Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 7 6 2007 10.5194/acp-7-1671-2007 http://www.atmos-chem-phys.net/7/1671/2007/ http://www.atmos-chem-phys.net/7/1671/2007/acp-7-1671-2007.html http://www.atmos-chem-phys.net/7/1671/2007/acp-7-1671-2007.pdf 1671 1681 2007-03-27 Systematic analysis of interannual and seasonal variations of model-simulated tropospheric NO₂ in Asia and comparison with GOME-satellite data I. Uno uno@riam.kyushu-u.ac.jp Y. He T. Ohara K. Yamaji J.-I. Kurokawa M. Katayama Z. Wang K. Noguchi S. Hayashida A. Richter J. P. Burrows Research Institute for Applied Mechanics, Kyushu University, Kasuga Park 6-1, Kasuga, Fukuoka, Japan Earth System Science and Technology, Kyushu University, Kasuga Park 6-1, Kasuga, Fukuoka, Japan National Institute for Environmental Studies, Tsukuba, Ibaraki, Japan Frontier Research Center for Global Change, Japan Agency for Marine-Earth Science and Technology, Yokohama, Japan NZC/LAPC, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China Information Science, Faculty of Science, Nara Women's University, Nara, Japan Institute of Environmental Physics, University of Bremen, Bremen, Germany Systematic analyses of interannual and seasonal variations of tropospheric NO₂ vertical column densities (VCDs) based on GOME satellite data and the regional scale chemical transport model (CTM), Community Multi-scale Air Quality (CMAQ), are presented for the atmosphere over eastern Asia between 1996 and June 2003. A newly developed year-by-year emission inventory (REAS) was used in CMAQ. The horizontal distribution of annual averaged GOME NO₂ VCDs generally agrees well with the CMAQ results. However, CMAQ/REAS results underestimate the GOME retrievals with factors of 2–4 over polluted industrial regions such as Central East China (CEC), a major part of Korea, Hong Kong, and central and western Japan. The most probable reasons for the underestimation typically over the CEC are accuracy of the basic energy statistic data, emission factors, and socio-economic data used for construction of emission inventory. For the Japan region, GOME and CMAQ NO₂ data show reasonable agreement with respect to interannual variation and show no clear increasing trend. For CEC, GOME and CMAQ NO₂ data indicate a very rapid increasing trend from 2000. Analyses of the seasonal cycle of NO₂ VCDs show that GOME data have larger dips than CMAQ NO₂ during February–April and September–November. Sensitivity experiments with fixed emission intensity reveal that the detection of emission trends from satellite in fall or winter has a larger error caused by the variability of meteorology. Examination during summer time and annual averaged NO₂ VCDs are robust with respect to variability of meteorology and are therefore more suitable for analyses of emission trends. Analysis of recent trends of annual emissions in China shows that the increasing trends of 1996–1998 and 2000–2002 for GOME and CMAQ/REAS show good agreement, but the rate of increase by GOME is approximately 10–11% yr^−1 after 2000; it is slightly steeper than CMAQ/REAS (8–9% yr^−1). The greatest difference was apparent between the years 1998 and 2000: CMAQ/REAS only shows a few percentage points of increase, whereas GOME gives a greater than 8% yr^−1 increase. The exact reason remains unclear, but the most likely explanation is that the emission trend based on the Chinese emission related statistics underestimates the rapid growth of emissions. Akimoto, H., Ohara, T., Kurokawa, J., and Horii, N.: Verification of energy consumption in China during 1996–2003 by satellite observation, Atmos. Environ., 40, 7663–7667, 2006. Boersma, K. F., Eskes, H. J., Meijer, E. W., and Kelder, H. M.: Estimates of lightning NOx production from GOME satellite observations, Atmos. Chem. Phys., 5, 2311–2331, 2005. Byun, D. W. and Ching, J. K. S. (Eds.): Science algorithms of the EPA Models-3 community multi-scale air quality (CMAQ) modeling system. \textitNERL, Research Triangle Park, NC EPA/ 600/R-99/030, 1999. Carter, W. P. L.: Documentation of the SAPRC-99 chemical mechanism for VOC reactivity assessment, Final report to California Air Resource Board, Contract No. 92-329 and 95-308, May, 2000. Irie, H., Sudo, K., Akimoto, H., et al.: Evaluation of long-term tropospheric NO2 data obtained by GOME over East Asia in 1996–2002, Geophys. Res. Lett., $32$, L11810, doi:10.1029/2005GL022770, 2005. Jaeglé, L., Steinberger, L., Martin, R. V., and Chance, K.: Global partitioning of NOx sources using satellite observations: Relative roles of fossil fuel combustion, biomass burning and soil emissions, Faraday Discuss., 130, 407–423, 2005. Koelemeijer, R. B. A., de Haan, J. F., and Stammes, P.: A database of spectral surface reflectivity in the range 335–772 nm derived from 5.5 years of GOME observations, J. Geophys. Res., 108(D2), 4070, doi:10.1029/2002JD002429, 2003. Ma, J., Richter, A., Burrows, J. P., Nüß, H., and van Aardenne, J. A.: Comparison of model-simulated tropospheric NO₂ over China with GOME-satellite data, Atmos. Environ., $40$, 593–604, 2006. Martin, R. V., Jacob, D. J., Chance, K., Kurosu, T. P., Palmer, P. I., and Evans, M. J.: Global inventory of nitrogen oxide emissions constrained by space-based observations of NO₂ columns, J. Geophys. Res., 108, 4537, doi:10.1029/2003JD003453, 2003. % %Ohara, T., Akimoto, H., Kurokawa, J., Horii, N., Yamaji, K., Yan, X., and Hayasaka, T.: REAS: Asian emission inventory for anthropogenic emission %sources during the period 1980–2020, Atmos. Chem. Phys. %Discuss., in preparation\blackbox\bf status?, 2007. Olivier, J. G. J., Berdowslki, J. J. M., Peters, J. A. H. W., Visschedijk, A. J. H., Bekker, J., and Bloos, J. P. J.: Applications of EDGAR: Emission Database for Global Atmospheric Research. Dutch National Research Programme on Global Air Pollution and Climate Change, report no. 410 200 051, 2002. Pielke, R. A., Cotton, W. R., Walko, R. L., Tremback, C. J., Lyons, W. A., Grasso, L. D., Nicholls, M. E., Moran, M. D., Wesley, D. A., Lee, T. J., and Copeland, J. H.: A comprehensive meteorological modeling system–-RAMS. Meteorol. Atmos. Phys., $49$, 69–91, 1992. 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, doi:10.1038/nature04092, 2005. Streets D. G., Bond, T. C., Carmichael, G. R., Fernandes, S. D., Fu, Q., He, D., Klimont, Z., Nelson, S. M., Tsai, N. Y., Wand, M. Q., Woo, J.-H., and Yarber, K. F.: An inventory of gaseous and primary aerosol emissions in Asia in the year 2000, J. Geophys. Res., $108$(D21), 8809, doi:10.1029/2002JD003093, 2003. Sudo, K., Takahashi, M., Kurokawa, J., and Akimoto, H.: CHASER: a global chemical model of the troposphere – 1. Model description, J. Geophys. Res.-Atmos., $107$(D17), 4339, doi:10.1029/2001JD001113, 2002. Tanimoto, H., Sawa, Y., Matsueda, H., Uno, I., Ohara, T., Yamaji, K., Kurokawa, J., and Yonemura, S.: Significant latitudinal gradient in the surface ozone spring maximum over East Asia, Geophys. Res. Lett., $32$, L21805, doi:10.1029/2005GL023514, 2005. Uno, I., Ohara, T., Sugata, S., Kurokawa, J., Furuhashi, N., Yamaji, K., Tanimoto, N., Yumimoto, K., and Uematsu, M.: Development of RAMS/CMAQ Asian scale chemical transport modeling system, J. Japan Soc. Atmos. Environ., 40(4), 148–164, [in Japanese], 2005. van Noiji, T. P. C., Eskes, H. J., Dentener, F. J., et al.: Multi-model ensemble simulations of tropospheric NO₂ compared with GOME retrievals for the year 2000, Atmos. Chem. Phys., $6$, 2943–2979, 2006. van der A, R. J., Peters, D. H. M. U., Eskes, H., Boersma, K. F., Van Roozendael, M., De Smedt, I., and Kelder, H. M.: Detection of the trend and seasonal variation in tropospheric NO₂ over China, J. Geophys. Res., $111$, D12317, doi:10.1029/2005JD006594, 2006. Yamaji, K., Ohara, T., Uno, I., Tanimoto, H., Kurokawa, J., and Akimoto, H.: Analysis of seasonal variation of ozone in the boundary layer in East Asia using the Community Multi-scale Air Quality model: What controls surface ozone level over Japan?, Atmos. Environ., $40$, 1856–1868, 2006a. Yamaji, K.: Modeling study of spatial-temporal variations of tropospheric ozone over East Asia, Ph. D. thesis for Kyushu University, 2006b. Zhang, M.-G., Uno, I., Sugata, S., Wang, Z.-F., D. W.,, and Akimoto, H.: Numerical study of boundary layer ozone transport and photochemical production in east Asia in the wintertime, Geophys. Res. Lett., $29$, 1545, doi:10.1029/2001GL014368, 2002. % %Zhang, Q., Streets, D. G., \blackbox\bf please name at least 3 authors before using et al. et al.: NO_x emission trends for China, 1995–2004: The %view from the ground and the view from space, in preparation, 2007.