Evaluating Ammonium, Nitrate and Sulfate Aerosols in 3-Dimensions

Abstract:

The spatial distribution of aerosols and their chemical composition dictates whether they would have a cooling or a warming effect on the climate system. Hence, properly modeling the 3-dimensonal distribution of aerosols is a crucial step for coherent climate simulations. Since surface networks only give 2-D data, and most satellites supply integrated column information, it is thus important to integrate aircraft measurements in climate model evaluation. In this study, the vertical distribution of ammonium, nitrate, and sulfate, is constrained against a collection of 14 AMS flight campaigns, and surface measurements from 2000-2010 in the USA and Europe. GISS modelE2, one of the only models to include nitrate aerosol in CIMP5, is used with multiple aerosol microphysics (MATRIX, OMA) and thermodynamic (ISORROPIA-II, EQSAM) configurations. Our results show that the MATRIX microphysical scheme improves the model performance for sulfate and that there is a systematic underestimation of ammonium and nitrate over the USA and Europe. In terms of gaseous precursors, underestimation of nitrate and ammonium is likely tied to ammonia emissions uncertainties, while nitric acid concentrations are largely overestimated in the higher levels of the model, influenced by strong strat-trop exchange. At high altitudes, nitrate formation is calculated to be ammonia limited, whose profile measurements are scarce.