Estimates of black carbon emissions in the western United States using the GEOS-Chem adjoint model

摘要

We estimate black carbon (BC) emissions in the western United States for July-September 2006 by inverting surface BC concentrations from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network using a global chemical transport model (GEOS-Chem) and its adjoint. Our best estimate of the BC emissions is 49.9 Gg at 2 degrees x 2.5 degrees (a factor of 2.1 increase) and 47.3 Gg at 0.5 degrees x 0.667 degrees (1.9 times increase). Model results now capture the observed major fire episodes with substantial bias reductions (similar to 35% at 2 degrees x 2.5 degrees and similar to 15% at 0.5 degrees x 0.667 degrees). The emissions are similar to 20-50% larger than those from our earlier analytical inversions (Mao et al., 2014). The discrepancy is especially drastic in the partitioning of anthropogenic versus biomass burning emissions. The August biomass burning BC emissions are 4.6-6.5 Gg and anthropogenic BC emissions 8.6-12.8 Gg, varying with the model resolution, error specifications, and subsets of observations used. On average both anthropogenic and biomass burning emissions in the adjoint inversions increase 2-fold relative to the respective a priori emissions, in distinct contrast to the halving of the anthropogenic and tripling of the biomass burning emissions in the analytical inversions. We attribute these discrepancies to the inability of the adjoint inversion system, with limited spatiotemporal coverage of the IMPROVE observations, to effectively distinguish collocated anthropogenic and biomass burning emissions on model grid scales. This calls for concurrent measurements of other tracers of biomass burning and fossil fuel combustion (e.g., carbon monoxide and carbon isotopes). We find that the adjoint inversion system as is has sufficient information content to constrain the total emissions of BC on the model grid scales.