Explosive formation of secondary organic aerosol due to aerosol-fog interactions

Abstract

Aerosol particles can profoundly affect the local environment and global climate. Explosive growths of secondary organic aerosol (SOA) are frequently observed during serious haze evens, but their fundamental mechanism remains unclear. We used chamber experiments and kinetic model simulations to reveal the microphysical mechanism for explosive organic aerosol formation. The evolution of SOA with organic vapors under dry and highly humid conditions was determined based on a high-resolution Orbitrap mass spectrometer. We found that the condensation of gas-phase organics could lead to the formation of cloud or fog droplets with relative humidity below 100 %; meanwhile, the aerosol-fog interaction could result in the explosive growth of SOA. Monomeric products from toluene oxidation were verified to primarily contribute to the increased SOA in super humid conditions, which are mainly assigned to be intermediate- and semi-volatile organic compounds. Moreover, we demonstrated that the decreasing temperatures could dramatically amplify organic compounds' co-condensing influence on SOA explosive formation and activation at relative humidity above 85 % and temperature below 20 °C. Our findings revealed that aerosol-fog interaction is the fundamental driving force for explosive organic aerosol formation. It indicates that overlooking the co-condensation of organic vapors with water could significantly underestimate SOA and liquid water content in 3D models.