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Partitioning Between Chlorine Reservoir Species Deduced from Observations in the Arctic Winter Stratosphere

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Abstract

Simultaneous observations of several chlorine source gases, as well asHCl and ClO, have been performed in the Arctic stratosphere on 1 and 9February 1994, using balloon-borne instrumentation as a contribution toSESAME (Second European Stratospheric Arctic and Mid latitude Experiment).The observed mixing ratios of HCl and N2O show a clearanticorrelation. No severe loss of HCl was observed inside the vortex duringour measurement. These measurements showed that during this period at 20 kmand above, HCl was either in excess, or at least as abundant, asClONO2 and comprised between 50 and 70% of theavailable chlorine, Cly. On 1 February, measurements were madeinside the polar vortex. The air mass sampled on this day showed a clearsignature of diabatic descent, and also enhanced levels of ClO with amaximum of 230 pptv at 22.5 km. A 10 day backward trajectory analysis showedthat these air masses had passed a large region of low temperatures a fewhours prior to the measurement. Temperatures along the back trajectory atthe 475 K and 550 K levels (20.1 and 23.7 km respectively) were cold enoughfor heterogeneous chlorine activation to occur, in agreement with theobserved elevated ClO mixing ratios.

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References

  • Anderson, J. G., Toohey, D. W., and Brune, W. H., 1991: Free radicals within the Antarctic vortex: The role of CFCs in Antarctic ozone loss, Science 251, 39–46.

    Google Scholar 

  • Bauer, R., Engel, A., Franken, H., Klein, E., Kulessa, G., Schiller, C., Schmidt, U., Borchers, R., and Lee, J., 1994: Monitoring the vertical structure of the Arctic polar vortex over northern Scandinavia during EASOE: Regular N2O profile observations, Geophys. Res. Lett. 21, 1211–1214.

    Google Scholar 

  • Considine, D. B., Douglass, A. R., and Jacman, C. H., 1994: Effects of a polar stratospheric cloud parametrization on ozone depletion due to stratospheric aircraft in a two-dimensional model, J. Geophys. Res. 99, 18,879–18,894.

    Google Scholar 

  • Dessler, A. E., Considine, D. B., Morris, G. A., Schoeberl, M. R., Russell III, J. M., Roche, A. E., Kumer, J. B., Mergenthaler, J. L., Waters, J. W., Gille, J. C., and Yue, G. K., 1995: Correlated observations of HCl and ClONO2 from UARS and implications for stratospheric chlorine partitioning, Geophys. Res. Lett. 22, 1721–1724.

    Google Scholar 

  • Engel, A. and Schmidt, U., 1994: Spurengasmessungen zur Charakterisierung der stratosphärischen Zirkulation in der Nordhemisphäre im Winter, Final report to project 01 VOZ 14/5 in the German ozone research program.

  • Farman, J. C., Gardiner, B. G., and Shanklin, J. D., 1985: Large losses of total ozone in Antarctica reveal seasonal ClOx/NOx interaction, Nature 315, 207–210.

    Google Scholar 

  • Gathen von der, P., Rex, M., Harris, N. R. P., Lusic, D., Knudsen, B. M., Braathen, G. O., De Backer, H., Fabian, R., Fast, H., Gil, M., Kyrö, E., Mikkelsen, I. S., Rummukainen, M., Stähelin, J., and Vorotsos, C., 1995: Observational evidence for chemical ozone depletion over the Arctic in winter 1991–92, Nature 375, 131–134.

    Google Scholar 

  • Kaye, J. A., Penkett, S. A., and Ormond, F. M., 1994: Report on the concentrations, lifetimes, and trends of CFCs, Halons, and related species, NASA Ref. Publ. 1339.

  • Knudsen, B. M. and Carver, G. D., 1994: Accuracy of the isentropic trajectories calculated for the EASOE campaign, Geophys. Res. Lett. 21, 1199–1202.

    Google Scholar 

  • Lait, L. R., 1994: An alternative form for potential vorticity, J. Atmos. Sci. 51, 1754–1759.

    Google Scholar 

  • Loewenstein, M., Podolske, J. R., Chan, K. R., and Strahan, S. E., 1990: N2O as a dynamical tracer in the arctic vortex, Geophys. Res. Lett. 17, 477–480.

    Google Scholar 

  • Manney, G. L., Froidevaux, L., Waters, J.W., Zurek, R. W., Read, W. G., Elson, L. S., Kumer, J. B., Mergenthaler, J. L., Roche, A. E., O’Neill, A., Harwood, R. S., MacKenzie, I., and Swinbank, R., 1994: Chemical depletion of ozone in the arctic lower stratosphere during winter 1992–93, Nature 370, 429–434.

    Google Scholar 

  • McCormich, M. P., 1992: Stratospheric ozone profile and total ozone trends derived from the SAGE I and SAGE II data, Geophys. Res. Lett. 19, 269–272.

    Google Scholar 

  • McIntyre, M. E., 1992: Atmospheric dynamics: Some fundamentals, with observational implications, Proc. Internat. School Phys. ‘Enrico Fermi’, 1–64.

  • Müller, R., Crutzen, P. J., Grooß, J.-U., Brühl, C., Russell III, J. M., and Tuck, A. F., 1996: Chlorine activation and ozone depletion in the Arctic vortex: Observations by the Halogen Occultation Experiment on the Upper Atmosphere Research Satellite, accepted for publication in J. Geophys. Res.

  • Naujokat, B., Labitzke, K., Lenschow, R., Rajewski, B., Wiesner, M., and Wohlfahrt, R.-C., 1994: The stratospheric winter 1993/1994: A winter with some minor warmings and an early final warming, Beilage zur Berliner Wetter Karte, SO 24/94.

  • Plumb, R. A. and Ko, M. K. W., 1992: Interrelationships between mixing ratios of long-lived stratospheric constituents, J. Geophys. Res. 97, 10,145–10,156.

    Google Scholar 

  • Poynter, R. L. and Pickett, H. M., 1985: Submillimeter, millimeter, and microwave spectral line catalog, Appl. Optics 24, 2235–2240.

    Google Scholar 

  • Proffitt, M. H., Fahey, D. W., Kelly, K. K., and Tuck, A. F., 1989: High-latitude ozone loss outside the Antarctic ozone hole, Nature 342, 233–237.

    Google Scholar 

  • Rinsland, C. P., Gunson, M. R., Abrams, M. C., Lowes, L. L., Zander, R., Mahieu, E., Goldman, A., and Irion, F. W., 1995: April 1993 Arctic profiles of stratospheric HCl, ClONO2, and CCl2F2 from atmospheric trace molecule spectroscopy/ATLAS 2 infrared solar occultation spectra, J. Geophys. Res. 100, 14,019–14,027.

    Google Scholar 

  • Salawitch, R. J., Wofsy, S. C., Wennberg, P. O., Cohen, R. C., Anderson, J. G., Fahey, D. W., Gao, R. S., Keim, E. R., Woodbridge, E. L., Stimpfle, R. M., Koplow, J. P., Kohn, D. W., Webster, C. R., May, R. D., Pfister, L., Gottlieb, E.W., Michelsen, H. A., Yue, G. K., Wilson, J. C., Brock, C. A., Jonsson, H. H., Dye, J. E., Baumgardner, D., Proffitt, M. H., Loewenstein, M., Podolske, J. R., Elkins, J. E., Dutton, G. S., Hintsa, E. J., Dessler, A. E., Weinstock, E. M., Kelly, K. K., Boering, K. A., Daube, B. C., Chan, K. R., and Bowen, S.W., 1994: The distribution of hydrogen, nitrogen, and chlorine radicals in the lower stratosphere: Implications for changes in O3 due to emission of NOy from supersonic aircraft, Geophys. Res. Lett. 21, 2547–2550.

    Google Scholar 

  • Schmidt, U., Bauer, R., Khedim, A., Klein, E., Kulessa, G., and Schiller, C., 1991: Profile observations of long-lived trace gases in the Arctic vortex, Geophys. Res. Lett. 18, 767–770.

    Google Scholar 

  • Schmidt, U., Bauer, R., Engel, A., Borchers, R., and Lee, J., 1994: The variation of available chlorine, Cly, in the Arctic polar vortex during EASOE, Geophys. Res. Lett. 21, 1215–1218.

    Google Scholar 

  • Schmidt, U. and Khedim, A., 1991: In situmeasurements of carbon dioxide in the winter Arctic vortex and at mid latitudes: An indicator of the ‘age’ of stratospheric air, Geophys. Res. Lett. 18, 763–766.

    Google Scholar 

  • Schmidt, U., Kulessa, G., Klein, E., Röth, E.-P., Fabian, P., and Borchers, R., 1987: Intercomparison of balloon-borne cryogenic whole air samplers during the MAP/GLOBUS 1983 campaign, Planet. Space Sci. 35, 647–656.

    Google Scholar 

  • Schoeberl, M. R., Lait, L. R., Newman, P. A., and Rosenfield, J. E., 1992: The structure of the polar vortex, J. Geophys. Res. 97, 7859–7882.

    Google Scholar 

  • Solomon, S., 1990: Progress towards a quantitative understanding of Antarctic ozone depletion, Nature 347, 347–354.

    Google Scholar 

  • Stachnik, R. A., Hardy, J. C., Tarsala, J. A., Waters, J.W., Erickson, N. R., 1992a: Submillimeterwave heterodyne measurements of stratospheric ClO, HCl, O3 and HO2: first results, Geophys. Res. Lett. 19, 1931–1934.

    Google Scholar 

  • Stachnik, R. A., Hardy, J. C., Tarsala, J. A., and Waters, J. W., 1992b: Balloon-borne submillimeterwave stratospheric measurements, in Optical Methods in Atmospheric Chemistry, SPIE Vol. 1715, pp. 433–440.

  • Stimpfle, R. M., Koplow, J. P., Cohen, R. C., Kohn, D. W., Wennberg, P. O., Judah, D. M., Toohey, D. W., Avallone, L. M., Anderson, J. G., Salawitch, R. J., Woodbridge, E. L., Webster, C. R., May, R. D., Proffitt, M. H., Aiken, A., Margitan, J., Loewenstein, M., Podolske, J. R., Pfister, L., and Chan, K. R., 1994: The response of the ClO radical concentrations to variations in NO2 radical concentrations in the lower stratosphere, Geophys. Res. Lett. 21, 2543–2546.

    Google Scholar 

  • Stolarski, R. S., Bloomfield, P., and McPeters, R. D., 1991: Total ozone trends deduced from Nimbus 7 TOMS data, Geophys. Res. Lett. 18, 1015–1018.

    Google Scholar 

  • Toohey, D. W., Avallone, L. M., Lait, L. R., Newman, P. A., Schoeberl, M. R., Fahey, D. W., Woodbridge, E. L., and Anderson, J. G., 1993: The seasonal evolution of reactive chlorine in the northern hemisphere stratosphere, Science 261, 1134–1136.

    Google Scholar 

  • Toumi, R., Jones, R. L., and Pyle, J. A., 1993: Stratospheric ozone depletion by ClONO2 photolysis, Nature 365, 37–39.

    Google Scholar 

  • Tuck, A. F., Webster, C. R., May, R. D., Scott, D. C., Hovde, S. J., Elkins, J.W., and Chan, K. R., 1995: Time and temperature dependence of fractional HCl abundances from airborne data in the southern hemisphere during 1994, Faraday Discuss. 100/22.

  • Waters, J. W., Froideveaux, L., Read, W. G., Manney, G. L., Elson, L. S., Flower, D. A., Jarnot, R. F., and Harwood, R. S., 1993: Stratospheric ClO and ozone from the microwave limb sounder on the upper atmosphere research satellite, Nature 362, 597–602.

    Google Scholar 

  • Webster, C. R., May, R. D., Jaeglé, L., Hu, H., Sander, S. P., Gunson, M. R., Toon, G. C., Russell III, J. M., Stimpfle, R. M., Koplow, J. P., Salawitch, R. J., and Michelsen, H. A., 1994: Hydrochloric acid and the chlorine budget of the lower stratosphere, Geophys. Res. Lett. 21, 2575–2578.

    Google Scholar 

  • Webster, S. R., May, R. D., Toohey, D. W., Avallone, L. M., Anderson, J. G., Newman, P., Lait, L., Schoeberl, M. R., Elkins, J.W., and Chan, K. R., 1993: Chlorine chemistry on polar stratospheric cloud particles in the Arctic winter, Science 261, 1130–1134.

    Google Scholar 

  • Wege, K. and Claude, H., 1994: On a period with very low ozone concentrations within the lower stratosphere, Geophys. Res. Lett. 21, 1395–1398.

    Google Scholar 

  • WMO, Scientific Assessment of Ozone Depletion: 1991, 1991: Report No. 25, World Meteorological Organisation, Geneva, Switzerland.

    Google Scholar 

  • WMO, Scientific Assessment of Ozone Depletion: 1994, 1994: Report No. 37, World Meteorological Organisation, Geneva, Switzerland.

    Google Scholar 

  • Zander, R., Gunson, M. R., Foster, J. C., Rinsland, C. P., and Namkung, J., 1990: Stratospheric ClONO2, HCl, and HF concentration profiles derived from Atmospheric Trace Molecule Spectroscopy Experiment Spacelab 3 observation: an update, J. Geophys. Res. 95, 20510–20525.

    Google Scholar 

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Engel, A., Schmidt, U. & Stachnik, R.a. Partitioning Between Chlorine Reservoir Species Deduced from Observations in the Arctic Winter Stratosphere. Journal of Atmospheric Chemistry 27, 107–126 (1997). https://doi.org/10.1023/A:1005781919448

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