Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 8 2 2008 10.5194/acpd-8-6469-2008 http://www.atmos-chem-phys-discuss.net/8/6469/2008/ http://www.atmos-chem-phys-discuss.net/8/6469/2008/acpd-8-6469-2008.html http://www.atmos-chem-phys-discuss.net/8/6469/2008/acpd-8-6469-2008.pdf 6469 6499 2008-04-01 A method for evaluating spatially-resolved NO_x emissions using Kalman filter inversion, direct sensitivities, and space-based NO₂ observations S. L. Napelenok napelenok.sergey@epa.gov R. W. Pinder A. B. Gilliland R. V. Martin Atmospheric Sciences Modeling Division, Air Resources Laboratory, National Oceanic and Atmospheric Administration, in partnership with the United States Environmental Protection Agency, 109 T.W. Alexander Drive, Research Triangle Park, NC 27711, USA Department of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, Canada Harvard-Smithsonian Center for Astrophysics, Cambridge, MA, USA An inverse modeling method was developed and tested for identifying possible biases in emission inventories using satellite observations. The relationships between emission inputs and modeled ambient concentrations were estimated using sensitivities calculated with the decoupled direct method in three dimensions (DDM-3D) implemented within the framework of the Community Multiscale Air Quality (CMAQ) regional model. As a case study to test the approach, the method was applied to regional ground-level NO_x emissions in the southeastern United States as constrained by the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) satellite derived observations of NO₂ column densities. A controlled "pseudodata" scenario with a known solution was used to establish that the methodology can achieve the correct solution, and the approach was then applied to a summer 2004 period where the satellite data are available. The results indicate that emissions biases differ in urban and rural areas of the southeast. The method suggested slight downward (less than 10%) adjustment to urban emissions, while rural region results were found to be highly sensitive to NO_x processes in the upper troposphere. As such, the bias in the rural areas is likely not solely due to biases in the ground-level emissions. It was found that CMAQ was unable to predict the significant level of NO₂ in the upper troposphere that was observed during the NASA Intercontinental Chemical Transport Experiment (INTEX) measurement campaign. The reasons for the underestimation likely include combination of a lack of lightning emissions and a short modeled lifetime of NO_x aloft. 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