Atmos. Chem. Phys. Discuss., 8, 6469-6499, 2008
www.atmos-chem-phys-discuss.net/8/6469/2008/
doi:10.5194/acpd-8-6469-2008
© Author(s) 2008. This work is distributed
under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
A method for evaluating spatially-resolved NOx emissions using Kalman filter inversion, direct sensitivities, and space-based NO2 observations
S. L. Napelenok1, R. W. Pinder1, A. B. Gilliland1, and R. V. Martin2,3
1Atmospheric 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
2Department of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, Canada
3Harvard-Smithsonian Center for Astrophysics, Cambridge, MA, USA

Abstract. 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 NOx 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 NOx 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 NOx aloft. Therefore, the best correlation between satellite observations and modeled NO2 column densities, as well as comparison to ground-level observations of NO2, was obtained from performing the inverse while accounting for the significant presence of NO2 in the upper troposphere not captured by the regional model.

Citation: Napelenok, S. L., Pinder, R. W., Gilliland, A. B., and Martin, R. V.: A method for evaluating spatially-resolved NOx emissions using Kalman filter inversion, direct sensitivities, and space-based NO2 observations, Atmos. Chem. Phys. Discuss., 8, 6469-6499, doi:10.5194/acpd-8-6469-2008, 2008.
 
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