Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 6 11 2006 10.5194/acp-6-3487-2006 http://www.atmos-chem-phys.net/6/3487/2006/ http://www.atmos-chem-phys.net/6/3487/2006/acp-6-3487-2006.html http://www.atmos-chem-phys.net/6/3487/2006/acp-6-3487-2006.pdf 3487 3503 2006-08-25 A Lagrangian analysis of the impact of transport and transformation on the ozone stratification observed in the free troposphere during the ESCOMPTE campaign A. Colette augustin.colette@aero.jussieu.fr G. Ancellet L. Menut S. R. Arnold Service d'Aéronomie/Institut Pierre-Simon Laplace, Centre National de la Recherche Scientifique, Université Pierre et Marie Curie, 4, place Jussieu, P.O. Box 102, 75252 Paris Cedex 05, France Laboratoire de Météorologie Dynamique/Institut Pierre-Simon Laplace, Centre National de la Recherche Scientifique, Ecole Polytechnique, 91128 Palaiseau Cedex, France Institute for Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK The ozone variability observed by tropospheric ozone lidars during the ESCOMPTE campaign is analyzed by means of a hybrid-Lagrangian modeling study. Transport processes responsible for the formation of ozone-rich layers are identified using a semi-Lagrangian analysis of mesoscale simulations to identify the planetary boundary layer (PBL) footprint in the free troposphere. High ozone concentrations are related to polluted air masses exported from the Iberian PBL. The chemical composition of air masses coming from the PBL and transported in the free troposphere is evaluated using a Lagrangian chemistry model. The initial concentrations are provided by a model of chemistry and transport. Different scenarios are tested for the initial conditions and for the impact of mixing with background air in order to perform a quantitative comparison with the lidar observations. For this meteorological situation, the characteristic mixing time is of the order of 2 to 6 days depending on the initial conditions. Ozone is produced in the free troposphere within most air masses exported from the Iberian PBL at an average rate of 0.2 ppbv h^−1, with a maximum ozone production of 0.4 ppbv h^−1. Transport processes from the PBL are responsible for an increase of 13.3 ppbv of ozone concentrations in the free troposphere compared to background levels; about 45% of this increase is attributed to in situ production during the transport rather than direct export of ozone. Ancellet, G. and Ravetta, F.: A compact airborne lidar for tropospheric ozone (ALTO): description and field measurements, Appl. Opt., 37, 5509–5521, 1998. Ancellet, G. and Ravetta, F.: Analysis and validation of ozone variability observed by lidar during the ESCOMPTE-2001 campaign, Atmos. Res., 74, 435–459, 2005. Bastin, S. and Drobinski, P.: Sea breeze induced mass transport over complex terrain in southeastern France: A case study, Quart. J. Roy. Met. Soc., 132, 405–423, 2006. Bastin, S., Drobinski, P., Dabas, A., Delville, P., Reitebuch O., and Werner, C.: Impact of the Rhône and Durance valleys on sea-breeze circulation in the Marseille area, Atmos. Res., 74, 303–328, 2005. Bernsten, T K., Isaksen, I S A., Myhre, G., Fuglestvedt, J S., Stordal, F., Larsen, T A., Freckleton, R S., and Shine, K P.: Effects of anthropogenic emissions on tropospheric ozone and its radiative forcing, J. Geophys. Res., 102, 28 101–28 126, 1997. Bevington, P R. and Robinson, D K.: Data reduction and error analysis for the physical sciences, 2nd edition, McGraw-Hill Book Co, New York, USA, 328 p., 1992. Coll I., Pinceloup, S., Perros, P. E., Laverdet, G., and Le Bras, G.: 3D analysis of the High Ozone Production Rates observed during the ESCOMPTE campaign, J. Atmos. Res., 74, 477–505, 2005. Cooper, O R., Moody, J L., Parrish, D D., Trainer, M., Ryerson, T B., Holloway, J S., Hubler, G., Fehsenfel, F C., and Evans, M J.: Trace gas composition of midlatitude cyclones over the western North Atlantic Ocean: A conceptual model, J. Geophys. Res., 107(D7), doi:10.1029/2001JD000901, 2002. Corsmeier, U., Behrendt, R., Drobinski P., and Kottmeier, C.: The mistral and its effect on air pollution transport and vertical mixing, Atmos. Res., 74, 275–302, 2005. Cotton, W R., Alexander, G D., Hertenstein, R., Walko, R L., McAnelly, R L., and Nicholls, M.: Cloud venting, A review and some new global annual estimates, Earth-Sci. Rev., 39(3–4), 169–206, 1995. Cousin, F., Tulet, P., and Rosset, R.: Interaction between local and regional pollution during ESCOMPTE 2001: impact on surface ozone concentrations (IOP2a and 2b), Atmos. Res., 74, 117–137, 2005. Cros, B. and Durand, P.: Preface, Guest editors, Atmos. Res., 74(1–4), 2005. Cros, B., Durand, P., Cachier, H., Drobinski, P., Fréjafon, E., Kottmeier, C., Perros, P. E., Peuch, V.-H., Ponche, J.-L., Robin, D., et al.: The ESCOMPTE program: an overview, Atmos. Res., 69, 241–279, 2004. Dufour, A., Amodei, M., Ancellet, G., and Peuch, V.-H.: Observed and modelled "chemical weather" during ESCOMPTE, Atmos. Res., 74, 161–189, 2005. Eckhardt, S., Stohl, A., Beirle, S., Spichtinger, N., James, P., Forster, C., Junker, C., Wagner, T., Platt, U., and Jennings, S. G.: The North Atlantic Oscillation controls air pollution transport to the Arctic, Atmos. Chem. Phys., 3, 1769–1778, 2003. ECMWF: User Guide to ECMWF Products 2.1, Meteorological Bulletin M3.2, ECMWF, Reading, UK, 49 p., 1995. Evans, M J., Shallcross, D E., Law, K S., Wild, J O F., Simmonds, P G., Spain, T G., Berrisford, P., Methven, J., Lewis, A C., McQuaid, J B., Pillinge, M J., Bandyf, B J., Penkettf, S A., and Pyle, J A.: Evaluation of a Lagrangian box model using field measurements from EASE (Eastern Atlantic Summer Experiment) 1996, Atmos. Environ., 34(23), 3843–3863, 2000. Gangoiti, G., Millán, M M., Salvador, R., and Mantilla, E.: Long-range transport and re-circulation of pollutants in the western Mediterranean during the project Regional Cycles of Air Pollution in the West-Central Mediterranean Area, Atmos. Environ., 35(36), 6267–6276, 2001. GENEMIS: Generation of European Emission Data for Episodes project, EUROTRAC annual report 1993, part 5, EUROTRAC international scientific secretariat, Garmisch-Partenkirchen, Germany, 1994. Gheusi, F. and Stein, J.: Lagrangian description of airflows using Eulerian passive tracers, Quart. J. Roy. Met. Soc., 128, 337–360, 2002. Gheusi, F., Cammas, J. -P., Cousin, F., Mari, C., and Mascart, P.: Quantification of mesoscale transport across the boundaries of the free troposphere: a new method and applications to ozone, Atmos. Chem. Phys. Discuss., 4, 8103–8139, 2004. Good, P., Giannakopoulos, C., O'Connor, F M., Arnold, S R., de Reus, M., and Schlager, H.: Constraining tropospheric mixing timescales using airborne observations and numerical models, Atmos. Chem. Phys., 3, 1023–1035, 2003. Hasel, M., Kottmeier, C., Corsmeier, U., and Wieser, A.: Airborne measurements of turbulent trace gas fluxes and analysis of eddy structure in the convective boundary layer over complex terrain, Atmos. Res., 74, 381–402, 2005. Hauf, T., Schulte, P., Alheit, R., and Schlager, H.: Rapid vertical trace gas transport by an isolated midlatitude thunderstorm, J. Geophys. Res., 100(D11), 22 957–22 970, 1995. Hauglustaine, D. A., Hourdin, F., Jourdain, L., Filiberti, M.-A., Walters, S., Lamarque, J.-F., and Holland, E A.: Interactive chemistry in the Laboratoire de Météorologie Dynamique general circulation model: Description and background tropospheric chemistry evaluation, J. Geophys. Res., 109, doi:10.1029/2003JD003957, 2004. Henne, S., Furger, M., Nyeki, S., Steinbacher, M., Neininger, B., deWekker, S F J., Dommen, J., Spichtinger, N., Stohl, A., and Prévôt, A S H.: Quantification of topographic venting of boundary layer air to the free troposphere, Atmos. Chem. Phys., 4, 497–509, 2004. Kalthoff, N., Kottmeier, C., Thürauf, J., Corsmeier, U., Sa\"\id, F., Fréjafon, E., and Perros, P E.: Mesoscale circulation systems and ozone concentrations during ESCOMPTE: a case study from IOP 2b, Atmos. Res., 74, 355–380, 2005. Kleinman, L. I., Daum, P. H., Lee, J. H., Lee, Y.-N., Nunnermacker, L. J., Springston, S. R., Newman, L., Weinstein-Lloyd, J., and Sillman, S., Dependence of ozone production on NO and hydrocarbons in the troposphere, Geophys. Res. Lett., 24(18), 2299–2302, doi:10.1029/97GL02279, 1997. Konovalov, I B., Beekmann, M., Vautard, R., Burrows, J P., Richter, A., Nüß, H., and Elansky, N.: Comparison and evaluation of modelled and GOME measurement derived tropospheric NO2 columns over Western and Eastern Europe, Atmos. Chem. Phys., 5, 169–190, 2005. Lafore, J.-P., Stein, J., Asencio, N., Bougeault, P., Ducrocq, V., Duron, J., Fischer, C., Héreil, P., Mascart, P., Masson, V., Pinty, J.-P., Redelsperger, J.-L., Richard, E., and Vilà-Guerau de Arellano, J.: The Meso-NH Atmospheric Simulation System. Part I: adiabatic formulation and control simulations. Scientific objectives and experimental design, Ann. Geophys., 16, 90–109, 1998. Lattuati, M.: Contribution à l'étude du bilan de l'ozone troposphérique à l'interface de l'Europe et de l'Atlantique Nord: Modélisation lagrangienne et mesures en altitude, Ph.D. Thesis, Université Paris 6, Paris, 1997. Lawrence, M G., Von Kuhlmann, R., Salzmann, M., and Rasch, P J.: The balance of effects of deep convective mixing on tropospheric ozone, Geophys. Res. Lett., 30(18), doi:10.1029/2003GL017644, 2003. Lelieveld, J., Berresheim, H., Borrmann, S., Crutzen, P J., Dentener, F. J., Fischer, H., Feichter, J., Flatau, P J., Heland, J., Holzinger, R., Korrmann, R., Lawrence, M. G., Levin, Z., Markowicz, K M., Mihalopoulos, N., Minikin, A., Ramanathan, V., de Reus, M., Roelofs, G J., Scheeren, H A., Sciare, J., Schlager, H., Schultz, M., Siegmund, P., Steil, B., Stephanou, E G., Stier, P., Traub, M., Warneke, C., Williams, J., and Ziereis, H.: Global Air Pollution Crossroads over the Mediterranean, Science, 298(5594), 794–799, 2002. Liang, J., Horowitz, L W., Jacob, D J., Wang, Y., Fiore, A M., Logan, J A., Gardner, G M., and Munger, J W.: Seasonal budgets of reactive nitrogen species and ozone over the United States, and export fluxes to the global atmosphere, J. Geophys. Res., 103(D11), doi:10.1029/97JD03126, 1998. 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), doi:10.1029/1998JD100096, 1999. MacQueen, J.: Some methods for classification and analysis multivariate observations, 5th Berkeley Symposium of Mathematical Statistics and Probability 1, 281–297, 1967. Marion, T., Perros, P E., Losno, R., and Steiner, E.: Ozone Production Efficiency in Savanna and Forested Areas during the EXPRESSO Experiment, J. Atmos. Chem., 38(1), doi:10.1023/A:1026585603100, 2001. Methven, J., Evans, M., Simmonds, P., and Spain, G.: Estimating relationships between air mass origin and chemical composition, J. Geophys. Res., 106(D5), 5005–5020, 2001. Methven, J., Arnold, S. R., O'Connor, F. M., Barjat, H., Dewey, K., Kent, J., and Brough, N.: Estimating photochemically produced ozone throughout a domain using flight data and a Lagrangian model, J. Geophys. Res., 108(D9), doi:10.1029/2002JD002955, 2003. Millán, M M., Salvador, R., Mantilla, E., and Kallos, G.: Photooxidant dynamics in the Mediterranean basin in summer: Results from European research projects, J. Geophys. Res., 102(D7), doi:10.1029/96JD03610, 1997. Norton, W A.: Breaking Rossby Waves in a Model Stratosphere Diagnosed by a Vortex-Following Coordinate System and a Technique for Advecting Material Contours, J. Atmos. Sci., 51, 654–673, 1994. Parrish, D. D., Ryerson, T. B., Holloway, J. S., Neuman, J. A., Roberts, J. M., Williams, J., Stroud, C. A., Frost, G. J., Trainer, M., Hübler, G., Fehsenfeld, F. C., Flocke, F., and Weinheimer, A. J.: Fraction and composition of NOy transported in air masses lofted from the North American continental boundary layer, J. Geophys. Res., 109, D09302, doi:10.1029/2003JD004226, 2004. Puygrenier, V., Lohou, F., Campistron, B., Sa\"\id, F., Pigeon, G., Bénech, B., and Serça, D.: Investigation on the fine structure of sea-breeze during ESCOMPTE experiment, Atmos. Res., 74, 329–353, 2005. Reeves, C E., Penkett, S A., Bauguitte, S., Law, K S., Evans, M J., Bandy, B J., Monks, P S., Edwards, G D., Phillips, G., Barjat, H., Kent, J., Dewey, K., Schmitgen, S., and Kley, D.: Potential for photochemical ozone formation in the troposphere over the North Atlantic as derived from aircraft observations during ACSOE, J. Geophys. Res., 107(D23), doi:10.1029/2002JD002415, 2002. Sa\"\id, F., Corsmeier, U., Kalthoff, N., Kottmeier, C., Lothon, M., Wieser, A., Hofherr, T., and Perros, P E.: ESCOMPTE experiment: intercomparison of four aircraft dynamical, thermodynamical, radiation and chemical measurements, Atmos. Res., 74, 217–252, 2005. Schmidt, H., Derognat, C., Vautard, R., and Beekmann, M.: A comparison of simulated and observed ozone mixing ratios for the summer of 1998 in Western Europe, Atmos. Environ., 35(36), 6277–6297, 2001. Sillman, S.: The relation between ozone, NOx and hydrocarbons in urban and polluted rural environments, Atmos. Env., 33, 1821–1845, 1999. Simeonov, P., Ristori, P., Balin, I., Calpini, B., and van den Bergh, H.: A new DIAL based on a N2 Raman converter for ozone monitoring; design and application during the ESCOMPTE Campaign, Proc. of the XX Quaternary Ozone Symposium, Greece, 109–110, 2004. Stohl, A. and Trickl, T.: A textbook example of long-range transport: Simultaneous observation of ozone maxima of stratospheric and North American origin in the free troposphere over Europe, J. Geophys. Res., 104, 30445–30462, 10.1029/1999JD900803, 1999. Stohl, A., Hittenberger, M., and Wotawa, G.: Validation of the Lagrangian particle dispersion model FLEXPART against large scale tracer experiment data, Atmos. Environ., 32(24), 4245–4264, 1998. Stohl, A., Forster, C., Frank, A., Seibert, P., and Wotawa, G.: Technical note: The Lagrangian particle dispersion model FLEXPART version 6.2, Atmos. Chem. Phys., 5, 2461–2474, 2005. Vautard, R., Beekmann, M., Roux, J., and Gombert, D.: Validation of a hybrid forecasting system for the ozone concentrations over the Paris area, Atmos. Environ., 35(14), 2449–2461, 2001. Vautard, R., Honoré, C., Beekmann, M., and Rouil, L.: Simulation of ozone during the August 2003 heat wave and emission control scenarios, Atmos. Environ., 39(16), 2957–2967, 2005. Wild, O., Law, K S., McKenna, D S., Bandy, B J., Penkett, S A., and Pyle, J A.: Photochemical trajectory modeling studies of the North Atlantic region during August 1993, J. Geophys. Res., 101, 29 269–29 288, 1996. Zhang, J. and Trivikrama Rao, S.: The Role of Vertical Mixing in the Temporal Evolution of Ground-Level Ozone Concentrations, J. Appl. Met., 38, 1674–1691, 1999.