Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 7 23 2007 10.5194/acp-7-5971-2007 http://www.atmos-chem-phys.net/7/5971/2007/ http://www.atmos-chem-phys.net/7/5971/2007/acp-7-5971-2007.html http://www.atmos-chem-phys.net/7/5971/2007/acp-7-5971-2007.pdf 5971 5987 2007-12-07 SCIAMACHY tropospheric NO₂ over Switzerland: estimates of NO_x lifetimes and impact of the complex Alpine topography on the retrieval D. Schaub D. Brunner dominik.brunner@empa.ch K. F. Boersma J. Keller D. Folini B. Buchmann H. Berresheim J. Staehelin Empa, Swiss Federal Laboratories for Materials Testing and Research, Ueberlandstrasse 129, 8600 Duebendorf, Switzerland School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA Paul Scherrer Institute (PSI), 5232 Villigen PSI, Switzerland German National Meteorological Service, DWD/MOHp, 82383 Hohenpeissenberg, Germany Swiss Federal Institute of Technology (ETH), Universitätstrasse 16, 8092 Zurich, Switzerland now at: National University of Ireland Galway, Department of Physics, University Road, Galway, Ireland This study evaluates NO₂ vertical tropospheric column densities (VTCs) retrieved from measurements of the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) above Switzerland and the Alpine region. The close correlation between pixel averaged NO_x emission rates from a spatially and temporally highly resolved inventory and the NO₂ VTCs under anticyclonic meteorological conditions demonstrates the general ability of SCIAMACHY to detect sources of NO_x pollution in Switzerland. This correlation is further used to infer seasonal mean NO_x lifetimes carefully taking into account the influence of the strong diurnal cycle in NO_x emissions on these estimates. Lifetimes are estimated to 3.6 (±0.8) hours in summer and 13.1 (±3.8) hours in winter, the winter value being somewhat lower than previous estimates. A comparison between the 2003-2005 mean NO₂ VTC distribution over Switzerland and the corresponding 1996–2003 mean from the Global Ozone Monitoring Experiment (GOME) illustrates the much better capability of SCIAMACHY to resolve regional scale pollution features. However, the comparison of seasonal averages over the Swiss Plateau with GOME and ground based in situ observations indicates that SCIAMACHY exhibits a too weak seasonal cycle with comparatively high values in summer and low values in winter. A problem likely contributing to the reduced values in winter (not reported in earlier literature) is the use of inaccurate satellite pixel surface pressures derived from a coarse resolution global model in the retrieval. The marked topography in the Alpine region can lead to deviations of several hundred meters between the model assumed and the real pixel-averaged surface height. A sensitivity study based on selected clear sky SCIAMACHY NO₂ VTCs over the Swiss Plateau and two fixed a priori NO₂ profile shapes indicates that inaccurate pixel surface pressures affect retrieved NO₂ columns over complex terrain by up to 40%. For retrievals in the UV-visible spectral range with a decreasing sensitivity towards the earth's surface, this effect is of major importance when the NO₂ resides close to the ground, a situation most frequently observed during winter. Beirle, S., Platt, U., Wenig, M., and Wagner, T.: Weekly cycle of NO₂ by GOME measurements: a signature of anthropogenic sources, Atmos. Chem. Phys., 3, 2225–2232, 2003. Beirle, S., Platt, U., Wenig, M., and Wagner, T.: Highly resolved global distribution of tropospheric NO₂ using GOME narrow swath mode data, Atmos. Chem. Phys., 4, 1913–1924, 2004. Blond, N., Boersma, K. F., Eskes, H. J., van der A, R. J., Van Roozendael, M., De Smedt, I., Bergamatti, G., and Vautard, R.: Intercomparison of SCIAMACHY nitrogen dioxide observations, in situ measurements and air quality modeling results over Western Europe, J. Geophys. Res., 112, D10311, doi:10.1029/2006JD007277, 2007. Boersma, K. F., Eskes, H. J., and Brinksma, E. J.: Error analysis for tropospheric NO₂ retrieval from space, J. Geophys. Res., 109, D04311, 2004. 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, 2007. Bovensmann, H., Burrows, J. P., Buchwitz, M., Frerick, J., No\"el, S., and Rozanov, V. V.: SCIAMACHY: Mission objectives and measurement modes, J. Atmos. Sci., 56, 2, 127–150, 1999. Burrows, J. P., Weber, M., Buchwitz, M., Rozanov, V., Ladstätter-Weissenmayer, A., Richter, A., DeBeek, R., Hoogen, R., Bramstedt, K., Eichmann, K. U., Eisinger, M., and Perner, D.: The global ozone monitoring experiment (GOME): Mission concept and first scientific results, J. Atmos. Sci., 56, 151–175, 1999. Chu, S. H. and Meyer, E. L.: Use of ambient ratios to estimate impact of NO_x sources on annual NO₂ concentrations, Proceedings, 84 Annual Meeting and Exhibition of the Air and Waste Management Association, Vancouver, B.C., 16–21 June 1991,91–180.6, 16 pp., 1991. Dentener, F. J. and Crutzen, P. J.: Reaction of N₂O$_5$ on tropospheric aerosols: impact on the global distributions of NO_x, O₃ and OH, J. Geophys. Res., 98, 7149–7163, 1993. Dentener, F. J., van Weele, M., Krol, M., Houweling, S., and van Velthoven, P.: Trends and inter-annual variability of methane emissions derived from 1979–1993 global CTM simulations, Atmos. Chem. Phys., 3, 73–88, 2003. Dommen, J., Prévôt, A. S. H., Hering, A. M., Staffelbach, T., Kok, G. L., and Schillawski, R. D.: Photochemical production and aging of an urban air mass, J. Geophys. Res., 104, D5, 5493–5509, 1999. Eskes, H. J.: Combined retrieval, modeling and assimilation approach to GOME NO₂, in GOA final report, European Commission 5th framework programme 1998–2002, EESD-ENV-99-2, 116–122, Eur. Comm., De Bilt, Netherlands, 2003. Finlayson-Pitts, B. J. and Pitts, J. N.: Chemistry of the upper and lower Atmosphere – Theory, Experiments and Applications, Academic Press, San Diego, CA, 2000. FOEN (Swiss Federal Office for the Environment, BAFU): Vom Menschen verursachte Luftschadstoffemissionen in der Schweiz von 1900 bis 2010, Schriftenreihe Umwelt Nr. 256, 1995. FOEN (Swiss Federal Office for the Environment, BAFU): NABEL – Luftbelastung 2004, Schriftenreihe Umwelt Nr. 388, 2005. Hueglin, C., Buchmann, B., and Weber, R. O.: Long-term observation of real-world road traffic emission factors on a motorway in Switzerland, Atmos. Environ., 40, 3696–3709, 2006. IPCC, Climate Change 2001: The Scientific Basis, Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge University Press, Cambridge, UK and New York, USA, 2001. Jaeglé, L., Jacob, D. J., Wang, Y., Weinheimer, A. J., Ridley, B. A., Campos, T. L., Sachse, G. W., and Hagen, D. E.: Sources and chemistry of NO_x in the upper troposphere over the United States, Geophys. Res. Lett., 25, 1705–1708, 1998. Keller, J., Andreani-Aksoyoglu, S., Tinguely, M., and Prévôt, A. S. H.: Emission Scenarios 1985–2010: Their Influence on Ozone in Switzerland, PSI Bericht Nr. 05–07, Paul Scherrer Institut, Villigen PSI, 2005. Keller, M. and Zbinden, R.: Luftschadstoffemissionen des Strassenverkehrs 1980–2030, Schriftenreihe Umwelt Nr. 355, FOEN (Swiss Federal Office for the Environment), 2004. Koelemeijer, R. B. A., Stammes, P., Hovenier, J. W., and de Haan, J. F.: A fast method for retrieval of cloud parameters using oxygen A-band measurements from Global Ozone Monitoring Experiment, J. Geophys. Res., 106, 3475–3490, 2001. Kramm, G., Dlugi, R., Dollard, G. J., Foken, T., Mölders, N., Müller, H., Seiler, W., and Sievering, H.: On the dry deposition of ozone and reactive nitrogen species, Atmos. Environ., 29, 3209–3231, 1995. Kühlwein, J.: Uncertainties in the arithmetical determination of pollutant emissions from road traffic and demands on future models, PhD thesis, University of Stuttgart, 2004. Kühlwein, J. and Friedrich, R.: Uncertainties of modelling emissions from road transport, Atmos. Environ., 34, 4603–4610, 2000. Kunhikrishnan, T., Lawrence, M. G., von Kuhlmann, R., Richter, A., Ladstätter-Weissenmayer, A., and Burrows, J. P.: Analysis of tropospheric NO_x over Asia using the model of atmospheric transport and chemistry (MATCH-MPIC) and GOME-satellite observations, Atmos. Environ., 38, 581–596, 2004. Leue, C., Wenig, M., Wagner, T., Klimm, O., Platt, U., and Jahne, B.: Quantitative analysis of NO_x emissions from Global Ozone Monitoring Experiment satellite image sequences, J. Geophys. Res., 106, 5493–5505, 2001. 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 NO$_2 $columns, J. Geophys. Res., 108, D17, 4537, doi:10.1029/2003JD003453, 2003. MeteoSwiss: Alpine Weather Statistics (Alpenwetterstatistik – Witterungskalender: Beschreibung der einzelnen Parameter), MeteoSwiss, Switzerland, 1985. Mihelcic, D., Holland, F., Hofzumahaus, A., Hoppe, L., Konrad, S., Müsgen, P., Pätz, H.-W., Schäfer, H.-J., Schmitz, T., Volz-Thomas, A., Bächmann, K., Schlomski, S., Platt, U., Geyer, A., Alicke, B., and Moortgat, G. K.: Peroxy radicals during BERLIOZ at Pabsttum: measurements, radical budgets and ozone production, J. Geophys. Res., 108, D4, 8254, doi:10.1029/2001JD001014, 2003. Nunnermacker, L. J., Kleinman, L. I., Imre, D., Daum, P. H., Lee, Y.-N., Lee, J. H., Springston, S. R., and Newman, L.: NO$_y$ lifetimes and O₃ production efficiencies in urban and power plant plumes: analysis of field data, J. Geophys. Res., 105, D7, 9165–9176, 2000. Palmer, P. I., Jacob, D. J., Chance, K., Martin, R. V., Spurr, R. J. D., Kurosu, T. P., Bey, I., Yantosca, R., Fiore, A., and Li, Q.: Air mass factor formulation for spectroscopic measurements from satellites: Application to formaldehyde retrievals from the Global Ozone Monitoring Experiment, J. Geophys. Res., 106, 14 539–14 550, 2001. Palmer, P. I., Jacob, D. J., Fiore, A. M., Martin, R. V., Chance, K., and Kurosu, T. P.: Mapping isoprene emissions over North America using formaldehyde column observations from space, J. Geophys. Res., 108, D6, 4180, doi:10.1029/2002JD002153, 2003. Petritoli, A., Bonasoni, P, Giovanelli, G., Ravegnani, F., Kostadinov, I., Bortoli, D., Weiss, A., Schaub, D., Richter, A., and Fortezza, F.: First comparison between ground-based and satellite-borne measurements of tropospheric nitrogen dioxide in the Po basin, J. Geophys. Res., 109, D15307, doi:10.1029/2004JD004547, 2004. Platt, U.: Differential optical absorption spectroscopy (DOAS), Chem. Anal. Series, 127, 27–83, 1994. Richter, A. and Burrows, J. P.: Tropospheric NO₂ from GOME measurements, Adv. Space Res., 29, 1673–1683, 2002. Richter, A., Burrows, J. P., Nüss, H., Granier, C., and Niemeier, U.: Increase in tropospheric nitrogen dioxide over China observed from space, Nature, 437, doi:10.1038/nature04092, 2005. Rohrer, F. and Berresheim, H.: Strong correlation between levels of tropospheric hydroxyl radicals and solar ultraviolet radiation, Nature, 442, 184–187, 2006. Ryerson, T. B., Buhr, M. P., Frost, G. J., Goldan, P. D., Holloway, J. S., Hübler, G., Jobson, B. T., Kuster, W. C., McKeen, S. A., Parrish, D. D., Roberts, J. M., Sueper, D. T., Trainer, M., Williams, J., and Fehsenfeld, F. C.: Emissions lifetimes and ozone formation in power plant plumes, J. Geophys. Res., 103, D17, 22 569–22 583, 1998. Schaub, D., Boersma, K. F., Kaiser, J. W., Weiss, A. K., Eskes, H. J., and Buchmann, B.: Comparison of GOME tropospheric NO₂ columns with NO₂ profiles deduced from ground-based in situ measurements, Atmos. Chem. Phys., 6, 3211–3229, 2006. Schaub, D., Weiss, A. K., Kaiser, J. W., Petritoli, A., Richter, A., Buchmann, B., and Burrows, J. P.: A transboundary transport episode of nitrogen dioxide as observed from GOME and its impact in the Alpine region, Atmos. Chem. Phys., 5, 23–37, 2005. Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics – from air pollution to climate change, John Wiley and Sons, New York, 1998. Sillman, S.: Ozone production efficiency and loss of NO_x in power plant plumes: photochemical model and interpretation of measurements in Tennessee, J. Geophys. Res., 105, D7, 9189–9202, 2000. Solomon, S., Portmann, W., Sanders, R. W., Daniel, J. S., Madsen, W., Bartram, B., and Dutton, E. G.: On the role of nitrogen dioxide in the absorption of solar radiation, J. Geophys. Res., 104, 12 047–12 058, 1999. Spicer, C. W.: Nitrogen oxide reactions in the urban plume of Boston, Science, 215, 4536, 1095–1097, 1982. Stammes, P.: Spectral radiance modelling in the UV-Visible Range, in IRS 2000: Current problems in Atmospheric Radiation, Edited by: Smith, W. L. and Timofeyev, Y. M.: A. Deepak Publ., Hampton (VA), 2001. Steinbacher, M., Zellweger, C., Schwarzenbach, B., Bugmann, S., Buchmann, B., Ordo\~nez, C., Prevot, A. S. H., and Hueglin, C.: Nitrogen dioxide measurements at rural sites in Switzerland: Bias of conventional measurement techniques, J. Geophys. Res., 112, D11307, doi:10.1029/2006JD007971, 2007. Uno, I., He, Y., Ohara, T., Yamaji, K., Kurokawa, J.-I., Katayama, M., Wang, Z., Noguchi, K., Hayashida, S., Richter, A., and Burrows, J. P.: Systematic analysis of interannual and seasonal variations of model-simulated tropospheric NO₂ in Asia and comparison with GOME-satellite data, Atmos. Chem. Phys. Disc., 6, 11 181–11 207, 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. Vandaele, A. C., Fayt, C., Hendrick, F., et al.: An intercomparison campaign of ground-based UV-visible measurements of NO₂, BrO, and OClO slant columns: Methods of analysis and results for NO₂, J. Geophys. Res., 110, D08305, doi:10.1029/2004JD005423, 2005. van Noije, T. P. C., Eskes, H. J., Dentener, F. J. , Stevenson, D. S., et al.: Multi-model ensemble simulations of tropospheric NO₂ compared with GOME retrievals for the year 2000, Atmos. Chem. Phys., 6, 2943–2979, 2006. Volz-Thomas, A., Geiss, H., Hofzumahaus, A., and Becker, K.-H.: Introduction to special section: photochemistry experiment in BERLIOZ, J. Geophys. Res., 108, D4, 8252, doi:10.1029/2001JD002029, 2003. Volz-Thomas, A. and Kolahgar, B: On the budget of hydroxyl radicals at Schauinsland during the Schauinsland Ozone Precursor Experiment (SLOPE96), J. Geophys. Res., 105, D1, 1611–1622, 2000. York, D.: Least-square fitting of a straight line, Can. J. Phys., 44, 1079–1086, 1966.