Modeling organic aerosol over Central Europe: Uncertainties linked to different chemical mechanisms, parameterizations, and boundary conditions

Abstract

This study explores the uncertainties in modeling organic aerosol (OA) over Central Europe, focusing on the roles of chemical mechanisms, emission parameterizations, and boundary conditions. Organic aerosols, particularly secondary organic aerosols (SOAs), significantly influence climate, health, and visibility, comprising up to 90 % of submicron particulate matter. Using the Comprehensive Air Quality Model with Extensions (CAMx) coupled with the Weather Research and Forecast Model, sensitivity analyses were conducted to assess the impact of intermediate-volatility organic compounds (IVOCs), semi-volatile organic compounds (SVOCs), and chemical boundary conditions on primary and secondary organic aerosol concentrations. Model evaluation against organic carbon measurements over the Czech Republic showed that including source-specific IVOC and SVOC emissions significantly improved CAMx's performance, particularly when using the 1.5-dimensional Volatility Basis Set framework with activated chemical aging. For example, the domain-averaged SOA concentrations increased by up to 1.17 μg m-3 during summer when both IVOC and SVOC emissions were included. Furthermore, incorporating OA into the boundary conditions enhanced model predictions, with the accuracy of modeled organic carbon concentrations significantly improved during summer at some monitoring sites. Despite these improvements, challenges remain due to uncertainties in emission estimates, parameterization schemes, and the spatial resolution of the models. The findings underscore the importance of refined parameterizations for IVOC and SVOC emissions, higher temporal and spatial resolution in chemical boundary conditions, and better representation of chemical aging. Addressing these gaps in future studies will further enhance the understanding and prediction of OA dynamics in regional air quality modeling.