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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.

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.