High-Resolution Satellite-Derived PM2.5 from Optimal Estimation and Geographically Weighted Regression over North America.

We used a geographically weighted regression (GWR) statistical model to represent bias of fine particulate matter concentrations (PM2.5) derived from a 1 km optimal estimate (OE) aerosol optical depth (AOD) satellite retrieval that used AOD-to-PM2.5 relationships from a chemical transport model (CTM) for 2004-2008 over North America. This hybrid approach combined the geophysical understanding and global applicability intrinsic to the CTM relationships with the knowledge provided by observational constraints. Adjusting the OE PM2.5 estimates according to the GWR-predicted bias yielded significant improvement compared with unadjusted long-term mean values (R(2) = 0.82 versus R(2) = 0.62), even when a large fraction (70%) of sites were withheld for cross-validation (R(2) = 0.78) and developed seasonal skill (R(2) = 0.62-0.89). The effect of individual GWR predictors on OE PM2.5 estimates additionally provided insight into the sources of uncertainty for global satellite-derived PM2.5 estimates. These predictor-driven effects imply that local variability in surface elevation and urban emissions are important sources of uncertainty in geophysical calculations of the AOD-to-PM2.5 relationship used in satellite-derived PM2.5 estimates over North America, and potentially worldwide.

Spatially refined aerosol direct radiative forcing efficiencies.

Global aerosol direct radiative forcing (DRF) is an important metric for assessing potential climate impacts of future emissions changes. However, the radiative consequences of emissions perturbations are not readily quantified nor well understood at the level of detail necessary to assess realistic policy options. To address this challenge, here we show how adjoint model sensitivities can be used to provide highly spatially resolved estimates of the DRF from emissions of black carbon (BC), primary organic carbon (OC), sulfur dioxide (SO(2)), and ammonia (NH(3)), using the example of emissions from each sector and country following multiple Representative Concentration Pathway (RCPs). The radiative forcing efficiencies of many individual emissions are found to differ considerably from regional or sectoral averages for NH(3), SO(2) from the power sector, and BC from domestic, industrial, transportation and biomass burning sources. Consequently, the amount of emissions controls required to attain a specific DRF varies at intracontinental scales by up to a factor of 4. These results thus demonstrate both a need and means for incorporating spatially refined aerosol DRF into analysis of future emissions scenario and design of air quality and climate change mitigation policies.