Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 8 3 2008 10.5194/acp-8-565-2008 http://www.atmos-chem-phys.net/8/565/2008/ http://www.atmos-chem-phys.net/8/565/2008/acp-8-565-2008.html http://www.atmos-chem-phys.net/8/565/2008/acp-8-565-2008.pdf 565 578 2008-02-07 The impact of transport across the polar vortex edge on Match ozone loss estimates J.-U. Grooß R. Müller P. Konopka H.-M. Steinhorst A. Engel T. Möbius C. M. Volk Forschungszentrum Jülich, Institut für Chemie und Dynamik der Geosphäre, ICG-1: Stratosphäre, Germany Johann Wolfgang Goethe-Universität, Frankfurt, Institut für Atmosphäre und Umwelt, Germany The Match method for the quantification of polar chemical ozone loss is investigated mainly with respect to the impact of the transport of air masses across the vortex edge. For the winter 2002/03, we show that significant transport across the vortex edge occurred and was simulated by the Chemical Lagrangian Model of the Stratosphere. In-situ observations of inert tracers and ozone from HAGAR on the Geophysica aircraft and balloon-borne sondes, and remote observations from MIPAS on the ENVISAT satellite were reproduced well by CLaMS. The model even reproduced a small vortex remnant that remained a distinct feature until June 2003 and was also observed in-situ by a balloon-borne whole air sampler. We use this CLaMS simulation to quantify the impact of transport across the vortex edge on ozone loss estimates from the Match method. We show that a time integration of the determined vortex average ozone loss rates, as performed in Match, results in a larger ozone loss than the polar vortex average ozone loss in CLaMS. The determination of the Match ozone loss rates is also influenced by the transport of air across the vortex edge. We use the model to investigate how the sampling of the ozone sondes on which Match is based represents the vortex average ozone loss rate. Both the time integration of ozone loss and the determination of ozone loss rates for Match are evaluated using the winter 2002/2003 CLaMS simulation. These impacts can explain the majority of the differences between CLaMS and Match column ozone loss. While the investigated effects somewhat reduce the apparent discrepancy in January ozone loss rates reported earlier, a distinct discrepancy between simulations and Match remains. However, its contribution to the accumulated ozone loss over the winter is not large. Becker, G., Müller, R., McKenna, D S., Rex, M., and Carslaw, K S.: Ozone loss rates in the Arctic stratosphere in the winter 1991/92: Model calculations compared with Match results, Geophys. Res. Lett., 25, 4325–4328, 1998. Becker, G., Müller, R., McKenna, D S., Rex, M., Carslaw, K S., and Oelhaf, H.: Ozone loss rates in the Arctic stratosphere in the winter 1994/1995: Model simulations underestimate results of the Match analysis, J Geophys. Res., 105, 15 175–15 184, 2000. Burkholder, J B., Orlando, J J., and Howard, C J.: Ultraviolet Absorption Cross Section of Cl₂O₂ between 210 and 410 nm, J Phys. Chem., 94, 687–695, 1990. Chipperfield, M P., Feng, W., and Rex, M.: Arctic ozone loss and climate sensitivity: Updated three-dimensional model study, Geophys. Res. Lett., 32, L11813, \doi10.1029/2005GL022674, 2005. Christensen, T., Knudsen, B M., Streibel, M., Anderson, S B., Benesova, A., Braathen, G., Davies, J., De Backer, H., Dier, H., Dorokhov, V., Gerding, M., Gil, M., Henchoz, B., Kelder, H., Kivi, R., Kyrö, E., Litynska, Moore, D., Peters, G., Skrivankova, P., Stübi, R., Turunen, T., Vaughan, G., Viatte, P., Vik, A F., von~der Gathen, P., and Zaitcev, I.: Vortex-averaged Arctic ozone depletion in the winter 2002/2003, Atmos. Chem. Phys., 5, 131–138, 2005. Douglass, A R., Stolarski, R S., Strahan, S E., and Polansky, B C.: Sensitivity of Arctic ozone loss to polar stratospheric cloud volume and chlorine and bromine loading in a chemistry and transport model, Geophys. Res. Lett., 33, L17809, \doi10.1029/2006GL026492, 2006. Feng, W., Chipperfield, M P., Davies, S., Sen, B., Toon, G., Blavier, J F., Webster, C R., Volk, C M., Ulanovsky, A., Ravegnani, F., von~der Gathen, P., Jost, H., Richard, E C., and Claude, H.: Three-dimensional model study of the Arctic ozone loss in 2002/2003 and comparison with 1999/2000 and 2003/2004, Atmos. Chem. Phys., 5, 139–152, 2005. Frieler, K., Rex, M., Salawitch, R J., Canty, T., Streibel, M., Stimpfle, R M., Pfeilsticker, K., Dorf, M., Weisenstein, D K., and Godin-Beekmann, S.: Toward a better quantitative understanding of polar stratospheric ozone loss, Geophys. Res. Lett., 33, L10812, \doi10.1029/2005GL025466, 2006. Goutail, F., Pommereau, J.-P., Lefèvre, F., Roozendael, M V., Andersen, S B., Kåstad-Høiskar, B.-A., Dorokhov, V., Kyrö, E., Chipperfield, M P., and Feng, W.: Early unusual ozone loss during the Arctic winter 2002/2003 compared to other winters, Atmos. Chem. Phys., 5, 665–677, 2005. Grooß, J.-U. and Müller, R.: The impact of mid-latitude intrusions into the polar vortex on ozone loss estimates, Atmos. Chem. Phys., 3, 395–402, 2003. Grooß, J.-U. and Russell, J M.: Technical note: A stratospheric climatology for O₃, H₂O, CH₄, NO_x, HCl and HF derived from HALOE measurements, Atmos. Chem. Phys., 5, 2797–2807, 2005. Grooß, J.-U., Günther, G., Müller, R., Konopka, P., Bausch, S., Schlager, H., Voigt, C., Volk, C M., and Toon, G C.: Simulation of denitrification and ozone loss for the Arctic winter 2002/2003, Atmos. Chem. Phys., 5, 1437–1448, 2005. Günther, G., Müller, R., von Hobe, M., Stroh, F., Konopka, P., and Volk, C M.: Quantification and Transport across the Boundary of the Lower Stratospheric Vortex during the Arctic Winter 2002/2003, Atmos. Chem. Phys. Discuss., 7, 17 559–17 597, 2007. Harris, N. R P., Rex, M., Goutail, F., Knudsen, B M., Manney, G L., Müller, R., and von~der Gathen, P.: Comparison of empirically derived ozone loss rates in the Arctic vortex, J Geophys. Res., 107, 8264, \doi10.1029/2001JD000482, 2002. Kilbane-Dawe, I., Harris, N. R P., Pyle, J A., Rex, M., Lee, A M., and Chipperfield, M P.: A comparison of Match and 3D model ozone loss rates in the Arctic polar vortex during the winters of 1994/95 and 1995/96, J. Atmos. Chem., 39, 123–138, 2001. Konopka, P., Steinhorst, H.-M., Grooß, J.-U., Günther, G., Müller, R., Elkins, J W., Jost, H.-J., Richard, E., Schmidt, U., Toon, G., and McKenna, D S.: Mixing and Ozone Loss in the 1999–2000 Arctic Vortex: Simulations with the 3-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS), J Geophys. Res., 109, D02315, \doi10.1029/2003JD003792, 2004. Lait, L R.: An alternative form for potential vorticity, J Atmos. Sci., 51, 1754–1759, 1994. McKenna, D S., Grooß, J.-U., Günther, G., Konopka, P., Müller, R., Carver, G., and Sasano, Y.: A new Chemical Lagrangian Model of the Stratosphere (CLaMS): 2. Formulation of chemistry scheme and initialization, J Geophys. Res., 107, 4256, \doi10.1029/2000JD000113, 2002a. McKenna, D S., Konopka, P., Grooß, J.-U., Günther, G., Müller, R., Spang, R., Offermann, D., and Orsolini, Y.: A new Chemical Lagrangian Model of the Stratosphere (CLaMS): 1. Formulation of advection and mixing, J Geophys. Res., 107, 4309, \doi10.1029/2000JD000114, 2002b. Möbius, T.: Untersuchungen zu Unterschieden in Tracer-Tracer Korrelationen innerhalb und auß erhalb des arktischen Polarwirbels, Diploma Thesis, University of Frankfurt, 2006. Morcrette, J.-J.: Radiation and Cloud Radiative Properties in the European Centre for Medium-Range Weather Forecasts Forecasting System, J Geophys. Res., 96, 9121–9132, 1991. Müller, R., Schmidt, U., Engel, A., McKenna, D S., and Proffitt, M H.: The O₃/N₂O relationship from balloon-borne observations as a measure of Arctic ozone loss in 1991–1992, Q J Roy. Meteor. Soc., 127, 1389–1412, 2001. Müller, R., Tilmes, S., Konopka, P., Grooß, J.-U., and Jost, H.-J.: Impact of mixing and chemical change on ozone-tracer relations in the polar vortex, Atmos. Chem. Phys., 5, 3139–3151, 2005. Müller, R., Tilmes, S., Grooß, J.-U., Engel, A., Oelhaf, H., Wetzel, G., Huret, N., Pirre, M., Catoire, V., Toon, G., and Nakajima, H.: Impact of mesospheric intrusions on ozone–tracer relations in the stratospheric polar vortex, J Geophys. Res., 112, D23307, \doi10.1029/2006JD008315, 2007. Nash, E R., Newman, P A., Rosenfield, J E., and Schoeberl, M R.: An objective determination of the polar vortex using Ertel's potential vorticity, J Geophys. Res., 101, 9471–9478, 1996. Naujokat, B. and Grunow, K.: The stratospheric arctic winter 2002/03: Balloon flight planning by trajectory calculation., in: Proceedings of the 16th ESA Symposium on European Rocket and Balloon Programmes and Related Research, ESA SP-530, St. Gallen, 421–425, 2003. Pope, F D., Hansen, J C., Bayes, K D., Friedl, R R., and Sander, S P.: Ultraviolet Absorption Spectrum of Chlorine Peroxide, ClOOCl, J Phys. Chem. A, 20, 4322–4332, \doi10.1021/jp067660w, 2007. Ray, E A., Moore, F L., Elkins, J W., Hurst, D F., Romashkin, P A., Dutton, G S., and Fahey, D W.: Descent and mixing in the 1999-2000 northern polar vortex inferred from in situ tracer measurements, J Geophys. Res., 107, 8285, \doi10.1029/2001JD000961, 2002. Rex, M., von der Gathen, P., Harris, N. R P., Lucic, D., Knudsen, B M., Braathen, G O., Reid, S J., De Backer, H., Claude, H., Fabian, R., Fast, H., Gil, M., Kyrö, E., Mikkelsen, I S., Rummukainen, M., Smit, H G., Stähelin, J., Varotsos, C., and Zaitcev, I.: In situ Measurements of stratospheric ozone depletion rates in the Arctic winter 1991/92: A Lagrangian approach, J Geophys. Res., 103, 5843–5853, 1998. Rex, M., von der Gathen, P., Braathen, G O., Reid, S J., Harris, N. R P., Chipperfield, M., Reimer, E., Beck, A., Alfier, R., Krüger-Carstensen, R., De Backer, J., Balis, D., Zerefos, Z., O' Connor, F., Dier, H., Dorokhov, V., Fast, H., Gamma, A., Gil, M., Kyrö, E., Rummukainen, M., Litynska, Z., Mikkelsen, I S., Molyneux, M., and Murphy, G.: Chemical Ozone Loss in the Arctic Winter 1994/95 as determined by the Match Technique, J Atmos. Chem., 32, 1–34, 1999. Rex, M., Salawitch, R J., Santee, M L., Waters, J W., Hoppel, K., and Bevilacqua, R.: On the unexplained stratospheric ozone losses during cold Arctic Januaries, Geophys. Res. Lett., 30, 1010, \doi10.1029/2002GL016008, 2003. Rex, M., Salawitch, R J., von~der Gathen, P., Harris, N. R P., Chipperfield, M P., and Naujokat, B.: Arctic ozone loss and climate change, Geophys. Res. Lett., 31, L04116, \doi10.1029/2003GL018844, 2004. Riediger, O., Volk, C M., Strunk, M., and Schmidt, U.: HAGAR – A new in-situ instrument for stratospheric balloons and high altitude aircraft, in: Stratospheric ozone 1999, in: Proceedings of the fifth European symposium, edited by: Harris, N. R P., Guirlet, M., and Amanatidis, G T., Air pollution research report 73, European Commission, 727–729, 2000. Sander, S P., Friedl, R R., Golden, D M., Kurylo, M J., Moortgat, G K., Keller-Rudek, H., Wine, P H., Ravishankara, A R., Kolb, C E., Molina, M J., Finlayson-Pitts, B J., Huie, R E., and Orkin, V L.: Chemical kinetics and photochemical data for use in atmospheric studies, JPL Publication 06-2, 2006. Schmidt, U., Kulessa, G., Klein, E., Röth, E.-P., Fabian, P., and Borchers, R.: Intercomparison of balloon-borne cryogenic whole air samplers during the MAP/GLOBUS 1983 campaign, Planet. Space Sci., 35, 647–656, 1987. Singleton, C G., Randell, C E., Chipperfield, M., Davies, S., Feng, W., Bevilacqua, R M., Hoppel, K W., Fromm, M D., Manney, G L., and Harvey, V L.: 2002–2003 Arctic ozone loss deduced from POAM III satellite observations and the SLIMCAT chemical transport model, Atmos. Chem. Phys., 5, 597–609, 2005. Steinhorst, H.-M., Konopka, P., Günther, G., and Müller, R.: How permeable is the edge of the Arctic vortex –- Model studies of the winter 1999–2000, J Geophys. Res., 110, D06105, \doi10.1029/2004JD005268, 2005. Streibel, M., Rex, M., von~der Gathen, P., Lehmann, R., Harris, N. R P., Braathen, G O., Reimer, E., Deckelmann, H., Chipperfield, M., Millard, G., Allaart, M., Andersen, S B., Claude, H., Davies, J., De Backer, H., Dier, H., Dorokov, V., Fast, H., Gerding, M., Kyrö, E., Litynska, Z., Moore, D., Moran, E., Nagai, T., Nakane, H., Parrondo, C., Skrivankova, P., Stübi, R., Vaughan, G., Viatte, P., and Yushkov, V.: Chemical ozone loss in the Arctic winter 2002/2003 determined with Match, Atmos. Chem. Phys., 6, 2783–2792, 2006. Tilmes, S., Müller, R., Grooß, J.-U., Höpfner, M., Toon, G C., and Russell, J M.: Very early chlorine activation and ozone loss in the Arctic winter 2002–2003, Geophys. Res. Lett., 30, 2201, \doi10.1029/2003GL018079, 2003. Tripathi, O P., Godin-Beekmann, S., Levèvre, F., Pazmino, A., Hauchecorne, A., Chipperfield, M., Feng, W., Millard, G., Rex, M., Streibel, M., and von~der Gathen, P.: Comparison of polar ozone loss rates simulated by 1-D and 3-D models with Match observations in recent Antarctic and Arctic winters, J Geophys. Res., 112, D12308, \doi10.1029/2006JD008370, 2007. Vogel, B., Feng, W., Streibel, M., and Müller, R.: The potential impact of ClO$_\mathrmx$ radical complexes on polar stratospheric ozone loss processes, Atmos. Chem. Phys., 6, 3099–3114, 2006. von Hobe, M., Salawitch, R J., Canty, T., Keller-Rudek, H., Moortgat, G K., Grooß, J.-U., Müller, R., and Stroh, F.: Understanding the kinetics of the ClO dimer cycle, Atmos. Chem. Phys., 7, 3055–3069, 2007. WMO: Scientific assessment of ozone depletion: 2006, Global Ozone Research and Monitoring Project-Report No. 50, Geneva, Switzerland, 2007.