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Heterogeneous reactions occurring at the surface of atmospheric aerosol particles regulate the production and lifetime of a wide array of atmospheric gases. Aerosol surface area plays a critical role in setting the rate of heterogeneous reactions in the atmosphere. Despite the central role of aerosol surface area, there are few assessments of the accuracy of aerosol surface area concentrations in regional and global models. In this study, we compare aerosol surface area concentrations in the EPA's Community Multiscale Air Quality (CMAQ) model with commensurate observations from the 2011 NASA flight-based DISCOVER-AQ (Deriving Information on Surface Conditions from COlumn and VERtically Resolved Observations Relevant to Air Quality) campaign. The study region includes the Baltimore and Washington, D.C. metropolitan area. Dry aerosol surface area was measured aboard the NASA P-3B aircraft using an ultra-high-sensitivity aerosol spectrometer (UHSAS). We show that modeled and measured dry aerosol surface area, Sa,mod and Sa,meas respectively, are modestly correlated (r2=0.52) and on average agree to within a factor of 2 (Sa,mod/Sa,meas=0.44) over the course of the 13 research flights. We show that Sa,mod/Sa,meas does not depend strongly on photochemical age or the concentration of secondary biogenic aerosol, suggesting that the condensation of low-volatility gas-phase compounds does not strongly affect model–measurement agreement. In comparison, there is strong agreement between measured and modeled aerosol number concentration (Nmod/Nmeas=0.87, r2=0.63). The persistent underestimate of Sa in the model, combined with strong agreement in modeled and measured aerosol number concentrations, suggests that model representation of the size distribution of primary emissions or secondary aerosol formed at the early stages of oxidation may contribute to the observed differences. For reactions occurring on small particles, the rate of heterogeneous reactions is a linear function of both Sa and the reactive uptake coefficient (γ). To assess the importance of uncertainty in modeled Sa for the representation of heterogeneous reactions in models, we compare both the mean and the variance in Sa,mod/Sa,meas to those in γ(N2O5)mod/γ(N2O5)meas. We find that the uncertainty in model representation of heterogeneous reactions is primarily driven by uncertainty in the parametrization of reactive uptake coefficients, although the discrepancy between Sa,mod and Sa,meas is not insignificant. Our analysis suggests that model improvements to aerosol surface area concentrations, in addition to more accurate parameterizations of heterogeneous kinetics, will advance the representation of heterogeneous chemistry in regional models.

Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of biomass burning (BB) smoke, including wildfires, on regional air quality depends on emissions, transport, and chemistry, including oxidation of emitted BB volatile organic compounds (BBVOCs) by the hydroxyl radical (OH), nitrate radical (NO3), and ozone (O3). During the daytime, when light penetrates the plumes, BBVOCs are oxidized mainly by O3 and OH. In contrast, at night or in optically dense plumes, BBVOCs are oxidized mainly by O3 and NO3. This work focuses on the transition between daytime and nighttime oxidation, which has significant implications for the formation of secondary pollutants and loss of nitrogen oxides (NOx=NO+NO2) and has been understudied. We present wildfire plume observations made during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality), a field campaign involving multiple aircraft, ground, satellite, and mobile platforms that took place in the United States in the summer of 2019 to study both wildfire and agricultural burning emissions and atmospheric chemistry. We use observations from two research aircraft, the NASA DC-8 and the NOAA Twin Otter, with a detailed chemical box model, including updated phenolic mechanisms, to analyze smoke sampled during midday, sunset, and nighttime. Aircraft observations suggest a range of NO3 production rates (0.1–1.5 ppbv h−1) in plumes transported during both midday and after dark. Modeled initial instantaneous reactivity toward BBVOCs for NO3, OH, and O3 is 80.1 %, 87.7 %, and 99.6 %, respectively. Initial NO3 reactivity is 10–104 times greater than typical values in forested or urban environments, and reactions with BBVOCs account for >97 % of NO3 loss in sunlit plumes (jNO2 up to 4×10-3s-1), while conventional photochemical NO3 loss through reaction with NO and photolysis are minor pathways. Alkenes and furans are mostly oxidized by OH and O3 (11 %–43 %, 54 %–88 % for alkenes; 18 %–55 %, 39 %–76 %, for furans, respectively), but phenolic oxidation is split between NO3, O3, and OH (26 %–52 %, 22 %–43 %, 16 %–33 %, respectively). Nitrate radical oxidation accounts for 26 %–52 % of phenolic chemical loss in sunset plumes and in an optically thick plume. Nitrocatechol yields varied between 33 % and 45 %, and NO3 chemistry in BB plumes emitted late in the day is responsible for 72 %–92 % (84 % in an optically thick midday plume) of nitrocatechol formation and controls nitrophenolic formation overall. As a result, overnight nitrophenolic formation pathways account for 56 %±2 % of NOx loss by sunrise the following day. In all but one overnight plume we modeled, there was remaining NOx (13 %–57 %) and BBVOCs (8 %–72 %) at sunrise.

During the NASA DISCOVER-AQ campaign over the US Baltimore, MD–Washington, D.C., metropolitan area in July 2011, the NASA P-3B aircraft performed extensive profiling of aerosol optical, chemical, and microphysical properties. These in situ profiles were coincident with ground-based remote sensing (AERONET) and in situ (PM2.5) measurements. Here, we use this data set to study the correlation between the PM2.5 observations at the surface and the column integrated measurements. Aerosol optical depth (AOD550 nm) calculated with the extinction (550 nm) measured during the in situ profiles was found to be strongly correlated with the volume of aerosols present in the boundary layer (BL). Despite the strong correlation, some variability remains, and we find that the presence of aerosol layers above the BL (in the buffer layer – BuL) introduces significant uncertainties in PM2.5 estimates based on column-integrated measurements (overestimation of PM2.5 by a factor of 5). This suggests that the use of active remote sensing techniques would dramatically improve air quality retrievals. Indeed, the relationship between the AOD550 nm and the PM2.5 is strongly improved by accounting for the aerosol present in and above the BL (i.e., integrating the aerosol loading from the surface to the top of the BuL). Since more than 15% of the AOD values observed during DISCOVER-AQ are dominated by aerosol water uptake, the f(RH)amb (ratio of scattering coefficient at ambient relative humidity (RH) to scattering coefficient at low RH; see Sect. 3.2) is used to study the impact of the aerosol hygroscopicity on the PM2.5 retrievals. The results indicate that PM2.5 can be predicted within a factor up to 2 even when the vertical variability of the f(RH)amb is assumed to be negligible. Moreover, f(RH = 80%) and RH measurements performed at the ground may be used to estimate the f(RH)amb during dry conditions (RHBL < 55%).

The western North Atlantic Ocean is strongly influenced by continental outflow, making it an ideal region to study the atmospheric transition from a polluted coastline to the marine environment. Utilizing eight transit flights between the NASA Langley Research Center (LaRC) in Hampton, Virginia, and the remote island of Bermuda from NASA's Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE), we examine the evolution of trace gas and aerosol properties off the US East Coast. The first pair of flights flew along the wind trajectory of continental outflow, while the other flights captured a mix of marine and continental air mass sources. For measurements within the boundary layer (BL), there was an offshore decline in particle N, N>100 nm, CH4, CO, and CO2 concentrations, all leveling off around ∼900 km offshore from the LaRC. These trends are strongest for the first pair of flights. In the BL, offshore declines in organic mass fraction and increases in sulfate mass fraction coincide with increasing hygroscopicity based on f(RH) measurements. Free troposphere measurements show a decline in N, but other measured parameters are more variable when compared to the prominent offshore gradients seen in the BL. Pollution layers exist in the free troposphere, such as smoke plumes, that can potentially entrain into the BL. This work provides detailed case studies with a broad set of high-resolution measurements to further our understanding of the transition between continental and marine environments.

Marine boundary layer clouds play a critical role in Earth's energy balance. Their microphysical and radiative properties are highly impacted by ambient aerosols and dynamic forcings. In this study, we evaluate the representation of these clouds and related aerosol–cloud interaction processes in the single-column version of the E3SM climate model (SCM) against field measurements collected during the NASA ACTIVATE campaign over the western North Atlantic, as well as intercompare results with high-resolution process level models. We show that E3SM SCM reproduces the macrophysical properties of post-frontal boundary layer clouds in a cold-air outbreak (CAO) case well. However, it generates fewer but larger cloud droplets compared to aircraft measurements. Further sensitivity tests show that the underestimation of both aerosol number concentration and vertical velocity variance contributes to this bias. Aerosol–cloud interactions are examined by perturbing prescribed aerosol properties in E3SM SCM with fixed dynamics. Higher aerosol number concentration or hygroscopicity leads to more numerous but smaller cloud droplets, resulting in a stronger cooling via shortwave cloud forcing. This apparent Twomey effect is consistent with prior climate model studies. The cloud liquid water path shows a weakly positive relation with cloud droplet number concentration due to precipitation suppression. This weak aerosol effect on cloud macrophysics may be attributed to the dominant impact of strong dynamical forcing associated with the CAO. Our findings indicate that the SCM framework is a key tool to bridge the gap between climate models, process level models, and field observations to facilitate process level understanding.

Remote marine regions comprise a high fraction of Earth's surface, but in situ vertically resolved measurements over these locations remain scarce. Here we use airborne data during 15 vertical spiral soundings (0.15–8.5 km) over Bermuda during the NASA Aerosol Cloud meTeorology Interactions over the western ATlantic Experiment (ACTIVATE) to investigate the impact of different source regions on the vertical structure of trace gases, aerosol particles, and meteorological variables over 1000 km offshore of the US East Coast. Results reveal significant differences in vertical profiles of variables between three different air mass source categories (North America, Ocean, Caribbean/North Africa) identified using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model: (i) the strongest pollution signature is from air masses from the North America category, while the weakest one is from the Ocean category; (ii) North America air has the highest levels of CO, CH4, submicron particle number concentration, aerosol mass spectrometer (AMS) mass, and organic mass fraction along with smoke layers in the free troposphere (FT); (iii) Ocean air has the highest relative amount of nitrate, non-sea-salt sulfate, and oxalate, which are key acidic species participating in chloride depletion; (iv) air masses from the Caribbean/North Africa showed a pronounced coarse aerosol signature in the FT and reduced aerosol hygroscopicity, which is associated with dust transport; and (v) there is considerable vertical heterogeneity for almost all variables examined, including higher O3 and submicron particle concentrations with altitude, suggesting that the FT is a potential contributor of both constituents in the marine boundary layer. This study highlights the importance of considering air mass source origin and vertical resolution to capture aerosol and trace gas properties over remote marine areas.

Ocean surface wind speed (i.e., wind speed 10 m above sea level) is a critical parameter used by atmospheric models to estimate the state of the marine atmospheric boundary layer (MABL). Accurate surface wind speed measurements in diverse locations are required to improve characterization of MABL dynamics and assess how models simulate large-scale phenomena related to climate change and global weather patterns. To provide these measurements, this study introduces and evaluates a new surface wind speed data product from the NASA Langley Research Center nadir-viewing High Spectral Resolution Lidar – generation 2 (HSRL-2) using data collected as part of the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. The HSRL-2 can directly measure vertically resolved aerosol backscatter and extinction profiles without additional constraints or assumptions, enabling the instrument to accurately derive atmospheric attenuation and directly determine surface reflectance (i.e., surface backscatter). Also, the high horizontal spatial resolution of the HSRL-2 retrievals (0.5 s or ∼ 75 m along track) allows the instrument to probe the fine-scale spatial variability in surface wind speeds over time along the flight track and over breaks in broken cloud fields. A rigorous evaluation of these retrievals is performed by comparing coincident HSRL-2 and National Center for Atmospheric Research (NCAR) Airborne Vertical Atmosphere Profiling System (AVAPS) dropsonde data, owing to the joint deployment of these two instruments on the ACTIVATE King Air aircraft. These comparisons show correlations of 0.89, slopes of 1.04 and 1.17, and y intercepts of −0.13 and −1.05 m s−1 for linear and bisector regressions, respectively, and the overall accuracy is calculated to be 0.15 ± 1.80 m s−1. It is also shown that the dropsonde surface wind speed data most closely follow the HSRL-2 distribution of wave slope variance using the distribution proposed by Hu et al. (2008) rather than the ones proposed by Cox and Munk (1954) and Wu (1990) for surface wind speeds below 7 m s−1, with this category comprising most of the ACTIVATE data set. The retrievals are then evaluated separately for surface wind speeds below 7 m s−1 and between 7 and 13.3 m s−1 and show that the HSRL-2 retrieves surface wind speeds with a bias of ∼ 0.5 m s−1 and an error of ∼ 1.5 m s−1, a finding not apparent in the cumulative comparisons. Also, it is shown that the HSRL-2 retrievals are more accurate in the summer (−0.18 ± 1.52 m s−1) than in the winter (0.63 ± 2.07 m s−1), but the HSRL-2 is still able to make numerous (N=236) accurate retrievals in the winter. Overall, this study highlights the abilities and assesses the performance of the HSRL-2 surface wind speed retrievals, and it is hoped that further evaluation of these retrievals will be performed using other airborne and satellite data sets.

Mesoscale organization of marine convective clouds into linear or clustered states is prevalent across the tropical and subtropical oceans, and its investigation served as a guiding focus for a series of process study flights conducted as part of the Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) during summer 2020, 2021, and 2022. These select ACTIVATE flights involved a novel strategy for coordinating two aircraft, with respective remote sensing and in situ sampling payloads, to probe regions of organized shallow convection for several hours. The main purpose of this measurement report is to summarize the aircraft sampling approach, describe the characteristics and evolution of the cases, and provide an overview of the datasets that can serve as a starting point for more detailed modeling and analysis studies. Six flights are described, involving a total of 80 dropsonde profiles that capture the environment surrounding clustered shallow convection. The flights include detailed observations of the vertical structure of cloud systems, comprising up to 20 in situ sampling levels. Four cases involved deepening convection rooted in the marine boundary layer that developed vertically to 2–5 km with varying precipitation amounts, while two cases captured more complex and developed cumulus congestus systems extending above 5 km. In addition to the thermodynamic and dynamic characterization afforded by dropsonde and in situ measurements, the datasets include cloud and aerosol microphysics, trace gas concentrations, aerosol and droplet composition, and cloud and aerosol remote sensing from high-spectral-resolution lidar and polarimetry.

NASA's Vapor In-cloud Profiling Radar (VIPR) is a tunable G-band radar designed for in-cloud and precipitation humidity remote sensing. VIPR estimates humidity using the differential absorption radar (DAR) technique. This technique exploits the difference between atmospheric attenuation at different frequencies (“on” and “off” an absorption line) and combines it with the ranging capabilities of the radar to estimate the absorbing gas concentration along the radar path. We analyze the VIPR humidity measurements during two NASA field campaigns: (1) the Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Snowstorms (IMPACTS) campaign, with the objective of studying wintertime snowstorms focusing on east coast cyclones; and (2) the Synergies Of Active optical and Active microwave Remote Sensing Experiment (SOA2RSE) campaign, which studied the synergy between DAR (VIPR) and differential absorption lidar (DIAL, the High altitude Lidar Observatory – HALO) measurements. We discuss a comparison with dropsondes launched during these campaigns as well as an intercomparison against the ERA5 reanalysis fields. Thus, this study serves as an additional evaluation of ERA5 lower tropospheric humidity fields. Overall, in-cloud and in-snowstorm comparisons suggest that ERA5 and VIPR agree within 20 % or better against the dropsondes. The exception is during SOA2RSE (i.e., in fair weather), where ERA5 exhibits up to a 50 % underestimation above 4 km. We also show a smooth transition in water vapor profiles between the in-cloud and clear-sky measurements obtained from VIPR and HALO respectively, which highlights the complementary nature of these two measurement techniques for future airborne and space-based missions.

A large part of the uncertainty in climate projections comes from uncertain aerosol properties and aerosol–cloud interactions as well as the difficulty in remotely sensing them. The southeastern Atlantic functions as a natural laboratory to study biomass-burning smoke and to constrain this uncertainty. We address these gaps by comparing the Weather Research and Forecasting with Chemistry Community Atmosphere Model (WRF-CAM5) to the multi-campaign observations ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS), CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing), and LASIC (Layered Atlantic Smoke Interactions with Clouds) in the southeastern Atlantic in August 2017 to evaluate a large range of the model's aerosol chemical properties, size distributions, processes, and transport, as well as aerosol–cloud interactions. Overall, while WRF-CAM5 is able to represent smoke properties and transport, some key discrepancies highlight the need for further analysis. Observations of smoke composition show an overall decrease in aerosol mean diameter as smoke ages over 4–12 d, while the model lacks this trend. A decrease in the mass ratio of organic aerosol (OA) to black carbon (BC), OA:BC, and the OA mass to carbon monoxide (CO) mixing ratio, OA:CO, suggests that the model is missing processes that selectively remove OA from the particle phase, such as photolysis and heterogeneous aerosol chemistry. A large (factor of ∼2.5) enhancement in sulfate from the free troposphere (FT) to the boundary layer (BL) in observations is not present in the model, pointing to the importance of properly representing secondary sulfate aerosol formation from marine dimethyl sulfide and gaseous SO2 smoke emissions. The model shows a persistent overprediction of aerosols in the marine boundary layer (MBL), especially for clean conditions, which multiple pieces of evidence link to weaker aerosol removal in the modeled MBL than reality. This evidence includes several model features, such as not representing observed shifts towards smaller aerosol diameters, inaccurate concentration ratios of carbon monoxide and black carbon, underprediction of heavy rain events, and little evidence of persistent biases in modeled entrainment. The average below-cloud aerosol activation fraction (NCLD/NAER) remains relatively constant in WRF-CAM5 between field campaigns (∼0.65), while it decreases substantially in observations from ORACLES (∼0.78) to CLARIFY (∼0.5), which could be due to the model misrepresentation of clean aerosol conditions. WRF-CAM5 also overshoots an observed upper limit on liquid cloud droplet concentration around NCLD= 400–500 cm−3 and overpredicts the spread in NCLD. This could be related to the model often drastically overestimating the strength of boundary layer vertical turbulence by up to a factor of 10. We expect these results to motivate similar evaluations of other modeling systems and promote model development to reduce critical uncertainties in climate simulations.

Due to their fast evolution and large natural variability in macro- and microphysical properties, the accurate representation of boundary layer clouds in current climate models remains a challenge. One of the regions with large intermodel spread in the Coupled Model Intercomparison Project Phase 6 ensemble is the western North Atlantic Ocean. Here, statistically representative in situ measurements can help to develop and constrain the parameterization of clouds in global models. To this end, we performed comprehensive measurements of boundary layer clouds, aerosol, trace gases, and radiation in the western North Atlantic Ocean during the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. In total, 174 research flights with 574 flight hours for cloud and precipitation measurements were performed with the HU-25 Falcon during three winter (February–March 2020, January–April 2021, and November 2021–March 2022) and three summer seasons (August–September 2020, May–June 2021, and May–June 2022). Here we present a statistical evaluation of 16 140 individual cloud events probed by the fast cloud droplet probe and the two-dimensional stereo cloud probe during 155 research flights in a representative and repetitive flight strategy allowing for robust statistical data analyses. We show that the vertical profiles of distributions of the liquid water content and the cloud droplet effective diameter (ED) increase with altitude in the marine boundary layer. Due to higher updraft speeds, higher cloud droplet number concentrations (Nliquid) were measured in winter compared to summer despite lower cloud condensation nucleus abundance. Flight cloud cover derived from statistical analysis of in situ data is reduced in summer and shows large variability. This seasonal contrast in cloud coverage is consistent with a dominance of a synoptic pattern in winter that favors conditions for the formation of stratiform clouds at the western edge of cyclones (post-cyclonic). In contrast, a dominant summer anticyclone is concomitant with the occurrence of shallow cumulus clouds and lower cloud coverage. The evaluation of boundary layer clouds and precipitation in the Nliquid ED phase space sheds light on liquid, mixed-phase, and ice cloud properties and helps to categorize the cloud data. Ice and liquid precipitation, often masked in cloud statistics by a high abundance of liquid clouds, is often observed throughout the cloud. The ACTIVATE in situ cloud measurements provide a wealth of cloud information useful for assessing airborne and satellite remote-sensing products, for global climate and weather model evaluations, and for dedicated process studies that address precipitation and aerosol–cloud interactions.

Cumulus clouds are common over maritime regions. They are important regulators of the global radiative energy budget and global hydrologic cycle, as well as a key contributor to the uncertainty in anthropogenic climate change projections due to uncertainty in aerosol–cloud interactions. These interactions are regionally specific owing to their strong influences on aerosol sources and meteorology. Here, our analysis focuses on the statistical properties of marine boundary layer (MBL) aerosol chemistry and the relationships of MBL aerosol to cumulus cloud properties just above cloud base as sampled in 2019 during the NASA Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex). The aerosol and clouds were sampled by instruments on the NASA P-3 aircraft over three distinct maritime regions around the Philippines: the West Pacific, the South China Sea, and the Sulu Sea. Our analysis shows three primary sources influenced the aerosol chemical composition: clean marine (ocean source), industrial (Southeast Asia, Manila, and cargo and tanker ship emissions), and biomass burning (Borneo and Indonesia). The clean marine aerosol chemical composition had low values of all sampled chemical signatures, specifically median values of 2.2 µg m−3 of organics (ORG), 2.3 µg m−3 of SO4, 0.3 µg m−3 of NO3, 1.4 µg m−3 of NH4, 0.04 µg m−3 of Cl, and 0.0074 µg m−3 of refractory black carbon (BC). Chemical signatures of the other two aerosol source regions were industrial, with elevated SO4 having a median value of 6.1 µg m−3, and biomass burning, with elevated median concentrations of ORG 21.2 µg m−3 and BC 0.1351 µg m−3. Based on chemical signatures, the industrial component was primarily from ship emissions, which were sampled within 60 km of ships and within projected ship plumes. Normalized cloud droplet size distributions in clouds sampled near the MBL passes of the P-3 showed that clouds impacted by industrial and biomass burning contained higher concentrations of cloud droplets, by as much as 1.5 orders of magnitude for diameters < 13 µm compared to clean marine clouds, while at size ranges between 13.0–34.5 µm the median concentrations of cloud droplets in all aerosol categories were nearly an order of magnitude less than the clean marine category. In the droplet size bins centered at diameters > 34.5 µm concentrations were equal to, or slightly exceeded, the concentrations of the clean marine clouds. These analyses show that anthropogenic aerosols generated from industrial and biomass burning sources significantly influenced cloud base microphysical structure in the Philippine region enhancing the small droplet concentration and reducing the concentration of mid-sized droplets.

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 as well as to 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, resulting in 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 HU-25 Falcon and King Air, respectively. The HU-25 Falcon 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. Under cloud-free conditions, the HU-25 Falcon similarly conducted profiling at different level legs within and immediately above the boundary layer. The King Air (the high-flying aircraft) flew at approximately ∼ 9 km and conducted remote sensing with a lidar and polarimeter while also launching dropsondes (785 in total). Collectively, simultaneous data from both aircraft help to characterize the same vertical column of the atmosphere. In addition to individual instrument files, data from the HU-25 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's 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. The data are publicly accessible through https://doi.org/10.5067/SUBORBITAL/ACTIVATE/DATA001 (ACTIVATE Science Team, 2020).

Abstract In-situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP2EX; ORACLES; SOCRATES; MARCUS; and CAPRICORN2. Each campaign involves aircraft measurements, ship-based measurements, or both. Measurements collected over the North and Central Atlantic, Indo-Pacific, and Southern Oceans, represent a range of clean to polluted conditions in various climate regimes. With the extensive range of environmental conditions sampled, this data collection is ideal for testing satellite remote detection methods of CDNC and CCN in marine environments. Remote measurement methods are vital to expanding the available data in these difficult-to-reach regions of the Earth and improving our understanding of aerosol-cloud interactions. The data collection includes particle composition and continental tracers to identify potential contributing CCN sources. Several of these campaigns include High Spectral Resolution Lidar (HSRL) and polarimetric imaging measurements and retrievals that will be the basis for the next generation of space-based remote sensors and, thus, can be utilized as satellite surrogates.

Abstract Heterogeneous chemical cycles of pyrogenic nitrogen and halides influence tropospheric ozone and affect the stratosphere during extreme Pyrocumulonimbus (PyroCB) events. We report field‐derived N2O5 uptake coefficients, γ(N2O5), and ClNO2 yields, φ(ClNO2), from two aircraft campaigns observing fresh smoke in the lower and mid troposphere and processed/aged smoke in the upper troposphere and lower stratosphere (UTLS). Derived φ(ClNO2) varied across the full 0–1 range but was typically

The NASA North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) ship and aircraft field campaign deployed to the western subarctic Atlantic between the years 2015 and 2018. One of the primary goals of NAAMES is to improve the understanding of aerosol–cloud interaction (ACI) over the Atlantic Ocean under different seasonal regimes. ACIs currently represent the largest source of uncertainty in global climate models. During three NAAMES field campaigns (NAAMES-1 in November 2015, NAAMES-2 in May 2016, and NAAMES-3 in September 2017), multiple 10 h science flights were conducted using the NASA C-130 aircraft to measure marine boundary layer aerosol and cloud properties. The standard flight pattern includes vertical spirals where the C-130 transitioned from high altitude to low altitude (and vice versa), collecting in situ measurements of aerosols, trace gases, clouds, and meteorological parameters as a function of altitude. We examine the data collected from 37 spirals during the three NAAMES field campaigns, and we present a comprehensive characterization of the vertical profiles of aerosol properties under different synoptic conditions and aerosol regimes. The vertical distribution of submicron aerosol particles exhibited strong seasonal variation, as well as elevated intra-seasonal variability depending on emission sources and aerosol processes in the atmospheric column. Pristine marine conditions and new particle formation were prevalent in the wintertime (NAAMES-1) due to low biogenic emissions from the surface ocean and reduced continental influence. Higher concentrations of submicron aerosol particles were observed in the spring (NAAMES-2) due to strong phytoplankton activity and the arrival of long-range-transported continental plumes in the free troposphere with subsequent entrainment into the marine boundary layer. Biomass burning from boreal wildfires was the main source of aerosol particles in the region during the late summer (NAAMES-3) in both the marine boundary layer and free troposphere.

Cloud processing is known to generate aerosol species such as sulfate and secondary organic aerosol, yet there is a scarcity of airborne data to examine this issue. The NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) was designed to build an unprecedented dataset relevant to aerosol–cloud interactions with two coordinated aircraft over the northwestern Atlantic, with aerosol mass spectrometer data used from four deployments between 2020–2021 to contrast aerosol composition below, in (using a counterflow virtual impactor) and above boundary layer clouds. Consistent features in all time periods of the deployments (January–March, May–June, August–September) include the mass fraction of organics and relative amount of oxygenated organics (m/z 44) relative to total organics (f44) increasing in droplet residuals relative to below and above cloud. Detailed analysis comparing data below and in cloud suggests a possible role for in-cloud aqueous processing in explaining such results; an intriguing aspect though requiring more attention is that only approximately a quarter of the cloud cases (29 of 110) showed higher organic mass fractions either below or above cloud. Of those 29 cases, the majority (25) showed higher organic mass fraction below cloud base where the cloud processing signature is presumably more evident as compared to above cloud. These results are consistent with the few past studies analyzing droplet residuals pointing to higher organic enrichment than in adjacent cloud-free areas. The data findings are important as other datasets (e.g., reanalysis) suggest that sulfate is both more abundant than organics (in contrast to this work) and more closely related to drop number concentrations in the winter when aerosol–cloud interactions are strongest. Here we show that organics are more abundant than sulfate in the droplet residuals and that aerosol interaction with clouds potentially decreases particle hygroscopicity due to the increase in organic:sulfate ratio for droplet residuals relative to surrounding cloud-free air. These results are important in light of the growing importance of organics over the northwestern Atlantic in recent decades relative to sulfate owing to the success of regulatory activity over the eastern United States to cut sulfur dioxide emissions.

The evolution of organic aerosol (OA) and aerosol size distributions within smoke plumes is uncertain due to the variability in rates of coagulation and OA condensation/evaporation between different smoke plumes and at different locations within a single plume. We use aircraft data from the FIREX-AQ campaign to evaluate differences in evolving aerosol size distributions, OA, and oxygen to carbon ratios (O:C) between and within smoke plumes during the first several hours of aging as a function of smoke concentration. The observations show that the median particle diameter increases faster in smoke of a higher initial OA concentration (>1000 µg m−3), with diameter growth of over 100 nm in 8 h – despite generally having a net decrease in OA enhancement ratios – than smoke of a lower initial OA concentration ( µg m−3), which had net increases in OA. Observations of OA and O:C suggest that evaporation and/or secondary OA formation was greater in less concentrated smoke prior to the first measurement (5–57 min after emission). We simulate the size changes due to coagulation and dilution and adjust for OA condensation/evaporation based on the observed changes in OA. We found that coagulation explains the majority of the diameter growth, with OA evaporation/condensation having a relatively minor impact. We found that mixing between the core and edges of the plume generally occurred on timescales of hours, slow enough to maintain differences in aging between core and edge but too fast to ignore the role of mixing for most of our cases.

Organic aerosol (OA) is an important fraction of submicron aerosols. However, it is challenging to predict and attribute the specific organic compounds and sources that lead to observed OA loadings, largely due to contributions from secondary production. This is especially true for megacities surrounded by numerous regional sources that create an OA background. Here, we utilize in situ gas and aerosol observations collected on board the NASA DC-8 during the NASA–NIER KORUS-AQ (Korea–United States Air Quality) campaign to investigate the sources and hydrocarbon precursors that led to the secondary OA (SOA) production observed over Seoul. First, we investigate the contribution of transported OA to total loadings observed over Seoul by using observations over the Yellow Sea coupled to FLEXPART Lagrangian simulations. During KORUS-AQ, the average OA loading advected into Seoul was ∼1–3 µg sm−3. Second, taking this background into account, the dilution-corrected SOA concentration observed over Seoul was ∼140 µgsm-3ppmv-1 at 0.5 equivalent photochemical days. This value is at the high end of what has been observed in other megacities around the world (20–70 µgsm-3ppmv-1 at 0.5 equivalent days). For the average OA concentration observed over Seoul (13 µg sm−3), it is clear that production of SOA from locally emitted precursors is the major source in the region. The importance of local SOA production was supported by the following observations. (1) FLEXPART source contribution calculations indicate any hydrocarbons with a lifetime of less than 1 day, which are shown to dominate the observed SOA production, mainly originate from South Korea. (2) SOA correlated strongly with other secondary photochemical species, including short-lived species (formaldehyde, peroxy acetyl nitrate, sum of acyl peroxy nitrates, dihydroxytoluene, and nitrate aerosol). (3) Results from an airborne oxidation flow reactor (OFR), flown for the first time, show a factor of 4.5 increase in potential SOA concentrations over Seoul versus over the Yellow Sea, a region where background air masses that are advected into Seoul can be measured. (4) Box model simulations reproduce SOA observed over Seoul within 11 % on average and suggest that short-lived hydrocarbons (i.e., xylenes, trimethylbenzenes, and semi-volatile and intermediate-volatility compounds) were the main SOA precursors over Seoul. Toluene alone contributes 9 % of the modeled SOA over Seoul. Finally, along with these results, we use the metric ΔOA/ΔCO2 to examine the amount of OA produced per fuel consumed in a megacity, which shows less variability across the world than ΔOA∕ΔCO.

This study was designed to determine the optimal intensity for verification phase testing (VP) in healthy, young adults. Thirty one young, active participants (16 females) completed a cycle ergometer graded exercise test (GXT) VO2max test and 4 VP tests at 80, 90, 100, and 105% of the maximum wattage achieved during the GXT. GXT and VP VO2max values showed a significant test x sex interaction (p = 0.02). The males elicited significantly higher VO2max values during the GXT, 80%, and 90% when compared to the 105%, (105 vs. GXT: p = 0.05; 105% vs. 80%: p < 0.01; 105% vs. 90%: p = 0.02). There were no significant differences in VO2max across the tests in the females (p > 0.05); 80% of the males achieved their highest VP VO2max during a submaximal VP test compared to only 37.5% of the females. A secondary study conducted showed excellent reliability (ICCs > 0.90) and low variation (CVs < 3%) for the 90% VP. Our findings show that a submaximal verification phase intensity is ideal for young healthy males to elicit the highest VO2max during cycle ergometer testing. For females, a range of intensities (80–105%) produce similar VO2max values. However, the 80% VP yields an unnecessarily high time to exhaustion.