Acidity variations across the cloud drop size spectrum and their influence on rates of atmospheric sulfate production

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Abstract

Measurements of pH variations within natural cloud drop populations reveal that small drops are often more acidic than large drops. Cloud samples collected from coastal stratus clouds, frontal clouds, and radiation fogs, from heavily polluted and pristine locations, had pH values ranging from below three to more than seven. Differences between small and large cloud drop acidities as large as two pH units were observed, although differences were generally below one pH unit. This chemical heterogeneity can significantly enhance oxidation of sulfur dioxide to sulfate within clouds, relative to oxidation rates predicted from the average cloudwater composition. One‐third of the sampled clouds were estimated to experience an increase of at least 20% in the rate of sulfur oxidation by ozone (8% of the clouds had increases exceeding 100%) as a result of acidity differences between large and small cloud drops. These findings suggest that sulfate production within clouds, a critical component of the global sulfur cycle, may be more rapid than previously thought.

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