surface-level SSA was nevertheless significantly lower by 0.12-0.17. This could be related to vertical heterogeneity and/or instrumental issues. DAK is at approximately 1,500 meters above sea level in heterogeneous terrain, and the resulting strong diurnal variability in planetary boundary layer depth above the site leads to high temporal variability in both surface and column measurements, and acts as a controlling factor to the ratio between surface particulate matter (PM) levels and column AOD. In contrast, while some hygroscopic effects were observed relating to aerosol particle size and Angstrom exponent, relative humidity variations appear to be less important for this ratio here. As part of the Seven South-East Asian Studies (7-SEAS) project, the Biomass-burning Aerosols & Stratocumulus Environment: Lifecycles and Interactions Experiment (BASELInE) was intended to probe physicochemical processes, interactions, and feedbacks related to biomass burning aerosols and clouds during the spring burning season (February-April) in southeast Asia (SEA).

biomass burning↗
DOE OSTI2016

The Two-Column Aerosol Project: Phase I-Overview and impact of elevated aerosol layers on aerosol optical depth

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). In addition, these layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. Lastly, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

A meteorological overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the southeastern Atlantic during 2016–2018: Part 1 – Climatology

In 2016–2018, the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project undertook 3-month-long deployments to the southeastern (SE) Atlantic Ocean using research aircraft to better understand the impact of biomass burning (BB) aerosol transport to the SE Atlantic Ocean on climate. In this (part 1 of the meteorological overview) paper, the climatological features at monthly timescales are investigated. The southern African easterly jet (AEJ-S), defined as the zonal easterlies over 600-700 hPa exceeding 6 m s-1 around 5-15°S, is a characteristic feature of the mid-level circulation over southern Africa that was also during the deployment months of August 2017, September 2016, and October 2018. Climatologically, the AEJ-S develops at lower altitudes (~3 km; 700 hPa) between 5-10° S in August, while it develops at around 4 km (~600 hPa) and further south (5-15 °S) in September and October, largely driven by the strong sensible heating over the African plateau. Notable meteorological anomalous characteristics during the 3 deployment months, compared to climatology (2000-2018), include the following: (1) during August 2017, the AEJ-S was weaker than the climatological mean, with an additional anomalous upper-level jet aloft (~6 km) around 10 °S. August 2017 was also drier over the SE Atlantic at 600-700 hPa than climatology, with a stronger Benguela low-level jet (LLJ) at 925-950 hPa along the Namibian coast of the SE Atlantic. Consistent with this, the southern Atlantic anticyclone was also stronger and closer to the coast than the August climatological mean. (2) During September 2016, the AEJ-S intensity was similar to the climatological mean, although the heat low and vertical motion over the land was slightly stronger compared to the September climatology. The LLJ and the large-scale southern Atlantic anticyclone were stronger than the climatological mean. (3) During October 2018, the AEJ-S was slightly weaker compared to the climatological mean, as was the LLJ and the southern Atlantic anticyclone. October 2018 was wetter over the Benguela coastal region at 600 hPa than the climatological mean. During all the deployment months, the sea surface temperatures (SST) over the SE Atlantic were warmer than the climatological means, but the monthly mean low cloud fraction was only noticeably reduced in August 2017. A weak August 2017 AEJ-S can explain low offshore black carbon (BC) mixing ratios within the European Centre for Medium-Range Weather Forecasts (ECMWF) Copernicus Atmosphere Monitoring Service (CAMS) reanalysis, although the BC peak altitude, at 2-3 km, is below that of the AEJ-S. The upper-level wave disturbance and the associated anomalous circulation also explain the weakening of AEJ-S through the reduction of the strength of the heat low over the land during August 2017.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Sensitivity of Regional WRF‐Chem Air Quality and Weather Simulations to Biomass‐Burning Emission Data Sets: A Case Study of the Impact of Canadian Wildfire on the US°

This study focuses on the period from June 26 to 29, 2023, when record‐breaking Canadian wildfires severely impacted air quality in the Midwest United States. Using the Weather Research and Forecasting Model with Chemistry (WRF‐Chem) and four biomass‐burning data sets (Fire Inventory from NCAR version 1, Fire Inventory from NCAR version 2.5, Quick Fire Emissions Data set [QFED], and Regional ABI‐VIIRS Emission), we analyzed aerosol transport from Canada to the US and assessed the model's accuracy in predicting PM 2.5 , O 3 , CO and aerosol weather feedback. Model simulations were compared with ground‐based and remote sensing observations as well as field measurements from the Community Research on Climate and Urban Science (CROCUS) project. Our findings show that the movement of a low‐pressure system from the Great Lakes to the Atlantic, combined with the high‐pressure system over the Atlantic, caused the transport of aerosols from Canadian wildfires to the US. Results show WRF‐Chem significantly underestimated key atmospheric components: aerosol optical depth (AOD) by over 50%, PM 2.5 by 65%–90% and peak O 3 concentrations by 50%–55% across four biomass burning data sets. Additionally, CO and NO 2 concentrations were underpredicted. The substantial underestimation of PM 2.5 led to an overestimation of temperature by up to 3.6 °C primarily due to excessive downward shortwave radiation, which resulted from the underestimation of direct aerosol effects and an increase in sensible heat flux. Among the biomass‐burning data sets, QFED produced the most accurate AOD and PM 2.5 predictions due to improved wildfire emission estimates, leading to a 1.0 to 1.5 °C reduction in temperature overestimation during the daytime. These findings underscore the need for improving wildfire emission estimates for trace gases and aerosols to enhance air quality and weather feedback predictions.

WRF-chem model↗
DOE OSTI2018

Final Technical Report

Southern Africa is the world’s largest emitter of biomass burning aerosols. Their westward transport over the remote southeast Atlantic ocean colocates some of the largest atmospheric loadings of absorbing aerosol with the least examined of the Earth’s major subtropical stratocumulus decks. Global aerosol model results highlight that the largest positive top-ofatmosphere forcing in the world occurs in the southeast Atlantic, but this region exhibits large differences in magnitude and sign between reputable models, in part because of high variability in the underlying model cloud distributions. Many uncertainties contribute to the highly variable model radiation fields: the aging of the shortwave-absorbing aerosol during transport, how much of the aerosol mixes into the cloudy boundary layer, and how the low clouds adjust to smokeradiation and smoke-cloud interactions. In addition, the ability of the biomass burning aerosol to absorb shortwave radiation is known to vary seasonally as the fuel type on land changes. LASIC (Layered Atlantic Smoke Interactions with Clouds) is a strategy to improve our understanding of aged carbonaceous aerosol, its seasonal evolution, and the mechanisms by which clouds adjust to the presence of the aerosol. The observational strategy centers on deploying the AMF1 cloud, aerosol, and atmospheric profiling instrumentation to Ascension Island, located within the trade-wind shallow cumulus regime (14.50W, 80S) 3000 km offshore of continental Africa. The location is within the latitude zone of the maximum outflow of aerosol, with the deepening boundary layer known to entrain free-tropospheric smoke. The primary activities for LASIC are: 1) to improve current knowledge on aged biomass burning aerosol and its radiative properties as a function of the seasonal cycle; 2) to use surface-based remote sensing to sensitively interrogate the atmosphere for the relative vertical location of aerosol and clouds; 3) to improve our understanding of the cloud adjustments to the presence of shortwave-absorbing aerosol within the vertical column, both through aerosol-radiation and through aerosol-cloud interactions; 4) to aid low cloud parameterization efforts for climate models. The measurements span June 1, 2016 - October 31, 2017, encompassing two July-October biomass burning seasons. The August-September, 2016, months include an Intensive Observing Period (IOP) with 8x/daily radiosondes. In 2017, from 16 August through 7 September, the UK FAAM Bae- 146 plane was deployed from Ascension, providing complementary data on the atmosphere’s vertical structure as part of the CLARIFY project, with similar scientific goals. The NASA ORACLES aircraft campaign, sharing similar objectives to LASIC, deployed from Namibia in September, 2016, and Sao Tome in August, 2017. The latter included a suitcase flight to Ascension spanning August 18-21. In 2017 a CAPS-SSA instrument belonging to Aerodyne was brought to Ascension, gathering data primarily for August, towards providing a second, independent measurement of aerosol absorption. Ascension Island is also an AERONET site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Simulation of the transport, vertical distribution, optical properties and radiative impact of smoke aerosols with the ALADIN regional climate model during the ORACLES-2016 and LASIC experiments

Estimates of the direct radiative effect (DRE) from absorbing smoke aerosols over the southeast Atlantic Ocean (SAO) require simulation of the microphysical and optical properties of stratocumulus clouds as well as of the altitude and shortwave (SW) optical properties of biomass burning aerosols (BBAs). In this study, we take advantage of the large number of observations acquired during the ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES-2016) and Layered Atlantic Smoke Interactions with Clouds (LASIC) projects during September 2016 and compare them with datasets from the ALADIN-Climate (Aire Limitée Adaptation dynamique Développement InterNational) regional model. The model provides a good representation of the liquid water path but the low cloud fraction is underestimated compared to satellite data. The modeled total-column smoke aerosol optical depth (AOD) and above-cloud AOD are consistent ( ~0.7 over continental sources and ~0.3 over the SAO at 550 nm) with the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2), Ozone Monitoring Instrument (OMI) or Moderate Resolution Imaging Spectroradiometer (MODIS) data. The simulations indicate smoke transport over the SAO occurs mainly between 2 and 4 km, consistent with surface and aircraft lidar observations. The BBA single scattering albedo is slightly overestimated compared to the Aerosol Robotic Network (AERONET) and more significantly when compared to Ascension Island surface observations. The difference could be due to the absence of internal mixing treatment in the ALADIN-Climate model. The SSA overestimate leads to an underestimation of the simulated SW radiative heating compared to ORACLES data. ALADIN-Climate simulates a positive (monthly mean) SW DRE of about +6 W m -2 over the SAO (20 ° S–10 ° N and 10 ° W–20 ° E) at the top of the atmosphere and in all-sky conditions. Over the continent, the presence of BBA is shown to significantly decrease the net surface SW flux, through direct and semi-direct effects, which is compensated by a decrease (monthly mean) in sensible heat fluxes ( -25 W m -2 ) and surface land temperature ( -1.5 ° C) over Angola, Zambia and the Democratic Republic of the Congo, notably. The surface cooling and the lower tropospheric heating decrease the continental planetary boundary layer height by about ~200 m.

54 ENVIRONMENTAL SCIENCES↗