Abstract
In 1978–1980 nine aircraft flights to an altitude of up to 15 km were made over western Europe. Sulfur dioxide was measured with a sensitive chemiluminescence method consisting of separate sampling and analysis stages and application of a wet chemical filter procedure (detection limit: 8 pptv SO2).
The measurements performed in the upper troposphere and lower stratosphere lead to some unexpected results: (a) the meteorological conditions at the tropopause level have an important influence on the observed SO2 mixing ratio; (b) between the 500 mb and the actual tropopause level the SO2 mixing ratio is found to be <100 pptv, and weak vertical gradients of SO2 suggest only a small flux of tropospheric SO2 into the stratosphere; (c) increasing SO2 mixing ratios within the first kilometers of the stratosphere give strong support to a stratospheric source of SO2.
In the light of improved one-dimensional models considering the vertical distribution of stratospheric sulfur compounds (Crutzen, 1981; Turco et al. 1981) it can be shown that the oxidation of organic sulfur compounds (e.g., OCS, CS2) seems to be a stratospheric source of SO2. Furthermore, the flux calculations based on the SO2 mixing ratios measured at the tropopause level indicate that the contribution of tropospheric (man-made) SO2 to the stratospheric aerosol layer is of only minor importance.
Similar content being viewed by others
References
Anjea, V. P., Anjea, A. P., and Adams, D. F., 1982, Biogenic sulfur compounds and the global sulfur cycle. J. Air Pollut. Control Assoc. 32, 803–806.
Bandy, A. R., Maroulis, P. J., Shalaby, L., and Wilner, L. A., 1983, Evidence for a short tropospheric residence time for carbon disulfide, Geophys. Res. Lett. 8, 1180–1183.
Baulch, D. L., Cox, R. A., Hampson, R. F., Jr., Kerr, J. A., Troe, J., and Watson, R. T., 1980, Evaluated kinetic and photochemical data for atmospheric chemistry, J. Phys. Chem. Ref. Data 9, (2).
Cadle, R. D., 1980, A comparison of volcanic with other fluxes of atmospheric trace gas constituents, Rev. Geophys. Space Phys. 18, 746–752.
Castleman, A. W., Munkelwitz, H. R., and Manowitz, B., 1974, Isotopic studies of the sulfur component of the stratospheric aerosol layer, Tellus 26, 222–234.
Crutcher, H. L. and Davies, O. M., 1969, U.S. Navy marine climatic atlas of the world 8, NAVAIR 50-1C-54, Chief of Naval Operations, Washington, D.C.
Crutzen, P. J., 1976, The possible importance of CSO for the sulfate layer of the stratosphere, Geophys. Res. Lett. 3, 73–76.
Crutzen, P. J., Heidt, L. E., Krasnec, J. P., Pollock, W. H., and Seiler, W., 1979, Biomass burning as a source of atmospheric gases CO, H2, N2O, NO, CH3Cl and COS, Nature 282, 253–256.
Crutzen, P. J., 1981, On the vertical distribution of gaseous sulfur compounds, unpublished manuscript.
Danielsen, E. F., 1959, The laminar structure of the atmosphere and its relation to the concept of a tropopause, Arch Meteorol. Geophys. Biokl., Ser. A 11, 293–332.
Friend, J. P., Leifer, R., and Trichon, M., 1973, On the formation of stratospheric aerosol, J. Atmos. Sci. 30, 465–479.
Georgii, H.-W. and Meixner, F. X., 1980, Measurements of the tropospheric and stratospheric SO2 distribution, J. Geophys. Res. 85, 7433–7438.
Harker, A. B., 1975, The formation of sulfate in the stratosphere through the gas phase oxidation of sulfur dioxide, J. Geophys. Res. 80, 3399–3401.
Harrison, H. and Larson, T., 1974, The oxidation of SO2 in the stratosphere, J. Geophys. Res. 79, 3095–3097.
Hofmann, D. J., Rosen, J. M., Kiernan, J. M., and Laby, J., 1976, Stratospheric aerosol measurements IV: Global time variations of the aerosol burden and source considerations, J. Atmos. Sci. 33, 1782–1788.
Inn, E. C. Y. and Vedder, J. F., 1981, Measurements of stratospheric sulfur constituents, Geophys. Res. Lett. 8, 5–8.
Iyer, R. S. and Rowland, F. S., 1980, A significant upper limit for the rate of formation of OCS from the reaction of OH with CS2, Geophys. Res. Lett. 7, 797–800.
Jaeschke, W., 1978, New methods for the analysis of SO2 and H2S in remote areas and their application to the atmosphere, Atmos. Environ. 12, 715–721.
Jaeschke, W., Georgii, H.-W., and Schmitt, R., 1976, Preliminary results of stratospheric SO2 measurements, Geophys. Res. Lett. 3, 517–519.
Junge, C. E., Chagnon, C. W., and Manson, J. E., 1961, Stratospheric aerosols, J. Meteorol. 18, 81–108.
Junge, C. E., 1966, The formation of the stratospheric aerosol layer, Tellus, 18, 685.
Junge, C. E., 1974, Sulfur budget of the stratospheric aerosol layer, Proc. of the IAMAP Conf. on Structure, Composition and General Circulation of the Upper and Lower Atmospheres, Vol. 1, Melbourne, January 1974, pp. 85–97.
Kurylo, M. J., 1978, Flash photolysis resonance fluorescence investigation of the reactions of OH radicals with OCS and CS2, Chem. Phys. Lett. 58, 238–242.
Lazrus, A. L. and Gandrud, B. W., 1974, Stratospheric sulfate aerosol, J. Geophys. Res. 79, 3424–3431.
Meixner, F. X., 1981, PhD dissertation, J. W. Goethe University, Frankfurt am Main, FRG.
Meixner, F. X., and Jaeschke, W. A., 1981, The detection of low atmospheric SO2 concentrations with a chemiluminescence technique, Int. J. Environ. Anal. Chem. 10, 51–67.
Meixner, F. X., Geogii, H.-W., Ockelmann, G., Jäger, H., and Reiter, R., 1981, The arrival of the Mount St Helens eruption cloud over Europe, Geophys. Res. Lett. 8, 163–166.
Meixner, F. X., 1983, A case study of stratospheric sulphur dioxide influx into the troposphere, CACGP-Conference on Tropospheric Chemistry, 28 August–2 September 1983, Oxford, England.
Moortgart, G. J., and Junge, C., 1977, The role of SO2 oxidation for the background stratospheric sulfate layer in the light of new reaction data, Pageoph 115, 769–774.
NASA, 1981, Chemical kinetic and photochemical data for use in stratospheric modelling evaluation, No. 4, NASA panel for data evaluation, Jan. 15, 1981, NASA Jet Prop. Lab., Calif. Inst. Technology, Pasadena, CA, USA.
Peyton, T. O., Steele, R. V., and Mabey, W. R., 1976, Carbon disulfide, carbonyl sulfide: Literature review and environmental assessment, Stanfort Research Institute Report 68-01-2940, 57 pp.
Ravinshankra, A. R., Kreutter, N. M., Shah, R. C., and Wine, P. H., 1980, Rate of reaction of OH with COS, Geophys. Res. Lett. 7, 861–864.
Reiter, E. R., 1972, Atmospheric transport processes, part 3: Hydrodynamic tracers, U.S. Atomic Energy Commission, Office of Information Services, TID-25731, National Technical Information Service, U.S. Department of Commerce, Springfield, VA, USA.
Reiter, E., 1975, Stratospheric-tropospheric exchange processes, Rev. Geophys. Space Phys. 13, 459–474.
Shapiro, M. A., Reiter, E. R., Cadle, R. D., and Sedlacek, W. A., 1980, Vertical mass- and trace constituent transports in the vicinity of jet streams, Arch. Meteorol. Geophys. Biokl., Ser. B., 28, 193–206.
Specker, H. and Kaiser, H., 1956, Bewertung und Vergleich von Analysenverfahren, Fres. Z. Anal. Chem. 149, 46–66.
Stauff, J. and Jaeschke, W., 1975, A chemiluminescence technique for measuring atmospheric trace concentrations of SO2, Atmos. Environ. 9, 1038–1039.
Torres, A. L., Maroulis, P. J., and Bandy, A. R., 1980, Atmospheric OCS measurements on Project GAMETAG, J. Geophys. Res. 85, 7357–7360.
Turco, R. P., Whitten, R. C., Toon, O. B., Inn, E. C. Y., and Hamill, P., 1981, Stratospheric hydroxyl radical concentrations: New limitations suggested by observations of gaseous and particulate sulfur, J. Geophys. Res. 86, 1129–1139.
Turco, R. P., Whitten, R. C., and Toon, O. B., 1982, Stratospheric aerosols: Observation and theory, Rev. Geophys. Space Phys. 20, 233–279.
U.S. Standard Atmosphere 1976: NOAA-S/T 76–1562, U.S. Government Printing Office, Washington, D.C. 20402, USA.
Whitten, R. C., Toon, O. B., and Turco, R. P., 1980, The stratospheric sulfate aerosol layer: Processes, models, observations, and simulations, Pageoph 118, 87–127.
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Meixner, F.X. The vertical sulfur dioxide distribution at the tropopause level. J Atmos Chem 2, 175–189 (1984). https://doi.org/10.1007/BF00114130
Received:
Revised:
Issue Date:
DOI: https://doi.org/10.1007/BF00114130