Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 7 22 2007 10.5194/acp-7-5815-2007 http://www.atmos-chem-phys.net/7/5815/2007/ http://www.atmos-chem-phys.net/7/5815/2007/acp-7-5815-2007.html http://www.atmos-chem-phys.net/7/5815/2007/acp-7-5815-2007.pdf 5815 5860 2007-11-26 A new tropospheric and stratospheric Chemistry and Transport Model MOCAGE-Climat for multi-year studies: evaluation of the present-day climatology and sensitivity to surface processes H. Teyssèdre hubert.teyssedre@meteo.fr M. Michou H. L. Clark B. Josse F. Karcher D. Olivié V.-H. Peuch D. Saint-Martin D. Cariolle J.-L. Attié P. Nédélec P. Ricaud V. Thouret R. J. van der A A. Volz-Thomas F. Chéroux GAME/CNRM (Météo-France, CNRS) Centre National de Recherches Météorologiques, Toulouse, France Centre Européen de Recherches et de Formation Avancée en Calcul Scientifique (CERFACS), Toulouse, France Laboratoire d'Aérologie (Université Toulouse III, CNRS), Toulouse, France KNMI (Royal Netherlands Meteorological Institute), De Bilt, The Netherlands Institute of Chemistry and Dynamics of the Geosphere, Juelich, Germany We present the configuration of the Météo-France Chemistry and Transport Model (CTM) MOCAGE-Climat that will be dedicated to the study of chemistry and climate interactions. MOCAGE-Climat is a state-of-the-art CTM that simulates the global distribution of ozone and its precursors (82 chemical species) both in the troposphere and the stratosphere, up to the mid-mesosphere (~70 km). Surface processes (emissions, dry deposition), convection, and scavenging are explicitly described in the model that has been driven by the ECMWF operational analyses of the period 2000–2005, on T21 and T42 horizontal grids and 60 hybrid vertical levels, with and without a procedure that reduces calculations in the boundary layer, and with on-line or climatological deposition velocities. Model outputs have been compared to available observations, both from satellites (TOMS, HALOE, SMR, SCIAMACHY, MOPITT) and in-situ instrument measurements (ozone sondes, MOZAIC and aircraft campaigns) at climatological timescales. The distribution of long-lived species is in fair agreement with observations in the stratosphere putting aside the shortcomings associated with the large-scale circulation. The variability of the ozone column, both spatially and temporarily, is satisfactory. However, because the Brewer-Dobson circulation is too fast, too much ozone is accumulated in the lower to mid-stratosphere at the end of winter. Ozone in the UTLS region does not show any systematic bias. In the troposphere better agreement with ozone sonde measurements is obtained at mid and high latitudes than in the tropics and differences with observations are the lowest in summer. Simulations using a simplified boundary layer lead to larger ozone differences between the model and the observations up to the mid-troposphere. NO_x in the lowest troposphere is in general overestimated, especially in the winter months over the Northern Hemisphere, which may result from a positive bias in OH. Dry deposition fluxes of O₃ and nitrogen species are within the range of values reported by recent inter-comparison model exercises. The use of climatological deposition velocities versus deposition velocities calculated on-line had greatest impact on HNO₃ and NO₂ in the troposphere. Andres, R. J. and Kasgnoc A. D.: A time-averaged inventory of subaerial volcanic sulfur emissions, J. Geophys. Res., 103, 25 251–25 261, 1998. Bechtold, P., Bazile, E., Guichard, F., Mascart, P., and Richard, E.: A mass flux convection scheme for regional and global models, Q. J. Roy. Meteor. Soc., 127, 869–886, 2001. Blond, N., Boersma, K. F., Eskes, H. J., van der A, R. J., Van Roozendael, M., De Smedt, I., Bergametti, 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. Bodeker, G. E., Shiona, H., and Eskes, H.: Antarctic ozone depletion indicators, Atmos. Chem. Phys., 5, 3811–3845, 2005. Boering, K. A., Wofsy, S. C., Daube, B. C., Schneider, H. R., Loewenstein, M., Podolske, J. R., and Conway, T. J.: Stratospheric mean ages and transport rates from observations of carbon dioxide and nitrous oxide, Science, 274, 1340–1343, 1996. Boersma, K. F., Eskes, H. J., and Brinksma, E. J.: Error analysis for tropospheric \chemNO_2 retrieval from space, J. Geophys. Res., 109, D04311, doi:10.1029/2003JD003962, 2004. Bousserez, N., Attié, J.-L., Peuch, V.-H., Michou, M., Pfister, G., Edwards, D., Emmons, L., Mari, C., Barret, B., Arnold, S. R., Heckel, A., Richter, A., Shlager, H., Lewis, A., Avery, M., Sachse, G., Browell, E. V., and Hair, J. W.: Evaluation of the MOCAGE chemistry transport model during the ICARTT/ITOP experiment, J. Geophys. Res., 112, D10S42, doi:10.1029/2006JD007595, 2007. Bouwman, A. F., Van der Hoek, K. W., and Olivier, J. G. J.: Uncertainties in the global source distribution of nitrous oxide, J. Geophys. Res., 100, 2785–2800, 1995. Bovensmann, H., Burrows, J. P., Buchwitz, M., Frerick, J., Noel, S., Rozanov, V. V., Chance, K. V., and Goede, A. P. H.: SCIAMACHY: Mission objectives and measurement modes, J. Atmos. Sci., 56, 127–150, 1999. Brasseur, G. P. and Solomon, S.: Aeoronomy of the middle atmosphere, D. Reidel Publishing Company, 452 pp., 1986. Brasseur, G. P., Hauglustaine, D. A., Walters, S., Rasch, P. J., Müller, J.-F., Granier, C., and Tie, X. X.: MOZART, a global chemical transport model for ozone and related chemical tracers. 1. Model description, J. Geophys. Res., 103, 28 265–28 289, 1998. Bregman, A., Meijer, E., and Scheele, R.: Key aspects of stratospheric tracer modeling using assimilated winds, Atmos. Chem. Phys., 6, 4529–4543, 2006. Brewer, A. W.: Evidence for a world circulation provided by the measurements of helium and water vapour distribution in the stratosphere, Q. J. Roy. Meteor. Soc., 75, 351–363, 1949. % %Brunner, D., J. Staehelin, H.L. Rogers, M.O. Köhler, J.A. Pyle, D. Hauglustaine, L. Jourdain, T.K. Berntsen, M. Gauss, I.S.A. Isaksen, E. Meijer, P. van Velthoven, G. Pitari, E. Mancini, V. Grewe, and R. Sausen, %An evaluation of the performance of chemistry transport models by comparison with research aircraft observations. Part I: concepts and overall model performance, %\textitAtmos. Chem. Phys., 3, 1609-1631, 2003. Cariolle, D. and Déqué, M.: Southern hemisphere medium-scale waves and total ozone disturbances in a spectral general circulation model, J. Geophys. Res., 91, 10 825–10 846, 1986. Cariolle, D., Lasserre-Bigorry, A., Royer, J.-F., and Geleyn, J.-F.: A general circulation model simulation of the springtime Antarctic ozone decrease and its impact on mid-latitudes, J. Geophys. Res., 95, 1883–1898, 1990. Cariolle, D. and Teyssèdre, H.: A revised linear ozone photochemistry parameterization for use in transport and general circulation models: multi-annual simulations Atmos. Chem. Phys., 7, 2183–2196, 2007. % %Carter, W.P.L., %Documentation of the SAPRC-99 chemical mechanism for VOC reactivity assessment, %\textitRapport du California Air Ressources Board, 1999. Cathala, M.-L., Pailleux, J., and Peuch, V.-H.: Improving global chemical simulations of the upper troposphere-lower stratosphere with sequential assimilation of MOZAIC data, Tellus, 55B, 1–10, 2003. Carslaw, K. S., Luo, B., Peter, T., and Clegg, S. L.: Vapour pressures of H₂SO₄/HNO₃/HBr/H₂O solutions to low stratospheric temperatures, Geophys. Res. Lett., 22, 247–250, 1995. Chapman, S.: A Theory of Upper-Atmospheric Ozone, Memoirs of the Royal Meteorological Society, 3, 103–25, 1930. Chipperfield, M. P., Cariolle, D., and Simon, P.: A 3D transport model study of chlorine activation during EASOE, Geophys. Res. Lett., 21, 1467–1470, 1994. Chipperfield M. P.: New version of the TOMCAT/SLIMCAT off-line chemical transport model: Intercomparison of stratospheric tracer experiments, Q. J. Roy. Meteor. Soc. , 132, 1179-1203, 2006. Clark H. L., Cathala, M.-L., Teyssèdre, H., Cammas, J.-P., and Peuch, V.-H.: Cross-tropopause fluxes of ozone using assimilation of MOZAIC measurements in a global CTM, Tellus, 59B, 39–49, 2007. Crassier, V., Suhre, K., Tulet, P., and Rosset, R.: Development of a reduced chemical scheme for use in mesoscale meteorological models, Atmos. Environ., 34, 2633–2644, 2000. Crutzen, P. J.: The influence of nitrogen oxide on the atmospheric ozone content, Q. J. Roy. Meteor. Soc., 96, 320–325, 1970. % %Cunnold, D.M., L.P. Steele, P.J. Fraser, P.G. Simmonds, R.G. Prinn, R.F. Weiss, L.W. Porter, S. O'Doherty, R.L. Langenfelds, P.B. Krummel, H.J. Wang, L. Emmons, X.X. Tie, and E.J. Dlugokencky, %In situ measurements of atmospheric methane at GAGE/AGAGE sites during 1985-2000 and resulting source inferences, %\textitJ. Geophys. Res., 107 (D14), doi: 10.1029/2001JD001226, 2002. Deeter, M. N., Emmons, L. K., Francis, G. L., et al.: Operational carbon monoxide retrieval algorithm and selected results for the MOPITT instrument, J. Geophys. Res., 108(D14), 4399, doi:10.1029/2002JD003186, 2003. Dentener, F., Stevenson, D., Cofala, J., Mechler, R., Amann, M., Bergamaschi, P., Raes, F., and Derwent, R.: The impact of air pollutant and methane emission controls on tropospheric ozone and radiative forcing: CTM calculations for the period 1990 2030, Atmos. Chem. Phys., 4, 8471–8538, 2004. Dentener, F., Drevet, J., Lamarque, J.-F., Bey, I., Eickhout, B., Fiore, A. M., Hauglustaine, D., Horowitz, L. W., Krol, M., Kulshrestha, U. C., Lawrence, M., Galy-Lacaux, C., Rast, S., Shindell, D., Stevenson, D., Van Noije, T., Atherton, C., Bell, N., Bergman, D., Butler, T., Cofala, J., Collins, B., Doherty, R., Ellingsen, K., Galloway, J., Gauss, M., Montanaro, V., Muller, J.-F., Pitari, G., Rodriguez, J., Sanderson, M., Solmon, F., Strahan, S., Schultz, M., Sudo, K., Szopa, S., and Wild, O.: Nitrogen and sulfur deposition on regional and global scales: A multimodel evaluation, Global Biogeochem. Cy., 20, GB4003, doi:10.1029/2005GB002672, 2006. Déqué, M., Dreveton, C., Braun, A., and Cariolle, D.: The ARPEGE-IFS atmosphere model: a contribution to the French community climate modelling, Clim. Dynam., 10, 249–266, 1994. % %Dlugokencky, E.J., B.P. Walter, K.A. Masarie, P.M. Lang, and E.S. Kasischke, %Measurements of an anomalous global methane increase during 1998, %\textitGeophys. Res. Lett., 28, p 499-502, 2001. Drummond, J. R. and Mand, G. S.: The Measurements of pollution in the troposphere (MOPITT) instrument: overall performance and calibration requirements, J. Atmos. Oceanic Technol., 13, 314–320, 1996. Dufour, A., Amodei, M., Ancellet, G., and Peuch, V.-H.: Observed and modelled "chemical weather" during ESCOMPTE, Atmos. Res., 74, 161–189, 2004. Drobinski, P., Sa\"id, F., Ancellet, G., Arteta, J., Augustin, P., Bastin, S., Brut, A., Caccia, J.-L., Campistron, B., Cautenet, S., Colette, A., Cros, B., Corsmeier, U., Coll, I., Dabas, A., Delbarre, H., Dufour, A., Durand, P., Guénard, V., Hasel, M., Kalthoff, N., Kottmeier, C., Lemonsu, A., Lohou, F., Masson, V., Menut, L., Moppert, C., Peuch, V.-H., Puygrenier, V., and Reitebuch, O.: Regional transport and dilution during high pollution episodes in southeastern France : summary of findings from the ESCOMPTE experiment, J. Geophys. Res., 112, D13105, doi:10.1029/2006JD007494, 2007. % %Dupuy, E., J. Urban, P. Ricaud, E. Le Flochmo\"en, N. Lautié, D. Murtagh, J. De La No\"e, L. El Amraoui, P%. Eriksson, P. Forkman, U. Frisk, F. Jégou, C. Jiménez, and M. Olberg, %Strato-mesospheric measurements of carbon monoxide with the Odin sub-millimeter radiometer: retrieval and first results, %\textitGeophys. Res. Lett., 31, L20101, doi:10.1029/2004GL020558, 2004. Edwards, D. P., Pétron, G., Novelli, P. C., Emmons, L. K., Gille, J. C., and Drummond, J. R.: Southern Hemisphere carbon monoxide interannual variability observed by Terra/Measurement of Pollution in the Troposphere (MOPITT), J. Geophys. Res., 111, D16303, doi:10.1029/2006JD007079, 2006. Egorova T., Rozanov, E., Zubov, V., Manzini, E., Schmutz, W., and Peter, T.: Chemistry-climate model SOCOL: a validation of the present-day climatology, Atmos. Chem. Phys., 5, 1557–1576, 2005. El Amraoui, L., Peuch, V.-H., Ricaud, P., Massart, S., Urban, J., Semane, N., Teyssèdre, H., Cariolle, D., and Karcher, F.: Ozone loss in the 2002/2003 Arctic vortex deduced from the assimilation of Odin/SMR \chemO_3 and \chemN_2O measurements: \chemH_2O as dynamical tracer, Q. J. Roy. Meteor. Soc., in press, 2007. Emmons, L. K., Hauglustaine, D. A., Muller, J.-F., Carroll, M. A., Brasseur, G. P., Brunner, D., Staehelin, J., Thouret, V., and Marenco, A.: Data composites of airborne observations of tropospheric ozone and its precursors, J. Geophys. Res., 105, 20 497–20 538, 2000. Emmons, L. K., Deeter, M. N., Gille, J. C., Edwards, D. P., Attié, J.-L., Warner, J., Ziskin, D., Francis, G., Khattatov, B., Yudin, V., Lamarque, J.-F., Ho, S.-P., Mao, D., Chen, J. S., Drummond, J., Novelli, P., Sachse, G., Coffey, M. T., Hannigan, J. W., Gerbig, C., Kawakami, S., Kondo, Y., Takegawa, N., Schlager, H., Baehr, J., and Ziereis, H.: Validation of Measurements of Pollution in the Troposphere (MOPITT) CO retrievals with aircraft in situ profiles, J. Geophys. Res., 109, D03309, doi:10.1029/2003JD004101, 2004. Emmons, L. K., Pfister, G. G., Edwards, D. P., Gille, J. C., Sachse, G., Blake, D., Wofsy, S., Gerbig, C., Matross, D., and Nédélec, P.: Measurements of Pollution in the Troposphere (MOPITT) validation exercises during summer 2004 field campaigns over North America: J. Geophys. Res., 112, D12S02, doi:10.1029/2006JD007833, 2007. Eskes, H. J. and Boersma, K. F.: Averaging kernels for DOAS total-column satellite retrievals, Atmos. Chem. Phys., 3, 1285–1291, 2003. % %Eyring, V., N.R.P. Harris, M. Rex, T.G. Shepherd, D.W. Fahey, G.T. Amanatidis, J. Austin, M.P. Chipperfield, M. Dameris, P.M. De F. Forster, A. Gettelman, H.F. Graf, T. Nagashima, P.A. Newman, S. Pawson, M.J. Prather, J.A. Pyle, R.J. Salawitch, B.D. Santer, and D.W. Waugh, %A strategy for process-oriented validation of coupled chemistry-climate models, %\textitBull. Am. Meteorol. Soc., 86, 111720131133, 2005. % %Eyring, V., Butchart, N., Waugh, D. W., Akiyoshi, H., Austin, J., Bekki, S., Bodeker, G. E., Boville, B. A., Bruhl, C., Chipperfield, M. P., Cordero, E., Dameris, M., Deushi, M., Fioletov, V. E., Frith, S. M., Garcia, R. R., Gettelman, A., Giorgetta, M. A., Grewe, V., Jourdain, L., Kinnison, D. E., Mancini, E., Manzini, E., Marchand, M., Marsh, D. R., Nagashima, T., Newman, P. A., Nielsen, J. E., Pawson, S., Pitari, G., Plummer, D. A., Rozanov, E., Schraner, M., Shepherd, T. G., Shibata, K., Stolarski, R. S., Struthers, H., Tian, W., and Yoshiki, M.: %Assessment of temperature, trace species, and ozone in chemistry-climate model simulations of the recent pas%t, %J. Geophys. Res., 111, D22308, doi:10.1029/2006JD007327, 2006. Farman, J. C., Gardiner, B. G., and Shanklin, J. D.: Large losses of total ozone in Antarctica reveal seasonal \chemClO_x/NO_x interaction, Nature, 315, 207–210, 1985. Feng, W., Chipperfield, M. P., Dorf, M., Pfeilsticker, K., and Ricaud, P.: Mid-latitude ozone changes: studies with a 3-D CTM forced by ERA-40 analyses, Atmos. Chem. Phys., 7, 2357–2369, 2007. % %Fortuin, J.P.F., and H. Kelder, %An ozone climatology based on ozonesonde and satellite measurements, %\textitJ. Geophys. Res., 103, 31,709-31,73, 1998. Frisk, U., Hagström, M., Ala-Laurinaho, J., et al.: The Odin satellite I: Radiometer design and test, Astron. Astrophys., 402(3), L27–L34, doi:10.1051/0004-6361:20030335, 2003. Fung, I., John, J., Lerner, J., Matthews, E., Prather, M., Steele, L. P., and Fraser, P. J.: Three-dimensional model synthesis of the global methane cycle, J. Geophys. Res., 96, 13 033–13 065, 1991. Ganzeveld, L. and Lelieveld, J.: Dry deposition parameterization in a chemistry general circulation model and its influence on the distribution of reactive trace gases, J. Geophys. Res., 100, 20 999–21 012, 1995. Ganzeveld, L., Lelieveld, J., and Roelofs, G.-J.: A dry deposition parameterization for sulfur oxides in a chemistry and general circulation model, J. Geophys. Res., 103, 5679–5694, 1998. Geer, A. J., Lahoz, W. A., Bekki, S., Bormann, N., Errera, Q., Eskes, H. J., Fonteyn, D., Jackson, D. R., Juckes, M. N., Massart, S., Peuch, V.-H., Rharmili, S., and Segers, A.: The ASSET intercomparison of ozone analyses: method and first results, Atmos. Chem. Phys., 6, 5445–5474, 2006. Giorgi, F. and Chamedeis, W. L.: Rainout lifetimes of highly soluble aerosols and gases as inferred from simulations with a general circulation model, J. Geophys. Res., 91, 14 367–14 376, 1986. Guenther, A., Hewitt, C. N., Erickson, D., Fall, R., Geron, C., Graedel, T., Harley, P., Klinger, L., Lerdau, M., McKay, W. A., Pierce, T., Scholes, B., Steinbrecher, R., Tallamraju, R., Taylor, J, and Zimmerman, P.: A global model of natural volatile compound emissions, J. Geophys. Res., 100, 8873–8892, 1995. Grooss, J.-U. and Russell III, J. M.: Technical note: A stratospheric climatology for \chemO_3, \chemH_2O, \chemCH_4, NO_x, \chemHCl and \chemHF derived from HALOE measurements, Atmos. Chem. Phys., 5, 2797–2807, 2005. Hadjinicolaou, P., Pyle, J. A., and Harris, N. R. P.: The recent turnaround in stratospheric ozone over northern middle latitudes: A dynamical modelling perspective, Geophys. Res. Lett., 32, L12821, doi:10.1029/2005GL022476, 2005. Hall, T. M. and Waugh, D. W.: Timescales for the stratospheric circulation derived from tracers, J. Geophys. Res., 102, 8991–9001, 1997. Harnisch, J., Borchers, R., Fabian, P., and Maiss, M.: Tropospheric trends for \chemCF_4 and \chemC_2F_6 since 1982 derived from \chemSF_6 dated stratospheric air, Geophys. Res. Lett., 23, 1099–1102, 1996. Hauchecorne, A., Bertaux, J.-L., Dalaudier, F., Cot, C., Lebrun, J.-C., Bekki, S., Marchand, M., Kyrola, E., Tamminen, J., Sofieva, V., Fussen, D., Vanhellemont, F., Fanton d'Andon, O., Barrot, G., Mangin, A., Théodore, B., Guirlet, M., Snoeij, P., Koopman, R., Saavedra de Miguel, L., Fraisse, R., and Renard, J.-B.: First simultaneous global measurements of nighttime stratospheric \chemNO_2 and \chemNO_3 observed by Global Ozone Monitoring by Occultation of Stars (GOMOS)/Envisat in 2003, J. Geophys. Res., 110, D18301, doi:10.1029/2004JD005711, 2005 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, D04314, doi:10.1029/2003JD003957, 2004. Holland, E. A., Braswell, B. H., Sulzman, J., and Lamarque, J.-F.: Nitrogen deposition onto the United States and western Europe: a synthesis of observations and models, Ecol. Appl., 15, 38–57, 2005. Honoré, C., Rouil, L., Vautard, R., Beekmann, M., Bessagnet, B., Dufour, A., Elichegaray, C., Flaud J-M., Malherbe, L., Meleux, F., Menut, L., Martin, D., Peuch, A., Peuch, V.-H., and Poisson, N.: Predictability of regional air quality in Europe: the assessment of three years of operational forecasts and analyses over France, J. Geophys. Res., in press, doi:2007JD008761R, 2007. Horowitz, L. W., Walters, S., Mauzerall D. L., et al.: A global simulation of tropospheric ozone and related tracers: description and evaluation of MOZART, version 2, J. Geophys. Res., 108, 4784, doi:10.1029/2002JD002853, 2003. Houghton, J. T., Ding, Y., Griggs, D. J., Noguer, M., van der Linden, P. J., and Xiaosu, D.: Climate Change 2001: The Scientific Basis, contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change (IPCC) Cambridge University Press (Eds.), UK, 2001. Intergovernmental Panel on Climate Change, Climate change 1994: radiative forcing of climate change and an evaluation of the IPCC IS92 emissions scenarios, Cambridge University Press (Eds.), UK, 1995. Jöckel, P., Tost, H., Pozzer, A., Brühl, C., Buchholz, J., Ganzeveld, L., Hoor, P., Kerkweg, A., Lawrence, M. G., Sander, R., Steil, B., Stiller, G., Tanarhte, M., Taraborrelli, D., van Aardenne, J., and Lelieveld, J.: The atmospheric chemistry general circulation model ECHAM5/MESSy1: consistent simulation of ozone from the surface to the mesosphere, Atmos. Chem. Phys., 6, 5067–5104, 2006. Josse, B., Simon, P., and Peuch, V.-H.: \chemRn-222 global simulations with the multiscale CTM MOCAGE, Tellus, 56B, 339–356, 2004. \bibitem[Kirkman et al.(2002)] Kirk02 Kirkman, G. A., Gut, A., Ammann, C., Gatti, L. V., Cordova, A. M., Moura, M. A. L., Andreae, M. O., and Meixner, F. X.: Surface exchange of nitric oxide, nitrogen dioxide, and ozone at a cattle pasture in Rondonia, Brazil, J. Geophys. Res., 107, 8083, doi:10.1029/2001JD000523, 2002. \bibitem[Labrador et al.(2005)] Labr05 Labrador L. J., von Kuhlmann, R., and Lawrence, M. G.: The effects of lightning-produced NOx and its vertical distribution on atmospheric chemistry: sensitivity simulations with MATCH-MPIC, Atmos. Chem. Phys., 5, 1815–1834, 2005. Lamarque, J.-F., Kiehl, J. T., Brasseur, G. P., Butler, T., Cameron-Smith, P., Collins, W. D., Collins, W. J., Granier, C., Hauglustaine, D., Hess, P. G., Holland, E. A., Horowitz, L., Lawrence, M. G., McKenna, D., Merilees, P., Prather, M. J., Rasch, P. J., Rotman, D., Shindell, D., and Thornton, P.: Assessing future nitrogen deposition and carbon cycle feedback using a multimodel approach: Analysis of nitrogen deposition, J. Geophys. Res., 110, D19303, doi:10.1029/2005JD005825, 2005. Law, K. S., Plantevin, P.-H., Shallcross, D. E., Rogers, H. L., Grouhel, C., Thouret, V., Marenco, A., and Pyle, J. A.: Evaluation of modelled \chemO_3 using MOZAIC data, J. Geophys. Res., 103, 25 721–25 740, 1998. Law, K. S., Plantevin, P.-H., Thouret, V., Marenco, A., Asman, W. A. H., Lawrence, M., Crutzen, P. J., Müller, 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, 1503–1526, 2000. Lefèvre, F., Brasseur, G. P., Folkins, I., Smith, A. K., and Simon, P.: Chemistry of the 1991–1992 stratospheric winter: three-dimensional model simulations, J. Geophys. Res., 99, 8183–8195, 1994. Li, Q., Jiang, J. H., Wu, D. L., Read, W. G., Livesey, N. J., Waters, J. W., Zhang, Y., Wang, B., Filipiak, M. J., Davis, C. P., Turquety, S., Wu, S., Park, R. J., Yantosca, R. M., and Jacob, D. J.: Convective outflow of South Asian pollution: A global CTM simulation compared with EOS MLS observations, Geophys. Res. Lett., 32, L14826, doi:10.1029/2005GL022762, 2006. Liang, J. and Jacobson, M. Z.: Effects of subgrid segregation on ozone production efficiency in a chemical model, Atmos. Environ., 34, 2975–2982, 2000. % %Liebmann, B. and C.A. Smith, %Description of a complete (Interpolated) Outgoing Longwave Radiation Dataset, %\textitBulletin of the American Meteorological Society, 77, 1275-1277, 1996. Liu, H., Jacob, D. J., Bey, I., and Yantosca, R. M.: Constraints from \chem^210Pb and \chem^7Be on wet deposition and transport in a global three-dimensional chemical-transport model driven by assimilated meteorological fields, J. Geophys. Res., 106, 12 109–12 128, 2001. % %Llewellyn, E.G., et al., %The OSIRIS instrument on the Odin spacecraft, %\textitCan. J. Phys., 82(6), 411-422, doi:10.1139/P04-005, 2004. 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, 16 115–16 149, 1999a. Logan, J. A.: An analysis of ozonesonde data for the lower stratosphere: Recommendations for testing models, J. Geophys. Res., 104, 16 151–16 170, 1999b. Louis, J.-F.: A parametric model of vertical eddy-fluxes in the atmosphere, Bound. Lay. Meteor., 17, 187–202, 1979. % %Leue, C., M. Wenig, T. Wagner, O. Klimm, U. Platt, and B. Jähne, %Quantitative analysis of NO_x emissions from Global Ozone Monitoring Experiment satellite image sequences, %\textitJ. Geophys. Res., 106, 5493-5505, 2001. McLinden, C., Olsen, S. C., Hannegan, B., Wild, O., Prather, M. J., and Sundet, J.: Stratospheric ozone in 3-D models: A simple chemistry and the cross-tropopause flux, J. Geophys. Res., 105, 14 653–14 665, 2000. Madronich, S. and Flocke, S.: The role of solar radiation in atmospheric chemistry, in: Handbook of Environmental Chemistry, edited by: Boule, P., Springer-Verlag, New York, 1–26, 1998. Marenco, A., Thouret, V., Nédélec, P., Smit, H., Helten, M., Kley, D., Karcher, F., Simon, P., Law, K., Pyle, J., Poschmann, G., Von Wrede, R., Hume, C., and Cook, T.: Measurement of ozone and vapor by Airbus in-service aircraft: The MOZAIC airborne program, An overview, J. Geophys. Res., 103, 631–642, 1998. McPeters, R. D. and Labow, G. J.: An assessment of the accuracy of 14.5 years of Nimbus 7 TOMS Version 7 ozone data by comparison with the Dobson network, Geophys. Res. Lett., 23, 3695–3698, 1996. Mari, C., Jacob, D. J., and Bechtold, P.: Transport and scavenging of soluble gases in a deep convective cloud, J. Geophys. Res., 105, 22 255–22 267, 2000. Matthews, E. and Fung, I.: Methane emissions from natural wetlands: Global distribution, area, and environmental characteristics of sources, Global Biogeochem. Cy., 1, 61–86, 1987. Michou, M. and Peuch, V.-H.: Surface exchanges in the MOCAGE multiscale Chemistry and Transport Model, J. Water Sci., 15, 173–203, 2002. Michou, M., Laville, P., Ser\c ca, D., Fotiadi, A., and Peuch, V.-H.: Measured and modeled dry deposition velocities over the ESCOMPTE area, Atmos. Res., 74, 89–116, 2004. Monge-Sanz, B. M., Chipperfield, M. P., Simmons, A. J., and Uppala, S. M.: Mean age of air and transport in a CTM: Comparison of different ECMWF analyses, Geophys. Res. Lett., 34, L04801, doi:10.1029/2006GL028515, 2007. Murtagh, D., Frisk, U., Merino, F., et al.: An overview of the Odin atmospheric mission, Can. J. Phys., 80, 309–319, 2002. Nédélec, P., Cammas, J.-P., Thouret, V., Athier, G., Cousin, J.-M., Legrand, C., Abonnel, C., Lecoeur, F., Cayez, G., and Marizy, C.: An Improved Infra-Red Carbon Monoxide Analyser for Routine Measurements aboard Commercial Airbus Aircraft : Technical Validation and First Scientific Results of the MOZAIC III Program, Atmos. Chem. Phys., 3, 1551–1564, 2003. % % Nevison C. D., D. E. Kinnison and R. F. Weiss, Stratospheric influences on the tropospheric seasonal cycles% of nitrous oxide and chlorofluorocarbons, %\textitGeophys. Res. Lett., 31, L20103, doi:10.1029/2004GL020398, 2004. Nho-Kim, E.-Y., Michou, M., and Peuch, V.-H.: Parameterization of size dependent particle dry deposition velocities for global modeling, Atmos. Environ., 38, 1933–1942, 2004. Noilhan, J. and Mahfouf, J.-F.: The ISBA land surface parameterisation, Glob. Plan. Change, 13, 145–159, 1996. Norton, W., Bregman, A., Chipperfield, M. P., et al.: TOwards the Prediction of stratospheric Ozone (TOPOZ-2), Final report, European Commission, ENV4-CT97-0542, 2000. Oikonomou, E. K., and O'Neill, A.: Evaluation of ozone and water vapor fields from the ECMWF reanalysis ERA-40 during 1991-1999 in comparison with UARS satellite and MOZAIC aircraft observations, J. Geophys. Res., 111, D14109, doi:10.1029/2004JD005341, 2006. Olivier, J. G. J., Bouwman, A. F., Van der Maas, C. W. M., Berdowski, J. J. M., Veldt, C., Bloos, J. P. J., Visschedijk, A. J. H., Zandveld, P. Y. J., and Haverlag, J. L.: Description of EDGAR Version 2.0: A set of global emission inventories of greenhouse gases and ozone-depleting substances for all anthropogenic and most natural sources on a per country basis and on 1$^\circ\times$1° grid, RIVM Rep 771060002/TNO MEP report nr R96/119, RIVM, Bilthoven, The Netherlands, 1996. % %Park, M., W.J. Randel, D.E. Kinnison, R.R. Garcia, and W. Choi, %Seasonal variation of methane, water vapor, and nitrogen oxides near the tropopause: Satellite observations and model simulations, %\textitJ. Geoph et al.(2004)]Park04 %Park, M., W.J. Randel, D.E. Kinnison, R.R. Garcia, and W. Choi, %Seasonal variation of methane, water vapor, and nitrogen oxides near the tropopause: Satellite observations and model simulations, %\textitJ. Geophys. Res., 109, D03302, doi:10.1029/2003JD003706, 2004. Park, J. H., Ko, M. K. W., Jackman, C. H., Plumb, R. A., Kaye, J. A., and Sage, K. H. (Eds.): Models and measurements intercomparison II, NASA/T-1999 209554, Natl. Aeronaut. And Space admin., Washington, D.C., 1999. Piters, A. J. M., Bramstedt, K., Lambert, J.-C., and Kirchhoff, B.: Overview of SCIAMACHY validation: 2002–2004, Atmos. Chem. Phys., 6, 127–148, 2006. Pradier, S., Attié, J.-L., Chong, M., Escobar, J., Peuch, V.-H., Lamarque, J.-F., Khattatov, B., and Edwards, D.: Evaluation of 2001 springtime CO transport over West Africa using MOPITT CO measurements assimilated in a global chemistry transport model, Tellus, 58B, 3, 163–176, 2006. Prather, M. and Ehhalt, D.: Atmospheric chemistry and greenhouse gases, in Climate Change 2001: The Scientific Basis. Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Houghton, J. T., Ding, Y., Griggs, D. J., et al., Cambridge Univ. Press, New York, 239–287, 2001. % %Prather, M.J, %Time scales in atmospheric chemistry: coupled perturbations to \chemN_2O, NO_y, and \chemO_3, %\textitScience 279, 1339-1341, 1998. Prinn, R. G., Weiss, R. F., Fraser, P. J., Simmonds,P. G., Cunnold, D. M., Alyea, F. N., O'Doherty, S., Salameh, P., Miller, B. R., Huang, J., Wang, R. H. J., Hartley, D. E., Harth, C., Steele, L. P., Sturrock, G., Midgley, P. M., and McCulloch, A.: A history of chemically and radiatively important gases in air deduced from ALE/GAGE/AGAGE, J. Geophys. Res., 105, 17 751–17 792, 2000. Ramaswamy, V., Boucher, O., Haigh, J., Hauglustaine, D., Haywood, J., Myhre, G., Nakajima, T., Shi, G. Y., and Solomon, S.: Radiative forcing of climate change, in Climate Change 2001: The Scientific Basis, Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change, edited by Houghton, J. T., Ding, Y., Griggs, D. J., et al., Cambridge Univ. Press, New York, 349–416, 2001. Randeniya, L. K., Vohralik, P. F., and Plumb, I. C.: Stratospheric ozone depletion at Northern mid latitudes in the $21^st$ century: the importance of future concentrations of greenhouse gases nitrous oxide and methane, Geophys. Res. Lett., 29(4) 1051, doi:10.1029/2001GL014295, 2002. Randel, W. J., Wu, F., Russell III, J. M., Roche, A., and Waters, J. W.: Seasonal cycles and QBO variations in stratospheric CH4 and H2O observed in UARS HALOE data J. Atmos. Sci., 55, 163–185, 1998. % %Read, W. G., D. L. Wu, J. W. Waters, and H. C. Pumphrey, %Dehydration in the tropical tropopause layer: Implications from the UARS Microwave Limb Sounder, %\textitJ. Geophys. Res., 109, D06110, doi:10.1029/2003JD004056, 2004. % %Reber, C.A., %The Upper Research Atmosphere Satellite (UARS), %\textitGeophys. Res. Lett., 20, 1215-1218, 1993. Ren, X., Brune W., Mao J., et al.: HO_x observation and model comparison during INTEX-NA 2004, J. Geophys. Res., in press., 2007. Ricaud, P., Barret, B., Attié, J.-L., Le Flochmo\"en, E., Motte, E., Teyssèdre, H., Peuch, V.-H., Livesey, N., Lambert, A., and Pommereau, J.-P.: Impact of land convection on troposphere-stratosphere exchange in the tropics, Atmos. Chem. Phys., 7, 5639–5657, 2007. % %Roche, A.E., J.B. Kumer, J.L. Mergentaler, G.A. Ely, W.G. Uplinger, J.F. Potter, T.C. James, and L.W. Sterritt, %The Cryogenic Limb Array Etalon Spectrometer (CLAES) on UARS: experiment description and performance, %\textitJ. Geophys. Res., 98, 10763-10776, 1993. Rodgers, C. D.: Inverse methods for atmospheric sounding: theory and practice, World Sci., River Edge, N. J., 1st ed., 256 pp., 2000. Russell, J. M., Gordley, L. L., Park, J. H., Drayson, S. R., Tuck, A. F., Harries, J. E., Ciccerone, R. J., Crutzen, P. J., and Frederick, J. E.: The Halogen Occultation Experiment, J. Geophys. Res., 98, 10 777–10 798, 1993. % %Santee, M.L., G.L. Manney, N.J. Livesey, and W.G. Read, %Three-dimensional structure and evolution of stratospheric \chemHNO_3 based on UARS Microwave Limb Sounder measurements, %\textitJ. Geophys. Res., 109, (D15), doi:10.1029/2004JD004578, 2004. Savage, N. H., Law, K. S., Pyle, J. A., Richter, A., Nub, H., and Burrows, J. P.: Using GOME NO2 satellite data to examine regional differences in TOMCAT model performance, Atmos. Chem. Phys., 4, 1895–1912, 2004. Schaub, D., Boersma, K. F., Keller, J., Folini, D., Brunner, D., Buchmann, B., Berresheim, H., and Staehelin, J.: SCIAMACHY tropospheric \chemNO_2 over the Alpine region and importance of pixel surface pressure for the column retrieval, Atmos. Chem. Phys. Discuss., 7, 429–468, 2007. Scheele, M. P., Siegmund, P.C., and van Velthoven, P. F. J.: Stratospheric age of air computed with trajectories based on various 3D-Var and 4D-Var data sets, Atmos. Chem. Phys., 5, 1–7, 2005. Simpson, I. J., Blake, D. R., Rowland, F. S., and Chen, T.-Y.: Implications of the recent fluctuations in the growth rate of tropospheric methane, Geophys. Res. Lett., 29(10), doi:10.1029/2001GL014521, 2002. % %Solomon, S., R.R. Garcia, F.S. Rowland, and D.J. Wuebbles, %On the depletion of Antarctic ozone, %\textitNature, 321, 755-758, 1986. Spivakovsky, C. M., Logan, J. A., Montzka, S. A., Balkanski, Y. J., Foreman-Fowler, M., Jones, D. B. A., Horowitz, L. W., Fusco, A. C., Brenninkmeijer, C. A. M., Prather, M. J., Wofsy, S. C., and McElroy, M. B.: Three-dimensional climatological distribution of tropospheric \chemOH: Update and evaluation, J. Geophys. Res., 105, 8931–8980, 2000. Shindell, D. T., Faluvegi, G., Stevenson, D. S., Krol, M. C., Emmons, L. K., Lamarque, J.-F., Pétron, G., Dentener, F. J., Ellingsen, K., Schultz, M. G., Wild, O., Amann, M., Atherton, C. S., Bergmann, D. J., Bey, I., Butler, T., Cofala, J., Collins, W. J., Derwent, R. G., Doherty, R. M., Drevet, J., Eskes, H. J., Fiore, A. M., Gauss, M., Hauglustaine, D. A., Horowitz, L. W., Isaksen, I. S. A., Lawrence, M. G., Montanaro, V., Müller, J.-F., Pitari, G., Prather, M. J., Pyle, J. A., Rast, S., Rodriguez, J. M., Sanderson, M. G., Savage, N. H., Strahan, S. E., Sudo, K., Szopa, S., Unger, N., van Noije, T. P. C., and Zeng, G.: Multimodel simulations of carbon monoxide: Comparison with observations and projected near-future changes, J. Geophys. Res., 111, D19306, doi:10.1029/2006JD007100, 2006. Stevenson, D. S., Dentener, F. J., Schultz, M. G., Ellingsen, K., van Noije, T. P. C., Wild, O., Zeng, G., Amann, M., Atherton, C. S., Bell, N., Bergmann, D. J., Bey, I., Butler, T., Cofala, J., Collins, W. J., Derwent, R. G., Doherty, R. M., Drevet, J., Eskes, H. J., Fiore, A. M., Gauss, M., Hauglustaine, D. A., Horowitz, L. W., Isaksen, I. S. A., Krol, M. C., Lamarque, J.-F., Lawrence, M. G., Montanaro, V., Müller, J.-F., Pitari, G., Prather, M. J., Pyle, J. A., Rast, S., Rodriguez, J. M., Sanderson, M. G., Savage, N. H., Shindell, D. T., Strahan, S. E., Sudo, K., and Szopa, S.: Multimodel ensemble simulations of present-day and near-future tropospheric ozone, J. Geophys. Res., 111, D08301, doi:10.1029/2005JD006338, 2006. Stockwell, W. R., Kirchner, F., Khun, M., and Seefeld, S.: A new mechanism for regional atmospheric chemistry modelling, J. Geophys. Res., 102, 25 847–25 879, 1997. Strahan, S. E. and Polansky, B. C.: Meteorological implementation issues in chemistry and transport models, Atmos. Chem. Phys., 6, 2895–2910, 2006. % %Taylor, F.W., C.D. Rodgers, J.G. Whitney, S.T. Werrett, J.J. Barnett, G.D. Peskett, P. Venters, J. Ballard, C.W.P. Palmer, R.J. Knight, P.E. Morris, and T.J. Nightingale, %Remote sensing of atmospheric structure and composition by pressure modulator radiometry from space: the ISAMS experiment on UARS, %\textitJ. Geophys. Res., 98, 10799-10814, 1993. Taylor, K. E.: Summarizing multiple aspects of model performance in a single diagram, J. Geophys. Res., 106, 7183–7192, 2001. % %Tiedtke, M., %A comprehensive mass flux scheme for cumulus parametrization in large scale models, %\textitMon. Wea. Rev., 117, 1779-1800, 1989. Trebs, I., Lara, L. L., Zeri, L. M. M., Gatti, L. V., Artaxo, P., Dlugi, R., Slanina, J., Andreae, M. O., and Meixner, F. X.: Dry and wet deposition of inorganic nitrogen compounds to a tropical pasture site (Rondonia, Brazil), Atmos. Chem. Phys., 6, 447–469, 2006. Urban, J., Lautié, N., Le Flochmo\"en, E., Jimenez, C., Eriksson, P., de la No\"e, J., Dupuy, E., El Amraoui, L., Frisk, U., Jegou, F., Murtagh, D., Olberg, M., Ricaud, P., Camy-Peyret, C., Payan, S., Dufour, G., Huret, N., Pirre, M., Robinson, A. D., Harris, N. R. D., Bremer, H., Kleinbohl, A., Kullmann, K., Kunzi, K., Kuttipurath, J., Ejiri, M., Nakajima, H., Sasano, Y., Sugita, T., Yokota, T., Piccolo, C., Raspollini, P., and Ridolfi, M.: Odin/SMR Limb Observations of Stratospheric Trace Gases: Validation of \chemN_2O, J. Geophys. Res., 110, D09301, doi:10.1029/2004JD005394, 2005. van der Werf, G. R., Randerson, J. T., Collatz, G. J., and Giglio, L.: Carbon emissions from fires in tropical and subtropical ecosystems, Global Change Biol., 9, 547–562, 2003. van Noije, T. P. C., Eskes, H. J., van Weele, M., and van Velthoven, P. F. J.: Implications of the enhanced Brewer-Dobson circulation in European Centre for Medium-Range Weather Forecasts reanalysis ERA-40 for the stratosphere-troposphere exchange of ozone in global chemistry transport models, J. Geophys. Res., 109(D19), D19308, doi:10.1029/2004JD004586, 2004. van Noije, T. P. C., Eskes, H. J., Dentener, F. J., Stevenson, D. S., Ellingsen, K., Schultz, M. G., Wild, O., Amann, M., Atherton, C. S., Bergmann, D. J., Bey, I., Boersma, K. F., Butler, T., Cofala, J., Drevet, J., Fiore, A. M., Gauss, M., Hauglustaine, D. A., Horowitz, L. W., Isaksen, I. S. A., Krol, M. C., Lamarque, J.-F., Lawrence,M. G., Martin, V., Montanaro, V., Müller, J.-F., Pitari, G., Prather, M. J., Pyle, J. A., Richter, A., Rodriguez, J. M., Savage, N. H., Strahan, S. E., Sudo, K., Szopa, S., and van Roozendael, M.: 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., Berg, M., Heil, T., Houben, N., Lerner, A., Petrick, W., Raak, D., and Pätz, H.-W.: Measurements of total odd nitrogen (NO_y) aboard MOZAIC in-service aircraft: instrument design, operation and performance, Atmos. Chem. Phys., 5, 583–595, 2005. % %Waters, J.W., %Microwave Limb Sounding, chapitre 8 de atmospheric remote sensing by microwave radiometry, %\textitM.A. Janssen, J. Wiley & sons, 1993. Wesely, M. L.: Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models, Atmos. Environ., 23, 1293–1304, 1989. Wesely, M. L. and Hicks, B. B.: A review of the current status of knowledge on dry deposition, Atmos. Environ., 34, 2261–2282, 2000. Wild, O.: Modelling the global tropospheric ozone budget: exploring the variability in current models, Atmos. Chem. Phys., 7, 2643–2660, 2007. Williamson, D. L. and Rash, P. J.: Two-dimensional semi-lagrangian transport with shape-preserving interpolation, Mon. Weather Rev., 117, 102–129, 1989. World Health Organization: Health aspects of air pollution with particulate matter, ozone, and nitrogen dioxide, Rep. EUR/03/5042688, Bonn, 2003. World Meteorological Organisation: Report of the international ozone trends panel-1988, WMO report, 18, 1988. World Meteorological Organisation: Scientific assessment of ozone depletion-1998, WMO report, 44, 1998. World Meteorological Organisation: Scientific assessment of ozone depletion-2002, WMO report, 47, 2002.