Global modeling of heterogeneous chemistry on mineral aerosol surfaces: Influence on tropospheric ozone chemistry and comparison to observations

Abstract

Mineral aerosols can affect gas phase chemistry in the troposphere by providing reactive sites for heterogeneous reactions. We present here a global modeling study of the influence of mineral dust on the tropospheric photochemical cycle. This work is part of the Mineral Dust and Tropospheric Chemistry (MINATROC) project, which focussed on measurement campaigns, laboratory experiments, and integrative modeling. The laboratory experiments provide uptake coefficients for chemical species on mineral aerosol surfaces, which are used to compute the heterogeneous reaction rates in the model. The field measurements at Mount Cimone, northern Italy, provide trace gas and aerosol measurements during a Saharan dust episode and are used to evaluate the model. The simulations include the reactions between mineral dust aerosols and the gas‐phase species O3, HNO3, NO3, and N2O5. Under the conditions for the year 2000 the model simulates a decrease in global tropospheric ozone mass by about 5% due to the heterogeneous reactions on dust aerosols. The most important heterogeneous reaction is the uptake of HNO3 on the dust surface, whereby the direct uptake of ozone on dust is not important in atmospheric chemistry. The comparison of the model results to observations indicates that the model simulates well the aerosol mass transported into the Mediterranean during the dust events and the arrival of all major dust events that were observed during a 7 month period. The decrease in ozone concentration during dust events is better simulated by the model when the heterogeneous reactions are included.