Aerosol responses to precipitation along North American air trajectories arriving at Bermuda.

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.

Particulate Oxalate-To-Sulfate Ratio as an Aqueous Processing Marker: Similarity Across Field Campaigns and Limitations.

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.

Contrasting wet deposition composition between three diverse islands and coastal North American sites.

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 SO2 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 Ca2+, NO 3 - , nss K+, nss Na+, nss Mg2+) 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 Ca2+) 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.