References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-6-2091-2006

Sensitivity analysis by the adjoint chemistry transport model DRAISfor an episode in the Berlin Ozone (BERLIOZ) experiment

Nester

¹ Panitz

H.-J.

Institut für Meteorologie und Klimaforschung (IMK), ForschungszentrumKarlsruhe/Universität Karlsruhe, Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany

20 06 2006

6 8 2091 2106

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys.net/6/2091/2006/acp-6-2091-2006.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/6/2091/2006/acp-6-2091-2006.pdf

The Berlin Ozone Experiment (BERLIOZ) was carried out in summer 1998. One of its purposes was the evaluation of Chemistry Transport Models (CTM). CTM KAMM/DRAIS was one of the models considered. The data of 20 July were selected for evaluation. On that day, a pronounced ozone plume developed downwind of the city. Evaluation showed that the KAMM/DRAIS model is able to reproduce the meteorological and ozone data observed, except at farther distances (60–80 km) downwind of the city. In that region, the DRAIS model underestimates the measured ozone concentrations by 10–15 ppb, approximately. Therefore, this study was conducted to detect possible reasons for this deviation. A comprehensive sensitivity analysis was carried out to determine the most relevant model parameters. The adjoint DRAIS model was developed for this purpose, because for this study the application of this model is the most effective method of calculating the sensitivities. The least squares of the measured and simulated ozone concentrations between 08:00 UTC and 16:00 UTC at two stations 30 km and 70 km downwind of the city centre were chosen as distance function. The model parameters considered in this study are the complete set of initial and boundary species concentrations, emissions, and reaction rates, respectively. A sensitivity ranking showing the relevance of the individual parameters in the set is determined for each parameter set. In order to find out which modification in the parameter sets most reduces the cost function, simplified 4-D data assimilation was carried out. The result of this data assimilation shows that modifications of the reaction rates provide the best agreement between the measured and the simulated ozone concentrations at both stations. However, the modified reaction rates seem to be unrealistic for the whole simulation period. Therefore, the good agreement should not be overestimated. The agreement is still acceptable when the parameters in the other sets are modified together. The investigation demonstrates that an analysis of this type can help to explain inconsistencies between observations and simulations. But in the case considered here the inconsistencies cannot be explained by an error in only one parameter set.

References 1

Adrian, G. and Fiedler, F.: Simulation of unstationary wind and temperature fields over complex terrain and comparison with observations, Contrib. Atmos. Phys., 64, 27-48, 1991.

Baer, M. and Nester, K.: Parametrization of trace gas dry deposition velocities for a regional mesoscale diffusion model, Ann. Geophys., 10, 912-923, 1992.

Becker, K. H., Donner, B., and Gäb, S.: BERLIOZ: A field experiment within the German Tropospheric Research Programme, in: Proc. of EUROTRAC Symposium 98, vol. 2, edited by: Borrell, P. M. and Borrell, P., WIT-Press, Southampton, 669-672, 1999.

Chang, J. S., Brost, A., Isaksen, I. S. A., Madronich, S., Middleton, P., Stockwell, W. R., and Walceck, C. J.: A three-dimensional Eulerian acid deposition model: Physical concepts and formulation, J. Geophys. Res., 92, 14 618-14 700, 1987.

Corsmeier, U., Kalthoff, N., Vogel, B., Hammer, M.-U., Fiedler, F., Kottmeier, Ch., Volz-Thomas, A., Konrad, S., Glaser, K., Neininger, B., Lehning, M., Jaeschke, W., Memmesheimer, M., Rappenglück, B., and Jakobi, G.: Ozone and PAN formation inside and outside of the BERLIN plume-Process analysis and numerical process simulation, J. Atmos. Chem., 42, 289-321, 2002.

Degrazia, G. A.: Anwendung von Ähnlichkeitsverfahren auf die turbulente Diffusion in der konvektiven und stabilen Grenzschicht, Dissertation, Fakultät für Physik der Universität Karlsruhe, Institut für Meteorologie und Klimaforschung, 1988.

Dufour, A., Amodel, M., Ancellet, G., and Peuch, V. H.: Observed and modelled "chemical weather" during ESCOMPTE, Atmos. Res., 74, 161-189, 2005.

Ebel, A., Elbern, H., Feldmann, H., Jakobs, H. J., Kessler, C., Memmesheimer, M., Oberreuter, A., and Piekorz, G.: Air pollution studies with the EURAD model system (3): EURAD-European air pollution dispersion model system, Mitteilungen aus dem Institut für Geophysik und Meteorologie der Universität Köln, Heft 120, p. 172, 1997.

Elbern, H., Schmidt, H., Talagrand, O., and Ebel, A.: 4D-variational data assimilation with an adjoint air quality model for emission analysis, Environ. Modelling & Software, 15, 539-548, 2000.

Elbern, H. and Schmidt, H.: Ozone episode analysis by four-dimensional variational chemistry data assimilation, J. Geophys. Res., 106(D4), 3569-3590, 2001.

Elbern, H. and Schmidt, H.: The development of a 4d variational chemistry data assimilation scheme for initial value and emission rate estimates, in: Proceedings of the 6th GLOREAM Workshop, Aveiro, Portugal, 4-6 September, edited by: Borego, C., Builtjes, P., Miranda, A. I., Santos, P., and Carvalho, A. C., 123-132, 2002.

Elizondo, D., Cappelaere, B., and Faure, Ch.: Automatic versus manual model differentiation to compute sensitivities and solve non-linear inverse problems, Computers & Geosciences, 28, 309-326, 2002.

Giering, R. and Kaminski, T.: Recipes for adjoint code construction, ACM Transactions on Mathematical Software, 24(4), 437-474, 1998.

Memmesheimer, M., Ebel, A., and Roemer, F.: Budget calculations for ozone and its precursors: Seasonal and episodic features based on model simulations, J. Atmos. Chem., 28, 283-317, 1997.

Menut, L.: Adjoint modelling for atmospheric pollution process sensitivity at regional scale, J. Geophys. Res., 108(D17), ESQ 5 1-17, 2003.

Nester, K. and Fiedler, F.: Modeling of the diurnal variation of air pollutants in a mesoscale area, Proceedings of the 9th World Clean Air Congress, Montreal, 5, Paper-No. IU-16C.02, 1992.

Nester, K., Fiedler, F. Panitz, H.-J., and Zhao, T.: Simulation of an episode of the BERLIOZ experiment and comparison with measured data, in: Proceedings 4th GLOREAM Workshop, Cottbus, Germany, 20-22 September, edited by: Schaller, E., Builtjes, P, and Münzenberg, A., 8-16, 2000.

Nester, K. and Panitz, H.-J.: Evaluation of the chemistry transport model system KAMM/DRAIS based on daytime ground level ozone data, Int. J. Environ. Pollut., 22(1/2), 87-107, 2004.

Palacios, M., Kirchner, F., Martilli, A., Clappier, A., Martin, F., and Rodrigues, M. E.: Summer ozone episodes in the Greater Madrid Area. Analyzing the ozone response to abatement strategies by modelling, Atmos. Environ., 36, 5323-5333, 2002.

Panitz, H.-J., Nester, K., and Fiedler, F.: Determination of mass balances of chemically reactive air pollutants over Baden-Württemberg (F.R.G.) - Study for the regions around the cities of Stuttgart and Freudenstadt, in: Air Pollution V, edited by: Power, H., Tirabassi, T., Brebbia, C. A., Computational Mechanics Publications, Southampton, Boston, 413-422, 1997.

Panitz, H.-J. and Nester, K.: Mass budget simulations of ozone in the city plume of Berlin for an episode of the BERLIOZ experiment, Companion CD-ROM of: Transport and Chemical Transformation in the Troposphere, edited by: Midgley, P. and Reuther, M., Proceedings of the EUROTRAC Symposium 2002, Garmisch-Partenkirchen, Germany, 11-15 March; see also http://www-fzk.imk.uni-karlsruhe.de/fi/fzk/imk/seite_1513.php, 2002.

Peleg, M., Luria, M., Sharf, G., Vanger, A., Kallos, G., Kotroni, V., Lagouvardos, K., and Varinou, M.: Observational evidence of an ozone episode over the Greater Athens Area, Atmos. Environ., 31, 3969-3983, 1997.

Plaza, J., Pujadas, M., and Artinano, B.: Formation and transport of the Madrid ozone plume, J. Air Waste Manage. Assoc., 47, 766-774, 1997.

Prevot, A. S. H., Staehlin, L., Kok, G. L., Schillawski, R. D., Neininger, B., Staffelbach, T., Neftel, A., Wernli, H., and Dommen, J.: The Milan photooxidant plume, J. Geophys. Res., 102, 23 375-23 388, 1997.

Pudykiewicz, J. A.: Application of adjoint tracer transport equations for evaluating source parameters, Atmos. Environ., 32(17), 3039-3050, 1998.

Rostaing, N., Dalmas, S., and Galligo, A.: Automatic differentiation in Odyssée, Tellus, 45A, 558-568, 1993.

Schädler, G., Kalthoff, N., and Fiedler, F.: Validation of a model for heat, mass and momentum exchange over vegetated surfaces using LOTREX-10E/HIBE88 data, Contrib. Atmos. Phys., 63, 85-100, 1990.

Schmidt, H. and Martin, D.: Adjoint sensitivity of episodic ozone in the Paris area to emissions on the continental scale, J. Geophys. Res., 108(D17), ESQ 4 1-16, 2003.

Slemr, F., Baumbach, G., Blank, P., Corsmeier, U., Fiedler, F., Friedrich, R., Habram, M., Kalthoff, N., Klemp, D., Kühlwein, J., Mannschreck, K., Möllmann-Coers, M., Nester, K., Panitz, H.-J., Rabl, P., Slemr, J., Vogt, U., and Wickert, B.: Evaluation of modelled spatially and temporally highly resolved emission inventories of photosmog precursors for the city of Augsburg: the experiment EVA and its major results, J. Atmos. Chem., 42, 207-233, 2002.

Stockwell, W. R., Middelton, P., and Chang, J. S.: The second generation Regional Acid Deposition Model, chemical mechanism for regional air quality modeling, J. Geophys. Res., 95(D10), 16 343-16 367, 1990.

Thuburn, J. and Haine, T. W. N.: Adjoints of nonoscillatory advection schemes, J. Comput. Phys., 171, 616-631, 2001.

Talagrand, O. and Courtier, P.: Variational assimilation of meteorological observations with the adjoint vorticity equation. I: Theory, Quart. J. Roy. Meteorol. Soc., 113, 1311-1328, 1987.

Ustinov, E. A.: Adjoint sensitivity analysis of atmospheric dynamics: Application to the case of multiple observables, J. Atmos. Sci., 58(21), 3340-3348, 2001.

Vautard, R., Beekmann, M., and Menut, L.: Applications of adjoint modelling in atmospheric chemistry: sensitivity and inverse modelling, Environ. Modelling & Software, 25, 703-709, 2000.

Vautard, R., Menut, L., Beekmann, M., Chazette, P., Flamant, P. H., Gombert, D., Kley, D., Lefebvre, M. P., Marti, D., Megie, G., Perros, P., and Toupance, G.: A synthesis of air pollution over the Paris region (ESQUIF) field campaign, J. Geophys. Res.-Atmos., 108(D17, 8558, doi:10.1029/2003JD003380, 2003.

Vogel, B., Fiedler, F., and Vogel, H.: Influence of topography and biogenic volatile organic compounds emission in the state of Baden-Württemberg on ozone concentrations during episodes of high air temperatures, J. Geophys. Res., 100, 22 907-22 928, 1995.

Wotawa, G., Stohl, A., and Neininger, B.: The urban plume of Vienna: Comparison between aircraft measurements and photochemical model results, Atmos. Environ., 32, 2479-2489, 1998.