Anthropogenic amplification of biogenic secondary organic aerosol production

Abstract

Biogenic secondary organic aerosols (SOAs) contribute to a large fraction of fine aerosols globally, impacting air quality and climate. The formation of biogenic SOA depends on not only emissions of biogenic volatile organic compounds (BVOCs) but also anthropogenic pollutants including primary organic aerosol, sulfur dioxide (SO2), and nitrogen oxides (NOx). However, the anthropogenic impact on biogenic SOA production (AIBS) remains unclear. Here we use the decadal trend and variability in observed organic aerosol (OA) in the southeast US, combined with a global chemistry-climate model, to better constrain AIBS. We show that the reduction in SO2 emissions can only explain 40ĝ€¯% of the decreasing decadal trend of OA in this region, constrained by the low summertime month-to-month variability in surface OA. We hypothesize that the rest of the OA decreasing trend is largely due to a reduction in NOx emissions. By implementing a scheme for monoterpene SOA with enhanced sensitivity to NOx, our model can reproduce the decadal trend and variability in OA in this region. Extending to a centennial scale, our model shows that global SOA production increases by 36ĝ€¯% despite BVOC reductions from the preindustrial period to the present day, largely amplified by AIBS. Our work suggests a strong coupling between anthropogenic and biogenic emissions in biogenic SOA production that is missing from current climate models.