Natural and transboundary pollution influences on sulfate-nitrate-ammonium aerosols in the United States: implications for policy

We use a global three-dimensional coupled oxidant-aerosol model (GEOS-CHEM) to estimate natural and transboundary pollution influences on sulfate-nitrate-ammonium aerosol concentrations in the United States. This work is motivated in part by the Regional Haze Rule of the U.S. Environmental Protection Agency (EPA), which requires immediate action to improve visibility in U.S. wilderness areas along a linear trajectory toward an endpoint of ‘‘natural visibility conditions’’ by 2064. We present full-year simulations for 1998 and 2001 and evaluate them with nationwide networks of observations in the United States and Europe (Interagency Monitoring of Protected Visual Environments (IMPROVE), Clean Air Status and Trends Network (CASTNET), National Atmospheric Deposition Program (NADP), European Monitoring and Evaluation Programme (EMEP)) and with Asian outflow observations from the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission. Shutting off U.S. anthropogenic emissions in the model defines ‘‘background’’ aerosol concentrations representing contributions from both natural and transboundary pollution sources. We find that transboundary transport of pollution from Canada, Mexico, and Asia dominates over natural influences for both sulfate and nitrate. Trans-Pacific transport of Asian pollution accounts for 30% of background sulfate in both the western and eastern United States. Our best estimates of natural concentrations for ammonium sulfate and ammonium nitrate in the United States are either consistent with or lower than the default values recommended by EPA for natural visibility calculations. However, the large transboundary pollution influence in our calculation suggests that a natural visibility objective cannot be approached without international emission controls.