Improving the representation of secondary organic aerosol (SOA) in the MOZART-4 global chemical transport model
Abstract. The secondary organic aerosol (SOA) module in the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) was updated by replacing existing two-product (2p) parameters with those obtained from two-product volatility basis set (2p-VBS) fits (MZ4-C1), and by treating SOA formation from the following additional volatile organic compounds (VOCs): isoprene, propene and lumped alkenes (MZ4-C2). Strong seasonal and spatial variations in global SOA distributions were demonstrated, with significant differences in the predicted concentrations between the base case and updated model simulations. Updates to the model resulted in significant increases in annual average SOA mass concentrations, particularly for the MZ4-C2 simulation in which the additional SOA precursor VOCs were treated. Annual average SOA concentrations predicted by the MZ4-C2 simulation were 1.00 ± 1.04 μg m−3 in South America, 1.57 ± 1.88 μg m−3 in Indonesia, 0.37 ± 0.27 μg m−3 in the USA, and 0.47 ± 0.29 μg m−3 in Europe with corresponding increases of 178, 406, 311 and 292% over the base-case simulation, respectively, primarily due to inclusion of isoprene. The increases in predicted SOA mass concentrations resulted in corresponding increases in SOA contributions to annual average total aerosol optical depth (AOD) by ~ 1–6%. Estimated global SOA production was 5.8, 6.6 and 19.1 Tg yr−1 with corresponding burdens of 0.22, 0.24 and 0.59 Tg for the base-case, MZ4-C1 and MZ4-C2 simulations, respectively. The predicted SOA budgets fell well within reported ranges for comparable modeling studies, 6.7 to 96 Tg yr−1, but were lower than recently reported observationally constrained values, 50 to 380 Tg yr−1. For MZ4-C2, simulated SOA concentrations at the surface also were in reasonable agreement with comparable modeling studies and observations. Total organic aerosol (OA) mass concentrations at the surface, however, were slightly over-predicted in Europe, Amazonian regions and Malaysian Borneo (Southeast Asia) during certain months of the year, and under-predicted in most sites in Asia; relative to those regions, the model performed better for sites in North America. Overall, with the inclusion of additional SOA precursors (MZ4-C2), namely isoprene, MOZART-4 showed consistently better skill (NMB (normalized mean bias) of −11 vs. −26%) in predicting total OA levels and spatial distributions of SOA as compared with unmodified MOZART-4. Treatment of SOA formation by these known precursors (isoprene, propene and lumped alkenes) may be particularly important when MOZART-4 output is used to generate boundary conditions for regional air quality simulations that require more accurate representation of SOA concentrations and distributions.