1Department of Civil and Environmental Engineering and Department of Earth, Atmospheric and Planetary Sciences, MIT, Cambridge, MA, USA
2Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
3Spectroscopie de l'Atmosphère, Service de Chimie Quantique et Photophysique, Université Libre de Bruxelles, Brussels, Belgium
4UPMC Univ. Paris 06, Université Versailles St-Quentin, CNRS/INSU, LATMOS-IPSL, Paris, France
5Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Canada
6US Environmental Protection Agency, Research Triangle Park, NC, USA
*now at: Earth Observatory of Singapore, Nanyang Technological University, Singapore
Received: 18 Jul 2012 – Discussion started: 06 Aug 2012
Abstract. We use in situ observations from the Interagency Monitoring of PROtected Visual Environments (IMPROVE) network, the Midwest Ammonia Monitoring Project, 11 surface site campaigns as well as Infrared Atmospheric Sounding Interferometer (IASI) satellite measurements with the GEOS-Chem model to investigate inorganic aerosol loading and atmospheric ammonia concentrations over the United States. IASI observations suggest that current ammonia emissions are underestimated in California and in the springtime in the Midwest. In California this underestimate likely drives the underestimate in nitrate formation in the GEOS-Chem model. However in the remaining continental United States we find that the nitrate simulation is biased high (normalized mean bias > = 1.0) year-round, except in Spring (due to the underestimate in ammonia in this season). None of the uncertainties in precursor emissions, the uptake efficiency of N2O5 on aerosols, OH concentrations, the reaction rate for the formation of nitric acid, or the dry deposition velocity of nitric acid are able to explain this bias. We find that reducing nitric acid concentrations to 75% of their simulated values corrects the bias in nitrate (as well as ammonium) in the US. However the mechanism for this potential reduction is unclear and may be a combination of errors in chemistry, deposition and sub-grid near-surface gradients. This "updated" simulation reproduces PM and ammonia loading and captures the strong seasonal and spatial gradients in gas-particle partitioning across the United States. We estimate that nitrogen makes up 15−35% of inorganic fine PM mass over the US, and that this fraction is likely to increase in the coming decade, both with decreases in sulfur emissions and increases in ammonia emissions.
Revised: 18 Oct 2012 – Accepted: 30 Oct 2012 – Published: 06 Nov 2012
Heald, C. L., Collett Jr., J. L., Lee, T., Benedict, K. B., Schwandner, F. M., Li, Y., Clarisse, L., Hurtmans, D. R., Van Damme, M., Clerbaux, C., Coheur, P.-F., Philip, S., Martin, R. V., and Pye, H. O. T.: Atmospheric ammonia and particulate inorganic nitrogen over the United States, Atmos. Chem. Phys., 12, 10295-10312, doi:10.5194/acp-12-10295-2012, 2012.