Contrast in Secondary Organic Aerosols between the Present Day and the Preindustrial Period: The Importance of Nontraditional Sources and the Changed Atmospheric Oxidation Capability

Abstract

Quantifying differences in secondary organic aerosols (SOAs) between the preindustrial period and the present day is crucial to assess climate forcing and environmental effects resulting from anthropogenic activities. The lack of vegetation information for the preindustrial period and the uncertainties in describing SOA formation are two leading factors preventing simulation of SOA. This study calculated the online emissions of biogenic volatile organic compounds (VOCs) in the Aerosol and Atmospheric Chemistry Model of the Institute of Atmospheric Physics (IAP-AACM) by coupling the Model of Emissions of Gases and Aerosols from Nature (MEGAN), where the input vegetation parameters were simulated by the IAP Dynamic Global Vegetation Model (IAP-DGVM). The volatility basis set (VBS) approach was adopted to simulate SOA formation from the nontraditional pathways, i.e., the oxidation of intermediate VOCs and aging of primary organic aerosol. Although biogenic SOAs (BSOAs) were dominant in SOAs globally in the preindustrial period, the contribution of nontraditional anthropogenic SOAs (ASOAs) to the total SOAs was up to 35.7%. In the present day, the contribution of ASOAs was 2.8 times larger than that in the preindustrial period. The contribution of nontraditional sources of SOAs to SOA was as high as 53.1%. The influence of increased anthropogenic emissions in the present day on BSOA concentrations was greater than that of increased biogenic emission changes. The response of BSOA concentrations to anthropogenic emission changes in the present day was more sensitive than that in the preindustrial period. The nontraditional sources and the atmospheric oxidation capability greatly affect the global SOA change.