Trends and drivers of aerosol vertical distribution over China from 2013 to 2020: Insights from integrated observations and modeling.

ABSTRACT

Understanding aerosol vertical distribution is of great importance to climate change and atmospheric chemistry, but there is a dearth of systematical analysis for aerosol vertical distribution amid rapid emission decline after 2013 in China. Here, the GEOS-Chem model and multiple-sourced observations were applied to quantify the changes of aerosol vertical distributions in response to clean air actions. In 2013-2020, the MODIS aerosol optical depth (AOD) presented extensive decreasing trends by -7.9 %/yr to -4.2 %/yr in summer and -6.1 %/yr to -5.8 %/yr in winter in polluted regions. Vertically, the aerosol extinction coefficient (AEC) from CALIPSO decreased by -8.0 %/yr to -5.5 %/yr below ~1 km, but the trends weakened significantly with increasing altitude. Compared with available measurements, the model can reasonably reproduce 2013-2020 trends and seasonality in AOD and vertical AEC. Model simulations confirm that emission reduction was the dominant driver of the 2013-2020 decline in AOD, while the effect of meteorology varied seasonally, with contributions ranging from -2 % to 13 % in summer and -67 % to -2 % in winter. Vertical distributions of emission-driven AEC trends strongly depended on emission reductions, local planetary boundary layer height, and relative humidity. For aerosol components, sulfate accounted for ~50 % of the AOD decline during summer, followed by ammonium and organic aerosol, while in winter the contribution of organic aerosol doubled (24 %-35 %), and nitrate exhibited a weak increasing trend. Chemical production and meteorological conditions (e.g., relative humidity) primarily drove the nitrate contribution, but emission reduction and hygroscopicity were decisive for other components. This work provides an integrated observational and modeling effort to better understand rapid changes in aerosol vertical distribution over China.