21st Century Change in Global Small-Size Aerosols from Combustion Emissions

Abstract

Changes in aerosol optical depth, both positive and negative, are observed across the globe during the 21rst Century. However, attribution of these changes to specific sources is largely uncertain as there are multiple contributing natural and anthropogenic sources that produce aerosols either directly or through secondary chemical reactions. Here we show that satellite-based changes in small-mode AOD between 2002 and 2019 observed in data from MISR can primarily be explained by changes, either directly or indirectly, in combustion emissions. We quantify combustion emissions using MOPITT total column CO observations and the adjoint of the GEOS-Chem global chemistry and transport model. The a priori fire emissions are taken from the Global Fire Emission Data base with small fires (GFED4s) but with fixed a priori for non-fire emissions. Aerosol precursor and direct emissions are updated by re-scaling them with the monthly ratio of the CO posterior to prior emissions. The correlation between modeled and observed AOD improves from a mean of 0.15 to 0.81 for the four industrial regions considered and from 0.52 to 0.75 for the four wildfire-dominant regions considered. Using these updated emissions in the GEOS-Chem global chemistry transport model, our results indicate that surface PM2.5 have declined across many regions of the globe during the 21rst century. For example, PM2.5 over China has declined by ~30% with smaller fractional declines in E. USA and Europe (from fossil emissions) and in S. America (from fires). These results highlight the importance of forest management and cleaner combustion sources in improving air-quality.