Simulation of nitrate, sulfate, and ammonium aerosols over the United States
1Department of Environmental Science and Engineering, California Institute of Technology, Pasadena, California, USA
2Department of Chemical Engineering, California Institute of Technology, Pasadena, California, USA
3Spectroscopie de l'Atmosphère, Service de Chimie Quantique et Photophysique, Université Libre de Bruxelles, Brussels, Belgium
4Université Paris 06, Université Versailles St.-Quentin, CNRS, INSU, LATMOS-IPSL, Paris, France
Abstract. Atmospheric concentrations of inorganic gases and aerosols (nitrate, sulfate, and ammonium) are simulated for 2009 over the United States using the chemical transport model GEOS-Chem. This work is motivated, in part, by the inability of previous modeling studies to reproduce observed high nitrate aerosol concentrations in California. Nitrate aerosol concentrations over most of the US are over-predicted relative to Interagency Monitoring of Protected Visual Environments (IMPROVE) and Clean Air Status and Trends Network (CASTNET) data. In California, on the other hand, nitrate and ammonium are under-predicted as compared to California Air Resources Board (CARB) measurements. Over-prediction of nitrate in the East and Midwest is consistent with results of recent studies, which have suggested that nighttime nitric acid formation by heterogeneous hydrolysis of N2O5 is over-predicted with current values of the N2O5 uptake coefficient, γ, onto aerosols. Accordingly, the value of γ is reduced here by a factor of 10. Despite this, predicted nitrate levels in the US Midwest remain higher than those measured and over-prediction of nitrate in this region remains to be explained. Data from the Infrared Atmospheric Sounding Interferometer (IASI) onboard the MetOp-A satellite indicate the presence of a strong ammonia maximum in central and southern California that is not present in the simulations, which are based on the EPA National Emissions Inventory (NEI) NH3 emission inventory. In order to predict ammonia columns similar to the satellite measurements in the San Joaquin Valley, CA and Riverside, CA, the current ammonia emission inventory in California would need to be increased substantially. Based on the sensitivity of ammonium nitrate formation to the availability of ammonia, the present results suggest that under-prediction of ammonia emissions is likely the main cause for the under-prediction of nitrate aerosol in California.