References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-1737-2012

Impact of lightning-NO on eastern United States photochemistry during the summer of 2006 as determined using the CMAQ model

Allen

D. J.

¹ Pickering

K. E.

² Pinder

R. W.

³ Henderson

B. H.

⁴ Appel

K. W.

³ Prados

⁵

Department of Atmospheric and Oceanic Science, University of Maryland, College Park, MD, USA

Atmospheric Chemistry and Dynamics Laboratory, Code 614 NASA-Goddard, Greenbelt, MD, USA

Atmospheric Modeling and Analysis Division, US EPA, Research Triangle Park, NC, USA

University of North Carolina Chapel Hill, NC, USA

Joint Center for Earth Sciences Technology (JCET), University of Maryland Baltimore County, Baltimore, MD, USA

16 02 2012

12 4 1737 1758

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A lightning-nitrogen oxide (NO) algorithm is implemented in the Community Multiscale Air Quality Model (CMAQ) and used to evaluate the impact of lightning-NO emissions (LNOx) on tropospheric photochemistry over the United States during the summer of 2006. For a 500 mole per flash lightning-NO source, the mean summertime tropospheric NO2 column agrees with satellite-retrieved columns to within −5 to +13%. Temporal fluctuations in the column are moderately well simulated; however, the addition of LNOx does not lead to a better simulation of day-to-day variability. The contribution of lightning-NO to the model column ranges from &sim;10% in the northern US to >45% in the south-central and southeastern US. Lightning-NO adds up to 20 ppbv to upper tropospheric model ozone and 1.5–4.5 ppbv to 8-h maximum surface layer ozone, although, on average, the contribution of LNOx to model surface ozone is 1–2 ppbv less on poor air quality days. LNOx increases wet deposition of oxidized nitrogen by 43% and total deposition of nitrogen by 10%. This additional deposition reduces the mean magnitude of the CMAQ low-bias in nitrate wet deposition with respect to National Atmospheric Deposition monitors to near zero. Differences in urban/rural biases between model and satellite-retrieved NO2 columns were examined to identify possible problems in model chemistry and/or transport. CMAQ columns were too large over urban areas. Biases at other locations were minor after accounting for the impacts of lightning-NO emissions and the averaging kernel on model columns. In order to obtain an upper bound on the contribution of uncertainties in NOy chemistry to upper tropospheric NOx low biases, sensitivity calculations with updated chemistry were run for the time period of the Intercontinental Chemical Transport Experiment (INTEX-A) field campaign (summer 2004). After adjusting for possible interferences in NO2 measurements and averaging over the entire campaign, these updates reduced 7–9 km biases from 32 to 17% and 9–12 km biases from 57 to 46%. While these changes lead to better agreement, a considerable unexplained NO2 low-bias remains in the uppermost troposphere.

References 1

Allen, D., Pickering, K., Duncan, B., and Damon, M.: Impact of lightning NO emissions on North American photochemistry as determined using the Global Modeling Initiative (GMI) model, J. Geophys. Res., 115, D22301, http://dx.doi.org/10.1029/2010JD014062doi:10.1029/2010JD014062, 2010.

Baughcum, S. L., Tritz, T. G., Henderson, S. C., and Pickett, D. C.: Scheduled civil aircraft emission inventories for 1992: Database development and analysis, NASA CR-4700, NASA, Washington DC, 1996.

Beirle, S., Huntrieser, H., and Wagner, T.: Direct satellite observation of lightning-produced NOx, Atmos. Chem. Phys., 10, 10965–10986, http://dx.doi.org/10.5194/acp-10-10965-2010doi:10.5194/acp-10-10965-2010, 2010.

Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. A., Field, B. D., Fiore, A. M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global modeling of tropospheric chemistry with assimilated meteorology: model description and evaluation, J. Geophys. Res., 106, 23073–23095, 2001.

Biagi, C. J., Cummins, K. L., Kehoe, K. E., and Krider, E. P.: National Lightning Detection Network (NLDN) performance in southern Arizona, Texas, and Oklahoma in 2003–2004, J. Geophys. Res., 112, D05208, doi:1029/2006DJ007341, 2007.

Boccippio, D., Cummins, K., Christian, H., and Goodman, S.: Combined Satellite- and Surface-Based Estimation of the Intracloud-Cloud-to-Ground Lightning Ratio over the Continental United States, Mon. Weather Rev., 129, 108–122, 2001.

Boccippio, D. J., Koshak, W. J., and Blakeslee, R. J.: Performance assessment of the Optical Transient Detector and Lightning Imaging Sensor, I: Predicted diurnal variability, J. Atmos. Ocean. Tech., 19, 1318–1332, 2002.

Boersma, K. F., Eskes, H. J., Veefkind, J. P., Brinksma, E. J., van der A, R. J., Sneep, M., van den Oord, G. H. J., Levelt, P. F., Stammes, P., Gleason, J. F., and Bucsela, E. J.: Near-real time retrieval of tropospheric NO2 from OMI, Atmos. Chem. Phys., 7, 2103–2118, http://dx.doi.org/10.5194/acp-7-2103-2007doi:10.5194/acp-7-2103-2007, 2007.

Boersma, K. F., Dirksen, R. J., Veefkind, J. P., Eskes, H. J., and van der A, R. J.: Dutch OMI NO2 (DOMINO) data product:, HE5 data file user manual, available at: http://www.temis.nl/docs/OMI_NO2_HE5_1.0.2.pdf, 2009.

Boersma, K. F., Eskes, H. J., Dirksen, R. J., van der A, R. J., Veefkind, J. P., Stammes, P., Huijnen, V., Kleipool, Q. L., Sneep, M., Claas, J., Leitão, J., Richter, A., Zhou, Y., and Brunner, D.: An improved tropospheric NO2 column retrieval algorithm for the Ozone Monitoring Instrument, Atmos. Meas. Tech., 4, 1905–1928, http://dx.doi.org/10.5194/amt-4-1905-2011doi:10.5194/amt-4-1905-2011, 2011.

Bousserez, N., Atti, J. L., Peuch, V. H., Michou, M., Pfister, G., Edwards, D., Emmons, L., Mari, C., Barret, B., Arnold, S. R., Heckel, A., Richter, A., Schlager, H., Lewis, A., Avery, M., Sachse, G., Browell, E. V., and Hair, J. W.: Evaluation of the MOCAGE chemistry transport model during the ICARTT/ITOP experiment, J. Geophys. Res., 112, D10S42, http://dx.doi.org/10.1029/2006JD007595doi:10.1029/2006JD007595, 2007.

Bovensmann, H., Burrows, J. P., Buchwitz, M., Frerick, J., No\"el, S., Rozanov, V. V., Chance, K. V., and Goede, A. P. H.: SCIAMACHY: Mission Objectives and Measurement Modes, J. Atmos. Sci., 56, 127–150, 1999.

Browne, E. C., Perring, A. E., Wooldridge, P. J., Apel, E., Hall, S. R., Huey, L. G., Mao, J., Spencer, K. M., Clair, J. M. St., Weinheimer, A. J., Wisthaler, A., and Cohen, R. C.: Global and regional effects of the photochemistry of CH3O2NO2: evidence from ARCTAS, Atmos. Chem. Phys., 11, 4209–4219, http://dx.doi.org/10.5194/acp-11-4209-2011doi:10.5194/acp-11-4209-2011, 2011.

Bucsela, E. J., Perring, A. E., Cohen, R. C., Boersma, K. F., Celarier, E. A., Gleason, J. F., Wenig, M. O., Bertram, T. H., Wooldridge, P. J., Dirksen, R., and Veefkind, J. P.: Comparison of tropospheric NO2 from in situ aircraft measurements with near-real-time and standard product data from OMI, J. Geophys. Res., 113, D16S31, http://dx.doi.org/10.1029/2007JD008838doi:10.1029/2007JD008838, 2008.

Byun, D. W. and Schere, K. L.: Review of the governing equations, computational algorithms, and other components of the Models-3 Community Multiscale Air Quality (CMAQ) modeling system, Appl. Mech. Rev., 59, 51–77, 2006.

Castellanos, P., Marufu, L. T., Doddridge, B. G., Taubman, B. F., Schwab, J. J., Hains, J. C., Ehrman, S. H., and Dickerson, R. R.: Ozone, oxides of nitrogen, and carbon monoxide during pollution events over the eastern United States: An evaluation of emissions and vertical mixing, J. Geophys. Res., 116, D16307, http://dx.doi.org/10.1029/2010JD014540doi:10.1029/2010JD014540, 2011.

Celarier, E. and Retscher, C.: OMINO2e data product readme file, available at: http://toms.gsfc.nasa.gov/omi/no2/OMNO2e_DP_Readme.pdf , 2009.

Choi, Y., Wang, Y., Yang, Q., Cunnold, D., Zeng, T., Shim, C., Luo, M., Eldering, A., Bucsela, E., and Gleason, J.: Spring to summer northward migration of high ozone over the western North Atlantic, Geophys. Res. Lett., 35, L04818, http://dx.doi.org/10.1029/2007GL032276doi:10.1029/2007GL032276, 2008.

Cooper, O. R., Stohl, A., Trainer, M., Thompson, A. M., Witte, J. C., Oltmans, S. J., Morris, G., Pickering, K. E., Crawford, J. H., Chen, G., Cohen, R. C., Bertram, T. H., Wooldridge, P., Perring, A., Brune, W. H., Merrill, J., Moody, J. L., Tarasick, D., N'ed'elec, P., Forbes, G., Newchurch, M. J., Schmidlin, F. J., Johnson, B. J., Turquety, S., Baughcum, S. L., Ren, X., Fehsenfeld, F. C., Meagher, J. F., Spichtinger, N., Brown, C. C., McKeen, S. A., McDermid, I. S., and Leblanc, T.: Large upper tropospheric ozone enhancements above midlatitude North America during summer: in situ evidence from the IONS and MOZAIC ozone measurement network, J. Geophys. Res., 111, D24S05, http://dx.doi.org/10.1029/2006JD007306doi:10.1029/2006JD007306, 2006.

Cooper, O. R., Trainer, M., Thompson, A. M., Oltmans, S. J., Tarasick, D. W., Witte, J. C., Stohl, A., Eckhardt, S., Lelieveld, J., Newchurch, M. J., Johnson, B. J., Portmann, R. W., Kalnajs, L., Dubey, M. K., Leblanc, T., McDermid, I. S., Forbes, G., Wolfe, D., Carey-Smith, T., Morris, G. A., Lefer, B., Rappenglück, B., Joseph, E., Schmidlin, F., Meagher, J., Fehsenfeld, F. C., Keating, T. J., van Curen, R. A., and Minschwaner, K: Evidence for a recurring Eastern North American upper tropospheric ozone maximum during summer, J. Geophys. Res., 112, D23304, http://dx.doi.org/10.1029/2007JD008710doi:10.1029/2007JD008710, 2007.

Cummins, K., Murphy, M., Bardo, E., Hiscox, W., Pyle, R., and Pifer, A.: A combined TOA/MDF Technology upgrade of the US National Lightning Detection Network, J. Geophys. Res., 103, 9035–9044, 1998.

DeCaria, A. J., Pickering, K. E., Stenchikov, G. L., and Ott, L. E.: Lightning-generated NOx and its impact on tropospheric ozone production: A three-dimensional modeling study of a STERAO-A thunderstorm, J. Geophys. Res., 110, D14303, http://dx.doi.org/10.1029/2004JD005556doi:10.1029/2004JD005556, 2005.

Dentener, F., Peter, W., Krol, M., van Weele, M., Bergamaschi, P., and Lelieveld, J.: Interannual variability and trend of OH and the lifetime of CH4: 1979–1993 global chemical transport model calculations, J. Geophys. Res., 108, 4442, http://dx.doi.org/10.1029/2002JD002916doi:10.1029/2002JD002916, 2003.

Fang, Y., Fiore, A. M., Horowitz, L. W., Levy, H., Hu, Y., and Russell, A. G.: Sensitivity of the NOy budget over the United States to anthropogenic and lightning NOx in summer, J. Geophys. Res., 115, D18312, http://dx.doi.org/10.1029/2010JD014079doi:10.1029/2010JD014079, 2010.

Fehr, T., Höller, H., and Huntrieser, H.: Model study on production and transport of lightning-produced NOx in a EULINOX supercell storm, J. Geophys. Res., 109, D09102, http://dx.doi.org/10.1029/2003JD003935doi:10.1029/2003JD003935, 2004.

Gilliland, A. B., Hogrefe, C., Pinder, R. W., Godowitch, J. M., Foley, K. L., and Rao, S. T.: Dynamic evaluation of regional air quality models: Assessing changes in ozone stemming from changes in emissions and meteorology, Atmos. Environ., 42, 5110–5123, 2008.

Grell, G., Dudhia, J., and Stauffer, D.: A description of the fifth generation Penn State/NCAR mesoscale model (MM5), NCAR Technical Note, NCAR/TN-398+STR, 1995.

Hansen, A. E., Fuelberg, H. E., and Pickering, K. E.: Vertical distributions of lightning sources and flashes over Kennedy Space Center, Florida, J. Geophys. Res., 115, D14203, http://dx.doi.org/10.1029/2009JD013143doi:10.1029/2009JD013143, 2010.

Henderson, B. H., Pinder, R. W., Crooks, J., Cohen, R. C., Hutzell, W. T., Sarwar, G., Goliff, W. S., Stockwell, W. R., Fahr, A., Mathur, R., Carlton, A. G., and Vizuete, W.: Evaluation of simulated photochemical partitioning of oxidized nitrogen in the upper troposphere, Atmos. Chem. Phys., 11, 275–291, http://dx.doi.org/10.5194/acp-11-275-2011doi:10.5194/acp-11-275-2011, 2011.

Herron-Thorpe, F. L., Lamb, B. K., Mount, G. H., and Vaughan, J. K.: Evaluation of a regional air quality forecast model for tropospheric NO2 columns using the OMI/Aura satellite tropospheric NO2 product, Atmos. Chem. Phys., 10, 8839–8854, http://dx.doi.org/10.5194/acp-10-8839-2010doi:10.5194/acp-10-8839-2010, 2010.

Hollingsworth, A., Engelen, R. J., Benedetti, A., Dethof, A., Flemming, J., Kaiser, J. W., Morcrette, J.-J., Simmons, A. J., Textor, C., Boucher, O., Chevallier, F., Rayner, P., Elbern, H., Eskes, H., Granier, C., Peuch, V.-H., Rouil, L., and Schultz, M. G.: Toward a monitoring and forecasting system for atmospheric composition: the Gems Project, B. Am. Meteor. Soc., 89, 1147–1164, http://dx.doi.org/10.1175/2008BAMS2355.1doi:10.1175/2008BAMS2355.1, 2008.

Hudman, R. C., Jacob, D. J., Turquety, S., Leibensperger, E. M., Murray, L. T., Wu, S., Gilliland, A. B., Avery, M., Bertram, T. H., Brune, W., Cohen, R. C., Dibb, J. E., Flocke, F. M., Fried, A., Holloway, J., Neuman, J. A., Orville, R., Perring, A., Ren, X., Sachse, G. W., Singh, H. B., Swanson, A., and Wooldridge, P. G.: Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow, J. Geophys. Res., 112, D12S05, http://dx.doi.org/10.1029/2006JD007912doi:10.1029/2006JD007912, 2007.

Huijnen, V., Eskes, H. J., Poupkou, A., Elbern, H., Boersma, K. F., Foret, G., Sofiev, M., Valdebenito, A., Flemming, J., Stein, O., Gross, A., Robertson, L., D'Isidoro, M., Kioutsioukis, I., Friese, E., Amstrup, B., Bergstrom, R., Strunk, A., Vira, J., Zyryanov, D., Maurizi, A., Melas, D., Peuch, V.-H., and Zerefos, C.: Comparison of OMI NO2 tropospheric columns with an ensemble of global and European regional air quality models, Atmos. Chem. Phys., 10, 3273–3296, http://dx.doi.org/10.5194/acp-10-3273-2010doi:10.5194/acp-10-3273-2010, 2010.

Huntrieser, H., Schumann, U., Schlager, H., Höller, H., Giez, A., Betz, H.-D., Brunner, D., Forster, C., Pinto Jr., O., and Calheiros, R.: Lightning activity in Brazilian thunderstorms during TROCCINOX: implications for NOx production, Atmos. Chem. Phys., 8, 921–953, http://dx.doi.org/10.5194/acp-8-921-2008doi:10.5194/acp-8-921-2008, 2008.

Huntrieser, H., Schlager, H., Lichtenstern, M., Roiger, A., Stock, P., Minikin, A., Höller, H., Schmidt, K., Betz, H.-D., Allen, G., Viciani, S., Ulanovsky, A., Ravegnani, F., and Brunner, D.: NOx production by lightning in Hector: first airborne measurements during SCOUT-O3/ACTIVE, Atmos. Chem. Phys., 9, 8377–8412, http://dx.doi.org/10.5194/acp-9-8377-2009doi:10.5194/acp-9-8377-2009, 2009.

Jourdain, L., Kulawik, S. S., Worden, H. M., Pickering, K. E., Worden, J., and Thompson, A. M.: Lightning NOx emissions over the USA constrained by TES ozone observations and the GEOS-Chem model, Atmos. Chem. Phys., 10, 107–119, http://dx.doi.org/10.5194/acp-10-107-2010doi:10.5194/acp-10-107-2010, 2010.

Kain, J. S. and Fritsch, J. M.: Convective parameterization for mesoscale models: The Kain-Fritsch scheme, The representation of cumulus convection in numerical models, edited by: Emanuel, K. A. and Raymond, D. J., Amer. Meteor. Soc., 246~pp., 1993.

Kaynak, B., Hu, Y., Martin, R. V., Russell, A. G., Choi, Y., and Wang, Y.: The effect of lightning NOx production on surface ozone in the continental United States, Atmos. Chem. Phys., 8, 5151–5159, http://dx.doi.org/10.5194/acp-8-5151-2008doi:10.5194/acp-8-5151-2008, 2008.

Koo, B., Chien, C.-J., Tonnesen, G., Morris, R., Johnson, J., Sakulyanontvittaya, T., Piyachaturawat, P., and Yarwood, G.: Natural emissions for regional modeling of background ozone and particulate matter and impacts on emissions control strategies, Atmos. Environ., 44, 2372–2382., http://dx.doi.org/10.1016/j.atmosenv.2010.02.041doi:10.1016/j.atmosenv.2010.02.041, 2010.

Koshak, W. J., Solakiewicz, R. J., Blakeslee, R. J., Goodman, S. J., Christian, H. J., Hall, J. M., Bailey, J. C., Krider, E. P., Bateman, M. G., Boccippio, D. J., Mach, D. M., McCaul, E. W., Stewart, M. F., Buechler, D. E., Petersen, W. A., and Cecil, D. J.: North Alabama Lightning Mapping Array (LMA): VHF source retrieval algorithm and error analyses, J. Atmos. Ocean. Tech., 21, 543–558, 2004.

Koshak, W. J., Peterson, H. S., McCaul, E. W., and Biazar, A.: Estimates of the lightning-NOx profile in the vicinity of the North Alabama Lightning Mapping Array, 21st International Lightning Detection Conference (ILDC)/Vaisala, 18–22~April~2010, Orlando, FL, United States, NASA Technical Report Document 20100021055, 2010.

Kunkrishnan, T. and Lawrence, M. G.: Sensitivity of NOx over the Indian Ocean to emissions from the surrounding continents and nonlinearities in atmospheric chemistry responses, Geophys. Res. Lett., 31, L15109, http://dx.doi.org/10.1029/2004GL020210doi:10.1029/2004GL020210, 2004.

Lamsal, L. N., Martin, R. V., van Donkelaar, A., Celarier, E. A., Bucsela, E. J., Boersma, K. F., Dirksen, R., Luo, C., and Wang, Y.: Indirect validation of tropospheric nitrogen dioxide retrieved from the OMI satellite instrument: Insight into the seasonal variation of nitrogen oxides at northern midlatitudes, J. Geophys. Res., 115, D05302, http://dx.doi.org/10.1029/2009JD013351doi:10.1029/2009JD013351, 2010.

Liu, X., Bhartia, P. K., Chance, K., Spurr, R. J. D., and Kurosu, T. P.: Ozone profile retrievals from the Ozone Monitoring Instrument, Atmos. Chem. Phys., 10, 2521–2537, http://dx.doi.org/10.5194/acp-10-2521-2010doi:10.5194/acp-10-2521-2010, 2010.

Mach, D. M., Christian, H. J., Blakeslee, R. J., Boccippio, D. J., Goodman, S. J., and Boeck, W. L.: Performance assessment of the Optical Transient Detector and Lightning Imaging Sensor, J. Geophys. Res., 112, D09210, http://dx.doi.org/10.1029/2006JD007787doi:10.1029/2006JD007787, 2007.

Martin, R. V., Jacob, D. J., Yantosca, R. M., Chin, M., and Ginoux, P.: Global and regional decreases in tropospheric oxidants from photochemical effects of aerosols, J. Geophys. Res., 108, 4097, http://dx.doi.org/10.1029/2002JD002622doi:10.1029/2002JD002622, 2003.

Martin, R. V., Sauvage, B., Folkins, I., Sioris, C. E., Boone, C., Bernath, P., and Ziemke, J.: Space-based constraints on the production of nitric oxide by lightning, J. Geophys. Res., 112, D09309, http://dx.doi.org/10.1029/2006JD007831doi:10.1029/2006JD007831, 2007.

Martini, M., Allen, D. J., Pickering, K. E., Stenchikov, G., Richter, A., Hyer, E., and Loughner, C.: The impact of North American anthropogenic emissions and lightning on long range transport of trace gases and their export from the continent during the summers of 2002 and 2004, J. Geophys. Res., 116, D07305, http://dx.doi.org/10.1029/2010JD014305doi:10.1029/2010JD014305, 2011.

Metwally, M.: Jet aircraft engine emissions database development – 1992 military, charter, and nonscheduled traffic, NASA CR-4684, NASA, Washington DC, 1995.

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., 8, 5603–5614, http://dx.doi.org/10.5194/acp-8-5603-2008doi:10.5194/acp-8-5603-2008, 2008.

National Acid Deposition program 2006 Annual Summary, NADP Data Report 2006-01, Illinois State Water Survey, University of Illinois at Urbana-Champaign, IL, 2006.

Novak, J. H. and Pierce, T. E.: Natural emissions of oxidant precursors, Water Air Soil Poll., 67, 57–77, 1993.

Orville, R. E., Huffines, R. E., Burrows, G. R., Holle, W. R., and Cummins, K. L., The North American Lightning Detection Network (NALDN)-first results: 1998–2000, Mon. Weather Rev., 130, 2098–2109, 2002.

Ott, L. E., Pickering, K. E., Stenchikov, G. L., Huntrieser, H., and Schumann, U.: Effects of lightning NOx production during the 21~July European Lightning Nitrogen Oxides Project storm studied with a three-dimensional cloud-scale chemical transport model, J. Geophys. Res., 112, D05307, http://dx.doi.org/10.1029/2006JD007365doi:10.1029/2006JD007365, 2007.

Ott, L. E., Pickering, K. E., Stenchikov, G. L., Allen, D. J., DeCaria, A. J., Ridley, B., Lin, R.-F., Lang, S., and Tao, W.-K.: Production of lightning NOx and its vertical distribution calculated from three-dimensional cloud-scale chemical transport model simulations, J. Geophys. Res., 115, D04301, http://dx.doi.org/10.1029/2009JD011880doi:10.1029/2009JD011880, 2010.

Petersen, W. A. and Rutledge, S. A.: On the relationship between cloud-to-ground lightning and convective rainfall, J. Geophys. Res., 103, 14025–14040, 1998.

Pierce, R. B., Schaack, T., Al-Saadi, J. A., Fairlie, T. D., Kittaka, C., Lingenfelser, G., Natarajan, M., Olson, J., Soja, A., Zapotocny, T., Lenzen, A., Stobie, J., Johnson, D., Avery, M. A., Sachse, G. W., Thompson, A., Cohen, R., Dibb, J. E., Crawford, J., Rault, D., Martin, R., Szykman, J., and Fishman, J.: Chemical data assimilation estimates of continental US ozone and nitrogen budgets during the Intercontinental Chemical Transport Experiment-North America, J. Geophys. Res., 112, D12S21, http://dx.doi.org/10.1029/2006JD007722doi:10.1029/2006JD007722, 2007.

Rao, S. T., Galmarini, S., and Puckett, S.: Air Quality Model Evaluation International Initiative (AQMEII): Advancing state-of-science in regional photochemical modeling and its applications, B. Am. Meteor. Soc., 92, 23–30, http://dx.doi.org/10.1175/2010BAMS3069.1doi:10.1175/2010BAMS3069.1, 2010.

Ren, X., Olson, J. R., Crawford, J. H., Brune, W. H., Mao, J., Long, R. B., Chen, Z., Chen, G., Avery, M. A., Sachse, G. W., Barrick, J. D., Diskin, G. S., Huey, L. G., Fried, A., Cohen, R. C., Heikes, B., Wennberg, P. O., Singh, H. B., Blake, D. R., and Shetter, R. E.: HOx chemistry during INTEX-A 2004: Observation, model calculation and comparison with previous studies, J. Geophys. Res., 113, D05310, http://dx.doi.org/10.1029/2007JD009166doi:10.1029/2007JD009166, 2008.

Richter, A., Burrows, J. P., Nüß, H., Granier, C., and Niemeier, U.: Increase in tropospheric nitrogen dioxide over China observed from space, Nature, 437, 129–132, http://dx.doi.org/10.1038/nature04092doi:10.1038/nature04092, 2005.

Sauvage, B., Martin, R. V., van Donkelaar, A., Liu, X., Chance, K., Jaeglé, L., Palmer, P. I., Wu, S., and Fu, T.-M.: Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone, Atmos. Chem. Phys., 7, 815–838, http://dx.doi.org/10.5194/acp-7-815-2007doi:10.5194/acp-7-815-2007, 2007a.

Sauvage, B., Martin, R. V., van Donkelaar, A., and Ziemke, J. R.: Quantification of the factors controlling tropical tropospheric ozone and the South Atlantic maximum, J. Geophys. Res., 112, D11309, http://dx.doi.org/10.1029/2006JD008008doi:10.1029/2006JD008008, 2007b.

Schumann, U. and Huntrieser, H.: The global lightning-induced nitrogen oxides source, Atmos. Chem. Phys., 7, 3823–3907, http://dx.doi.org/10.5194/acp-7-3823-2007doi:10.5194/acp-7-3823-2007, 2007.

Singh, H. B., Brune, W. H., Crawford, J. H., Jacob, D. J., and Russell, P. B.: Overview of the summer 2004 Intercontinental Chemical Transport Experiment-North America (INTEX-A), J. Geophys. Res., 111, D24S01, http://dx.doi.org/10.1029/2006JD007905doi:10.1029/2006JD007905, 2006.

Singh, H. B., Salas, L., Herlth, D., Kolyer, R., Czech, E., Avery, M., Crawford, J. H., Pierce, R. B., Sachse, G. W., Blake, D. R., Cohen, R. C., Bertram, T. H., Perring, A., Wooldridge, P. J., Dibb, J., Huey, G., Hudman, R. C., Turquety, S., Emmons, L. K., Flocke, F., Tang, Y., Carmichael, G. R., and Horowitz, L. W.: Reactive nitrogen distribution and partitioning in the North American troposphere and lowermost stratosphere, J. Geophys. Res., 112, D12S04, http://dx.doi.org/10.1029/2006JD007664doi:10.1029/2006JD007664, 2007.

Sioris, C. E., Kurosu, T. P., Martin, R. V., and Chance, K.: Stratospheric and tropospheric NO2 observed by SCIAMACHY: first results, Adv. Space Res., 34, 780–785, 2004.

Skamarock, W. C., Klemp, J. B., Dudhia, J., Gill, D. O., Barker, D. M., Wang, W., and Powers, J. G.: A description of the advanced research WRF version 2, NCAR/TN-468+STR, 2005.

Smith, S. N. and Mueller, S. F.: Modeling natural emissions in the Community Multiscale Air Quality (CMAQ) Model�I: building an emissions data base, Atmos. Chem. Phys., 10, 4931–4952, http://dx.doi.org/10.5194/acp-10-4931-2010doi:10.5194/acp-10-4931-2010, 2010.

SMOKE v2.6 User's Manual, The Institute for the Environment, University of North Carolina, available at: http://www.smoke-model.org/version2.6/SMOKE_v26_manual.pdf, 504~pp., 2009.

Tapia, A. J., Smith, A., and Dixon, M.: Estimation of convective rainfall from lightning observations, J. Appl. Meteorol., 37, 1497–1509, 1998.

Thompson, A. M., Stone, J. B., Witte, J. C., Miller, S. K., Pierce, R. B., Chatfield, R. B., Oltmans, S. J., Cooper, O. R., Loucks, A. L., Taubman, B. F., Johnson, B. J., Joseph, E., Kucsera, T. L., Merrill, J. T., Morris, G. A., Hersey, S., Forbes, G., Newchurch, M. J., Schmidlin, F. J., Tarasick, D. W., Thouret, V., and Cammas, J.-P.: Intercontinental Chemical Transport Experiment Ozonesonde Network Study (IONS) 2004: 2. Tropospheric ozone budgets and variability over Northeastern North America, J. Geophys. Res., 112, D12S13, http://dx.doi.org/10.1029/2006JD007670doi:10.1029/2006JD007670, 2007a.

Thompson, A. M., Stone, J. B., Witte, J. C., Miller, S. K., Oltmans, S. J., Kucsera, T. L., Ross, K. L., Pickering, K. E., Merrill, J. T., Forbes, G., Tarasick, D. W., Joseph, E., Schmidlin, F. J., McMillan, W. W., Warner, J., Hintsa, E. J., and Johnson, J. E.: Intercontinental Chemical Transport Experiment Ozonesonde Network Study (IONS) 2004: 1. Summertime upper troposphere/lower stratosphere ozone over Northeastern North America, J. Geophys. Res., 112, D12S12, http://dx.doi.org/10.1029/2006JD007441doi:10.1029/2006JD007441, 2007b.

Tost, H., Jöckel, P., and Lelieveld, J.: Lightning and convection parameterisations – uncertainties in global modelling, Atmos. Chem. Phys., 7, 4553–4568, http://dx.doi.org/10.5194/acp-7-4553-2007doi:10.5194/acp-7-4553-2007, 2007.

Vukovich, J. M. and Pierce, T.: The implementation of BEIS3 within the SMOKE modeling framework, available at: http://www.epa.gov/ttn/chief/conference/ei11/modeling/vukovich.pdf, 2002.

Zhang, R., Tie, X., and Bond, D. W.: Impacts of anthropogenic and natural NOx sources over the US on tropospheric chemistry, P. Natl. Acad. Sci. USA, 100, 1505–1509, http://dx.doi.org/10.1073/pnas.252763799doi:10.1073/pnas.252763799, 2003.

Zhao, C., Wang, Y., Choi, Y., and Zeng, T.: Summertime impact of convective transport and lightning NOx production over North America: modeling dependence on meteorological simulations, Atmos. Chem. Phys., 9, 4315–4327, http://dx.doi.org/10.5194/acp-9-4315-2009doi:10.5194/acp-9-4315-2009, 2009.