Numerical simulation of the interaction between ammonium nitrate aerosol and convective boundary-layer dynamics

Abstract

We investigate the interaction between the ammonium nitrate aerosol ((NO3)-N-A) abundance and convective boundary-layer (CBL) dynamics by means of a large-eddy simulation (LES) framework In our LES model the CBL dynamics is solved coupled with radiation, chemistry, and surface exchange. Concerning the aerosol coupling we assume a simplified representation that accounts for black carbon, aerosol water and inorganic aerosols, focusing on the semi-volatile ammonium nitrate aerosol within the CBL. The aerosol absorption and scattering of shortwave radiation is also taken into consideration. We use a data set of observations taken at the Cabauw Experimental Site for Atmospheric Research during the IMPACT/EUCAARI (European Integrated Project on Aerosol, Cloud, Climate, and Air Quality Interactions) campaign to successfully evaluate our LES approach. We highlight that our LES framework reproduces the observations of the ratio between gas-phase nitrate and total nitrate at the surface, with a diurnally-averaged overestimation of only approximate to 12%. We show that the dependence between gas-aerosol conversion of nitrate and CBL (thermo)dynamics produces highly non-linear concentration and turbulent flux vertical profiles. The flux profiles maximize at around 1/3 of the CBL. Close to the surface, we show that the outgassing of (NO3)-N-A affects the dry deposition of nitrate. This outgassing is responsible for the high deposition velocities obtained from the concentration and flux measurements during observational campaigns. To account for the influence of CBL (thermo)dynamics on gas-aerosol conversion we propose an effective turbulent exchange coefficient based on an analysis of the flux budget equation of aerosol nitrate calculated by our LES. The implementation of this effective turbulent exchange coefficient in a 1D model leads to a better agreement with the LES results and with surface observations. (C) 2015 Elsevier Ltd. All rights reserved.