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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.

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.

Fireworks degrade air quality, reduce visibility, alter atmospheric chemistry, and cause short-term adverse health effects. However, there have not been any comprehensive physicochemical and optical measurements of fireworks and their associated impacts in a Southeast Asia megacity, where fireworks are a regular part of the culture. Size-resolved particulate matter (PM) measurements were made before, during, and after New Year 2019 at the Manila Observatory in Quezon City, Philippines, as part of the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex). A high-spectral-resolution lidar (HSRL) recorded a substantial increase in backscattered signal associated with high aerosol loading ∼440 m above the surface during the peak of firework activities around 00:00 (local time). This was accompanied by PM2.5 concentrations peaking at 383.9 µg m−3. During the firework event, water-soluble ions and elements, which affect particle formation, growth, and fate, were mostly in the submicrometer diameter range. Total (>0.056 µm) water-soluble bulk particle mass concentrations were enriched by 5.7 times during the fireworks relative to the background (i.e., average of before and after the firework). The water-soluble mass fraction of PM2.5 increased by 18.5 % above that of background values. This corresponded to increased volume fractions of inorganics which increased bulk particle hygroscopicity, kappa (κ), from 0.11 (background) to 0.18 (fireworks). Potassium and non-sea-salt (nss) SO42- contributed the most (70.9 %) to the water-soluble mass, with their mass size distributions shifting from a smaller to a larger submicrometer mode during the firework event. On the other hand, mass size distributions for NO3-, Cl−, and Mg2+ (21.1 % mass contribution) shifted from a supermicrometer mode to a submicrometer mode. Being both uninfluenced by secondary aerosol formation and constituents of firework materials, a subset of species were identified as the best firework tracer species (Cu, Ba, Sr, K+, Al, and Pb). Although these species (excluding K+) only contributed 2.1 % of the total mass concentration of water-soluble ions and elements, they exhibited the highest enrichments (6.1 to 65.2) during the fireworks. Surface microscopy analysis confirmed the presence of potassium/chloride-rich cubic particles along with capsule-shaped particles in firework samples. The results of this study highlight how firework emissions change the physicochemical and optical properties of water-soluble particles (e.g., mass size distribution, composition, hygroscopicity, and aerosol backscatter), which subsequently alters the background aerosol's respirability, influence on surroundings, ability to uptake gases, and viability as cloud condensation nuclei (CCN).

Aerosol–cloud interactions are the largest source of uncertainty in quantifying anthropogenic radiative forcing. The large uncertainty is, in part, due to the difficulty of predicting cloud microphysical parameters, such as the cloud droplet number concentration (Nd). Even though rigorous first-principle approaches exist to calculate Nd, the cloud and aerosol research community also relies on empirical approaches such as relating Nd to aerosol mass concentration. Here we analyze relationships between Nd and cloud water chemical composition, in addition to the effect of environmental factors on the degree of the relationships. Warm, marine, stratocumulus clouds off the California coast were sampled throughout four summer campaigns between 2011 and 2016. A total of 385 cloud water samples were collected and analyzed for 80 chemical species. Single- and multispecies log–log linear regressions were performed to predict Nd using chemical composition. Single-species regressions reveal that the species that best predicts Nd is total sulfate (Radj2=0.40). Multispecies regressions reveal that adding more species does not necessarily produce a better model, as six or more species yield regressions that are statistically insignificant. A commonality among the multispecies regressions that produce the highest correlation with Nd was that most included sulfate (either total or non-sea-salt), an ocean emissions tracer (such as sodium), and an organic tracer (such as oxalate). Binning the data according to turbulence, smoke influence, and in-cloud height allowed for examination of the effect of these environmental factors on the composition–Nd correlation. Accounting for turbulence, quantified as the standard deviation of vertical wind speed, showed that the correlation between Nd with both total sulfate and sodium increased at higher turbulence conditions, consistent with turbulence promoting the mixing between ocean surface and cloud base. Considering the influence of smoke significantly improved the correlation with Nd for two biomass burning tracer species in the study region, specifically oxalate and iron. When binning by in-cloud height, non-sea-salt sulfate and sodium correlated best with Nd at cloud top, whereas iron and oxalate correlated best with Nd at cloud base.

This study provides a detailed characterization of stratocumulus clearings off the US West Coast using remote sensing, reanalysis, and airborne in situ data. Ten years (2009–2018) of Geostationary Operational Environmental Satellite (GOES) imagery data are used to quantify the monthly frequency, growth rate of total area (GRArea), and dimensional characteristics of 306 total clearings. While there is interannual variability, the summer (winter) months experienced the most (least) clearing events, with the lowest cloud fractions being in close proximity to coastal topographical features along the central to northern coast of California, including especially just south of Cape Mendocino and Cape Blanco. From 09:00 to 18:00 (PST), the median length, width, and area of clearings increased from 680 to 1231, 193 to 443, and ∼67 000 to ∼250 000 km2, respectively. Machine learning was applied to identify the most influential factors governing the GRArea of clearings between 09:00 and 12:00 PST, which is the time frame of most rapid clearing expansion. The results from gradient-boosted regression tree (GBRT) modeling revealed that air temperature at 850 hPa (T850), specific humidity at 950 hPa (q950), sea surface temperature (SST), and anomaly in mean sea level pressure (MSLPanom) were probably most impactful in enhancing GRArea using two scoring schemes. Clearings have distinguishing features such as an enhanced Pacific high shifted more towards northern California, offshore air that is warm and dry, stronger coastal surface winds, enhanced lower-tropospheric static stability, and increased subsidence. Although clearings are associated obviously with reduced cloud fraction where they reside, the domain-averaged cloud albedo was actually slightly higher on clearing days as compared to non-clearing days. To validate speculated processes linking environmental parameters to clearing growth rates based on satellite and reanalysis data, airborne data from three case flights were examined. Measurements were compared on both sides of the clear–cloudy border of clearings at multiple altitudes in the boundary layer and free troposphere, with results helping to support links suggested by this study's model simulations. More specifically, airborne data revealed the influence of the coastal low-level jet and extensive horizontal shear at cloud-relevant altitudes that promoted mixing between clear and cloudy air. Vertical profile data provide support for warm and dry air in the free troposphere, additionally promoting expansion of clearings. Airborne data revealed greater evidence of sea salt in clouds on clearing days, pointing to a possible role for, or simply the presence of, this aerosol type in clearing areas coincident with stronger coastal winds.

This paper presents novel results from size-resolved particulate matter (PM) mass, composition, and morphology measurements conducted during the 2018 southwest monsoon (SWM) season in Metro Manila, Philippines. Micro-orifice uniform deposit impactors (MOUDIs) were used to collect PM sample sets composed of size-resolved measurements at the following aerodynamic cut-point diameters (Dp): 18, 10, 5.6, 3.2, 1.8, 1.0, 0.56, 0.32, 0.18, 0.10, and 0.056 µm. Each sample set was analyzed for composition of the water-soluble fraction. Analysis for mass was carried out on two sample sets, whereas black carbon (BC) and morphology analysis were analyzed on a single sample set. The bulk of the PM mass was between 0.18 and 1.0 µm with a dominant mode between 0.32 and 0.56 µm. Similarly, most of the black carbon (BC) mass was found between 0.10 and 1.0 µm, peaking between 0.18 and 0.32 µm. These peaks are located in the Greenfield gap, or the size range between 0.10 and 1.0 µm, where wet scavenging by rain is relatively inefficient. In the range between 0.10 and 0.18 µm, BC constituted 78.1 % of the measured mass. Comparable contributions of BC (26.9 %) and the water-soluble fraction (33.4 %) to total PM were observed and most of the unresolved mass, which amounted to 39.6 % in total, was for diameters exceeding 0.32 µm. The water-soluble ions and elements exhibited an average combined concentration of 8.53 µg m−3, with SO42-, NH4+, NO3-, Na+, and Cl− as the major contributors. Positive matrix factorization (PMF) was applied to identify the possible aerosol sources and estimate their contribution to the water-soluble fraction of collected PM. The factor with the highest contribution was attributed to “aged aerosol” (48.0 %), while “sea salt” (22.5 %) and “combustion” emissions (18.7 %) had comparable contributions. “Vehicular/resuspended dust” (5.6 %) and “waste processing” emissions (5.1 %) were also identified. Microscopy analysis highlighted the ubiquity of nonspherical particles regardless of size, which is significant when considering calculations of parameters such as single scattering albedo, the asymmetry parameter, and the extinction efficiency. The significant influence from aged aerosol to Metro Manila during the SWM season indicates that local sources in this megacity do not fully govern this coastal area's aerosol properties. The fact that the majority of the regional aerosol mass burden is accounted for by BC and other insoluble components has important downstream effects on the aerosol hygroscopic properties, which depend on composition. The results are relevant for understanding the impacts of monsoonal features on size-resolved aerosol properties, notably aqueous processing and wet scavenging. Finally, the results of this work provide contextual data for future sampling campaigns in Southeast Asia such as the airborne component of the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex) planned for the SWM season in 2019.

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.

This study uses airborne data from two field campaigns off the California coast to characterize aerosol size distribution characteristics in the entrainment interface layer (EIL), a thin and turbulent layer above marine stratocumulus cloud tops, which separates the stratocumulus-topped boundary layer (STBL) from the free troposphere (FT). The vertical bounds of the EIL are defined in this work based on considerations of buoyancy and turbulence using thermodynamic and dynamic data. Aerosol number concentrations are examined from three different probes with varying particle diameter (Dp) ranges: > 3 nm, > 10 nm, and 0.11–3.4 µm. Relative to the EIL and FT layers, the sub-cloud (SUB) layer exhibited lower aerosol number concentrations and higher surface area concentrations. High particle number concentrations between 3 and 10 nm in the EIL are indicative of enhanced nucleation, assisted by high actinic fluxes, cool and moist air, and much lower surface area concentrations than the STBL. Slopes of number concentration versus altitude in the EIL were correlated with the particle number concentration difference between the SUB and lower FT layers. The EIL aerosol size distribution was influenced by varying degrees from STBL aerosol versus subsiding FT aerosol depending on the case examined. These results emphasize the important role of the EIL in influencing nucleation and aerosol–cloud–climate interactions.

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.

Biomass burning (BB) aerosol events were characterized over the U.S. East Coast and Bermuda over the western North Atlantic Ocean (WNAO) between 2005 and 2018 using a combination of ground-based observations, satellite data, and model outputs. Days with BB influence in an atmospheric column (BB days) were identified using criteria biased toward larger fire events based on anomalously high AERONET aerosol optical depth (AOD) and MERRA-2 black carbon (BC) column density. BB days are present year-round with more in June-August (JJA) over the northern part of the East Coast, in contrast to more frequent events in March-May (MAM) over the southeast U.S. and Bermuda. BB source regions in MAM are southern Mexico and by the Yucatan, Central America, and the southeast U.S. JJA source regions are western parts of North America. Less than half of the BB days coincide with anomalously high PM 2.5 levels in the surface layer, according to data from 14 IMPROVE sites over the East Coast. Profiles of aerosol extinction suggest that BB particles can be found in the boundary layer and into the upper troposphere with the potential to interact with clouds. Higher cloud drop number concentration and lower drop effective radius are observed during BB days. In addition, lower liquid water path is found during these days, especially when BB particles are present in the boundary layer. While patterns are suggestive of cloud-BB aerosol interactions over the East Coast and the WNAO, additional studies are needed for confirmation.

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.

Coastal southeast Florida experiences a wide range of aerosol conditions, including African dust, biomass burning (BB) aerosols, as well as sea salt and other locally-emitted aerosols. These aerosols are important sources of cloud condensation nuclei (CCN), which play an essential role in governing cloud radiative properties. As marine environments dominate the surface of Earth, CCN characteristics in coastal southeast Florida have broad implications for other regions with the added feature that this site is perturbed by both natural and anthropogenic emissions. This study investigates the influence of different air mass types on CCN concentrations at 0.2% (CCN 0.2% ) and 1.0% (CCN 1.0% ) supersaturation (SS) based on ground site measurements during selected months in 2013, 2017, and 2018. Average CCN 0.2% and CCN 1.0% concentrations were 373 ± 200 cm -3 and 584 ± 323 cm -3 , respectively, for four selected days with minimal presence of African dust and BB (i.e., background days). CCN concentrations were not elevated on the four days with highest influence of African dust (289 ± 104 cm -3 [0.2% SS] and 591 ± 302 cm -3 [1.0% SS]), consistent with high dust mass concentrations comprised of coarse particles that are few in number. In contrast, CCN concentrations were substantially enhanced on the five days with the greatest impact from BB (1408 ± 976 cm -3 [0.2% SS] and 3337 ± 1252 cm -3 [1.0% SS]). Ratios of CCN 0.2% :CCN 1.0% were used to compare the hygroscopicity of the aerosols associated with African dust, BB, and background days. Average ratios were similar for days impacted by African dust and BB (0.54 ± 0.17 and 0.55 ± 0.17, respectively). A 29% higher average ratio was observed on background days (0.71 ± 0.14), owing in part to a strong presence of sea salt and reduced presence of more hydrophobic species such as those of a carbonaceous or mineral-dust nature. Finally, periods of heavy rainfall were shown to effectively decrease both CCN 0.2% and CCN 1.0% concentrations. However, the rate varied at which such concentrations increased after the rain. This work contributes knowledge on the nucleating ability of African dust and BB in a marine environment after varying periods of atmospheric transport (days to weeks). The results can be used to understand the hygroscopicity of these air mass types, predict how they may influence cloud properties, and provide a valuable model constraint when predicting CCN concentrations in comparable situations., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Aerosol characteristics and aerosol-cloud interactions remain uncertain in remote marine regions. We use over a decade of data (2000-2012) from the NASA AErosol RObotic NETwork, aerosol and wet deposition samples, satellite remote sensors, and models to examine aerosol and cloud droplet number characteristics at a representative open ocean site (Bermuda) over the Western North Atlantic Ocean (WNAO). Annual mean values were as follows: aerosol optical depth (AOD) = 0.12, Ångström Exponent (440/870 nm) = 0.95, fine mode fraction = 0.51, asymmetry factor = 0.72 (440 nm) and 0.68 (1020 nm), and Aqua-MODIS cloud droplet number concentrations = 51.3 cm -3 . The winter season (December-February) was characterized by high sea salt optical thickness and the highest aerosol extinction in the lowest 2 km. Extensive precipitation over the WNAO in winter helps contribute to the low FMFs in winter (~0.40-0.50) even though air trajectories often originate over North America. Spring and summer had more pronounced influence from sulfate, dust, organic carbon, and black carbon. Volume size distributions were bimodal with a dominant coarse mode (effective radii: 1.85-2.09 μm) and less pronounced fine mode (0.14-0.16 μm), with variability in the coarse mode likely due to different characteristic sizes for transported dust (smaller) versus regional sea salt (larger). Extreme pollution events highlight the sensitivity of this site to long-range transport of urban emissions, dust, and smoke. Differing annual cycles are identified between AOD and cloud droplet number concentrations, motivating a deeper look into aerosol-cloud interactions at this site.

This study examined spatial variations of precipitation accumulation and chemistry for six sites located on the West and East Coasts of the U.S., and one site each on the islands of Hawaii, Bermuda, and Luzon of the Philippines (specifically Manila). The nine coastal sites ranged widely in both mean annual precipitation accumulation, ranging from 40 cm (Mauna Loa, Hawaii) to 275 cm (Washington), and in terms of monthly profiles. The three island sites represented the extremes of differences in terms of chemical profiles, with Bermuda having the highest overall ion concentrations driven mainly by sea salt, Hawaii having the highest SO 4 2 - mass fractions due to the nearby influence of volcanic SO 2 emissions and mid-tropospheric transport of anthropogenic pollution, and Manila exhibiting the highest concentration of non-marine ions ( NH 4 + non-sea salt [nss] SO 4 2 - , nss Ca 2+ , NO 3 - , nss K + , nss Na + , nss Mg 2+ ) linked to anthropogenic, biomass burning, and crustal emissions. The Manila site exhibited the most variability in composition throughout the year due to shifting wind directions and having diverse regional and local pollutant sources. In contrast to the three island sites, the North American continental sites exhibited less variability in precipitation composition with sea salt being the most abundant constituent followed by some combination of SO 4 2 - , NO 3 - , and NH 4 + . The mean-annual pH values ranged from 4.88 (South Carolina) to 5.40 (central California) with NH 4 + exhibiting the highest neutralization factors for all sites except Bermuda where dust tracer species (nss Ca 2+ ) exhibited enhanced values. The results of this study highlight the sensitivity of wet deposition chemistry to regional considerations, elevation, time of year, and atmospheric circulations., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

This study focuses on the long-term aerosol and precipitation chemistry measurements from colocated monitoring sites in Southern Florida between 2013 and 2018. A positive matrix factorization (PMF) model identified six potential emission sources impacting the study area. The PMF model solution yielded the following source concentration profiles: (i) combustion; (ii) fresh sea salt; (iii) aged sea salt; (iv) secondary sulfate; (v) shipping emissions; and (vi) dust. Based on these results, concentration-weighted trajectory maps were developed to identify sources contributing to the PMF factors. Monthly mean precipitation pH values ranged from 4.98 to 5.58, being positively related to crustal species and negatively related to SO 4 2- . Sea salt dominated wet deposition volume-weighted concentrations year-round without much variability in its mass fraction in contrast to stronger seasonal changes in PM 2.5 composition where fresh sea salt was far less influential. The highest mean annual deposition fluxes were attributed to Cl - , NO 3 - , SO 4 2- , and Na + between April and October. Nitrate is strongly correlated with dust constituents (unlike sea salt) in precipitation samples, indicative of efficient partitioning to dust. Interrelationships between precipitation chemistry and aerosol species based on long-term surface data provide insight into aerosol-cloud-precipitation interactions., Competing Interests: Conflicts of Interest: The authors declare no conflict of interest.

Aerosol-cloud interactions are the largest source of uncertainty in quantifying anthropogenic radiative forcing. The large uncertainty is, in part, due to the difficulty of predicting cloud microphysical parameters, such as the cloud droplet number concentration ( N d ). Even though rigorous first-principle approaches exist to calculate N d , the cloud and aerosol research community also relies on empirical approaches such as relating N d to aerosol mass concentration. Here we analyze relationships between N d and cloud water chemical composition, in addition to the effect of environmental factors on the degree of the relationships. Warm, marine, stratocumulus clouds off the California coast were sampled throughout four summer campaigns between 2011 and 2016. A total of 385 cloud water samples were collected and analyzed for 80 chemical species. Single- and multispecies log-log linear regressions were performed to predict N d using chemical composition. Single-species regressions reveal that the species that best predicts N d is total sulfate ( R adj 2 = 0.40 ). Multispecies regressions reveal that adding more species does not necessarily produce a better model, as six or more species yield regressions that are statistically insignificant. A commonality among the multispecies regressions that produce the highest correlation with N d was that most included sulfate (either total or non-sea-salt), an ocean emissions tracer (such as sodium), and an organic tracer (such as oxalate). Binning the data according to turbulence, smoke influence, and in-cloud height allowed for examination of the effect of these environmental factors on the composition- N d correlation. Accounting for turbulence, quantified as the standard deviation of vertical wind speed, showed that the correlation between N d with both total sulfate and sodium increased at higher turbulence conditions, consistent with turbulence promoting the mixing between ocean surface and cloud base. Considering the influence of smoke significantly improved the correlation with N d for two biomass burning tracer species in the study region, specifically oxalate and iron. When binning by in-cloud height, non-sea-salt sulfate and sodium correlated best with N d at cloud top, whereas iron and oxalate correlated best with N d at cloud base., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

The MONterey Aerosol Research Campaign (MONARC) in May-June 2019 featured 14 repeated identical flights off the California coast over the open ocean at the same time each flight day. The objective of this study is to use MONARC data along with machine learning analysis to evaluate relationships between both supermicrometer sea salt aerosol number (N >1 ) and volume (V >1 ) concentrations and wind speed, wind direction, sea surface temperature (SST), ambient temperature (T amb ), turbulent kinetic energy (TKE), relative humidity (RH), marine boundary layer (MBL) depth, and drizzle rate. Selected findings from this study include the following: (i) Near surface (<60 m) N >1 and V >1 concentration ranges were 0.1-4.6 cm -3 and 0.3-28.2 μm 3 cm -3 , respectively; (ii) four meteorological regimes were identified during MONARC with each resulting in different N >1 and V >1 concentrations and also varying horizontal and vertical profiles; (iii) the relative predictive strength of the MBL properties varies depending on predicting N >1 or V >1 , with MBL depth being more highly ranked for predicting N >1 and with TKE being higher for predicting V >1 ; (iv) MBL depths >400 m (<200 m) often correspond to lower (higher) N >1 and V >1 concentrations; (v) enhanced drizzle rates coincide with reduced N >1 and V >1 concentrations; (vi) N >1 and V >1 concentrations exhibit an overall negative relationship with SST and RH and an overall positive relationship with T amb ; and (vii) wind speed and direction were relatively weak predictors of N >1 and V >1 .

This study examines 14 years (2004-2017) of surface aerosol composition data from the EPA IMPROVE network with a focus on the monthly profile, sources, and chemical nature of extreme dust events (>92nd percentile of fine soil concentration each month) impacting ten sites along the United States East Coast ranging in latitude from Florida to Maine. Based on trajectory, remote sensing, and reanalysis data, dust events were categorized into four source categories: African, Asian, Mix (African + Asian), and Other (anything other than African and Asian). The results reveal that extreme dust events account for between 3.3% and 4.6% of total available days depending on the site. March-April-May (MAM) had the most (174) dust events, followed by June-July-August (JJA) with 172, and then by September-October-November (SON) with 160 and December-January-February (DFJ) with 150. There is a variability in the predominant dust sources based on latitude, with African and Other sources more influential from North Carolina to the south, while Asian and Other were most important from New Jersey to the north. The Mix category is consistently the least frequent dust category at all sites. The African dust category was linked to the highest fine soil levels across the entire East Coast relative to other sources regardless of location. JJA is mostly impacted by African dust for sites ranging from Florida to New Jersey, while MAM is dominated by Asian dust for all sites. Mix events occurred mostly between April and October and Other events were most common outside of MAM and JJA seasons. Seven out of ten sites had Other as the most dominant source. Aerosol constituents organic carbon (OC) and elemental carbon (EC) had higher average concentrations in Other events (2.39 ± 0.78 μg m -3 and 0.79 ± 0.81 μg m -3 , respectively) as compared to the other three source categories, suggestive of regional anthropogenic emissions. Moreover, the ratios of elements (Si:Al, K:Fe, Fe:Ca, Al:Ca) contributing to fine soil and PM 2.5 :PM 10 exhibited distinct values depending on the dust source category and the site. This study builds on the growing evidence of the importance of long-range transport of dust in impacting distant regions and how a variety of sources can impact the U.S. East Coast at all times of the year., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

This study provides a detailed characterization of stratocumulus clearings off the US West Coast using remote sensing, reanalysis, and airborne in situ data. Ten years (2009-2018) of Geostationary Operational Environmental Satellite (GOES) imagery data are used to quantify the monthly frequency, growth rate of total area (GR Area ), and dimensional characteristics of 306 total clearings. While there is interannual variability, the summer (winter) months experienced the most (least) clearing events, with the lowest cloud fractions being in close proximity to coastal topographical features along the central to northern coast of California, including especially just south of Cape Mendocino and Cape Blanco. From 09:00 to 18:00 (PST), the median length, width, and area of clearings increased from 680 to 1231, 193 to 443, and ~ 67000 to ~ 250000km 2 , respectively. Machine learning was applied to identify the most influential factors governing the GR Area of clearings between 09:00 and 12:00PST, which is the time frame of most rapid clearing expansion. The results from gradient-boosted regression tree (GBRT) modeling revealed that air temperature at 850 hPa ( T 850 ), specific humidity at 950 hPa ( q 950 ), sea surface temperature (SST), and anomaly in mean sea level pressure (MSLP anom ) were probably most impactful in enhancing GR Area using two scoring schemes. Clearings have distinguishing features such as an enhanced Pacific high shifted more towards northern California, offshore air that is warm and dry, stronger coastal surface winds, enhanced lower-tropospheric static stability, and increased subsidence. Although clearings are associated obviously with reduced cloud fraction where they reside, the domain-averaged cloud albedo was actually slightly higher on clearing days as compared to non-clearing days. To validate speculated processes linking environmental parameters to clearing growth rates based on satellite and reanalysis data, airborne data from three case flights were examined. Measurements were compared on both sides of the clear-cloudy border of clearings at multiple altitudes in the boundary layer and free troposphere, with results helping to support links suggested by this study's model simulations. More specifically, airborne data revealed the influence of the coastal low-level jet and extensive horizontal shear at cloud-relevant altitudes that promoted mixing between clear and cloudy air. Vertical profile data provide support for warm and dry air in the free troposphere, additionally promoting expansion of clearings. Airborne data revealed greater evidence of sea salt in clouds on clearing days, pointing to a possible role for, or simply the presence of, this aerosol type in clearing areas coincident with stronger coastal winds., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

This study reports on airborne measurements of stratocumulus cloud properties under varying degrees of influence from biomass burning (BB) plumes off the California coast. Data are reported from five total airborne campaigns based in Marina, California, with two of them including influence from wildfires in different areas along the coast of the western United States. The results indicate that subcloud cloud condensation nuclei number concentration and mass concentrations of important aerosol species (organics, sulfate, nitrate) were better correlated with cloud droplet number concentration ( N d ) as compared to respective above-cloud aerosol data. Given that the majority of BB particles resided above cloud tops, this is an important consideration for future work in the region as the data indicate that the subcloud BB particles likely were entrained from the free troposphere. Lower cloud condensation nuclei activation fractions were observed for BB-impacted clouds as compared to non-BB clouds due, at least partly, to less hygroscopic aerosols. Relationships between N d and either droplet effective radius or drizzle rate are preserved regardless of BB influence, indicative of how parameterizations can exhibit consistent skill for varying degrees of BB influence as long as N d is known. Lastly, the composition of both droplet residual particles and cloud water changed significantly when clouds were impacted by BB plumes, with differences observed for different fire sources stemming largely from effects of plume aging time and dust influence.

This study examines co-located aerosol and precipitation chemistry data between 2010 and 2016 at Pinnacles National Monument ~65 km east of the coastline in central California. Positive matrix factorization analysis of the aerosol composition data revealed seven distinct pollutant sources: aged sea salt (25.7% of PM 2.5 ), biomass burning (24.2% of PM 2.5 ), fresh sea salt (15.0% of PM 2.5 ), secondary sulfate (11.7% of PM 2.5 ), dust (10.0% of PM 2.5 ), vehicle emissions (8.2% of PM 2.5 ), and secondary nitrate (5.2% of PM 2.5 ). The influence of meteorology and transport on monthly patterns of PM 2.5 composition is discussed. Only secondary sulfate exhibited a statistically significant change (a reduction) over time among the PM 2.5 source factors. In contrast, PM coarse exhibited a significant increase most likely due to dust influence. Monthly profiles of precipitation chemistry are summarized showing that the most abundant species in each month was either SO 4 2- , NO 3 - , or Cl - . Intercomparisons between the precipitation and aerosol data revealed several features: (i) precipitation pH was inversely related to factors associated with more acidic aerosol constituents such as secondary sulfate and aged sea salt, in addition to being reduced by uptake of HNO 3 in the liquid phase; (ii) two aerosol source factors (dust and aged sea salt) and PM coarse exhibited a positive association with Ca 2+ in precipitation, suggestive of directly emitted aerosol types with larger sizes promoting precipitation; and (iii) sulfate levels in both the aerosol and precipitation samples analyzed were significantly correlated with dust and aged sea salt PMF factors, pointing to the partitioning of secondary sulfate to dust and sea salt particles. The results of this work have implications for the region's air quality and hydrological cycle, in addition to demonstrating that the use of co-located aerosol and precipitation chemistry data can provide insights relevant to aerosol-precipitation interactions., (Copyright © 2018 Elsevier B.V. All rights reserved.)

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.

This study uses airborne cloud water composition measurements to characterize the vertical structure of air-equivalent mass concentrations of water-soluble species in marine stratocumulus clouds off the California coast. A total of 385 cloud water samples were collected in the months of July and August between 2011 and 2016 and analyzed for water-soluble ionic and elemental composition. Three characteristic profiles emerge: (i) a reduction of concentration with in-cloud altitude for particulate species directly emitted from sources below cloud without in-cloud sources (e.g., Cl - and Na + ), (ii) an increase of concentration with in-cloud altitude (e.g., NO 2 - and formate), and (iii) species exhibiting a peak in concentration in the middle of cloud (e.g., non-sea-salt SO 4 2- , NO 3 - , and organic acids). Vertical profiles of rainout parameters such as loss frequency, lifetime, and change in concentration with respect to time show that the scavenging efficiency throughout the cloud depth depends strongly on the thickness of the cloud. Thin clouds exhibit a greater scavenging loss frequency at cloud top, while thick clouds have a greater scavenging loss frequency at cloud base. The implications of these results for treatment of wet scavenging in models are discussed.

Water samples from marine stratus clouds were collected during 16 aircraft flights above the Pacific Ocean near the Central California coast during the summer of 2016. These samples were analyzed for total mercury (THg), monomethyl mercury (MMHg), and 32 other chemical species in addition to aerosol physical parameters. The mean concentrations of THg and MMHg in the cloudwater samples were 9.2 ± 6.0 ng L -1 (2.3-33.8 ng L -1 ) ( N = 97) and 0.87 ± 0.66 ng L -1 (0.17-2.9 ng L -1 ) ( N = 22), respectively. This corresponds to 9.5% (3-21%) MMHg as a fraction of THg. Low and high nonsea salt calcium ion (nss-Ca 2+ ) concentrations in cloudwater were used to classify flights as "marine" and "continental", respectively. Mean [MMHg] marine was significantly higher ( p < 0.05) than [MMHg] continental consistent with an ocean source of dimethyl Hg (DMHg) to the atmosphere. Mean THg in cloudwater was not significantly different between the two categories, indicating multiple emissions sources. Mean [THg] continental was correlated with pH, CO, NO 3 - , NH 4 + , and other trace metals, whereas [THg] marine was correlated with MMHg and Na + . THg concentrations were negatively correlated with altitude, consistent with ocean and land emissions, coupled with removal at the cloud-top due to drizzle formation.

Airborne measurements of meteorological, aerosol, and stratocumulus cloud properties have been harmonized from six field campaigns during July-August months between 2005 and 2016 off the California coast. A consistent set of core instruments was deployed on the Center for Interdisciplinary Remotely-Piloted Aircraft Studies Twin Otter for 113 flight days, amounting to 514 flight hours. A unique aspect of the compiled data set is detailed measurements of aerosol microphysical properties (size distribution, composition, bioaerosol detection, hygroscopicity, optical), cloud water composition, and different sampling inlets to distinguish between clear air aerosol, interstitial in-cloud aerosol, and droplet residual particles in cloud. Measurements and data analysis follow documented methods for quality assurance. The data set is suitable for studies associated with aerosol-cloud-precipitation-meteorology-radiation interactions, especially owing to sharp aerosol perturbations from ship traffic and biomass burning. The data set can be used for model initialization and synergistic application with meteorological models and remote sensing data to improve understanding of the very interactions that comprise the largest uncertainty in the effect of anthropogenic emissions on radiative forcing.

This study examines major wildfires in the western United States between 2005 and 2015 to determine which species exhibit the highest percent change in mass concentration on day of peak fire influence relative to preceding nonfire days. Forty-one fires were examined using the Environmental Protection Agency (EPA) Interagency Monitoring of Protected Visual Environments (IMPROVE) data set. Organic carbon (OC) and elemental carbon (EC) constituents exhibited the highest percent change increase. The sharpest enhancements were for the volatile (OC1) and semivolatile (OC2) OC fractions, suggestive of secondary organic aerosol formation during plume transport. Of the noncarbonaceous constituents, Cl, P, K, NO 3 - , and Zn levels exhibited the highest percent change. Dust was significantly enhanced in wildfire plumes, based on significant enhancements in fine soil components (i.e., Si, Ca, Al, Fe, and Ti) and PM coarse (i.e., PM 10 -PM 2.5 ). A case study emphasized how transport of wildfire plumes significantly impacted downwind states, with higher levels of fine soil and PM coarse at the downwind state (Arizona) as compared to the source of the fires (California). A global model (Navy Aerosol Analysis and Prediction System, NAAPS) did not capture the dust influence over California or Arizona during this case event because it is not designed to resolve dust dynamics in fires, which motivates improved treatment of such processes. Significant chloride depletion was observed on the peak EC day for almost a half of the fires examined. Size-resolved measurements during two specific fires at a coastal California site revealed significant chloride reductions for particle aerodynamic diameters between 1 and 10 μm.

This work examines particulate chloride (Cl - ) and bromide (Br - ) depletion in marine aerosol particles influenced by wildfires at a coastal California site in the summers of 2013 and 2016. Chloride exhibited a dominant coarse mode due to sea salt influence, with substantially diminished concentrations during fire periods as compared to nonfire periods. Bromide exhibited a peak in the submicrometer range during fire and nonfire periods, with an additional supermicrometer peak in the latter periods. Chloride and Br - depletions were enhanced during fire periods as compared to nonfire periods. The highest observed %Cl - depletion occurred in the submicrometer range, with maximum values of 98.9% (0.32-0.56 μm) and 85.6% (0.56-1 μm) during fire and nonfire periods, respectively. The highest %Br - depletion occurred in the supermicrometer range during fire and nonfire periods with peak depletion between 1.8-3.2 μm (78.8% and 58.6%, respectively). When accounting for the neutralization of sulfate by ammonium, organic acid particles showed the greatest influence on Cl - depletion in the submicrometer range. These results have implications for aerosol hygroscopicity and radiative forcing in areas with wildfire influence owing to depletion effects on composition.