SO2 emissions and lifetimes: Estimates from inverse modeling using in situ and global, space-based (SCIAMACHY and OMI) observations

Top-down constraints on global sulfur dioxide (SO2) emissions are inferred through inverse modeling using SO2 column observations from two satellite instruments (SCIAMACHY and OMI). We first evaluated the SO2 column observations with surface SO2 measurements by applying local scaling factors from a global chemical transport model (GEOS-Chem) to SO2 columns retrieved from the satellite instruments. The resulting annual mean surface SO2 mixing ratios for 2006 exhibit a significant spatial correlation (r = 0.86, slope = 0.91 for SCIAMACHY and r = 0.80, slope = 0.79 for OMI) with coincident in situ measurements from monitoring networks throughout the United States and Canada. We evaluate the GEOS-Chem simulation of the SO2 lifetime with that inferred from in situ measurements to verify the applicability of GEOS-Chem for inversion of SO2 columns to emissions. The seasonal mean SO2 lifetime calculated with the GEOS-Chem model over the eastern United States is 13 h in summer and 48 h in winter, compared to lifetimes inferred from in situ measurements of 19 +/- 7 h in summer and 58 +/- 20 h in winter. We apply SO2 columns from SCIAMACHY and OMI to derive a top-down anthropogenic SO2 emission inventory over land by using the local GEOS-Chem relationship between SO2 columns and emissions. There is little seasonal variation in the top-down emissions (< 15%) over most major industrial regions providing some confidence in the method. Our global estimate for annual land surface anthropogenic SO2 emissions (52.4 Tg S yr(-1) from SCIAMACHY and 49.9 Tg S yr(-1) from OMI) closely agrees with the bottom-up emissions (54.6 Tg S yr(-1)) in the GEOS-Chem model and exhibits consistency in global distributions with the bottom-up emissions (r = 0.78 for SCIAMACHY, and r = 0.77 for OMI). However, there are significant regional differences.