Contrasting seasonal responses of sulfate aerosols to declining SO2 emissions in the Eastern US: Implications for the efficacy of SO2 emission controls

Stringent controls have reduced U.S. SO2 emissions by over 60% since the late 1990s. These controls have been more effective at reducing surface SO42- in summer (June, July, and August) than in winter (December, January, and February (DJF)), a seasonal contrast that is not robustly captured by Climate Model Intercomparison Project 5 global models. We use the Geophysical Fluid Dynamics Laboratory AM3 chemistry-climate model to show that oxidant limitation during winter causes SO42- (DJF) to be sensitive to primary SO42- emissions, in-cloud titration of H2O2, and in-cloud oxidation by O-3. The observed contrast in the seasonal response of SO42- to decreasing SO2 emissions is best explained by the O-3 reaction, whose rate coefficient has increased over the past decades as a result of increasing NH3 emissions and decreasing SO2 emissions, both of which lower cloud water acidity. The fraction of SO2 oxidized to SO42- is projected to keep increasing in future decades, delaying improvements in wintertime air quality.