Modern agricultural practices have greatly increased the emission of ammonia (NH3) to the atmosphere. Recent controls to reduce the emissions of sulfur and nitrogen oxides (SOX and NOX) have increased the importance of understanding the role ammonia plays in the formation of surface fine inorganic particulate matter (PM2.5) in the United States. In this study, we identify the interannual variability in ammonia concentration, explore the sources of this variability and determine their contribution to the variability in surface PM2.5 concentration. Over the summers of 2008-2012, measurements from the Ammonia Monitoring Network (AMoN) and the Infrared Atmospheric Sounding Interferometer (IASI) satellite instrument show considerable variability in both surface and column ammonia concentrations (+/- 29% and 28% of the mean), respectively. This observed variability is larger than that simulated by the GEOS-Chem chemical transport model, where meteorology dominates the variability in ammonia and PM2.5 concentrations compared to the changes caused by SOX and NOX reductions. Our initial simulation does not include year-to-year changes in ammonia agricultural emissions. We use county-wide information on fertilizer sales and livestock populations, as well as meteorological variations to account for the interannual variability in agricultural activity and ammonia volatilization. These sources of ammonia emission variability are important for replicating observed variations in ammonia and PM2.5, highlighting how accurate ammonia emissions characterization is central to PM air quality prediction.