Nonlinear Processes in Geophysics www.nonlin-processes-geophys.net 1023-5809 1607-7946 16 3 2009 10.5194/npg-16-409-2009 http://www.nonlin-processes-geophys.net/16/409/2009/ http://www.nonlin-processes-geophys.net/16/409/2009/npg-16-409-2009.html http://www.nonlin-processes-geophys.net/16/409/2009/npg-16-409-2009.pdf 409 418 2009-06-19 Upper stratospheric ozone decrease events due to a positive feedback between ozone and the ozone dissociation rate G. R. Sonnemann sonnemann@iap-kborn.de P. Hartogh Leibniz-Institute of Atmospheric Physics at the University of Rostock, Schloss-Str. 6, 18225 Ostseebad Kühlungsborn, Germany Max-Planck-Institute for Solar System Research, Max-Planck-Str. 2, 37191 Katlenburg-Lindau, Germany Ozone measurements taken with a ground based microwave instrument at Lindau (51.66° N, 10.13° E) over some years showed strong ozone decrease events within the stratopause region, particularly during the winter half-year. These events are characterized by a marked drop of the ozone mixing ratio from two to three ppmv to less than half a ppmv in extreme cases. Simultaneous water vapor measurements at the same place, also carried out by a microwave instrument, showed a strong increase of its mixing ratio and the temperature was also enhanced during these episodes. The theoretical analysis brought evidence that these events result from a positive feedback in the complex radiatively-chemical system between the ozone column density and the ozone dissociation rate. % vor jede Referenz Bittner, M., Offermann, D., and Graef, D.: Mesopause temperature variability above midlatitudev station in Europe, J. Geophys. Res., 105, 2045–2058, 2000. CIRA-86: Part~II Middle Atmosphere Models, edited by: Rees, D., Barnett, J. J., Labitzke, K. Clancy, R. T., and Rusch, D. W., Solar Mesosphere Explorer Temperature Climatology of the mesosphere as compared to CIRA Model, Adv. Space Res., 10(12), 187–206, 1986. Clancy, R. T., Rusch, D. W., Thomas, R. J., Allen, M., and Eckman, R. S.: Model ozone photochemistry on the basis of solar mesospheric explorer mesospheric observations, J. Geophys. Res., 92, 3067–3080, 1987. Crutzen, P. J., Grooß, J.-U., Brühl, C., Müller, R., and Russel III, J. M.: A reevaluation of the ozone budget with HALOE UARS data: No evidence of the ozone deficit, Science, 268, 705–708, 1995. Dessler, A. E., Burrage, M. D., Grooss, J.-U., et al.: Selected science highlights from the first 5 years of the Upper Atmospheric Research Satellite (UARS) program, Rev. Geophys., 36, 183–210, 1998. Dlugokencky, E. J., Houweling, S., Bruhwiler, L., Masarie, K. A., Lang, P. M., Miller, J. B., and Tans, P. P.: Atmospheric methane levels off: Temporary pause or a new steady-state?, Geophys. Res. Lett., 30, 1992, doi:10.1029/2003GL018126, 2003. Eluszkiewicz, J. and Allen, M.: A global analysis of the ozone deficit in the upper stratosphere and lower mesosphere, J. Geophys. Res., 98, 1069–1082, 1993. Evans, S. J., Toumi, R., Harries, J. E., Chipperfield, M. P., and Russel, J. M.: Trends in stratospheric humidity and the sensitivity of ozone to these trends, J. Geophys. Res., 103, 8715–8725, 1998. Feigin, A. M. and Konovalov, I. B.: On the possibility of the complicated dynamic behavior of atmospheric photochemical system: Instability of the Antarctic photochemistry during ozone hole formation, J. Geophys. Res., 101, 26023–26038, 1996. Fichtelmann, B. and Sonnemann, G.: On the variation of ozone in the upper mesosphere and lower thermosphere: A comparison between theory and observation, Z. Meteorol., 39, 297–308, 1989. Fichtelmann, B. and Sonnemann, G.: Non-linear behaviour of the photochemistry of minor constituents in the mesosphere, Ann. Geophys., 10, 719–728, 1992. Foster, P. M. de F. and Shine, K. P.: Stratospheric water vapour changes as a possible contributor to observed stratospheric cooling, Geophys. Res. Lett., 26, 3309–3312, 1999. Fox, J. L., Wofsy, S. C., McElroy, M. B., and Prather, M. J.: A stratospheric chemical instability, J. Geophys. Res., 87, 11126–11132, 1982. Frederick, J. E.: Seasonal variations in high-latitude ozone and metastable molecular oxygen emissions: A theoretical interpretation, J. Geophys. Res., 85, 1611–1617, 1980. Hedin, A.: Extension of the MSIS thermosphere model into the middle and lower atmosphere, J. Geophys. Res., 96, 1159–1167, 1991. Kasting, J. F. and Ackerman, T. P.: High atmospheric NO_x levels and multiple photochemical steady states, J. Atmos. Chem., 3, 321–340, 1985. Hartogh, P., Jarchow, C., Sonnemann, G. R., and Grygalashvyly, M.: On the spatiotemporal behavior of ozone within the mesosphere/mesopause region under nearly polar night conditions, J. Geophys. Res., 109, D18303, doi:10.1029/2004JD004576, 2004. Keating, G. M., Brasseur, G. P., Nicholson III, J. Y., and de Rudder, A.: Detection of the response of ozone in the middle atmosphere to short-term solar ultraviolet variations, Geophys. Res. Lett., 12, 449–452, 1985. Khalil, M. A. K., Rasmussen, R. A., and Moraes, F.: Atmospheric methane at Cap Meares: Analysis of a high-resolution data base and its environmental implications, J. Geophys. Res., 98, 14753–14770, 1993. Kheshgi, H. S., Jain, A. K., Kotamarthi, V. R., and Wuebbles, D. J.: Future atmospheric methane concentrations in the context of stabilization of greenhouse gas concentrations, J. Geophys. Res., 104, 19183–19190, 1999. Kleinman, L. I.: The low and high NO_x regime, J. Geophys. Res., 96, 20721–20733, 1991. Kley, D. J., Russell III, M., and Phillips, C. (Eds.): SPARC Assessment of Upper Tropospheric and Stratospheric Water Vapor, SPARC Tech. Rep., 2, 312~pp., 2000. Körner, U. and Sonnemann, G. R.: Global 3D-modeling of water vapor concentration of the mesosphere/mesopause region and implications with respect to the NLC region, J. Geophys. Res., 106, 9639–9651, 2001. Lebonnois, S., Quémerais, E., Montmessin, F., Lefèvre, F., Perrier, S., Bertaux, J.-L., and Forget, F.: Vertical distribution of ozone on Mars as measured by SPICAM/Mars Express using stellar occultations, J. Geophys. Res., 111, E09S05, doi:10.1029/2005JE002643, 2006. Lefèvre, F., Lebonnois, S., Montmessin, F., and Forget, F.: Three-dimensional modeling of ozone on Mars, J. Geophys. Res., 109, E07004, doi:10.1029/2004JE002268, 2004. McKenna, D. S., Groß, 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(D15), 4256, doi:10.1029/2000JD000113, 2002. Mcpeters, R. D.: The Behavior of Ozone Near the Stratopause From Two Years of BUV Observations, J. Geophys. Res., 85(C8), 4545–4550, 1980. McPherson, R. S., Bergman, K. H., Kistler, R. E., Rasch, G. E., and Gordon, D. S.: The NMC Operational Global Data Assimilation System, Mon. Weather Rev., 107, 1445–1461, 1979. Oldmans, S. J. and Hofmann, D. J.: Increase in lower stratospheric water vapour and a midlatitude northern hemisphere site from 1981–1994, Nature, 374, 146–149, 1995. Poppe, D. and Lustfeld, H.: Nonlinearities in the gas phase chemistry of the troposphere: Oscillating concentrations in a simplified mechanism, J. Geophys. Res., 101, 14373–14380, 1996. Prather, M. J., McElroy, M. B., Wofsy, S. C., and Logan, J. A.: Stratospheric chemistry: Multiple solutions, Geophys. Res. Lett., 6, 163–164, 1979. Randel, W. J., Wu, F., Vömel, H., Nedoluha, G. E., and Forster, P.: Decreases in stratospheric water vapor after 2001: Links to changes in the tropical tropopause and the Brewer-Dobson circulation, J. Geophys. Res., 111, D12312, doi:10.1029/2005JD006744, 2006. Rasmussen, R. A. and Khalil, M. A. K.: Atmospheric methane in the recent and ancient atmospheres: Concentrations, trends, and interhemispheric gradients, J. Geophys. Res., 89, 11599–11605, 1984. Reinsel, G. C., Tiao, G. C., DeLuisi, J. J., Mateer, C. L., Miller, A. J., and Frederick, J. E.: Analysis of upper stratospheric Umkehr ozone profile data for trends and the effects of stratospheric aerosols, J. Geophys. Res., 89, 4833–4840, 1984. Reinsel, G. C., Tiao, G. C., Miller, A. J., Wuebbles, D. J., Connell, P. S., Mateer, C. L., and DeLuisi, J. J.: Statistical analysis of total ozone and stratospheric Umkehr data for trends and solar cycle relationship, J. Geophys. Res., 92, 2201–2209, 1987. Röth, E.-P.: Fast algorithm to calculate the photon flux in optically dense media for use in photochemical models, Ber. Bunsen-Gesellsch, Phys. Chem., 96, 417–420, 1994. Rusch, D. W., Mount, G. H., Barth, C. A., Rottman, G. J., Thomas, R. J., Thomas, G. E., Sanders, R. W., Lawrence, G. N., and Eckman, R. S.: Ozone density in the lower mesosphere measured by a limb scanning ultraviolet spectrometer, Geophys. Res. Lett., 10, 241–244, 1983. Scherer, M., Vömel, H., Fueglistaler, S., Oltmans, S. J., and Staehelin, J.: Trends and variability of midlatitude stratospheric water vapour deduced from the re-evaluated Boulder balloon series and HALOE, Atmos. Chem. Phys., 8, 1391–1402, 2008. Seele, C. P. and Hartogh, P.: Water vapor of the polar middle atmosphere: Annual variation and summer mesosphere conditions as observed by ground-based microwave spectroscopy, Geophys. Res. Lett., 26, 1517–1720, 1999. Seele, C. P. and Hartogh, P.: A case study on middle atmospheric water vapor transport during the February 1998 stratospheric warming, Geophys. Res. Lett., 27, 3309–3312, 2000. Siskind, D. E., Connor, B. J., Eckman, R. S., Remsberg, E. E., Tsou, J. J., and Parrish, A.: An intercomparison of model ozone deficits in the upper stratosphere and mesosphere from two data sets, J. Geophys. Res., 100, 11191–11201, 1995. Solomon, S., Rusch, D. W., Thomas, R. J., and Eckman, R. S.: Comparison of mesospheric ozone abundances measured by the Solar Mesospheric Explorer and model calculations, Geophys. Res. Lett., 10, 249–252, 1983. Sonnemann, G.: On the formation of particlelike pattern, the amplitude modulated route to chaos and the wave-particle dualism in three-dimensional systems under global constraints, Prog. Theor. Phys., 99(6), 931–962, 1998. Sonnemann, G. and Fichtelmann, B.: Subharmonics, cascades of period doubling, and chaotic behavior of photochemistry of the mesopause region, J. Geophys. Res., 102, 1193–1203, 1997. Sonnemann, G., Kremp, Ch., Ebel, A., and Berger, U.: A three-dimensional dynamic model of minor constituents of the mesosphere, Atmos. Environm., 32, 3157–3172, 1998. Sonnemann, G. R. and Feigin, A. M.: Nonlinear behavior of a reaction-diffusion system of the photochemistry within the mesopause region, Phys. Rev. E, 59, 1719–1726, 1999. Sonnemann, G. R. and Grygalashvyly, M.: Solar influence on mesospheric water vapor with impact on NLCs, J. Atmos. Sol.-Terr. Phy., 67, 177–190, 2005. Sonnemann, G. R., Grygalashvyly, M., and Berger, U.: Autocatalytic water vapor production as a source of large mixing ratios within the middle to upper mesosphere, J. Geophys. Res., 110, D15303, doi:10.1029/2004JD005593, 2005. Sonnemann, G. R., Hartogh, P., Jarchow, C., Grygalashvyly, M., and Berger, U.: On the winter anomaly of the night-to-day ratio of ozone in the middle to upper mesosphere in middle to high latitudes, Adv. Space Res., 40, 846–854, 2007. Sonnemann, G. R., Hartogh, P., Grygalashvyly, M., Li, S., and Berger, U.: The quasi 5-day signal in the mesospheric water vapor concentration in high latitudes in 2003 – a comparison between observations at ALOMAR and calculations, J. Geophys. Res., 113, D04101, doi:10.1029/2007JD008875, 2008. Stewart, R. W.: Multiple steady states in atmospheric chemistry, J. Geophys. Res., 98, 20601–20611, 1993. Stewart, R. W.: Dynamics of the low to high NO_x transition in a simplified tropospheric photochemical model, J. Geophys. Res., 100, 8929–8943, 1995. Summers, M. E., Conway, R. R., Siskind, D. E., Bevilacqua, R., Strobel, D. F., and Zasadil, S.: Mesospheric HO_x photochemistry: Constraints from recent satellite measurements of OH and H₂O, Geophys. Res. Lett., 23, 2097–2100, 1996. Summers, M. E., Conway, R. R., Siskind, D. E., Stevens, M. H., Offermann, D., Riese, M., Preusse, P., Strobel, D. F., and Russel III, J. M.: Implications of satellite OH observations for middle atmospheric H₂O and ozone, Science, 277, 1967–1970, 1997. Thomas, G. E., Olivero, J. J., Jensen, E. J., Schröder, W., and Toon, O. B.: Relation between increasing methane and the presence of ice clouds at the mesopause, Nature, 338, 490–492, 1989. Thomas, G. E. and Olivero, J. J.: Noctilucent clouds as possible indicators of global change in the mesosphere, Adv. Space Res., 28(7), 937–946, 2001. White, W. H. and Dietz, D.: Does the photochemistry of the troposphere admit more than one steady state?, Nature, 309, 242–244, 1984. Yang, P. and Brasseur, G.: Dynamics of the oxygen-hydrogen system in the mesosphere, 1. Photochemical equilibria and catastrophe, J. Geophys. Res., 99, 20955–20965, 1994. Zimmermann, J. and Poppe, D.: Nonlinear chemical couplings in the tropospheric NO_x-HO_x gas phase chemistry, J. Atmos. Chem., 17, 141–155, 1993.