Enhanced daytime secondary aerosol formation driven by gas-particle partitioning in downwind urban plumes

Abstract

Abstract. Anthropogenic emissions from city clusters can significantly enhance secondary organic aerosol (SOA) formation in the downwind regions, while the mechanism is poorly understood. To investigate the effect of pollutants within urban plumes on organic aerosol (OA) evolution, a field campaign was conducted at a downwind site of the Pearl River Delta region of China in the fall of 2019. A time-of-flight chemical ionization mass spectrometer coupled with a Filter Inlet for Gases and Aerosol (FIGAERO-CIMS) was used to probe the gas- and particle-phase molecular composition and thermograms of organic compounds. For air masses influenced by urban pollution, strong daytime SOA formation through gas-particle partitioning was observed, resulting in higher OA volatility. The obvious SOA enhancement was mainly attributed to the equilibrium partitioning of non-condensable (C * ≥ 100.5 μg m-3) organic vapors. We speculated that the elevated NOx concentration could suppress the formation of highly oxidized products, resulting in a smooth increase of condensable (C * < 100.5 μg m-3) organic vapors. Evidence showed that urban pollutants (NOx and VOCs) could enhance the oxidizing capacity, while the elevated VOCs was mainly responsible for promoting daytime SOA formation by increasing the RO2 production rate. Our results highlight the important role of urban anthropogenic pollutants in SOA control in the suburban region.