References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-7073-2012

Record-breaking ozone loss in the Arctic winter 2010/2011: comparison with 1996/1997

Kuttippurath

¹ Godin-Beekmann

¹ Lefèvre

¹ Nikulin

² Santee

M. L.

³ Froidevaux

UPMC Université Paris 06, LATMOS-IPSL, CNRS/INSU, UMR8190, 75005 Paris, France

Swedish Meteorological Hydrological Institute, Kiruna, Sweden

JPL/NASA, California Institute of Technology, Pasadena, California, USA

06 08 2012

12 15 7073 7085

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/12/7073/2012/acp-12-7073-2012.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/7073/2012/acp-12-7073-2012.pdf

We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.

References 1

Andersen, S. B. and Knudsen, B. M.: The influence of vortex ozone depletion on Arctic ozone trends, Geophys. Res. Lett., 29, 2013, http://dx.doi.org/10.1029/2001GL014595doi:10.1029/2001GL014595, 2002.

Balis, D., Isaksen, I. S. A., Zerefos, C., Zyrichidou, I., Eleftheratos, K., Tourpali, K., Bojkov, R., Rognerud, B., Stordal, F., Søvde, O. A., and Orsolini, Y.: Observed and Modelled record ozone decline over the Arctic during winter/spring 2011, Geophys. Res. Lett., 38, L23801, http://dx.doi.org/10.1029/2011GL049259doi:10.1029/2011GL049259, 2011.

Burkholder, J. B., Orlando, J. J., and Howard, C. J.: Ultraviolet absorption cross-sections of Cl2O2 between 210 and 410 nm, J. Phys. Chem., 94, 687–695, 1990.

Butz, A., Bösch, H., Camy-Peyret, C., Dorf, M., Engel, A., Payan, S., and Pfeilsticker, K.: Observational constraints on the kinetics of the ClO-BrO and ClO-ClO ozone loss cycles in the Arctic winter stratosphere, Geophys. Res. Lett., 34, L05801, http://dx.doi.org/10.1029/2006GL028718doi:10.1029/2006GL028718, 2007.

Coy, L., Nash, E. R., and Newman, P. A.: Meteorology of the polar vortex: Spring 1997, Geophys. Res. Lett., 24, 2693–2696, 1997.

Froidevaux, L., Jiang, Y. B., Lambert, A., Livesey, N. J., Read, W. G., Waters, J. W., Browell, E. V., Hair, J. W., Avery, M. A., McGee, T. J., Twigg, L. W., Sumnicht, G. K., Jucks, K. W., Margitan, J. J., Sen, B., Stachnik, R. A., Toon, G. C., Bernath, P. F., Boone, C. D., Walker, K. A., Filipiak, M. J., Harwood, R. S., Fuller, R. A., Manney, G. L., Schwartz, M. J., Daffer, W. H., Drouin, B. J., Cofield, R. E., Cuddy, D. T., Jarnot, R. F., Knosp, B. W., Perun, V. S., Snyder, W. V., Stek, P. C., Thurstans, R. P., Wagner, P. A.: Validation of Aura Microwave Limb Sounder stratospheric ozone measurements, J. Geophys. Res., 113, D15S20, http://dx.doi.org/10.1029/2007JD008771doi:10.1029/2007JD008771, 2008.

Goutail, F., Pommereau, J.-P., Lefèvre, F., van Roozendael, M., 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, http://dx.doi.org/10.5194/acp-5-665-2005doi:10.5194/acp-5-665-2005, 2005.

Grooß, J.-U., Konopka, P., and Müller, R.: Ozone chemistry during the 2002 Antarctic vortex split, J. Atmos. Sci., 62, 860–870, 2005.

Hanson, D. and Mauersberger, K.: Laboratory studies of the nitric acid trihydrate: implications for the south polar stratosphere, Geophys. Res. Lett., 15, 855–858, 1998.

Hanson, G. and Chipperfield, M.: Ozone loss at the edge of the polar vortex, J. Geophys. Res., 104, 1837–1845, 1999.

Harris, N. R. P., Lehmann, R., Rex, M., and von der Gathen, P.: A closer look at Arctic ozone loss and polar stratospheric clouds, Atmos. Chem. Phys., 10, 8499–8510, http://dx.doi.org/10.5194/acp-10-8499-2010doi:10.5194/acp-10-8499-2010, 2010.

Hurwitz, M. M., Newman, P. A., and Garfinkel, C. I.: The Arctic vortex in March 2011: a dynamical perspective, Atmos. Chem. Phys., 11, 11447–11453, http://dx.doi.org/10.5194/acp-11-11447-2011doi:10.5194/acp-11-11447-2011, 2011.

Kleinböhl, A., Bremer, H., Küllmann, H., Kuttippurath, J., Browell, E. V., Canty, T., Salawitch, R. J., Toon, G. C., and Notholt, J.: Denitrification in the Arctic mid-winter 2004/2005 observed by airborne submillimeter radiometry, Geophys. Res. Lett., 32, L19811, http://dx.doi.org/10.1029/2005GL023408doi:10.1029/2005GL023408, 2005.

Knudsen, B. M., Larsen, N., Mikkelsen, I. S., Morcrette, J.-J., Braathen, G. O., Kyro, E., Fast, H., Gernandt, H., Kanzawa, H., Nakane, H., Dorokhov, V., Yushkov, V., Hansen, G., Gil, M., and Shearman, R. J.: Ozone depletion in and below the Arctic vortex for 1997, Geophys. Res. Lett., 25, 627–630, 1998.

Kondo, Y., H. Irie, M. Koike, and G. E. Bodeker: Denitrification and nitrification in the Arctic stratosphere during the winter of 1996–1997, Geophys. Res. Lett., 27, 337–340, http://dx.doi.org/10.1029/1999GL011081doi:10.1029/1999GL011081, 2000.

Kuttippurath, J., Goutail, F., Pommereau, J.-P., Lefèvre, F., Roscoe, H. K., Pazmiño, A., Feng, W., Chipperfield, M. P., and Godin-Beekmann, S.: Estimation of Antarctic ozone loss from ground-based total column measurements, Atmos. Chem. Phys., 10, 6569–6581, http://dx.doi.org/10.5194/acp-10-6569-2010doi:10.5194/acp-10-6569-2010, 2010a.

Kuttippurath, J., Godin-Beekmann, S., Lefèvre, F., and Goutail, F.: Spatial, temporal, and vertical variability of polar stratospheric ozone loss in the Arctic winters 2004/2005–2009/2010, Atmos. Chem. Phys., 10, 9915–9930, http://dx.doi.org/10.5194/acp-10-9915-2010doi:10.5194/acp-10-9915-2010, 2010b.

Lefèvre F., Figarol, F., Carslaw, K. S., and Peter, T.: The 1997 Arctic ozone depletion quantified from three-dimensional model simulations, Geophys. Res. Lett., 25, 2425–2428, 1998.

Livesey, N. J., Read, W. G., Froidevaux, L., Waters, J. W., Santee, M. L., Pumphrey, H. C., Wu, D. L., Shippony, Z., and Jarnot, R. F.: The UARS Microwave Limb Sounder version 5 data set: Theory, characterization, and validation, J. Geophys. Res., 108, 4378, http://dx.doi.org/10.1029/2002JD002273doi:10.1029/2002JD002273, 2003.

Livesey, N. J., Read, W. G., Froidevaux, L., Lambert, A., Manney, G. L., Pumphrey, H. C., Santee, M. L., Schwartz, M. J., Wang, S., Cofeld, R. E., Cuddy, D. T., Fuller, Jarnot, R. F., Jiang, J. H., Knosp, B. W., Stek, P. C., Wagner, P. A., and Wu, D. L.: Earth Observing System (EOS) Aura Microwave Limb Sounder (MLS) Version 3.3 Level 2 data quality and description document, JPL D-33509, Jet Propulsion Laboratory California Institute of Technology, Pasadena, California, USA, 91109–8099, 2011.

Manney, G. L., Froidevaux, L., Santee, M. L., Zurek, R. W., and Waters, J. W.: MLS observations of Arctic ozone loss in 1996–1997, Geophys. Res. Lett., 24, 2697–2700, 1997.

Manney, G. L., Froidevaux, L., Santee, M., Livesey, N., Sabutis, J., and Waters, J.: Variability of ozone loss during Arctic winter (1991–2000) estimated from UARS Microwave Limb Sounder measurements, J. Geophys. Res., 108, 4149, http://dx.doi.org/10.1029/2002JD002634doi:10.1029/2002JD002634, 2003.

Manney, G. L., Santee, M. L., Rex, M., Livesey, N. J., Pitts, M. C., Veefkind, P., Nash, E. R., Wohltmann, I., Lehmann, R., Froidevaux, L., Poole, L. R., Schoeberl, M. R., Haffner, D. P., Davies, J., Dorokhov, V., Gernandt, H., Johnson, B., Kivi, R., Kyro, E., Larsen, N., Levelt, P. F., Makshtas, A., McElroy, C. T., Nakajima, H., Parrondo, M. C., Tarasick, D. W., von der Gathen, P., Walker, K. A., and Zinoviev, N. S.: Unprecedented Arctic ozone loss in 2011, Nature, 478, 469–475, http://dx.doi.org/10.1038/nature10556doi:10.1038/nature10556, 2011.

Papanastasiou, D. K., Papadimitriou, V. C., Fahey, D. W., and Burkholder, J. B.: UV Absorption Spectrum of the ClO Dimer (Cl2O2) between 200 and 420 nm, J. Phys. Chem. A, 113, 13711–13726, 2009.

Pitts, M. C., Thomason, L. W., Poole, L. R., and Winker, D. M.: Characterization of Polar Stratospheric Clouds with spaceborne lidar: CALIPSO and the 2006 Antarctic season, Atmos. Chem. Phys., 7, 5207–5228, http://dx.doi.org/10.5194/acp-7-5207-2007doi:10.5194/acp-7-5207-2007, 2007.

Randall, C. E., Harvey, V. L., Siskind, D. E., France, J., Bernath, P. F., Boone, C. D., and Walker, K. A.: NO$_\mathrm x$ descent in the Arctic middle atmosphere in early 2009, Geophys. Res. Lett., 36, L18811, http://dx.doi.org/10.1029/2009GL039706doi:10.1029/2009GL039706, 2009.

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, http://dx.doi.org/10.1029/2003GL018844doi:10.1029/2003GL018844, 2004.

Sander, S., Friedl, R., Ravishankara, A., Golden, D., Kolb, C., Kurylo, M., Molina, M., Moortgat, G., Keller-Rudek, H., Finlayson-Pitts, B., Wine, P., Huie, R., and Orkin, V.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies (Evaluation Number 15), JPL Publication: 06–2, 2006.

Santee, M. L., Manney, G. L., Froidevaux, L., Zurek, R. W., and Waters, J. W.: MLS observations of ClO and HNO3 in the 1996–97 Arctic polar vortex, Geophys. Res. Lett., 24, 2713–2716, 1997.

Santee, M. L., Manney, G. L., Froidevaux, L., Read, W. G., and Waters, J. W.: Six years of UARS Microwave Limb Sounder HNO3 observations: Seasonal, interhemispheric, and interannual variations in the lower stratosphere, J. Geophys. Res., 104, 8225–8246, 1999.

Santee, M. L., Lambert, A., Read, W. G., Livesey, N. J., Manney, G. L., Cofield, R. E., Cuddy, D. T., Daffer, W. H., Drouin, B. J., Froidevaux, L., Fuller, R. A., Jarnot, R. F., Knosp, B. W., Perun, V. S., Snyder, W. V., Stek, P. C., Thurstans, R. P., Wagner, P. A., Waters, J. W., Connor, B., Urban, J., Murtagh, D., Ricaud, P., Barrett, B., Kleinböhl, A., Kuttippurath, J., Küllmann, H., von Hobe, M., Toon, G. C., and Stachnik, R. A.: Validation of the Aura Microwave Limb Sounder ClO measurements, J. Geophys. Res., 113, D15S22, http://dx.doi.org/10.1029/2007JD008762doi:10.1029/2007JD008762, 2008.

Shine, K. P.: The middle atmosphere in the absence of dynamical heat fluxes, Q. J. Roy. Meteorol. Soc., 113, 603–633, 1987.

Singleton, C. S., Randall, C. E., Chipperfield, M. P., 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, http://dx.doi.org/10.5194/acp-5-597-2005doi:10.5194/acp-5-597-2005, 2005.

Sinnhuber, B.-M., Stiller, G. P., Ruhnke, R., von Clarmann, T., Kellmann, S., and Aschmann, J.: Arctic winter 2010/2011 at the brink of an ozone hole, Geophys. Res. Lett., 38, L24814, http://dx.doi.org/10.1029/2011GL049784doi:10.1029/2011GL049784, 2011.

Solomon, S., Crutzen, P. J., and Roble, R. G.: Photochemical coupling between the thermosphere and the lower atmosphere: 1. Odd nitrogen from 50 to 120 km, J. Geophys. Res., 87, 7206–7220, 1982.

Solomon, S., Portmann, R. W., and Thompson, D. W. J.: Contrasts between Antarctic and Arctic ozone depletion, P. Natl. Acad. Sci. USA, 104, 445–449, 2007.

Sonkaew, T., von Savigny, C., Eichmann, K.-U., Weber, M., Rozanov, A., Bovensmann, H., and Burrows, J. P.: Chemical ozone loss in Arctic and Antarctic polar winter/spring season derived from SCIAMACHY limb measurements 2002–2009, Atmos. Chem. Phys. Discuss., 11, 6555–6599, http://dx.doi.org/10.5194/acpd-11-6555-2011doi:10.5194/acpd-11-6555-2011, 2011. \hack

Stimpfle, R. M., Wilmouth, D. M., Salawitch, R. J., and Anderson, J. G.: First measurements of ClOOCl in the stratosphere: the coupling of ClOOCl and ClO in the Arctic polar vortex, J. Geophys. Res., 109, D03301, http://dx.doi.org/10.1029/2003JD003811doi:10.1029/2003JD003811, 2004

Terao, Y., Sasano, Y., Nakajima, H., Tanaka, H., and Yasunari, T.: Stratospheric ozone loss in the 1996/1997 Arctic winter: Evaluation based on multiple trajectory analysis for doublesounded air parcels by ILAS, J. Geophys. Res., 107, 8210, http://dx.doi.org/10.1029/2001JD000615doi:10.1029/2001JD000615, 2002.

Tilmes, S., Müller, R., Engel, A., Rex, M., and Russell III, J.: Chemical ozone loss in the Arctic and Antarctic stratosphere between 1992 and 2005, Geophys. Res. Lett., 33, L20812, http://dx.doi.org/10.1029/2006GL026925doi:10.1029/2006GL026925, 2006.

Tripathi, O. P., Godin-Beekmann, S., Lefèvre, F., Marchand, M., Pazmiño, A., Hauchecorne, A., Goutail, F., Schlager, H., Volk, C. M., Johnson, B., Konig-Langlo, G., Balestri, S., Stroh, F., Bui, T. P., Jost, H. J., Deshler, T., and von der Gathen, P.: High resolution simulation of recent Arctic and Antarctic stratospheric chemical ozone loss compared to observations, J. Atmos. Chem., 55, 205–226, http://dx.doi.org/10.1007/s10874-006-9028-8doi:10.1007/s10874-006-9028-8, 2006.

Vogel, B., Konopka, P., Grooß, J.-U., Müller, R., Funke, B., López-Puertas, M., Reddmann, T., Stiller, G., von Clarmann, T., and Riese, M.: Model simulations of stratospheric ozone loss caused by enhanced mesospheric NO$_\rm x $ during Arctic Winter 2003/2004, Atmos. Chem. Phys., 8, 5279–5293, http://dx.doi.org/10.5194/acp-8-5279-2008doi:10.5194/acp-8-5279-2008, 2008.

Woyke, T., Müller, R., Stroh, F., McKenna, D. S., Engel, A., Margitan, J. J., Rex, M., and Carslaw, K. S.: A test of our understanding of the ozone chemistry in the Arctic polar vortex based on in situ measurements of ClO, BrO, and O3 in the 1994/1995 winter, J. Geophys. Res., 104, 18755–18768, 1999.

WMO (World Meteorological Organisation): Scientific assessment of ozone depletion: 2006, Global Ozone Research and Monitoring Project-Report No 50, 572~pp., Geneva, Switzerland, 2007.

WMO (World Meteorological Organisation): Scientific assessment of ozone depletion: 2006, Global Ozone Research and Monitoring Project-Report No 52, 516~pp., Geneva, Switzerland, 2011.

Woods, A.: Medium-Range Weather Prediction - the European Approach, Springer, ISBN 978-0387269283, 2006.