Cloud Chemistry in the United States: Problems and Prospects

Clouds cover 60% of the Earth's surface at a given time and are the primary means by which atmospheric trace species are lofted from the polluted boundary layer to the free troposphere. Clouds also play an important role as atmospheric aqueous phase reactors, scavenging soluble gas phase precursors and providing a medium for oxidation reactions that yield lower volatility products that contribute to increased aerosol mass when cloud drops evaporate. On a global average, most sulfate particles are formed during cloud processing, and organic particles known to form through aqueous phase pathways are found above clouds. However, atmospheric chemistry observations are generally biased for clear sky conditions. For example, aircraft field deployments typically avoid clouds. Satellite retrievals impacted by clouds are often screened from the final data products. This hinders knowledge of cloud chemistry and the impacts on tropospheric composition. In this work, we explore temporal and geospatial trends in trace species related to cloud processing in the U.S. with a focus on organic chemistry. We apply 3-dimensional and 0-dimensional models to recent campaigns and mountaintop cloud sampling sites, and compare to measurements.