A method for evaluating spatially-resolved NO x emissions using Kalman filter inversion, direct sensitivities, and space-based NO 2 observations

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 observations of NO 2 column densities derived from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) satellite instrument. 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 NO 2 in the upper troposphere that was observed during the NASA Intercontinental Chemical Transport Experiment (INTEX) measurement campaign. The best correlation between satellite observations and modeled NO 2 column densities, as well as comparison to ground-level observations of NO 2 , was obtained by performing the inverse while accounting for the significant presence of NO 2 in the upper troposphere not captured by the regional model.

[1]  Kelly Chance,et al.  Global partitioning of NOx sources using satellite observations: relative roles of fossil fuel combustion, biomass burning and soil emissions. , 2005, Faraday discussions.

[2]  John H. Seinfeld,et al.  Inverse air pollution modelling of urban-scale carbon monoxide emissions , 1995 .

[3]  James F. Gleason,et al.  Algorithm for NO/sub 2/ vertical column retrieval from the ozone monitoring instrument , 2006, IEEE Transactions on Geoscience and Remote Sensing.

[4]  H. Christopher Frey,et al.  Uncertainties in predicted ozone concentrations due to input uncertainties for the UAM-V photochemical grid model applied to the July 1995 OTAG domain , 2001 .

[5]  Armistead G Russell,et al.  Nonlinear response of ozone to emissions: source apportionment and sensitivity analysis. , 2005, Environmental science & technology.

[6]  Steffen Beirle,et al.  Weekly cycle of NO 2 by GOME measurements: a signature of anthropogenic sources , 2003 .

[7]  A. M. Dunker,et al.  Implementing the decoupled direct method for sensitivity analysis in a particulate matter air quality model. , 2007, Environmental science & technology.

[8]  John P. Burrows,et al.  Satellite‐observed U.S. power plant NOx emission reductions and their impact on air quality , 2006 .

[9]  Gary A. Morris,et al.  Large upper tropospheric ozone enhancements above midlatitude North America during summer: In situ evidence from the IONS and MOZAIC ozone measurement network , 2006 .

[10]  A. M. Dunker.  The decoupled direct method for calculating sensitivity coefficients in chemical kinetics , 1984 .

[11]  F. Fehsenfeld,et al.  An efficient photolysis system for fast-response NO2 measurements , 2000 .

[12]  John P. Burrows,et al.  Satellite measurement based estimates of decadal changes in European nitrogen oxides emissions , 2008 .

[13]  Alan Fried,et al.  Surface and Lightning Sources of Nitrogen Oxides over the United States: Magnitudes, Chemical Evolution, and Outflow , 2007 .

[14]  D. Byun,et al.  Review of the Governing Equations, Computational Algorithms, and Other Components of the Models-3 Community Multiscale Air Quality (CMAQ) Modeling System , 2006 .

[15]  Christian Hogrefe,et al.  Dynamic evaluation of regional air quality models: Assessing changes in O3 stemming from changes in emissions and meteorology , 2008 .

[16]  R. Martin,et al.  Seasonal variability of NOx emissions over east China constrained by satellite observations: Implications for combustion and microbial sources , 2007 .

[17]  Trissevgeni Stavrakou,et al.  Inversion of CO and NO x emissions using the adjoint of the IMAGES model , 2004 .

[18]  Ronald G. Prinn,et al.  Feasibility of determining surface emissions of trace gases using an inverse method in a three‐dimensional chemical transport model , 1993 .

[19]  H. Rabitz,et al.  Sensitivity analysis of the atmospheric reaction-diffusion equation , 1987 .

[20]  D. Blake,et al.  Direct Measurements of the Convective Recycling of the Upper Troposphere , 2007, Science.

[21]  Philip B. Russell,et al.  Overview of the Summer 2004 Intercontinental Chemical Transport Experiment–North America (INTEX-A) , 2006 .

[22]  M. Buchwitz,et al.  SCIAMACHY: Mission Objectives and Measurement Modes , 1999 .

[23]  Eugene P. Dougherty,et al.  Further developments and applications of the Green’s function method of sensitivity analysis in chemical kinetics , 1979 .

[24]  A. Gilliland,et al.  A sensitivity study of the discrete Kalman filter (DKF) to initial condition discrepancies , 2001 .

[25]  James G. Wilkinson,et al.  Fast, Direct Sensitivity Analysis of Multidimensional Photochemical Models , 1997 .

[26]  Iterative Inverse Modeling and Direct Sensitivity Analysis of a Photochemical Air Quality Model , 2000 .

[27]  M. Koda,et al.  Sensitivity analysis of distributed parameter systems , 1982 .

[28]  G. Grell,et al.  A description of the fifth-generation Penn State/NCAR Mesoscale Model (MM5) , 1994 .

[29]  Yongtao Hu,et al.  Decoupled direct 3D sensitivity analysis for particulate matter (DDM-3D/PM) , 2006 .

[30]  G. Grell,et al.  Satellite-observed US power plant NOx emission reductions and their impact on air quality - article no. L22812 , 2006 .

[31]  John P. Burrows,et al.  TROPOSPHERIC NO2 FROM GOME MEASUREMENTS , 2002 .

[32]  Clive D Rodgers,et al.  Inverse Methods for Atmospheric Sounding: Theory and Practice , 2000 .

[33]  James F. Gleason,et al.  An improved retrieval of tropospheric nitrogen dioxide from GOME , 2002 .

[34]  Henk Eskes,et al.  Error analysis for tropospheric NO2 retrieval from space , 2004 .

[35]  C. Rosenzweig,et al.  Assessing Ozone-Related Health Impacts under a Changing Climate , 2004, Environmental health perspectives.

[36]  Thomas P. Kurosu,et al.  Global inventory of nitrogen oxide emissions constrained by space‐based observations of NO2 columns , 2003 .

[37]  John P. Burrows,et al.  Inverse modelling of the spatial distribution of NO x emissions on a continental scale using satellite data , 2005 .

[38]  Matthias Beekmann,et al.  Bayesian Monte Carlo analysis applied to regional‐scale inverse emission modeling for reactive trace gases , 2007 .

[39]  Robin L. Dennis,et al.  Seasonal NH3 emission estimates for the eastern United States , 2003 .

[40]  G. Carmichael,et al.  Direct and adjoint sensitivity analysis of chemical kinetic systems with KPP: Part I—theory and software tools , 2003, Atmospheric Environment.

[41]  G. Carmichael,et al.  Reactive nitrogen distribution and partitioning in the North American troposphere and lowermost stratosphere , 2007 .

[42]  A. M. Dunker,et al.  Efficient calculation of sensitivity coefficients for complex atmospheric models , 1981 .

[43]  William P L Carter,et al.  Documentation of the SAPRC-99 chemical mechanism for VOC reactivity assessment. Volume 2. , 2000 .

[44]  G. Hidy,et al.  The Southeastern Aerosol Research and Characterization Study: Part 1—Overview , 2003, Journal of the Air & Waste Management Association.

[45]  R. Prinn,et al.  Optimizing an inverse method to deduce time‐varying emissions of trace gases , 1996 .

[46]  Michael E. Chang,et al.  Inverse modeling of biogenic isoprene emissions , 1996 .

[47]  Aaron L. Swanson,et al.  Evaluation of space‐based constraints on global nitrogen oxide emissions with regional aircraft measurements over and downwind of eastern North America , 2006 .

[48]  Greg Yarwood,et al.  The decoupled direct method for sensitivity analysis in a three-dimensional air quality model--implementation, accuracy, and efficiency. , 2002, Environmental science & technology.

[49]  Vivien Mallet,et al.  Inverse modeling of NOx emissions at regional scale over northern France: Preliminary investigation of the second‐order sensitivity , 2005 .

[50]  Henk Eskes,et al.  Intercomparison of SCIAMACHY nitrogen dioxide observations, in situ measurements and air quality modeling results over Western Europe , 2007 .

[51]  J. Burrows,et al.  TROPOSPHERIC NO 2 FROM GOME MEASUREMENTS , 2002 .