Journal of Atmospheric Chemistry

, Volume 32, Issue 1, pp 147–164 | Cite as

Ground Based FTIR Measurements of Stratospheric Species from Harestua, Norway During Sesame and Comparison with Models

  • B. Galle
  • J. Mellqvist
  • D.W. Arlander
  • I. Fløisand
  • M.P. Chipperfield
  • A.M. Lee


Vertical columns of HF, HCl, HNO3, ClONO2, N2O, ClO and COF2 were measured at Harestua, Norway (60.22° N, 10.75° E, Elevation 600 a.s.l.) beginning on 24′ November 1994 and concluding on 1′ May 1995 during Phase-III of the SESAME (Second European Stratospheric Arctic and Mid-latitude Experiment) measurement campaign. The vertical columns of HCl, HNO3 and ClONO2 measured on 81 days were compared with columns calculated by the 3-D Cambridge model SLIMCAT. In addition the results were also interpreted by comparison with a photochemical trajectory model. Good agreement was seen for HCl while the nitrogen compounds showed larger discrepancies, especially for ClONO2. Evidence for chlorine activation was seen with 65% reduction of the chlorine reservoirs (HCl + ClONO2) while the levels of ClO were greatly enhanced. Interpretation of the loss with the trajectory model indicated condensation of chlorine on PSCs. The vertical column ratio of COF2 and HF was measured to 0.21 outside the vortex and a factor of two lower inside. The recovery of ClONO2 was seen to be much faster than that of HCl in the early spring.

SESAME polar vortex arctic stratosphere ground based FTIR hydrogen fluoride hydrogen chloride nitric acid chlorine nitrate nitrous oxide chlorine monoxide carbonyl fluoride 3D-Model photochemical trajectory model 


Unable to display preview. Download preview PDF.

Unable to display preview. Download preview PDF.


  1. Adrian G.P., et al., 1994. First results of groundbased FTIR measurements of atmospheric trace gases in north Sweden and Greenland during EASOE; Geophys. Res. Lett., 21, 1343–1346.Google Scholar
  2. Ballard J., Johnston, W.B., and M.R. Gunson, M.R., 1988, Absolute absorption coefficients of CIONO2 infrared bands at stratospheric temperature, J. Geophys. Res., 93, 1659–1665.Google Scholar
  3. Bell W., N.A. Martin, T.A. Gardiner, N.R. Swann, P.T. Woods, P.F. Fogal and J.W. Waters, 1994, Column measurements of stratospheric trace species over Åre, Sweden, in the winter of 1991–1992, Geophys. Res. Lett. vol 21, 1347–1350.Google Scholar
  4. Bell W., C. Paton-Walsh, T.D. Gardiner, P.T. Woods, L. Donohoe, A. Gould, D. Secker, S. Naughten, N.R. Swann, N.A. Martin and L.E. Page, 1997, Groundbased FTIR measurements of stratospheric trace species from Aberdeen during winter and spring 1993/94 and 1994/95 and comparison with a 3D model, submitted to JAC.Google Scholar
  5. Chipperfield M.P., M.L. Santee, L. Froidevaux, G.L. Manney, W.G. Read, J.W. Waters, A.E. Roche and J.M. Russell, 1996, Analysis of UARS data in the southern polar vortex in September 1992 using a chemical transport model, J. Geophys. Res., 101, 18861–18881.Google Scholar
  6. Chipperfield M.P., Burton, M., Bell, W., Paton Walsh, C., Blumenstock, T., Coffey, M.T., Hannigan, J.W., Mankin, W.G., Galle, B., Mellqvist, J., Mahieu, E., Zander, R., Notholt, J., Sen, B., and Toon, G.C., 1997, On the use of HF as a reference for stratespheric observations, JGR 102,D11, 12,901–12,919Google Scholar
  7. Ennis C. A. et al., 1994, Scientific assessment of ozone depletion: 1994, WMO Global ozone research and monitoring project report No. 37.Google Scholar
  8. Fløisand, I., Stordal, F., Rognerud, B., Isaksen, I.S.A., Larsen, N., and Knudsen, B.M., 1996, Modelled Chemical Ozone Change over Europe during the winters 1992 to 1995, 1997, Proceedings of the Quadrennial Ozone Symposium, l'Aquila, September 1996.Google Scholar
  9. Galle, B., Mellqvist, J., Arlander, D.W., and Karisen, K., 1995, Ground based high resolution FTIR measurements of stratospheric molecules at Harestua Norway, Proceedings of the Third Annual Symposium on Polar Stratospheric Ozone, Schliersee, Bavaria, September 1995.Google Scholar
  10. Griffith, D.W.T., 1996, Synthetic calibration and quantitative analysis of gas-phase FTIR spectra, Appl. Spectros., 50, 59–70.Google Scholar
  11. Gunson, M.R., et al., 1996, The Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment deployment on the ATLAS-3 Space Shuttle Mission, Geophys. Res. Lett., 23,17, 2333–2336.Google Scholar
  12. De Haan, D.O., Fløisand, I., and Stordal, F., 1997. Modelling studies of the effects of the heterogeneous reaction ClOOCl + HCl − > Cl2 + HOOCl on stratospheric chlorine activation and ozone depletion, Journal of Geophys. Res., 102, 1251–1258.Google Scholar
  13. Hanson, D.R, and Ravishankara, A.R., 1991, The loss of CF2O on ice, NAT, and sulfuric acid solutions, Geophys. res. Lett., 18, 1699–1701.Google Scholar
  14. Holton, J.R., Haynes. P.H., McIntyre, M.E., Douglass, A.N., Rood, R.B., and Pfister, L., 1995, Stratosphere-Troposphere Exchange, Rev. of Geophys., 33,4, 403–439.Google Scholar
  15. Kaye, J.A., Douglass, A.R., Jackman, C.H., Stolarski, R.S., Zander, R., and Roland, G., 1991, Two dimensional model calculations of fluorine containing reservoir species in the stratosphere, J. Geophys. Res., 96, 12865–12881.Google Scholar
  16. Kinnersley J.S., 1996, The climatology of the stratospheric THIN AIR model, Q. J. R. Meteorol. Soc., 122, 219–252.Google Scholar
  17. Koop, T., et al., 1995, Do stratospheric aerosol droplets freeze above the ice frost point?, Geophys. Res. Lett., 22,8, 917–920.Google Scholar
  18. Larsen, N., 1991, Polar Stratospheric Clouds: A Microphysical Simulation Model. Copenhagen, Danish Meteorological Institute (DMI Scientific Report 91–2).Google Scholar
  19. Larsen, N., 1994, The Impact of Freezing of Sulfate Aerosols on the Formation of Polar Stratospheric Clouds, Geophys. Res. Lett. 21, 425–428.Google Scholar
  20. Luo, M., et al., 1994, Observations of stratospheric hydrogen fluoride by halogen occultation experiment (HALOE), J. Geophys. Res., 99,D8, 16,691–16,705.Google Scholar
  21. MacKenzie, AR., 1995, On the theories of type 1 polar stratospheric cloud formation, J. Geophys. Res., 100,D6, 11,275–11,288.Google Scholar
  22. Notholt J., O. Schrems, 1994, Ground based FTIR measurements of vertical column densities of several trace gases above Spitsbergen, Geophys. Res. Lett., 21, 1355–1358.Google Scholar
  23. Paton-Walsh, C., Bell, W., Gardiner, T., Swann, N., Woods, P., Notholt, J., Schutt, H., Galle, B., Arlander, W., and Mellqvist, J., 1997. An uncertainty budget for ground-based FTIR column measurements of HCl, HF, N2O and HNO3 deduced from results of side-by-side instrument intercomparisons. J. Geophys. Res., 102,D7, 8867–8873.Google Scholar
  24. Reisinger, A.R., Jones, N.B., Matthews, W.A., and Rinsland, C.P., 1994, Southern hemisphere ground based measurements of Carbonyl Fluoride (COF2) and Hydrogen Fluoride (HF): Partitioning between Fluoride reservoir species, Geophys. Res. Lett., 21,9, 797–800.Google Scholar
  25. Rothman, L., et. al., 1992, The HITRAN molecular database: Edition of 1991 and 1992, J. Quant. Spectrosc. Radiat. Transfer., 48, 469–479.Google Scholar
  26. Stolarski, R.S., and Rundel, R.D., 1978, Fluorine photochemistry in the stratosphere, J. Geophys. Res., 5, 781–783.Google Scholar
  27. Stordal, F., Isaksen, I.S.A. and Horntvedt, K., 1985. A Diabatic Circulation Two-Dimensional Model With Photochemistry: Simulations of Ozone and Long-Lived Tracers With Surface Sources., J. Geophys. Res., 90, 5757–5776.Google Scholar
  28. Toon, G.C., Farmer, C.B., Loves, L.L., Schaper, P.W., Blavier, J.-F., and Norton R.H., 1989, Infrared aircraft measurements of stratospheric composition over Antarctica during September 1987. J. Geophys. Res., 94,D14, 16571–16596.Google Scholar
  29. Toon, G.C., Blavier, J.T., and Szeto, J.T., 1994, Latitude variations of stratospheric gases, Geophys. Res. Lett., 21,23, 2599–2602Google Scholar
  30. Van Roozendael, M., Hermans, C., Kabbadj, Y., Lambert, J.-C., Vandaele, A.-C., Simon, P.C., Carleer, M., Guilmot, J.-M., and Colin, R., 1995, Ground-based measurements of stratospheric OClO, NO2 and O3 at Harestua, Norway (60°N, 10°E) during SESAME, Proceedings 12th ESA Symposium on Rocket and Balloon Programmes and Related Research, Lillehammer, Norway, June 1995, ESA SP-370 (September 1995).Google Scholar
  31. Webster, C.R., May, R.D., Toohey, D.W., Avallone, L.M., Anderson, J.G., Newman, P.A., Lait, L.R., 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
  32. World Meteorological Organisation, 1994, Scientific Assessment of Ozone Depletion, World Meteorolog. Organiz. Global Ozone Res. and Monit. Proj., Rep. 37, Geneva, 1994Google Scholar
  33. Wofsy, S.C., Yatteau, J.H., Salawitch, R.J., McElroy, M.B., Toon, G.C., Mankin, W.G., and Coffey, M.T., 1990, Heterogeneous conversion, of COF2 to HF in polar stratospheric clouds, Geophys. Res. Lett., 17,9, 461–464.Google Scholar
  34. R. Zander, Gunson, M.R., Farmer, C.B., Rinsland, C.P., Irion, F.W., and Mahieu, E., 1992, “The 1985 chlorine and fluorine inventories in the stratosphere based on ATMOS observations at 30 North latitude”, J. Atm. Chem., 15, 171–186.Google Scholar
  35. Zander, R., Mahieu, E., Meilen, F., Demoulin, P., Roland, G., Delbouille, L., and Servais, C., 1995, Stratospheric changes monitored above the Jungfraujoch — The budgets of inorganic chlorine and fluorine since 1995, Proceedings of the Third Annual Symposium on Polar Stratospheric Ozone, Schliersee, Bavaria, September 1995.Google Scholar

Copyright information

© Kluwer Academic Publishers 1999

Authors and Affiliations

  • B. Galle
    • 1
  • J. Mellqvist
    • 1
    • 2
  • D.W. Arlander
    • 3
  • I. Fløisand
    • 3
  • M.P. Chipperfield
    • 4
  • A.M. Lee
    • 4
  1. 1.Swedish Environmental Research Institute (IVL)GöteborgSweden
  2. 2.Department of PhysicsChalmers University of Technology and University of GöteborgGöteborgSweden
  3. 3.Norwegian Institute for Air ResearchKjellerNorway
  4. 4.Department of ChemistryUniversity of CambridgeCambridgeUnited Kingdom

Personalised recommendations