The Significant Contribution of Small-Sized and Spherical Aerosol Particles to the Decreasing Trend in Total Aerosol Optical Depth over Land from 2003 to 2018

The optical and microphysical properties of aerosols remain one of the greatest uncertainties associated with evaluating the climate forcing attributed to aerosols.Although the trends in aerosol optical depth(AOD)at global and regional scales have been widely examined,little attention has been paid to the trends in type-dependent AODs related to aerosol particle properties.Here,using the aerosol optical component dataset from the Multi-angle Imaging SpectroRadiometer(MISR)instrument,we investigate decadal-scale trends in total aerosol loading as well as AODs for five aerosol components by particle size and morphology during 2003–2018 over land.Relationships between the total AOD(TAOD)trends and type-dependent AOD changes were examined,and the relative contribution of each type-dependent AOD to the overall TAOD trends was quantified.By dividing the TAOD values into four different aerosol pollution levels(APLs)with splits at 0.15,0.40,and 0.80,we further explored the relationships between TAOD changes and interannual variations in the frequency-of-occurrences(FoOs)of these APLs.Long-term trends in FoOs in the different APLs show that there was a significant improvement in air quality between 2003 and 2018 in most land areas,except South Asia,corresponding to a shift from lightly polluted to clean conditions.However,the effects of different APLs on TAOD changes are regionally dependent and their extent of correlation varied spatially.Moreover,we observed that the annual mean TAOD has decreased by 0.47%.a^(-1)over land since 2003(P<0.05).This significant reduction was mainly attributed to the continued reduction in small-sized(<0.7 mm diameter)AOD(SAOD)(-0.74%.a^(-1))and spherical AOD(SPAOD)(-0.46%.a^(-1)).Statistical analysis shows that SAOD and SPAOD respectively accounted for 57.5%and 89.6%of the TAOD,but contributed 82.6%and 90.4%of the trend in TAOD.Our study suggests that small-sized and spherical aerosols composed of sulfate,organic matter,and black carbon play a dominant role in determining interannual variability in land TAOD.