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The NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) produced a unique dataset for research into aerosol-cloud-meteorology interactions with applications extending from process-based studies to multi-scale model intercomparison and improvement, and remote sensing algorithm assessments and advancements. ACTIVATE used two NASA Langley Research Center aircraft, a HU-25 Falcon and King Air, to conduct systematic and spatially coordinated flights over the northwest Atlantic Ocean amounting to 162 joint flights and 17 other single-aircraft flights between 2020 and 2022 across all seasons. Data cover 574 and 592 cumulative flights hours for the Falcon and King Air, respectively. The HU-25 Falcon flew conducted profiling at different level legs below, in, and just above boundary layer clouds (< 3 km) and obtained in situ measurements of trace gases, aerosol particles, clouds, and atmospheric state parameters. In cloud-free conditions, the Falcon similarly conducted profiling at different level legs within and immediately above the boundary layer. The King Air (the high-flyer) flew at approximately ~9 km conducting remote sensing with a lidar and polarimeter while also launching dropsondes. Collectively, simultaneous data collected from both aircraft help characterize the same vertical column of the atmosphere. In addition to individual instrument files, data from the Falcon aircraft are combined into “merge files” on the publicly available data archive that are created at different time resolutions of interest (e.g., 1, 5, 10, 15, 30, 60 s, or matching an individual data product start and stop times). This paper describes the ACTIVATE flight strategy, instrument and complementary dataset products, data access and usage details, and data application notes.

Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated, highly spectrally resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in situ bulk aerosol particle light absorption measured at three wavelengths (405, 532 and 664 nm) with a photoacoustic spectrometer (PAS). A light-absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS-measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm−1 ppbv−1; emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions, the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion or constant levels with age were all observed in the first 8 h after emission in different plumes. Within 8 h following emissions, 4-nitrocatechol, a well-characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped, possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 h) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer timescales and spatial scales, where its environmental impacts are likely to be greater.

Carbonaceous emissions from wildfires are a dynamic mixture of gases and particles that have important impacts on air quality and climate. Emissions that feed atmospheric models are estimated using burned area and fire radiative power (FRP) methods that rely on satellite products. These approaches show wide variability and have large uncertainties, and their accuracy is challenging to evaluate due to limited aircraft and ground measurements. Here, we present a novel method to estimate fire plume-integrated total carbon and speciated emission rates using a unique combination of lidar remote sensing aerosol extinction profiles and in situ measured carbon constituents. We show strong agreement between these aircraft-derived emission rates of total carbon and a detailed burned area-based inventory that distributes carbon emissions in time using Geostationary Operational Environmental Satellite FRP observations (Fuel2Fire inventory, slope = 1.33 ± 0.04, r2 = 0.93, and RMSE = 0.27). Other more commonly used inventories strongly correlate with aircraft-derived emissions but have wide-ranging over- and under-predictions. A strong correlation is found between carbon monoxide emissions estimated in situ with those derived from the TROPOspheric Monitoring Instrument (TROPOMI) for five wildfires with coincident sampling windows (slope = 0.99 ± 0.18; bias = 28.5%). Smoke emission coefficients (g MJ–1) enable direct estimations of primary gas and aerosol emissions from satellite FRP observations, and we derive these values for many compounds emitted by temperate forest fuels, including several previously unreported species.

UCATS (the UAS Chromatograph for Atmospheric Trace Species) was designed and built for observations of important atmospheric trace gases from unmanned aircraft systems (UAS) in the upper troposphere and lower stratosphere (UT/LS). Initially it measured major chlorofluorocarbons (CFCs) and the stratospheric transport tracers nitrous oxide (N2O) and sulfur hexafluoride (SF6), using gas chromatography with electron capture detection. Compact ozone (O3) and water vapor (H2O) instruments were added to enhance science missions on platforms with relatively small payloads. Over the past decade, UCATS has been reconfigured to measure methane (CH4), carbon monoxide (CO), and molecular hydrogen (H2) instead of CFCs and has undergone numerous upgrades to its subsystems. It has served as part of large payloads on stratospheric UAS missions to probe the tropical tropopause region and transport of air into the stratosphere, in piloted aircraft studies of greenhouse gases, transport, and chemistry in the troposphere, and will soon return to the study of stratospheric ozone depletion, one of the original goals for UCATS. Each deployment brought different challenges, which were largely met or resolved. The design, capabilities, modifications and some results from UCATS are shown and described here, including changes for upcoming missions.

The details of aerosol processes and size distributions in the stratosphere are important for both heterogeneous chemistry and aerosol-radiation interactions. Using in-situ, global-scale measurements of the size distribution of particles with diameters > 3 nm from the NASA Atmospheric Tomography Mission (ATom), we identify a mode of ultrafine aerosol in the lowermost stratosphere (LMS) at mid and high latitudes. This mode is substantial only in the northern hemisphere (NH), and was observed in all four seasons. We also observe elevated SO2, an important precursor for new particle formation (NPF) and growth, in the NH LMS. We use box modelling and thermodynamic calculations to show that NPF can occur in the LMS conditions observed on ATom. Aircraft emissions are shown as likely sources of this SO2, as well as a potential source of ultrafine particles directly emitted by, or formed in the plume of the engines. These ultra-fine particles have the potential to grow to larger sizes, and to coagulate with larger aerosol, affecting heterogeneous chemistry and aerosol-radiation interactions. Understanding all sources and characteristics of stratospheric aerosol is important in the context of anthropogenic climate change as well as proposals for climate intervention via stratospheric sulphur injection. This analysis not only adds to the, currently sparse, observations of the global impact of aviation, but also introduces another aspect of climate influence, namely a size distribution shift of the background aerosol distribution in the LMS.

Wildland fires involve complicated processes that are challenging to represent in chemical transport models. Recent airborne measurements reveal remarkable chemical tomography in fresh wildland fire plumes, which remain yet to be fully explored using models. Here, we present a high-resolution large eddy simulation model coupled to chemistry to study the chemical evolution in fresh wildland fire plume. The model is configured for a large fire heavily sampled during the Fire Influence on Regional to Global Environments and Air Quality field campaign, and a variety of airborne measurements are used to evaluate the chemical heterogeneity revealed by the model. We show that the model captures the observed cross-transect variations of a number of compounds quite well, including ozone (O3), nitrous acid (HONO), and peroxyacetyl nitrate. The combined observational and modeling results suggest that the top and edges of fresh plume drive the photochemistry, while dark chemistry is also present but in the lower part of the plume. The model spatial resolution is shown to be very important as it may shift the chemical regime, leading to biases in O3 and NOx chemistry. Based on findings in this work, we speculate that the impact of small fires on air quality may be largely underestimated in models with coarse spatial resolutions.

We analyse aerosol particle composition measurements from five research missions between 2014 and 2018 to assess the meridional extent of particles containing meteoric material in the upper troposphere and lower stratosphere (UTLS). Measurements from the Jungfraujoch mountaintop site and a low-altitude aircraft mission show that meteoric material is also present within middle- and lower-tropospheric aerosol but within only a very small proportion of particles. For both the UTLS campaigns and the lower- and mid-troposphere observations, the measurements were conducted with single-particle laser ablation mass spectrometers with bipolar-ion detection, which enabled us to measure the chemical composition of particles in a diameter range of approximately 150 nm to 3 µm. The five UTLS aircraft missions cover a latitude range from 15 to 68∘ N, altitudes up to 21 km, and a potential temperature range from 280 to 480 K. In total, 338 363 single particles were analysed, of which 147 338 were measured in the stratosphere. Of these total particles, 50 688 were characterized by high abundances of magnesium and iron, together with sulfuric ions, the vast majority (48 610) in the stratosphere, and are interpreted as meteoric material immersed or dissolved within sulfuric acid. It must be noted that the relative abundance of such meteoric particles may be overestimated by about 10 % to 30 % due to the presence of pure sulfuric acid particles in the stratosphere which are not detected by the instruments used here. Below the tropopause, the observed fraction of the meteoric particle type decreased sharply with 0.2 %–1 % abundance at Jungfraujoch, and smaller abundances (0.025 %–0.05 %) were observed during the lower-altitude Canadian Arctic aircraft measurements. The size distribution of the meteoric sulfuric particles measured in the UTLS campaigns is consistent with earlier aircraft-based mass-spectrometric measurements, with only 5 %–10 % fractions in the smallest particles detected (200–300 nm diameter) but with substantial (> 40 %) abundance fractions for particles from 300–350 up to 900 nm in diameter, suggesting sedimentation is the primary loss mechanism. In the tropical lower stratosphere, only a small fraction (< 10 %) of the analysed particles contained meteoric material. In contrast, in the extratropics the observed fraction of meteoric particles reached 20 %–40 % directly above the tropopause. At potential temperature levels of more than 40 K above the thermal tropopause, particles containing meteoric material were observed in much higher relative abundances than near the tropopause, and, at these altitudes, they occurred at a similar abundance fraction across all latitudes and seasons measured. Above 440 K, the observed fraction of meteoric particles is above 60 % at latitudes between 20 and 42∘ N. Meteoric smoke particles are transported from the mesosphere into the stratosphere within the winter polar vortex and are subsequently distributed towards low latitudes by isentropic mixing, typically below a potential temperature of 440 K. By contrast, the findings from the UTLS measurements show that meteoric material is found in stratospheric aerosol particles at all latitudes and seasons, which suggests that either isentropic mixing is effective also above 440 K or that meteoric fragments may be the source of a substantial proportion of the observed meteoric material.

Large industrial facilities, such as petrochemical complexes, have decisive effects on regional air quality: directly due to their own hazardous volatile organic compounds (VOCs) emissions and indirectly due to their contribution to secondary air pollution. In South Korea, pronounced ozone and particulate matter issues have been reported in industrial areas. In this study, we develop a new top-down VOC emission rate estimation method using in situ airborne formaldehyde (HCHO) observations in the downwind plume of the Daesan Petrochemical Complex (DPC) in South Korea during the 2016 Korea–United States Air Quality (KORUS-AQ) mission. On May 22, we observed a peak HCHO mole fraction of 12 ppb after a transport time of 2.5 h (distance approximately 36 km) under conditions where the HCHO photochemical lifetime was 1.8 h. Box model calculations indicate that this elevated HCHO is mainly due to secondary production (more than 90% after 2 h of plume aging) from various VOC precursors including ethene, propene, and 1,3-butadiene. We estimate a lower limit for yearly DPC VOC emissions of 31 (±8.7) × 103 MT/year for HCHO precursors and 53 (±15) × 103 MT/year for all measured primary VOCs. These estimates are 1.5–2.5 times higher than the latest Korean emission inventories, KORUSv5. This method is beneficial not only by tracking the sources, sinks, and evolution of HCHO but also by validating existing emission inventories.

Acetone is one of the most abundant oxygenated volatile organic compounds (VOCs) in the atmosphere. The oceans impose a strong control on atmospheric acetone, yet the oceanic fluxes of acetone remain poorly constrained. In this work, the global budget of acetone is evaluated using two global models: CAM‐chem and GEOS‐Chem. CAM‐chem uses an online air‐sea exchange framework to calculate the bidirectional oceanic acetone fluxes, which is coupled to a data‐oriented machine‐learning approach. The machine‐learning algorithm is trained using a global suite of seawater acetone measurements. GEOS‐Chem uses a fixed surface seawater concentration of acetone to calculate the oceanic fluxes. Both model simulations are compared to airborne observations from a recent global‐scale, multiseasonal campaign, the NASA Atmospheric Tomography Mission (ATom). We find that both CAM‐chem and GEOS‐Chem capture the measured acetone vertical distributions in the remote atmosphere reasonably well. The combined observational and modeling analysis suggests that (i) the ocean strongly regulates the atmospheric budget of acetone. The tropical and subtropical oceans are mostly a net source of acetone, while the high‐latitude oceans are a net sink. (ii) CMIP6 anthropogenic emission inventory may underestimate acetone and/or its precursors in the Northern Hemisphere. (iii) The MEGAN biogenic emissions model may overestimate acetone and/or its precursors, and/or the biogenic oxidation mechanisms may overestimate the acetone yields. (iv) The models consistently overestimate acetone in the upper troposphere‐lower stratosphere over the Southern Ocean in austral winter. (v) Acetone contributes up to 30–40% of hydroxyl radical production in the tropical upper troposphere/lower stratosphere.

The Korea-United States Air Quality Study (KORUS-AQ) took place in spring 2016 to better understand air pollution in Korea. In support of KORUS-AQ, 2554 whole air samples (WAS) were collected aboard the NASA DC-8 research aircraft and analyzed for 82 C1–C10 volatile organic compounds (VOCs) using multi-column gas chromatography. Together with fast-response measurements from other groups, the air samples were used to characterize the VOC composition in Seoul and surrounding regions, determine which VOCs are major ozone precursors in Seoul, and identify the sources of these reactive VOCs. (1) The WAS VOCs showed distinct signatures depending on their source origins. Air collected over Seoul had abundant ethane, propane, toluene and n-butane while plumes from the Daesan petrochemical complex were rich in ethene, C2–C6 alkanes and benzene. Carbonyl sulfide (COS), CFC-113, CFC-114, carbon tetrachloride (CCl4) and 1,2-dichloroethane were good tracers of air originating from China. CFC-11 was also elevated in air from China but was surprisingly more elevated in air over Seoul. (2) Methanol, isoprene, toluene, xylenes and ethene were strong individual contributors to OH reactivity in Seoul. However methanol contributed less to ozone formation based on photochemical box modeling, which better accounts for radical chemistry. (3) Positive Matrix Factorization (PMF) and other techniques indicated a mix of VOC source influences in Seoul, including solvents, traffic, biogenic, and long-range transport. The solvent and traffic sources were roughly equal using PMF, and the solvents source was stronger in the KORUS-AQ emission inventory. Based on PMF, ethene and propene were primarily associated with traffic, and toluene, ethylbenzene and xylenes with solvents, especially non-paint solvents for toluene and paint solvents for ethylbenzene and xylenes. This suggests that VOC control strategies in Seoul could continue to target vehicle exhaust and paint solvents, with additional regulations to limit the VOC content in a variety of non-paint solvents.

The Seoul Metropolitan Area (SMA) has a population of 24 million and frequently experiences unhealthy levels of ozone (O3). In this work, measurements taken during the Korea-United States Air Quality Study (KORUS-AQ, 2016) are used to explore regional gradients in O3 and its chemical precursors, and an observationally-constrained 0-D photochemical box model is used to quantify key aspects of O3 production including its sensitivity to precursor gases. Box model performance was evaluated by comparing modeled concentrations of select secondary species to airborne measurements. These comparisons indicate that the steady state assumption used in 0-D box models cannot describe select intermediate species, highlighting the importance of having a broad suite of trace gases as model constraints. When fully constrained, aggregated statistics of modeled O3 production rates agreed with observed changes in O3, indicating that the box model was able to represent the majority of O3 chemistry. Comparison of airborne observations between urban Seoul and a downwind receptor site reveal a positive gradient in O3 coinciding with a negative gradient in NOx, no gradient in CH2O, and a slight positive gradient in modeled rates of O3 production. Together, these observations indicate a radical-limited (VOC-limited) O3 production environment in the SMA. Zero-out simulations identified C7+ aromatics as the dominant VOC contributors to O3 production, with isoprene and anthropogenic alkenes making smaller but appreciable contributions. Simulations of model sensitivity to decreases in NOx produced results that were not spatially uniform, with large increases in O3 production predicted for urban Seoul and decreases in O3 production predicted for far-outlying areas. The policy implications of this work are clear: Effective O3 mitigation strategies in the SMA must focus on reducing local emissions of C7+ aromatics, while reductions in NOx emissions may increase O3 in some areas but generally decrease the regional extent of O3 exposure.

The Korea – United States Air Quality Study (May – June 2016) deployed instrumented aircraft and ground-based measurements to elucidate causes of poor air quality related to high ozone and aerosol concentrations in South Korea. This work synthesizes data pertaining to aerosols (specifically, particulate matter with aerodynamic diameters

We present the first data on the concentration of sea-salt aerosol throughout most of the depth of the troposphere and over a wide range of latitudes, which were obtained during the Atmospheric Tomography (ATom) mission. Sea-salt concentrations in the upper troposphere are very small, usually less than 10 ng per standard m3 (about 10 parts per trillion by mass) and often less than 1 ng m−3. This puts stringent limits on the contribution of sea-salt aerosol to halogen and nitric acid chemistry in the upper troposphere. Within broad regions the concentration of sea-salt aerosol is roughly proportional to water vapor, supporting a dominant role for wet scavenging in removing sea-salt aerosol from the atmosphere. Concentrations of sea-salt aerosol in the winter upper troposphere are not as low as in the summer and the tropics. This is mostly a consequence of less wet scavenging in the drier, colder winter atmosphere. There is also a source of sea-salt aerosol over pack ice that is distinct from that over open water. With a well-studied and widely distributed source, sea-salt aerosol provides an excellent test of wet scavenging and vertical transport of aerosols in chemical transport models.

Author(s): Tang, Wenfu; Emmons, Louisa K; Jr, Arellano Avelino F; Gaubert, Benjamin; Knote, Christoph; Tilmes, Simone; Buchholz, Rebecca R; Pfister, Gabriele G; Diskin, Glenn S; Blake, Donald R; Blake, Nicola J; Meinardi, Simone; DiGangi, Joshua P; Choi, Yonghoon; Woo, Jung-Hun; He, Cenlin; Schroeder, Jason R; Suh, Inseon; Lee, Hyo-Jung; Jo, Hyun-Young; Kanaya, Yugo; Jung, Jinsang; Lee, Youngjae; Kim, Danbi