Numerical simulation of the interaction between ammonium nitrate aerosol and convective boundary-layer dynamics. (March 2015)

• Record Type: Journal Article
• Authors: Barbaro, E.; Krol, M.C.; Vilà-Guerau de Arellano, J.
• Is Part Of: Atmospheric environment. Volume 105(2015)
• Page Start: 202
• Page End: 211
• Publication Date: 2015-03
• Subjects: Gas-aerosol conversion -- Convective boundary-layer dynamics -- Aerosol nitrate deposition -- Reactive turbulent exchange coefficient -- Large-Eddy simulation; Air -- Pollution -- Periodicals; Air -- Pollution -- Meteorological aspects -- Periodicals; 551.51
• DOI: 10.1016/j.atmosenv.2015.01.048
• Languages: English
• ISSNs: 1352-2310

Abstract

Abstract: We investigate the interaction between the ammonium nitrate aerosol ( N A O 3 ) 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 ≈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 N A O 3 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. Highlights: Using a LES model we find a strong interaction between 3D-turbulence and A NO3 . The apparent deposition of A NO3 is larger for shorter equilibration timescales. The transport of A NO3 in 1D models needs a larger exchange coefficient than heat.