ACP Atmospheric Chemistry and Physics ACP Atmos. Chem. Phys. 1680-7324 Copernicus Publications Göttingen, Germany 10.5194/acp-10-12073-2010 Attribution of stratospheric ozone trends to chemistry and transport: a modelling study Kiesewetter G. 1 Sinnhuber B.-M. 1 2 Weber M. 1 Burrows J. P. 1 Institute of Environmental Physics, University of Bremen, Otto-Hahn-Allee 1, 28359 Bremen, Germany now at: Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany 17 12 2010 10 24 12073 12089 Copyright: © 2010 G. Kiesewetter et al. 2010 This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/ This article is available from https://acp.copernicus.org/articles/10/12073/2010/acp-10-12073-2010.html The full text article is available as a PDF file from https://acp.copernicus.org/articles/10/12073/2010/acp-10-12073-2010.pdf

The decrease of the concentration of ozone depleting substances (ODSs) in the stratosphere over the past decade raises the question to what extent observed changes in stratospheric ozone over this period are consistent with known changes in the chemical composition and possible changes in atmospheric transport. Here we present a series of ozone sensitivity calculations with a stratospheric chemistry transport model (CTM) driven by meteorological reanalyses from the European Centre for Medium-Range Weather Forecasts, covering the period 1978–2009. In order to account for the reversal in ODS trends, ozone trends are analysed as piecewise linear trends over two periods, 1979–1999 and 2000–2009. Modelled column ozone (TO3) inter-annual variability and trends are in excellent agreement with observations from the Total Ozone Mapping Spectrometer (TOMS) and Solar Backscatter UV (SBUV/2) as well as the Global Ozone Monitoring Experiment (GOME/GOME2) and Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) instruments. In the period 1979–1999, modelled TO3 trends at mid-latitudes are dominated by changes in in situ gas-phase chemistry, which contribute to about 50% or more of the TO3 trend in most seasons. Changes in meteorology contribute around 35% to mid-latitude TO3 trends, with strong differences between different seasons. In springtime, export of ozone depleted air from polar latitudes contributes about 35–50% to the modelled TO3 trend at SH mid-latitudes and about 15–30% at NH mid-latitudes. Over the period 2000–2009 positive linear trends in modelled TO3, which agree well with observed TO3 trends, are dominated by changes in meteorology, as expected for the yet small decrease in stratospheric halogen loading over this period. While the TO3 trends themselves are not statistically significant over the period 2000–2009, changes in linear trends between 1978–1999 and 2000–2009 are significant at mid- and high latitudes of both hemisphere during most seasons. However, changes in meteorology have contributed substantially to these TO3 trend changes.

 References Bovensmann, H., Burrows, J.&nbsp;P., Buchwitz, M., Frerick, J., Noel, S., Rozanov, V.&nbsp;V., Chance, K.&nbsp;V., and Goede, A. P.&nbsp;H.: {SCIAMACHY}: {M}ission objectives and measurement modes, J. Atmos. Sci., 56, 127–150, 1999. Bracher, A., Lamsal, L. N., Weber, M., Bramstedt, K., Coldewey-Egbers, M., and Burrows, J. P.: Global satellite validation of SCIAMACHY O<sub>3</sub> columns with GOME WFDOAS, Atmos. Chem. Phys., 5, 2357–2368, https://doi.org/10.5194/acp-5-2357-2005, 2005. Braesicke, P. and Pyle, J.&nbsp;A.: Changing ozone and changing circulation in northern mid-latitudes: Possible feedbacks?, Geophys. Res. Lett., 30, 1059, <a href="http://dx.doi.org/10.1029/2002GL015973">https://doi.org/10.1029/2002GL015973</a>, 2003. Callies, J., Corpaccioli, E., Eisinger, M., Hahne, A., and Lefebvre, A.: GOME-2 – {METOP}'s second-generation sensor for operational ozone monitoring, ESA Bull., 102, 28–36, 2000. Chipperfield, M. P.: A three-dimensional model study of long-term mid-high latitude lower stratosphere ozone changes, Atmos. Chem. Phys., 3, 1253–1265, https://doi.org/10.5194/acp-3-1253-2003, 2003. Coldewey-Egbers, M., Weber, M., Lamsal, L. N., de Beek, R., Buchwitz, M., and Burrows, J. P.: Total ozone retrieval from GOME UV spectral data using the weighting function DOAS approach, Atmos. Chem. Phys., 5, 1015–1025, https://doi.org/10.5194/acp-5-1015-2005, 2005. Dhomse, S., Weber, M., Wohltmann, I., Rex, M., and Burrows, J. P.: On the possible causes of recent increases in northern hemispheric total ozone from a statistical analysis of satellite data from 1979 to 2003, Atmos. Chem. Phys., 6, 1165–1180, https://doi.org/10.5194/acp-6-1165-2006, 2006. Eyring, V., Shepherd, T.&nbsp;G., and Waugh, D.&nbsp;W.&nbsp;(Eds.): SPARC {R}eport on the Evaluation of Chemistry-Climate Models, SPARC {R}eport N}o. 5, {WCRP-132, {WMO/TD}-{N}o. 1526, 2010. 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, https://doi.org/10.5194/acp-7-2357-2007, 2007. Fortuin, J. F.&nbsp;P. and Kelder, H.: An ozone climatology based on ozonesondes and satellite measurements, J. Geophys. Res., 103, 31709–31734, 1998. Hadjinicolaou, P., Jrrar, A., Pyle, J.&nbsp;A., and Bishop, L.: The dynamically driven long-term trend in stratospheric ozone over northern middle latitudes, Q. J. Roy Meteor. Soc., 128, 1393–1412, 2002. Hadjinicolaou, P., Pyle, J.&nbsp;A., and Harris, N. R.&nbsp;P.: The recent turnaround in stratospheric ozone over northern middle latitudes: A dynamical modeling perspective, Geophys. Res. Lett., 32, 12821, <a href="http://dx.doi.org/10.1029/2005GL022476">https://doi.org/10.1029/2005GL022476</a>, 2005. Harris, N., Hudson, R., and Phillips, C.&nbsp;(Eds.): Assessment of trends in the vertical distribution of ozone. SPARC {R}ep. 1, {WMO}-{O}zone {R}esearch and {M}onitoring {P}roject {R}ep. 43, 1998. Harris, N. R. P., Kyrö, E., Staehelin, J., Brunner, D., Andersen, S.-B., Godin-Beekmann, S., Dhomse, S., Hadjinicolaou, P., Hansen, G., Isaksen, I., Jrrar, A., Karpetchko, A., Kivi, R., Knudsen, B., Krizan, P., Lastovicka, J., Maeder, J., Orsolini, Y., Pyle, J. A., Rex, M., Vanicek, K., Weber, M., Wohltmann, I., Zanis, P., and Zerefos, C.: Ozone trends at northern mid- and high latitudes –- a European perspective, Ann. Geophys., 26, 1207–1220, https://doi.org/10.5194/angeo-26-1207-2008, 2008. Harris, N. R.&nbsp;P., Lehmann, R., Rex, M., and von der Gathen, P.: A closer look at {A}rctic ozone loss and polar stratospheric clouds, Atmos. Chem. Phys., 10, 8499–8510, <a href="http://dx.doi.org/10.5194/acp-10-8499-2010">https://doi.org/10.5194/acp-10-8499-2010</a>, 2010. Hood, L.&nbsp;L., Mc{C}ormack, J.&nbsp;P., and Labitzke, K.: An investigation of dynamical contributions to midlatitude ozone trends in winter, J. Geophys. Res., 102, 13079–13093, 1997. Hsu, J. and Prather, M.&nbsp;J.: Stratospheric variability and tropospheric ozone, J. Geophys. Res., 114, D06102, <a href="http://dx.doi.org/10.1029/2008JD010942">https://doi.org/10.1029/2008JD010942</a>, 2009. Kiesewetter, G., Sinnhuber, B.-M., Vountas, M., Weber, M., and Burrows, J.&nbsp;P.: A Long-term Stratospheric Ozone Dataset from Assimilation of Satellite Observations: {H}igh-Latitude Ozone Anomalies, J. Geophys. Res., 115, D10307, <a href="http://dx.doi.org/10.1029/2009JD013362">https://doi.org/10.1029/2009JD013362</a>, 2010. McLinden, C.&nbsp;A., Olsen, S.&nbsp;C., Hannegan, B., Wild, O., Prather, M.&nbsp;J., and Sundet, J.: Stratospheric ozone in 3-D models: A simple chemistry and the cross-tropopause flux, J. Geophys. Res., 105, 14653–14665, 2000. Newchurch, M.&nbsp;J., Yang, E.-S., Cunnold, D.&nbsp;M., Reinsel, G.&nbsp;C., Zawodny, J.&nbsp;M., and Russell III, J.&nbsp;M.: Evidence for slowdown in stratospheric ozone loss: {F}irst stage of ozone recovery, J. Geophys. Res., 108, 4507, <a href="http://dx.doi.org/10.1029/2003JD003471">https://doi.org/10.1029/2003JD003471</a>, 2003. Newman, P.&nbsp;A., Nash, E.&nbsp;R., Kawa, S.&nbsp;R., Montzka, S.&nbsp;A., and Schauffler, S.&nbsp;M.: When will the Antarctic ozone hole recover?, Geophys. Res. Lett., 33, L12814, <a href="http://dx.doi.org/10.1029/2005GL025232">https://doi.org/10.1029/2005GL025232</a>, 2006. Prather, M.: Catastrophic Loss of Stratospheric Ozone in Dense Volcanic Clouds, J. Geophys. Res., 97, 10187–10191, 1992. Randel, W. and Wu, F.: Cooling of the Arctic and Antarctic Polar Stratospheres due to Ozone Depletion, J. Clim., 12, 1467–1469, 1999. Randel, W.&nbsp;J., Wu, F., Russell III, J.&nbsp;M., Waters, J.&nbsp;W., and Froidevaux, L.: Ozone and temperature changes in the stratosphere following the eruption of Mt. Pinatubo, J. Geophys. Res., 100, 16753–16764, 1995. Randel, W.&nbsp;J., Wu, F., and Stolarski, R.: Changes in column ozone correlated with the stratospheric EP flux, J. Met. Soc. Japan, 80, 849–862, 2002. Reinsel, G.&nbsp;C., Weatherhead, E.&nbsp;C., Tiao, G.&nbsp;C., Miller, A.&nbsp;J., Nagatani, R.&nbsp;M., Wuebbles, D.&nbsp;J., and Flynn, L.&nbsp;E.: On detection of turnaround and recovery in trend for ozone, J. Geophys. Res., 107, 4078, <a href="http://dx.doi.org/10.1029/2001JD000500">https://doi.org/10.1029/2001JD000500</a>, 2002. Reinsel, G.&nbsp;C., Miller, A.&nbsp;J., Weatherhead, E.&nbsp;J., Flynn, L.&nbsp;E., Nagatani, R.&nbsp;M., Tiao, G.&nbsp;C., and Wuebbles, D.&nbsp;J.: Trend analysis of total ozone data for turnaround and dynamical contributions, J. Geophys. Res., 110, 16306, <a href="http://dx.doi.org/10.1029/2004JD004662">https://doi.org/10.1029/2004JD004662</a>, 2005. Rex, M., Salawitch, R.&nbsp;J., von&nbsp;der Gathen, P., Harris, N. R.&nbsp;P., Chipperfield, M.&nbsp;P., and Naujokat, B.: Arctic ozone loss and climate change, Geophys. Res. Lett., 31, L04116, <a href="http://dx.doi.org/10.1029/2003GL018844">https://doi.org/10.1029/2003GL018844</a>, 2004. Searle, K.&nbsp;R., Chipperfield, M.&nbsp;P., Bekki, S., and Pyle, J. A.&nbsp;.: The impact of spatial averaging on calculated polar ozone loss. 2. {T}heoretical analysis, J. Geophys. Res., 103, 25409–25416, 1998. Shine, K.&nbsp;P.: The middle atmosphere in the absence of dynamical heat fluxes, Q. J. Roy. Meteor. Soc., 113, 603–633, 1987. Sinnhuber, B.-M., Weber, M., Amankwah, A., and Burrows, J.&nbsp;P.: Total ozone during the unusual {A}ntarctic winter of 2002, Geophys. Res. Lett., 30, 1580, <a href="http://dx.doi.org/10.1029/2002GL016798">https://doi.org/10.1029/2002GL016798</a>, 2003. Solomon, S., Portmann, R.&nbsp;W., Garcia, R., Thomason, L.&nbsp;W., Poole, L.&nbsp;R., and McCormick, M.: The role of aerosol variations in anthropogenic ozone depletion at northern midlatitudes, J. Geophys. Res., 101, 6713 – 6727, 1996. Solomon, S., Portmann, R.&nbsp;W., Garcia, R.&nbsp;R., Randel, W., Wu, F., Nagatani, R., Gleason, J., Thomason, L., Poole, L.&nbsp;R., and Mc-Cormick, M.&nbsp;P.: Ozone depletion at mid-latitudes: Coupling of volcanic aerosols and temperature variability to anthropogenic chlorine, Geophys. Res. Lett., 28, 1871–1874, 1998. Soukharev, B.&nbsp;E. and Hood, L.&nbsp;L.: Solar cycle variation of stratospheric ozone: {M}ultiple regression analysis of long-term satellite data sets and comparisons with models, J. Geophys. Res., 111, D20314, <a href="http://dx.doi.org/10.1029/2006JD007107">https://doi.org/10.1029/2006JD007107</a>, 2006. Steinbrecht, W., Claude, H., K{ö}hler, U., and Hoinka, K.&nbsp;P.: Correlations between tropopause height and total ozone: {I}mplications for long-term changes, J. Geophys. Res., 103, 19183–19192, 1998. Stolarski, R. S. and Frith, S. M.: Search for evidence of trend slow-down in the long-term TOMS/SBUV total ozone data record: the importance of instrument drift uncertainty, Atmos. Chem. Phys., 6, 4057–4065, https://doi.org/10.5194/acp-6-4057-2006, 2006. Stolarski, R.&nbsp;S., Douglass, A.&nbsp;R., Steenrood, S., and Pawson, S.: Trends in stratospheric ozone: Lessons learned from a 3D chemical transport model, J. Atmos. Sci., 63, 1028–1041, 2006. Thomason, L.&nbsp;W. and Peter, T.&nbsp;(Eds.): Assessment of Stratospheric Aerosol Properties ({ASAP}). SPARC {R}ep. 4, 2006. Thomason, L.&nbsp;W., Poole, L.&nbsp;R., and Deshler, T.: A global climatology of stratospheric aerosol surface area density deduced from S}tratospheric {A}erosol and {G}as {E}xperiment {II measurements: 1984&nbsp;1994, J. Geophys. Res., 102, 8967–8976, 1997. Waibel, A.&nbsp;E., Peter, T., Carslaw, K.&nbsp;S., Oelhaf, H., Wetzel, G., Crutzen, P.&nbsp;J., Pöschl, U., Tsias, A., Reimer, E., and Fischer, H.: Arctic Ozone Loss Due to Denitrification, Science, 283, 2064–2069, <a href="http://dx.doi.org/10.1126/science.283.5410.2064">https://doi.org/10.1126/science.283.5410.2064</a>, 1999. Weber, M., Dohmse, S., Wittrock, F., Richter, A., Sinnhuber, B.-M., and Burrows, J.&nbsp;P.: Dynamical control of NH and SH winter/spring total ozone from GOME observations 1995–2002, Geophys. Res. Lett., 30, 1583, <a href="http://dx.doi.org/10.1029/2002GL016799">https://doi.org/10.1029/2002GL016799</a>, 2003. Weber, M., Lamsal, L. N., Coldewey-Egbers, M., Bramstedt, K., and Burrows, J. P.: Pole-to-pole validation of GOME WFDOAS total ozone with groundbased data, Atmos. Chem. Phys., 5, 1341–1355, https://doi.org/10.5194/acp-5-1341-2005, 2005. Weber, M., Lamsal, L.&nbsp;N., and Burrows, J.&nbsp;P.: Improved SCIAMACHY WFDOAS total ozone retrieval: Steps towards homogenising long-term total ozone datasets from GOME, SCIAMACHY, and GOME2, in: Proc. "Envisat Symposium 2007", Montreux, Switzerland, 23–27 April 2007, ESA SP-636, 2007. Wohltmann, I., Lehmann, R., Rex, M., Brunner, D., and Mader, J.: A process-oriented regression model for column ozone, J. Geophys. Res., 112, D12 304, <a href="http://dx.doi.org/10.1029/2006JD007573">https://doi.org/10.1029/2006JD007573</a>, 2007. World Meteorological Organization: Scientific Assessment of of Ozone Depletion: 2006. Global Ozone Research and Monitoring Project – {R}eport {N}o. 50, 2007. Yang, E.-S., Cunnold, D.&nbsp;M., Newchurch, M.&nbsp;J., Salawitch, R.&nbsp;J., McCormick, M.&nbsp;P., Russell III, J.&nbsp;M., Zawodny, J.&nbsp;M., and Oltmans, S.&nbsp;J.: First stage of {A}ntarctic ozone recovery, J. Geophys. Res., 113, D20308, <a href="http://dx.doi.org/10.1029/2007JD009675">https://doi.org/10.1029/2007JD009675</a>, 2008.