New positive feedback mechanism between boundary layer meteorology and secondary aerosol formation during severe haze events

摘要

Severe haze events during which particulate matter (PM) increases quickly from tens to hundreds of microgram per cubic meter in 1–2 days frequently occur in China. Although it has been known that PM is influenced by complex interplays among emissions, meteorology, and physical and chemical processes, specific mechanisms remain elusive. Here, a new positive feedback mechanism between planetary boundary layer (PBL), relative humidity (RH), and secondary PM (SPM) formation is proposed based on a comprehensive field experiment and model simulation. The decreased PBL associated with increased PM increases RH by weakening the vertical transport of water vapor; the increased RH in turn enhances the SPM formation through heterogeneous aqueous reactions, which further enhances PM, weakens solar radiation, and decreases PBL height. This positive feedback, together with the PM-Radiation-PBL feedback, constitutes a key mechanism that links PM, radiation, PBL properties (e.g. PBL height and RH), and SPM formation, This mechanism is self-amplifying, leading to faster PM production, accumulation, and more severe haze pollution.