Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 7 4 2007 10.5194/acpd-7-9795-2007 http://www.atmos-chem-phys-discuss.net/7/9795/2007/ http://www.atmos-chem-phys-discuss.net/7/9795/2007/acpd-7-9795-2007.html http://www.atmos-chem-phys-discuss.net/7/9795/2007/acpd-7-9795-2007.pdf 9795 9828 2007-07-05 Tropospheric ozone climatology over Beijing: analysis of aircraft data from the MOZAIC program A. J. Ding T. Wang cetwang@polyu.edu.hk V. Thouret J.-P. Cammas P. Nédélec Department of Civil and Structural Engineering, The Hong Kong Polytechnic University, Hong Kong, China Laboratoire d'Aérologie, UMR 5560, Université Paul Sabatier, Toulouse, France Ozone (O₃) profiles recorded over Beijing from 1995 to 2005 by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program were analyzed to provide a first climatology of tropospheric O₃ over Beijing and the North China Plains (NCPs), one of the most populated and polluted regions in China. A pooled method was adopted in the data analysis to reduce the influence of irregular sampling frequency. The tropospheric O₃ over Beijing shows a seasonal and vertical distribution typical of mid-latitude locations in the Northern Hemisphere, but has higher daytime concentrations in the lower troposphere, when compared to New York City, Tokyo, and Paris at similar latitude. The tropospheric O₃ over Beijing exhibits a common summer maximum and a winter minimum, with a broad summer maximum in the middle troposphere and a narrower early summer (June) peak in the lower troposphere. Examination of meteorological and satellite data suggests that the lower tropospheric O₃ maximum in June is a result of strong photochemical production, transport of regional pollution, and possibly also more intense burnings of biomass in Central-Eastern China. Trajectory analysis indicates that in summer the regional pollution sources from the NCPs, maybe mixed with urban plumes from Beijing, played important roles on the high O₃ concentrations in the boundary layer, but had limited impact on the O₃ concentrations in the middle troposphere. A comparison of the data recorded before and after 2000 reveals that O₃ in the lower troposphere over Beijing had a strong positive trend (approximately 2% per year from 1995 to 2005) in contrast to a flat or a decreasing trend over Tokyo, New York City, and Paris, indicating worsening photochemical pollution in Beijing and the NCPs. Akimoto, H., Nakane, H., and Matsumoto, Y.: The chemistry of oxidant generation: tropospheric ozone increase in Japan, Chemistry of the Atmosphere: The Impact on Global Change, edited by: Calvert, J., Blackwell Scientific Publications, Oxford, UK, 261–273, 1994. Akimoto, H.,and Narita, H.: Distribution of SO₂, NO_x, and CO₂ emissions from fuel combustion and industrial activities in Asia with 1°×1° resolution, Atmos. Environ., 28(2), 213–225, 1994. Austin, J. F. and Midgley, R. P.: The climatology of the jet-stream and stratospheric intrusions of ozone over Japan, Atmos. Environ., 28(1), 39–52,1994. Beekmann, M. Ancellet, G., and Megie, G.: Climatology of tropospheric ozone in southern Europe and its relation to potential vorticity, J. Geophys. Res., 99, 12 841–12 853, 1994. Bojkov, R. D.: Ozone changes at the surface and in the free troposphere, in: Tropospheric Ozone: Regional and Global Scale Interactions, edited by: Isaksen, I. S. A., and Reidel, D., 83–96, Dordrecht, Netherlands, 1988. Chan, C. Y., Chan, L. Y., Chang, W. L., Zheng, Y. G., Cui, H., Zheng, X. D., Qin, Y., and Li, Y. S.: Characteristics of a tropospheric ozone profile and implications for the origin of ozone over subtropical China in the spring of 2001, J. Geophys. Res., 108(D20), 8800, doi:10.1029/2003JD003427, 2003. Cheung, V. T. F. and Wang, T.: Observational study of ozone pollution in rural site in the Yangtze Delta of China, Atmos. Environ., 35, 4947–4958, 2001. Cooper, O. R., Stohl, A., Eckhardt, S., Parrish, D. D., Oltmans, S. J., Johnson, B. J., Nedelec, P., Schmidlin, F. J., Newchurch, M. J., Kondo, Y., and Kita, K.: A springtime comparison of tropospheric ozone and transport pathways on the east and west coasts of the United States, J. Geophys. Res., 110, D05S90, doi:10.1029/2004JD005183, 2005. Crutzen, P. J: A discussion of the chemistry of some minor constituents of the stratosphere and troposphere, Pure Appl. Geophys., 106–108, 1385–1399, 1973. Ding, A. and Wang, T.: Influence of stratosphere-to-troposphere exchange on the seasonal cycle of surface ozone at Mount Waliguan in western China, Geophys. Res. Lett., 33(3), L03803, doi:10.1029/2005GL024760, 2006. Ding, Y.: Monsoons Over China, Kluwer Acd., Norwell, Mass., 420pp., 1994. Fishman, J., Ramanathan, V., Crutzen, P. J., and Liu, S. C.: Tropospheric ozone and climate, Nature, 282, 818–820, 1979. Fishman, J., Wozniak, A. E., and Creilson, J. K.: Global distribution of tropospheric ozone from satellite measurements using the empirically corrected tropospheric ozone residual technique: Identification of the regional aspects of air pollution, Atmos. Chem. Phys., 3, 893–907, 2003. Gao, J., Wang, T., Ding, A. J., and Liu, C.: Observation study of ozone and carbon monoxide at the summit of mount Tai (1534 m a.s.l.) in central-eastern China, Atmos. Environ., 39, 4779–4791, 2005. Hidy, G. M.: Ozone process insights from field experiments Part~I: Overview, Atmos. Environ., 34, 2001–2022, 2000. Kleinman, L., Lee, Y.-N., Springston, S. R., Nunnermacker, L., and Zhou, X. L.: Ozone formation at a rural site in the southeastern United States, J. Geophys. Res., 99, 3469–3482, 1994. Lam, K. S., Wang, T. J., Chan, L. Y., Wang, T., and Harris, J.: Flow patterns influencing the seasonal behaviors of surface ozone and carbon monoxide at a coastal site near Hong Kong, Atmos. Environ., 35, 3121–3135, 2001. Law, K. S., Plantevin, P. H., Thouret, V., Marenco, A., Asman, W. A. H., Lawrence, M., Crutzen, P. J., Muller, J. F., Hauglustaine, D. A., and Kanakidou, M.: Comparison between global chemistry transport model results and Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) data, J. Geophys. Res., 105(D1), 1503–1525, 2000. Liu, J., Zhang, X. L., Zhang, X. C., and Tang, J.: Surface ozone characteristics and the correlated factors at Shangdianzi atmospheric background monitoring station, Research of Environmental Sciences (in Chinese), 19(4), 19–25, 2006. Liu, S. C., Trainer, M., Fehsenfeld, F. C., Parrish, D. D., Williams, E. J., Fahey, D. W., Hubler, G., and Murphy, P. C.: Ozone production in the rural troposphere and the implications for regional and global ozone production, J. Geophys. Res., 92, 4191–5207, 1987. Logan, J. A.: Tropospheric ozone: seasonal behavior trends, and anthropogenic influence. J. Geophys. Res., D6, 10 463–10 482, 1985. Logan, J. A.: Ozone in rural areas of the United States, J. Geophys. Res., 94, 8511–8532, 1989. Logan, J. A.: Trends in the vertical distribution of ozone: An analysis of ozonesonde data, J. Geophys. Res., 99, 25, 553–25, 585, 1994. Logan, J. A.: An analysis of ozonesonde data for the troposphere: Recommendations for testing 3-D models and development of a gridded climatology for tropospheric ozone, J. Geophys. Res., 104(D13), 16 115–16 149, 1999. Luo, C, John, J. C. S., Zhou, X. J., Lam, K. S., Wang, T., and Chameides, W. L.:A nonurban ozone air pollution eipsode over eastern China: Observations and model simulations, J. Geophys. Res., 105(D2), 1889–1908, 2000. Marenco, A., Thouret, V., Nedelec, P., Smit, H., Helten, M., Kley, D., Karcher, F., Simon, P., Law, K., Pyle, J., Poschmann, G., Wrede, R. V., Hume, C., and Cook, T: Measurement of ozone and water vapor by Airbus in-service aircraft: The MOZAIC airborne program, An overview, J. Geophys. Res., 103(D19), 25 631–25 642, 1998. McKee, D. J.: Tropospheric ozone: human health and agricultural impacts, Lewis Publishers, New York, 9–18, 1994. McKendry, I. G. and Lundgren, J.: Tropospheric layering of ozone in regions of urbanized complex and/or coastal terrain: a review, Prog. Phys. Geog., 24, 3, 329–354, 2000. Monks, P. S.: A review of the observations and origins of the spring ozone maximum, Atmos. Environ., 34, 3545–3561, 2000. Naja, M., and Akimoto H.: Contribution of regional pollution and long-range transport to the Asia – Pacific Region: Analysis of long-term ozonesonde data over Japan, J. Geophys. Res., 109, D21306, doi:10.1029/2004JD004687,2004. Nedelec, P., Thouret, V., Biroude, J., Sauvage, B., Cammas, J.-P., and Stohl, A.: Extreme CO concentrations in the upper troposphere over the northeast Asia in June 2003 from the in situ MOZAIC aircraft data, Geophys. Res. Lett. 32, L14807, doi:10.1029/2005GL023141, 2005. Neu, U., Kunzle, T., and Wanner, H.: On the relation between ozone storage in the residual layer and daily variation in near-surface ozone concentration – a case study, Bound. Lay. Meteorol., 69, 221–247, 1994. NRC (National Research Council): Rethinking the Ozone Problem in Urban and Regional Air Pollution, National Academy Press, Washington, D.C., 1991. Oltmans, S. J., Lefohn, A. S., Scheel, H. E., Harris, J. M., Levy II, H., Galbally, I. E., Brunke, E. G., Meyer, C. P., Lathrop, J. A., Johnson, B. J., Shadwick, D. S., Cuevas, E., Schmidlin, F. J., Tarasick, D. W., Claude, H., Kerr, J. B., Uchino, O., and Mohnen, V.: Trends of ozone in the troposphere, Geophys. Res. Lett., 25, 139–142, 1998. Pochanart, P., Akimoto, H., Kinjo, Y., and Tanimoto, H.: Surface ozone at four remote island sites and the preliminary assessment of the exceedances of its critical level in Japan, Atmos. Environ., 36, 4235–4250, 2002. Pochanart, P., Akimoto, H., Kajii, Y., Potemkin, V. M., and Khodzher, T. V.: Regional background ozone and carbon monoxide variations in remote Siberia/East Asia, J. Geophy. Res., 108(D1), 4028, doi:10.1029/2001JD001412, 2003. Qin, S. G., Ding, A. J., and Wang, T.: Transport pattern of biomass burnings air masses in Eurasia and the impacts on China, China Environment Science, 26(6), 641–645, 2006. Real, E., Law, K. S., Weinzierl, B., Fiebig, M., Petzold, A., Wild, O., Methven, J., Arnold, S., Stohl, A., Huntrieser, H., Roiger, A., Schlager, H., Stewart, D., Avery, M., Sachse, G., Browell, E., Ferrare, R., and Blake, D.: Processes influencing ozone levels in Alaskan forest fire plumes during long-range transport over the North Atlantic, J. Geophys. Res., 112, D10S41, doi:10.1029/2006JD007576, 2007. Reiter, R.: On the mean daily and seasonal variations of the vertical ozone profiles in the lower troposphere, Atmos. Environ., 25A, 1751–57, 1991. Richter, A., Burrows, J. P., Nub, H., Granier, C., and Niemeier, U.: Increase in tropospheric nitrogen dioxide over China observed from space, Nature, 437, 129–132, 2005. Shao, M., Tang, X. Y., Zhang, Y. H., and Li, W. J.: City clusters in China: air and surface water pollution, Frontiers in Ecology and the Environment, 4(7), 353–361, 2006. Streets, D. G., Bond T. C., Carmichael, G. R., Fernandes, S. D., Fu, Q., He, D., Klimont, Z., Nelson, S. M., Tsai, N. Y., Wang, 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. Taylor, J. K. and Cihon, C.: Statistical Techniques for data analysis, Second Edition, Chapman and Hall/CRC, 2004. Thouret, V., Marenco, A., Nedelec, P., and Grouhel, C.: Ozone climatologies at 9–12 km altitude as seen by the MOZAIC airborne program between September 1994 and August 1996, J. Geophys. Res., 103(D19), 25 653–25 679, 1998a. Thouret, V., Marenco, A., Logan, J. A., Nedelec, P., and Grouhel, C.: Comparison of ozone measurements from the MOZAIC airborne program and the ozone sounding network at eight locations, J. Geophys. Res., 103(D19), 25 695–25 720, 1998b. Thouret, V., Cammas, J. P., Sauvage, B., Athier, G., Zbinden, R., Nedelec, P., Simon, P., and Karcher, F.: Tropopause referenced ozone climatology and inter-annual variability (1994–2003) from the MOZAIC programme, Atmos. Chem. Phys., 6, 1033–1051, 2006. Wang, T., Cheung, T. F., Anson, M., and Li, Y. S.: Ozone and related gaseous pollutants in the boundary layer of eastern China: Overview of the recent measurements at a rural site, Geophys. Res. Lett., 28, 2373–2376, 2001. Wang, T., Cheung, T. F., Li, Y. S., Yu, X. M., and Blake, D. R.: Emission characteristics of CO, NO_x, SO₂ and indications of biomass burning observed at a rural site in eastern China, J. Geophys. Res., 107, 4157–4167, 2002. Wang, T., Ding, A. J., Gao., J., and Wu, W. S.: Strong ozone production in urban plumes from Beijing, China, Geophys. Res. Lett., 33(21), L21806, doi:10.1029/2006GL027689, 2006a. Wang, T., Guo, H., Blake, D. R., Kwok, Y. H., Simpson, I. J., and Li, Y. S.: Measurements of trace gases in the inflow of South China Sea background air and outflow of regional pollution at Tai'O, Southern China, J. Atmos. Chem., 52(3), 295–317, 2005. Wang, T. and Kwok, J. Y. H.: Measurement and analysis of a multiday photochemical smoge episode in the Pearl River Delta of China, J. Appl. Meteorol., 42, 404–416, 2003. Wang, T., Wong, H. L. A., Tang, J., Ding, A., Wu, W. S., and Zhang, X. C.: On the origin of surface ozone and reactive nitrogen observed at a remote mountain site in the northeastern Qinhai-Tibetan Plateau, western China, J. Geophys. Res., 111, D08303, doi:10.1029/2005JD006527, 2006b. Xu, X. B., Lin, W. L., Wang, T., Yan, P., Tang, J., Meng, Z. Y., and Wang, Y.: Enhanced variability of surface ozone at a regional background station in eastern China 1991–2006, Geophys. Res. Lett., unpublished results, 2007. Zbinden, R. M., Cammas, J. P., Thouret, V., Nedelec, P., Karcher, F., and Simon, P.: Mid-latitude tropospheric ozone columns from the MOZAIC program: climatology and inter-annual variability, Atmos. Chem. Phys., 6, 1053–1073, 2006. Zheng, X. D., Zhou, X. J., Tang, J., Qin, Y., and Chan, C. Y.: A meteorological analysis on a low tropospheric ozone event over Xining, North Western China on 26–27 July 1996, Atmos. Environ., 38(2), 261–271, 2004.