Abstract

Observed surface organic aerosols (OA) concentrations slightly increased in the western US (WUS) but significantly decreased in the eastern US (EUS) in summer, and continuously decreased in winter over the US region. To understand the driving factors for the long-term surface OA trend, we apply a... Show moreObserved surface organic aerosols (OA) concentrations slightly increased in the western US (WUS) but significantly decreased in the eastern US (EUS) in summer, and continuously decreased in winter over the US region. To understand the driving factors for the long-term surface OA trend, we apply a revised version of the Community Atmosphere Model version 6 with comprehensive tropospheric and stratospheric chemistry representation, considering the heterogeneous formation of isoprene-epoxydiol-derived secondary organic aerosols (SOAIE) and fast photolysis rate of monoterpene-derived secondary organic aerosols (MTSOA) to diagnose the OA evolution in 1988-2019. Compared to older versions, the revised model better reproduces the climatology, seasonal cycle, and long-term trend of surface OA as evaluated against the Interagency Monitoring of Protected Visual Environments measurements. We find the decrease in EUS summertime OA is likely attributed to the interplay between SOAIE and MTSOA. With anthropogenic emissions reduction, primary organic aerosols (POA) declined, SOAIE decreased along with sulfate, while MTSOA increased along with biogenic emissions driven by a warming climate. POA from wildfires with a significant trend of 2.9% yr(-1) and considerable interannual variation of 62.8% drive the statistically insignificant but increasing WUS summertime OA, while anthropogenic POA dominates the decreasing wintertime OA in the US. Through sensitivity experiments, we find MTSOA show linear responses to the increasing monoterpenes emissions and negligible responses to NOx emissions reduction due to the mutual offsets between MTSOA components from different oxidation pathways. This study reveals the increasingly important role of MTSOA in summertime OA under a warming climate. Show less