An improved framework for efficiently modeling organic aerosol (OA) considering primary OA evaporation and secondary OA formation from VOCs, IVOCs, and SVOCs†

Abstract

Organic aerosols (OA) constitute an important fraction of fine particulate matter (PM_2.5) air pollution, yet accurate and efficient OA modeling within chemical transport models (CTM) remains a challenge. Volatility basis set (VBS) schemes for OA have demonstrated improved performance in simulating OA, particularly for primary organic aerosol (POA), but their computational complexity impedes application to advanced modeling tasks, such as detailed source apportionment. Conversely, simpler “two-product” schemes are efficient and compatible with source apportionment techniques but many of them tend to overestimate POA by treating it as non-volatile. Either VBS or 2-product schemes can perform well for secondary organic aerosol (SOA) depending upon the data and assumptions used to model SOA formation from precursors. In this study, we update the Comprehensive Air Quality Model with extensions (CAMx) “SOAP” 2-product modeling framework by (1) treating POA as semivolatile using an efficient scheme, (2) adding SOA formation from semivolatile organic compounds (SVOCs), and (3) adopting SOA yields derived from the widely-used Community Multiscale Air Quality (CMAQ) AERO7 scheme. The first update allows temperature-dependent partial evaporation of POA to SVOC, which is subsequently oxidized in the gas phase. For the latter two updates, SOA yields are updated to emulate the AERO7 scheme based on an offline conceptual model. We implemented these changes within the existing SOAP2 scheme of CAMx to create a new scheme called “SOAP3”. A series of CTM simulations were conducted with the SOAP3 scheme to simulate OA and its components in China during July and November 2018. Results were validated against surface observations and compared to the SOAP2 and AERO7 schemes. Compared to SOAP2, SOAP3 substantially reduced POA proportions (by 10–24%) and increased SOA concentrations (by 45–193%) for selected regions. SOAP3 performs more like the AERO7 scheme than SOAP2 in terms of the simulated OA components and improved accuracy compared to observations. Uncertainties and limitations of the current SOAP3 scheme are also discussed. Our study demonstrates a feasible and readily implemented methodology for improving two-product OA modeling, which is currently employed in many CTMs.