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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.

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.

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.

To determine the impact of dynamic and aerosol processes on marine low clouds, we examine the seasonal impact of updraft speed w and cloud condensation nuclei concentration at 0.43 % supersaturation (NCCN0.43%) on the cloud droplet number concentration (NC) of low-level clouds over the western North Atlantic Ocean. Aerosol and cloud properties were measured with instruments on board the NASA LaRC Falcon HU-25 during the ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment) mission in summer (August) and winter (February–March) 2020. The data are grouped into different NCCN0.43% loadings, and the density functions of NC and w near the cloud bases are compared. For low updrafts (w < 1.3 m s−1), NC in winter is mainly limited by the updraft speed and in summer additionally by aerosols. At larger updrafts (w > 3 m s−1), NC is impacted by the aerosol population, while at clean marine conditions cloud nucleation is aerosol-limited, and for high NCCN0.43% it is influenced by aerosols and updraft. The aerosol size distribution in winter shows a bimodal distribution in clean marine environments, which transforms to a unimodal distribution in high NCCN0.43% due to chemical and physical aerosol processes, whereas unimodal distributions prevail in summer, with a significant difference in their aerosol concentration and composition. The increase of NCCN0.43% is accompanied with an increase of organic aerosol and sulfate compounds in both seasons. We demonstrate that NC can be explained by cloud condensation nuclei activation through upwards processed air masses with varying fractions of activated aerosols. The activation highly depends on w and thus supersaturation between the different seasons, while the aerosol size distribution additionally affects NC within a season. Our results quantify the seasonal influence of w and NCCN0.43% on NC and can be used to improve the representation of low marine clouds in models.

North American pollution outflow is ubiquitous over the western North Atlantic Ocean, especially in winter, making this location a suitable natural laboratory for investigating the impact of precipitation on aerosol particles along air mass trajectories. We take advantage of observational data collected at Bermuda to seasonally assess the sensitivity of aerosol mass concentrations and volume size distributions to accumulated precipitation along trajectories (APT). The mass concentration of particulate matter with aerodynamic diameter less than 2.5 µm normalized by the enhancement of carbon monoxide above background (PM2.5/ΔCO) at Bermuda was used to estimate the degree of aerosol loss during transport to Bermuda. Results for December–February (DJF) show that most trajectories come from North America and have the highest APTs, resulting in a significant reduction (by 53 %) in PM2.5/ΔCO under high-APT conditions (> 13.5 mm) relative to low-APT conditions (< 0.9 mm). Moreover, PM2.5/ΔCO was most sensitive to increases in APT up to 5 mm (−0.044 µg m−3 ppbv−1 mm−1) and less sensitive to increases in APT over 5 mm. While anthropogenic PM2.5 constituents (e.g., black carbon, sulfate, organic carbon) decrease with high APT, sea salt, in contrast, was comparable between high- and low-APT conditions owing to enhanced local wind and sea salt emissions in high-APT conditions. The greater sensitivity of the fine-mode volume concentrations (versus coarse mode) to wet scavenging is evident from AErosol RObotic NETwork (AERONET) volume size distribution data. A combination of GEOS-Chem model simulations of the 210Pb submicron aerosol tracer and its gaseous precursor 222Rn reveals that (i) surface aerosol particles at Bermuda are most impacted by wet scavenging in winter and spring (due to large-scale precipitation) with a maximum in March, whereas convective scavenging plays a substantial role in summer; and (ii) North American 222Rn tracer emissions contribute most to surface 210Pb concentrations at Bermuda in winter (∼ 75 %–80 %), indicating that air masses arriving at Bermuda experience large-scale precipitation scavenging while traveling from North America. A case study flight from the ACTIVATE field campaign on 22 February 2020 reveals a significant reduction in aerosol number and volume concentrations during air mass transport off the US East Coast associated with increased cloud fraction and precipitation. These results highlight the sensitivity of remote marine boundary layer aerosol characteristics to precipitation along trajectories, especially when the air mass source is continental outflow from polluted regions like the US East Coast.

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.

This work focuses on total organic carbon (TOC) and contributing species in cloud water over Southeast Asia using a rare airborne dataset collected during NASA's Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex), in which a wide variety of maritime clouds were studied, including cumulus congestus, altocumulus, altostratus, and cumulus. Knowledge of TOC masses and their contributing species is needed for improved modeling of cloud processing of organics and to understand how aerosols and gases impact and are impacted by clouds. This work relies on 159 samples collected with an axial cyclone cloud-water collector at altitudes of 0.2–6.8 km that had sufficient volume for both TOC and speciated organic composition analysis. Species included monocarboxylic acids (glycolate, acetate, formate, and pyruvate), dicarboxylic acids (glutarate, adipate, succinate, maleate, and oxalate), methanesulfonic acid (MSA), and dimethylamine (DMA). TOC values range between 0.018 and 13.66 ppm C with a mean of 0.902 ppm C. The highest TOC values are observed below 2 km with a general reduction aloft. An exception is samples impacted by biomass burning for which TOC remains enhanced at altitudes as high as 6.5 km (7.048 ppm C). Estimated total organic matter derived from TOC contributes a mean of 30.7 % to total measured mass (inorganics + organics). Speciated organics contribute (on a carbon mass basis) an average of 30.0 % to TOC in the study region and account for an average of 10.3 % to total measured mass. The order of the average contribution of species to TOC, in decreasing contribution of carbon mass, is as follows (±1 standard deviation): acetate (14.7 ± 20.5 %), formate (5.4 ± 9.3 %), oxalate (2.8 ± 4.3 %), DMA (1.7 ± 6.3 %), succinate (1.6 ± 2.4 %), pyruvate (1.3 ± 4.5 %), glycolate (1.3 ± 3.7 %), adipate (1.0 ± 3.6 %), MSA (0.1 ± 0.1 %), glutarate (0.1 ± 0.2 %), and maleate (< 0.1 ± 0.1 %). Approximately 70 % of TOC remains unaccounted for, highlighting the complex nature of organics in the study region; in samples collected in biomass burning plumes, up to 95.6 % of TOC mass is unaccounted for based on the species detected. Consistent with other regions, monocarboxylic acids dominate the speciated organic mass (∼ 75 %) and are about 4 times more abundant than dicarboxylic acids. Samples are categorized into four cases based on back-trajectory history, revealing source-independent similarity between the bulk contributions of monocarboxylic and dicarboxylic acids to TOC (16.03 %–23.66 % and 3.70 %–8.75 %, respectively). Furthermore, acetate, formate, succinate, glutarate, pyruvate, oxalate, and MSA are especially enhanced during biomass burning periods, which is attributed to peat emissions transported from Sumatra and Borneo. Lastly, dust (Ca2+) and sea salt (Na+/Cl-) tracers exhibit strong correlations with speciated organics, supporting how coarse aerosol surfaces interact with these water-soluble organics.

Cloud drop number concentrations (Nd) over the western North Atlantic Ocean (WNAO) are generally highest during the winter (DJF) and lowest in summer (JJA), in contrast to aerosol proxy variables (aerosol optical depth, aerosol index, surface aerosol mass concentrations, surface cloud condensation nuclei (CCN) concentrations) that generally peak in spring (MAM) and JJA with minima in DJF. Using aircraft, satellite remote sensing, ground-based in situ measurement data, and reanalysis data, we characterize factors explaining the divergent seasonal cycles and furthermore probe into factors influencing Nd on seasonal timescales. The results can be summarized well by features most pronounced in DJF, including features associated with cold-air outbreak (CAO) conditions such as enhanced values of CAO index, planetary boundary layer height (PBLH), low-level liquid cloud fraction, and cloud-top height, in addition to winds aligned with continental outflow. Data sorted into high- and low-Nd days in each season, especially in DJF, revealed that all of these conditions were enhanced on the high-Nd days, including reduced sea level pressure and stronger wind speeds. Although aerosols may be more abundant in MAM and JJA, the conditions needed to activate those particles into cloud droplets are weaker than in colder months, which is demonstrated by calculations of the strongest (weakest) aerosol indirect effects in DJF (JJA) based on comparing Nd to perturbations in four different aerosol proxy variables (total and sulfate aerosol optical depth, aerosol index, surface mass concentration of sulfate). We used three machine learning models and up to 14 input variables to infer about most influential factors related to Nd for DJF and JJA, with the best performance obtained with gradient-boosted regression tree (GBRT) analysis. The model results indicated that cloud fraction was the most important input variable, followed by some combination (depending on season) of CAO index and surface mass concentrations of sulfate and organic carbon. Future work is recommended to further understand aspects uncovered here such as impacts of free tropospheric aerosol entrainment on clouds, degree of boundary layer coupling, wet scavenging, and giant CCN effects on aerosol–Nd relationships, updraft velocity, and vertical structure of cloud properties such as adiabaticity that impact the satellite estimation of Nd.

The tropical Northwest Pacific (TNWP) is a receptor for pollution sources throughout Asia and is highly susceptible to climate change, making it imperative to understand long-range transport in this complex aerosol-meteorological environment. Measurements from the NASA Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex; 24 August to 5 October 2019) and back trajectories from the National Oceanic and Atmospheric Administration Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT) were used to examine transport into the TNWP from the Maritime Continent (MC), peninsular Southeast Asia (PSEA), East Asia (EA), and the West Pacific (WP). A mid-campaign monsoon shift on 20 September 2019 led to distinct transport patterns between the southwest monsoon (SWM; before 20 September) and monsoon transition (MT; after 20 September). During the SWM, long-range transport was a function of southwesterly winds and cyclones over the South China Sea. Low- (high-) altitude air generally came from MC (PSEA), implying distinct aerosol processing related to convection and perhaps wind shear. The MT saw transport from EA and WP, driven by Pacific northeasterly winds, continental anticyclones, and cyclones over the East China Sea. Composition of transported air differed by emission source and accumulated precipitation along trajectories (APT). MC air was characterized by biomass burning tracers while major components of EA air pointed to Asian outflow and secondary formation. Convective scavenging of PSEA air was evidenced by considerable vertical differences between aerosol species but not trace gases, as well as notably higher APT and smaller particles than other regions. Finally, we observed a possible wet scavenging mechanism acting on MC air aloft that was not strictly linked to precipitation. These results are important for understanding the transport and processing of air masses with further implications for modeling aerosol lifecycles and guiding international policymaking to public health and climate, particularly during the SWM and MT.

A new aircraft-mounted probe for collecting samples of cloud water has been designed, fabricated, and extensively tested. Following previous designs, the probe uses inertial separation to remove cloud droplets from the airstream, which are subsequently collected and stored for offline analysis. We report details of the design, operation, and modelled and measured probe performance.Computational fluid dynamics (CFD) was used to understand the flow patterns around the complex interior geometrical features that were optimized to ensure efficient droplet capture. CFD simulations coupled with particle tracking and multiphase surface transport modelling provide detailed estimates of the probe performance across the entire range of flight operating conditions and sampling scenarios.Physical operation of the probe was tested on a Lockheed C-130 Hercules (fuselage mounted) and de Havilland Twin Otter (wing pylon mounted) during three airborne field campaigns. During C-130 flights on the final field campaign, the probe reflected the most developed version of the design and a median cloud water collection rate of 4.5 mL min−1 was achieved. This allowed samples to be collected over 1–2 min under optimal cloud conditions. Flights on the Twin Otter featured an inter-comparison of the new probe with a slotted-rod collector, which has an extensive airborne campaign legacy. Comparison of trace species concentrations showed good agreement between collection techniques, with absolute concentrations of most major ions agreeing within 30 %, over a range of several orders of magnitude.

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 use of alternative fuels for aviation is likely to increase due to concerns over fuel security, price stability, and the sustainability of fuel sources. Concurrent reductions in particulate emissions from these alternative fuels are expected because of changes in fuel composition including reduced sulfur and aromatic content. The NASA Alternative Aviation Fuel Experiment (AAFEX) was conducted in January–February 2009 to investigate the effects of synthetic fuels on gas-phase and particulate emissions. Standard petroleum JP-8 fuel, pure synthetic fuels produced from natural gas and coal feedstocks using the Fischer–Tropsch (FT) process, and 50% blends of both fuels were tested in the CFM-56 engines on a DC-8 aircraft. To examine plume chemistry and particle evolution with time, samples were drawn from inlet probes positioned 1, 30, and 145 m downstream of the aircraft engines. No significant alteration to engine performance was measured when burning the alternative fuels. However, leaks in the aircraft fuel system were detected when operated with the pure FT fuels as a result of the absence of aromatic compounds in the fuel. Dramatic reductions in soot emissions were measured for both the pure FT fuels (reductions in mass of 86% averaged over all powers) and blended fuels (66%) relative to the JP-8 baseline with the largest reductions at idle conditions. At 7% power, this corresponds to a reduction from 7.6 mg kg−1 for JP-8 to 1.2 mg kg−1 for the natural gas FT fuel. At full power, soot emissions were reduced from 103 to 24 mg kg−1 (JP-8 and natural gas FT, respectively). The alternative fuels also produced smaller soot (e.g., at 85% power, volume mean diameters were reduced from 78 nm for JP-8 to 51 nm for the natural gas FT fuel), which may reduce their ability to act as cloud condensation nuclei (CCN). The reductions in particulate emissions are expected for all alternative fuels with similar reductions in fuel sulfur and aromatic content regardless of the feedstock. As the plume cools downwind of the engine, nucleation-mode aerosols form. For the pure FT fuels, reductions (94% averaged over all powers) in downwind particle number emissions were similar to those measured at the exhaust plane (84%). However, the blended fuels had less of a reduction (reductions of 30–44%) than initially measured (64%). The likely explanation is that the reduced soot emissions in the blended fuel exhaust plume results in promotion of new particle formation microphysics, rather than coating on pre-existing soot particles, which is dominant in the JP-8 exhaust plume. Downwind particle volume emissions were reduced for both the pure (79 and 86% reductions) and blended FT fuels (36 and 46%) due to the large reductions in soot emissions. In addition, the alternative fuels had reduced particulate sulfate production (near zero for FT fuels) due to decreased fuel sulfur content. To study the formation of volatile aerosols (defined as any aerosol formed as the plume ages) in more detail, tests were performed at varying ambient temperatures (−4 to 20 °C). At idle, particle number and volume emissions were reduced linearly with increasing ambient temperature, with best fit slopes corresponding to −8 × 1014 particles (kg fuel)−1 °C−1 for particle number emissions and −10 mm3 (kg fuel)−1 °C−1 for particle volume emissions. The temperature dependency of aerosol formation can have large effects on local air quality surrounding airports in cold regions. Aircraft-produced aerosols in these regions will be much larger than levels expected based solely on measurements made directly at the engine exit plane. The majority (90% at idle) of the volatile aerosol mass formed as nucleation-mode aerosols, with a smaller fraction as a soot coating. Conversion efficiencies of up to 2.8% were measured for the partitioning of gas-phase precursors (unburned hydrocarbons and SO2) to form volatile aerosols. Highest conversion efficiencies were measured at 45% power.

In the spring of 2008 NASA and NOAA funded the ARCTAS and ARCPAC field campaigns as contributions to POLARCAT, a core IPY activity. During the campaigns the NASA DC-8, P-3B and NOAA WP-3D aircraft conducted over 160 h of in-situ sampling between 0.1 and 12 km throughout the Western Arctic north of 55° N (i.e. Alaska to Greenland). All aircraft were equipped with multiple wavelength measurements of aerosol optics, trace gas and aerosol chemistry measurements, as well as direct measurements of the aerosol size distributions and black carbon mass. Late April of 2008 proved to be exceptional in terms of Asian biomass burning emissions transported to the Western Arctic. Though these smoke plumes account for only 11–14 % of the samples within the Western Arctic domain, they account for 42–47 % of the total burden of black carbon. Dust was also commonly observed but only contributes to 4–12 % and 3–8 % of total light absorption at 470 and 530 nm wavelengths above 6 km. Below 6 km, light absorption by carbonaceous aerosol derived from urban/industrial and biomass burning emissions account for 97–99 % of total light absorption by aerosol. Stratifying the data to reduce the influence of dust allows us to determine mass absorption efficiencies for black carbon of 11.2±0.8, 9.5±0.6 and 7.4±0.7 m2 g−1 at 470, 530 and 660 nm wavelengths. These estimates are consistent with 35–80 % enhancements in 530 nm absorption due to clear or slightly absorbing coatings of pure black carbon particulate. Assuming a 1/λ wavelength dependence for BC absorption, and assuming that refractory aerosol (420 °C, τ = 0.1 s) in low-dust samples is dominated by brown carbon, we derive mass absorption efficiencies for brown carbon of 0.83±0.15 and 0.27±0.08 m2 g−1 at 470 and 530 nm wavelengths. Estimates for the mass absorption efficiencies of Asian dust are 0.034 m2 g−1 and 0.017 m2 g−1. However the absorption efficiency estimates for dust are highly uncertain due to the limitations imposed by PSAP instrument noise. In-situ ARCTAS/ARCPAC measurements during the IPY provide valuable constraints for absorbing aerosol over the Western Arctic, species which are currently poorly simulated over a region that is critically under-sampled.

In-situ airborne measurements of trace gases, aerosol size distributions, chemistry and optical properties were conducted over Mexico and the Eastern North Pacific during MILAGRO and INTEX-B. Heterogeneous reactions between secondary aerosol precursor gases and mineral dust lead to sequestration of sulfur, nitrogen and chlorine in the supermicrometer particulate size range. Simultaneous measurements of aerosol size distributions and weak-acid soluble calcium result in an estimate of 11 wt% of CaCO3 for Asian dust. During transport across the North Pacific, ~5–30% of the CaCO3 is converted to CaSO4 or Ca(NO3)2 with an additional ~4% consumed through reactions with HCl. The 1996 to 2008 record from the Mauna Loa Observatory confirm these findings, indicating that, on average, 19% of the CaCO3 has reacted to form CaSO4 and 7% has reacted to form Ca(NO3)2 and ~2% has reacted with HCl. In the nitrogen-oxide rich boundary layer near Mexico City up to 30% of the CaCO3 has reacted to form Ca(NO3)2 while an additional 8% has reacted with HCl. These heterogeneous reactions can result in a ~3% increase in dust solubility which has an insignificant effect on their optical properties compared to their variability in-situ. However, competition between supermicrometer dust and submicrometer primary aerosol for condensing secondary aerosol species led to a 25% smaller number median diameter for the accumulation mode aerosol. A 10–25% reduction of accumulation mode number median diameter results in a 30–70% reduction in submicrometer light scattering at relative humidities in the 80–95% range. At 80% RH submicrometer light scattering is only reduced ~3% due to a higher mass fraction of hydrophobic refractory components in the dust-affected accumulation mode aerosol. Thus reducing the geometric mean diameter of the submicrometer aerosol has a much larger effect on aerosol optical properties than changes to the hygroscopic:hydrophobic mass fractions of the accumulation mode aerosol. In the presence of dust, nitric acid concentrations are reduced to y as a fraction of total nitrogen (NOy plus particulate nitrate), is reduced from >85% to 60–80% in the presence of dust. These observations support previous model studies which predict irreversible sequestration of reactive nitrogen species through heterogeneous reactions with mineral dust during long-range transport.

Combined lidar and polarimeter retrievals of aerosol, cloud, and ocean microphysical properties involve single-scattering cloud calculations that are time consuming. We create a look-up table to speed up these calculations for water droplets in the atmosphere. In our new Lorenz-Mie look-up table we tabulate the light scattering by an ensemble of homogeneous isotropic spheres at wavelengths starting from 0.35 µm. The look-up table covers liquid water cloud particles with radii in the range of 0.001-500 µm while gaining an increase of up to 10 4 in computational speed. The covered complex refractive indices range from 1.25 to 1.36 for the real part and from 0 to 0.001 for the imaginary part. We show that we can precisely compute inherent optical properties for the particle size distributions ranging up to 100 µm for the effective radius and up to 0.6 for the effective variance. We test wavelengths from 0.35 to 2.3 µm and find that the elements of the normalized scattering matrix as well as the asymmetry parameter, the absorption, backscatter, extinction, and scattering coefficients are precise to within 1% for 96.7%-100% of cases depending on the inherent optical property. We also provide an example of using the look-up table with in situ measurements to determine agreement with remote sensing. The table together with C++, Fortran, MATLAB, and Python codes to interpolate the complex refractive index and apply different particle size distributions are freely available online.

Aerosol mass extinction efficiency (MEE) is a key aerosol property used to connect aerosol optical properties with aerosol mass concentrations. Using measurements of smoke obtained during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign we find that mid-visible smoke MEE can change by a factor of 2-3 between fresh smoke (<2 hr old) and one-day-old smoke. While increases in aerosol size partially explain this trend, changes in the real part of the aerosol refractive index (real(n)) are necessary to provide closure assuming Mie theory. Real(n) estimates derived from multiple days of FIREX-AQ measurements increase with age (from 1.40 - 1.45 to 1.5-1.54 from fresh to one-day-old) and are found to be positively correlated with organic aerosol oxidation state and aerosol size, and negatively correlated with smoke volatility. Future laboratory, field, and modeling studies should focus on better understanding and parameterizing these relationships to fully represent smoke aging., Competing Interests: The authors declare no conflicts of interest relevant to this study., (© 2022 The Authors.)

Leveraging aerosol data from multiple airborne and surface-based field campaigns encompassing diverse environmental conditions, we calculate statistics of the oxalate-sulfate mass ratio (median: 0.0217; 95% confidence interval: 0.0154-0.0296; R = 0.76; N = 2,948). Ground-based measurements of the oxalate-sulfate ratio fall within our 95% confidence interval, suggesting the range is robust within the mixed layer for the submicrometer particle size range. We demonstrate that dust and biomass burning emissions can separately bias this ratio toward higher values by at least one order of magnitude. In the absence of these confounding factors, the 95% confidence interval of the ratio may be used to estimate the relative extent of aqueous processing by comparing inferred oxalate concentrations between air masses, with the assumption that sulfate primarily originates from aqueous processing.

North American pollution outflow is ubiquitous over the western North Atlantic Ocean, especially in winter, making this location a suitable natural laboratory for investigating the impact of precipitation on aerosol particles along air mass trajectories. We take advantage of observational data collected at Bermuda to seasonally assess the sensitivity of aerosol mass concentrations and volume size distributions to accumulated precipitation along trajectories (APT). The mass concentration of particulate matter with aerodynamic diameter less than 2.5 μm normalized by the enhancement of carbon monoxide above background (PM 2.5 /ΔCO) at Bermuda was used to estimate the degree of aerosol loss during transport to Bermuda. Results for December-February (DJF) show that most trajectories come from North America and have the highest APTs, resulting in a significant reduction (by 53 %) in PM 2.5 /ΔCO under high-APT conditions (> 13.5 mm) relative to low-APT conditions (< 0.9 mm). Moreover, PM 2.5 /ΔCO was most sensitive to increases in APT up to 5 mm (-0.044 μg m -3 ppbv -1 mm -1 ) and less sensitive to increases in APT over 5 mm. While anthropogenic PM 2.5 constituents (e.g., black carbon, sulfate, organic carbon) decrease with high APT, sea salt, in contrast, was comparable between high- and low-APT conditions owing to enhanced local wind and sea salt emissions in high-APT conditions. The greater sensitivity of the fine-mode volume concentrations (versus coarse mode) to wet scavenging is evident from AErosol RObotic NETwork (AERONET) volume size distribution data. A combination of GEOS-Chem model simulations of the 210 Pb submicron aerosol tracer and its gaseous precursor 222 Rn reveals that (i) surface aerosol particles at Bermuda are most impacted by wet scavenging in winter and spring (due to large-scale precipitation) with a maximum in March, whereas convective scavenging plays a substantial role in summer; and (ii) North American 222 Rn tracer emissions contribute most to surface 210 Pb concentrations at Bermuda in winter (~75 %-80 %), indicating that air masses arriving at Bermuda experience large-scale precipitation scavenging while traveling from North America. A case study flight from the ACTIVATE field campaign on 22 February 2020 reveals a significant reduction in aerosol number and volume concentrations during air mass transport off the US East Coast associated with increased cloud fraction and precipitation. These results highlight the sensitivity of remote marine boundary layer aerosol characteristics to precipitation along trajectories, especially when the air mass source is continental outflow from polluted regions like the US East Coast.

Cloud drop number concentrations ( N d ) over the western North Atlantic Ocean (WNAO) are generally highest during the winter (DJF) and lowest in summer (JJA), in contrast to aerosol proxy variables (aerosol optical depth, aerosol index, surface aerosol mass concentrations, surface cloud condensation nuclei (CCN) concentrations) that generally peak in spring (MAM) and JJA with minima in DJF. Using aircraft, satellite remote sensing, ground-based in situ measurement data, and reanalysis data, we characterize factors explaining the divergent seasonal cycles and furthermore probe into factors influencing N d on seasonal timescales. The results can be summarized well by features most pronounced in DJF, including features associated with cold-air outbreak (CAO) conditions such as enhanced values of CAO index, planetary boundary layer height (PBLH), low-level liquid cloud fraction, and cloud-top height, in addition to winds aligned with continental outflow. Data sorted into high- and low- N d days in each season, especially in DJF, revealed that all of these conditions were enhanced on the high- N d days, including reduced sea level pressure and stronger wind speeds. Although aerosols may be more abundant in MAM and JJA, the conditions needed to activate those particles into cloud droplets are weaker than in colder months, which is demonstrated by calculations of the strongest (weakest) aerosol indirect effects in DJF (JJA) based on comparing N d to perturbations in four different aerosol proxy variables (total and sulfate aerosol optical depth, aerosol index, surface mass concentration of sulfate). We used three machine learning models and up to 14 input variables to infer about most influential factors related to N d for DJF and JJA, with the best performance obtained with gradient-boosted regression tree (GBRT) analysis. The model results indicated that cloud fraction was the most important input variable, followed by some combination (depending on season) of CAO index and surface mass concentrations of sulfate and organic carbon. Future work is recommended to further understand aspects uncovered here such as impacts of free tropospheric aerosol entrainment on clouds, degree of boundary layer coupling, wet scavenging, and giant CCN effects on aerosol- N d relationships, updraft velocity, and vertical structure of cloud properties such as adiabaticity that impact the satellite estimation of N d ., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

A particle-into-liquid sampler (PILS) was coupled to a flow-through conductivity cell to provide a continuous, nondestructive, online measurement in support of offline ion chromatography analysis. The conductivity measurement provides a rapid assessment of the total ion concentration augmenting slower batch-sample data from offline analysis and is developed primarily to assist airborne measurements, where fast time-response is essential. A conductivity model was developed for measured ions and excellent closure was derived for laboratory-generated aerosols (97% conductivity explained, R 2 > 0.99). The PILS-conductivity measurement was extensively tested throughout the NASA Cloud, Aerosol and Monsoon Processes: Philippines Experiment (CAMP 2 Ex) during nineteen research flights. A diverse range of ambient aerosol was sampled from biomass burning, fresh and aged urban pollution, and marine sources. Ambient aerosol did not exhibit the same degree of closure as the laboratory aerosol, with measured ions only accountable for 43% of the conductivity. The remaining fraction of the conductivity was examined in combination with ion charge balance and found to provide additional supporting information for diagnosing and modeling particle acidity. An urban plume case study was used to demonstrate the utility of the measurement for supplementing compositional data and augmenting the temporal capability of the PILS., Competing Interests: Disclosure statement The authors declare no conflicts of interest, financial interests or benefits.

A new aircraft-mounted probe for collecting samples of cloud water has been designed, fabricated, and extensively tested. Following previous designs, the probe uses inertial separation to remove cloud droplets from the airstream, which are subsequently collected and stored for offline analysis. We report details of the design, operation, and modelled and measured probe performance. Computational fluid dynamics (CFD) was used to understand the flow patterns around the complex interior geometrical features that were optimized to ensure efficient droplet capture. CFD simulations coupled with particle tracking and multiphase surface transport modelling provide detailed estimates of the probe performance across the entire range of flight operating conditions and sampling scenarios. Physical operation of the probe was tested on a Lockheed C-130 Hercules (fuselage mounted) and de Havilland Twin Otter (wing pylon mounted) during three airborne field campaigns. During C-130 flights on the final field campaign, the probe reflected the most developed version of the design and a median cloud water collection rate of 4.5 mL min -1 was achieved. This allowed samples to be collected over 1-2 min under optimal cloud conditions. Flights on the Twin Otter featured an inter-comparison of the new probe with a slotted-rod collector, which has an extensive airborne campaign legacy. Comparison of trace species concentrations showed good agreement between collection techniques, with absolute concentrations of most major ions agreeing within 30 %, over a range of several orders of magnitude., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

Aviation-related aerosol emissions contribute to the formation of contrail cirrus clouds that can alter upper tropospheric radiation and water budgets, and therefore climate. The magnitude of air-traffic-related aerosol-cloud interactions and the ways in which these interactions might change in the future remain uncertain. Modelling studies of the present and future effects of aviation on climate require detailed information about the number of aerosol particles emitted per kilogram of fuel burned and the microphysical properties of those aerosols that are relevant for cloud formation. However, previous observational data at cruise altitudes are sparse for engines burning conventional fuels, and no data have previously been reported for biofuel use in-flight. Here we report observations from research aircraft that sampled the exhaust of engines onboard a NASA DC-8 aircraft as they burned conventional Jet A fuel and a 50:50 (by volume) blend of Jet A fuel and a biofuel derived from Camelina oil. We show that, compared to using conventional fuels, biofuel blending reduces particle number and mass emissions immediately behind the aircraft by 50 to 70 per cent. Our observations quantify the impact of biofuel blending on aerosol emissions at cruise conditions and provide key microphysical parameters, which will be useful to assess the potential of biofuel use in aviation as a viable strategy to mitigate climate change.

The emissions from a Garrett-AiResearch (now Honeywell) Model GTCP85-98CK auxiliary power unit (APU) were determined as part of the National Aeronautics and Space Administration's (NASA's) Alternative Aviation Fuel Experiment (AAFEX) using both JP-8 and a coal-derived Fischer Tropsch fuel (FT-2). Measurements were conducted by multiple research organizations for sulfur dioxide (SO2, total hydrocarbons (THC), carbon monoxide (CO), carbon dioxide (CO2), nitrogen oxides (NOx), speciated gas-phase emissions, particulate matter (PM) mass and number, black carbon, and speciated PM. In addition, particle size distribution (PSD), number-based geometric mean particle diameter (GMD), and smoke number were also determined from the data collected. The results of the research showed PM mass emission indices (EIs) in the range of 20 to 700 mg/kg fuel and PM number EIs ranging from 0.5 x 10(15) to 5 x 10(15) particles/kg fuel depending on engine load and fuel type. In addition, significant reductions in both the SO2 and PM EIs were observed for the use of the FT fuel. These reductions were on the order of approximately 90% for SO2 and particle mass EIs and approximately 60% for the particle number EI, with similar decreases observed for black carbon. Also, the size of the particles generated by JP-8 combustion are noticeably larger than those emitted by the APU burning the FT fuel with the geometric mean diameters ranging from 20 to 50 nm depending on engine load and fuel type. Finally, both particle-bound sulfate and organics were reduced during FT-2 combustion. The PM sulfate was reduced by nearly 100% due to lack of sulfur in the fuel, with the PM organics reduced by a factor of approximately 5 as compared with JP-8.