References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-397-2010

More evidence for very short-lived substance contribution to stratospheric chlorine inferred from HCl balloon-borne in situ measurements in the tropics

Mébarki

¹ Catoire

¹ Huret

¹ Berthet

¹ Robert

¹ Poulet

Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), UMR 6115 CNRS–Université d'Orléans, 45071 Orléans cedex 2, France

18 01 2010

10 2 397 409

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/10/397/2010/acp-10-397-2010.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/397/2010/acp-10-397-2010.pdf

Volume mixing ratio (vmr) vertical profiles of hydrogen chloride (HCl) are retrieved from in situ measurements performed by a balloon-borne infrared tunable diode laser absorption spectrometer (SPIRALE) during two balloon flights in the tropics (Teresina, Brazil, 5.1° S–42.9° W) in June 2005 and June 2008. HCl vertical profiles obtained from 15 to 31 km are presented and analysed to estimate the contribution of very short-lived substances (VSLS) to total stratospheric chlorine. Both retrieved vertical profiles of HCl from these flights agree very well with each other, with estimated overall uncertainties of 6% on vmr between 23 and 31 km. Upper limits of HCl vmr as low as 20 pptv in June 2008 and 30 pptv in June 2005 are inferred in the upper part of the tropical tropopause layer (TTL). Backward trajectory calculations and such low amounts suggest that the air masses sampled correspond to typical background conditions, i.e. neither influenced by recent tropospheric nor stratospheric air. Taking into account the recently reported VSL source gas measurements obtained in similar conditions (Laube et al., 2008) and the main intermediate degradation product gas COCl2 (Fu et al., 2007), a total VSLS contribution of 85±40 pptv to stratospheric chlorine is inferred. This refines the WMO (2007) estimation of 50 to 100 pptv, which was not taking into account any HCl contribution. In addition, comparisons of HCl measurements between SPIRALE and the Aura MLS satellite instrument in the tropical lower and middle stratosphere lead to a very good agreement. The previous agreement between MLS-deduced upper stratospheric total chlorine content and modelled values including 100 pptv of VSLS (Froidevaux et al., 2006) is thus supported by our present result about the VSLS contribution.

References 1

Bernath, P. F., McElroy, C. T., Abrams, M. C., Boone, C. D., Butler, M., Camy-Peyret, C., Carleer, M., Clerbaux, C., Coheur, P.-F., Colin, R., DeCola, P., DeMazière, M., Drummond, J. R., Dufour, D.,~Evans, W. F. J., Fast, H., Fussen, D., Gilbert, K., Jennings, D. E., Llewellyn, E. J., Lowe, R. P., Mahieu, E., McConnell, J. C., McHugh, M., McLeod, S. D., Michaud, R., Midwinter, C., Nassar, R., Nichitiu, F., Nowlan, C., Rinsland, C. P., Rochon, Y. J., Rowlands, N., Semeniuk, K., Simon, P., Skelton, R., Sloan, J. J., Soucy, M.-A., Strong, K., Tremblay, P., Turnbull, D., Walker, K. A., Walkty, I., Wardle, D. A., Wehrle, V., Zander, R., and Zou, J.: Atmospheric Chemistry Experiment (ACE): Mission overview, Geophys. Res. Lett., 32, L15S01, doi:10.1029/2005GL022386, 2005.

Berthet, G., Huret, N., Lef�vre, F., Moreau, G., Robert, C., Chartier, M., Catoire, V., Barret, B., Pisso, I., and Pomathiod, L.: On the ability of chemical transport models to simulate the vertical structure of the N2O, NO2 and HNO3 species in the mid-latitude stratosphere, Atmos. Chem. Phys., 6, 1599–1609, 2006.

Berthet, G., Renard, J.-B., Catoire, V. Chartier, M. Robert, C., Huret, N., Coquelet, F., Bourgeois, Q., Rivière, E. D., Barret, B., Lefèvre, F., and Hauchecorne, A.: Remote sensing measurements in the polar vortex: comparison to in situ observations and implications for the simultaneous retrievals and analysis of the NO2 and OClO species, J. Geophys. Res., 112, D21310, doi:10.1029/2007JD008699, 2007a.

Berthet, G., Esler, J. G., and Haynes, P. H.: A Lagrangian perspective of the tropopause and the ventilation of the lowermost stratosphere, J. Geophys. Res., 112, D18102, doi:10.1029/2006JD008295, 2007b.

Cooper, D. E. and Warren, R. E.: Two-tones optical heterodyne spectroscopy with diode lasers: Theory of line shapes and experimental results, J. Opt. Soc. Am. B, 4, 470–480, 1987.

Chen, Y., Shi, C., and Zheng, B.: HCl Quasi-Biennal Oscillation in the stratosphere and a comparison with ozone QBO, Adv. Atmos. Sci., 22(5), 751–758, 2005.

Edmonds, M., Pyle, D., and Oppenheimer, C.: HCl emissions at Soufrière Hills Volcano, Montserrat, West Indies, during a second phase of dome building: November 1999 to October 2000, B. Volcanol., 64, 21–30, 2002.

Engel, A., Möbius, T., Haase, H.-P., Bönisch, H., Wetter, T., Schmidt, U., Levin, I., Reddmann, T., Oelhaf, H., Wetzel, G., Grunow, K., Huret, N., and Pirre, M.: Observation of mesospheric air inside the arctic stratospheric polar vortex in early 2003, Atmos. Chem. Phys., 6, 267–282, 2006.

Folkins, I., Loewenstein, M., Podolske, J., Oltmans, S. J., and Proffitt, M.: A barrier to vertical mixing at 14 km in the tropics: Evidence from ozonesondes and aircraft measurements, J. Geophys. Res., 104(D18), 22095–22102, 1999.

Froidevaux, L., Livesey, N. J., Read, W. G., Salawitch, R. J., Waters, J. W., Drouin, B., MacKenzie, I. A., Pumphrey, H. C., Bernath, P., Boone, C., Nassar, R., Montzka, S., Elkins, J., Cunnold, D., and Waugh, D.: Temporal decrease in atmospheric chlorine, Geophys. Res. Lett., 22, L23812, doi:10.1029/2006GL027600, 2006.

Froidevaux, L., Jiang, Y. B, Lambert, A., Livesey, N. J., Read, W. G., Waters, J. W., Fuller, R. A., Marcy, T. P., Popp, P. J., Gao, R. S., Fahey, D. W., Jucks, K. W., Stachnik, R. A., Toon, G. C., Christensen, L. E., Webster, C. R., Bernath, P. F., Boone, C. D., Walker, K. A., Pumphrey, H. C., Harwood, R. S., 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., Synder, W. V., Stek, P. C., Thurstans, R. P., and Wagner, P. A.: Validation of Aura Microwave Limb Sounder HCl measurements, J. Geophys. Res., 113, D15S25, doi:10.1029/2007JD009025, 2008.

Fu, D., Boone, C. D., Bernath, P. F., Walker, K. A., Nassar, R., Manney, G. L., and McLeod, S. D.: Global phosgene observations from the Atmospheric Chemistry Experiment (ACE) mission, Geophys. Res. Lett., 34, L17815, doi:10.1029/2007GL029942, 2007.

Fueglistaler, S., Dessler, A. E., Dunkerton, T. J., Folkins, I., Fu, Q., and Mote, P. W.: Tropical Tropopause Layer, Rev. Geophys., 47, RG1004, doi:10.1029/2008RG000267, 2008.

Gettelman, A., Forster, P. M., de Fujiwara, M., Fu, Q., Vomel, H., Gohar, L. K., Johanson, C., and Ammerman, M.: Radiation balance of the tropical tropopause layer, J. Geophys. Res., 109, D07103, doi:10.1029/2003JD004190, 2004.

Grossel, A., Huret, N., Catoire, V., Berthet, G., Renard, J.-B., Robert, C., and Gaubicher, B.: In situ balloon-borne measurements of HNO3 and HCl stratospheric vertical profiles influenced by PSC formation during winter 2006, J. Geophys. Res., in revision, 2010.

Hauchecorne, A., Godin, S., Marchand, M., Heese, B., and Souprayen, C.: Quantification of the Transport of Chemical Constituents from the Polar Vortex to Middle Latitudes in the Lower Stratosphere using the High-Resolution Advection Model MIMOSA and Effective Diffusivity, J. Geophys. Res., 107, 8289–8302, 2002.

Huret, N., Pirre, M., Hauchecorne, A., Robert, C., and Catoire, V.: On the vertical structure of the stratosphere at midlatitudes during the first stage of the polar vortex formation and in the polar region in the presence of a large mesospheric descent, J. Geophys. Res., 111, D06111, doi:10.1029/2005JD006102, 2006.

Kim, S., Huey, L. G., Stickel, R. E., Pierce, R. B., Chen, G., Avery, M. A., Dibb, J. E., Diskin, G. S., Sachse, G. W., McNaughton, C. S., Clarke, A. D., Anderson, B. E., and Blake, D. R.: Airborne measurements of HCl from the marine boundary layer to the lower stratosphere over the North Pacific Ocean during INTEX-B, Atmos. Chem. Phys. Discuss., 8, 3563–3595, 2008.

Laube, J. C., Engel, A., Bönisch, H., Möbius, T., Worton, D. R., Sturges, W. T., Grunow, K., and Schmidt, U.: Contribution of very short-lived organic substances to stratospheric chlorine and bromine in the tropics – a case study, Atmos. Chem. Phys., 8, 7325–7334, 2008.

Livesey, N. J., Read, Lambert, A., Cofield, R. E., Cuddy, D. T., Froidevaux, L., Fuller, R. A., Jarnot, R. F., Jiang, J. H., Jiang, Y. B., Knosp, B. W., Kovalenko, L. J., Pickett, H. M., Pumphrey, H. C., Santee, M. L., Schwartz, M. J., Stek, P. C., Wagner, P. A., Waters, J. W., and Wu, D. L.: Version 2.2 level 2 data quality and description document, Tech. Rep. JPL D-33509, Jet Propul. Lab., Pasadena, Calif., 2007.

McHugh, M., Magill, B., Walker, K. A., Boone, C. D., Bernath, P. F., and Russell III, J. M.: Comparison of atmospheric retrievals from ACE and HALOE, Geophys. Res. Lett., 32, L15S10, doi:10.1029/2005GL022403, 2005.

Mahieu, E., Duchatelet, P., Demoulin, P., Walker, K. A., Dupuy, E., Froidevaux, L., Randall, C., Catoire, V., Strong, K., Boone, C. D., Bernath, P. F., Blavier, J.-F., Blumenstock, T., Coffey, M., De Mazière, M., Griffith, D., Hannigan, J., Hase, F., Jones, N., Jucks, K. W., Kagawa, A., Kasai, Y., Mebarki, Y., Mikuteit, S., Nassar, R., Notholt, J., Rinsland, C. P., Robert, C., Schrems, O., Senten, C., Smale, D., Taylor, J., Tétard, C., Toon, G. C., Warneke, T., Wood, S. W., Zander, R., and Servais, C.: Validation of ACE-FTS v2.2 measurements of HCl, HF, CCl3F and CCl2F2 using space-, balloon- and ground-based instrument observations, Atmos. Chem. Phys., 8, 6199–6221, 2008.

Marcy, T. P., Fahey, D. W., Gao, R. S., Popp, P. J., Richard, E. C., Thompson, T. L., Rosenlof, K. H., Ray, E. A., Salawitch, R. J., Atherton, C. S., Bergmann, D. J., Ridley, B. A., Weinheimer, A. J., Loewenstein, M., Weinstock, E. M., and Mahoney, M. J.: Quantifying stratospheric ozone in the upper troposphere with in situ measurements of HCl, Science, 304, 261–265, 2004.

Marcy, T. P., Popp, P. J., Gao, R. S., Fahey, D. W., Ray, E. A., Richard, E. C., Thompson, T. L., Atlas, E. L., Loewenstein, M., Wofsy, S. C., Park, S., Weinstock, E. M., Swartz, W. H., and Mahoney, M. J.: Measurements of trace gases in the tropical tropopause layer, Atmos. Environ., 41, 7253–7261, 2007.

Michelsen, H., Salawitch, R. J., Gunson, M. R., Aellig, C., Kämpfer, N., Abbas, M. M., Brown, T. L., Chang, A. Y., Goldman, A., Irion, F. W., Newchurch, M. J., Rinsland, C. P., Stiller, G. P., and Zander, R.: Stratospheric chlorine partitioning: Constraints from shuttle-borne measurements of [HCl], [ClNO3], and [ClO], Geophys. Res. Lett., 23, 2361–2364, 1996.

Moreau, G., Robert, C., Catoire, V., Chartier, M., Camy-Peyret, C., Huret, N., Pirre, M., Pomathiod, L., and Chalumeau, G.: SPIRALE: A multispecies in situ balloon-borne experiment with six tunable diode laser spectrometers, Appl. Opt., 44(28), 5972–5989, 2005.

Müller, R., Tilmes, S., Grooß, J.-U., Engel, A., Oelhalf, H., Wetzel, G., Huret, N., Pirre, M., Catoire, V., Toon, G, and Nakajima, H.: Impact of mesospheric intrusions on ozone-tracer relations in the stratospheric polar vortex, J. Geophys. Res., 112, D23307, doi:10.1029/2006JD008315, 2007.

Nassar, R., Bernath, P. F., Boone, C. D., Clerbaux, C., Coheur, P. F., Dufour, G., Froidevaux, L., Mahieu, L., McConell, J. C., McLeod, S. D., Murtagh, D. P., Rinsland, C. P., Semeniuk, K., Skelton, R., Walker, K. A., and Zander, R.: A global inventory of stratospheric chlorine in 2004, J. Geophys. Res., 111, D22312, doi:10.1029/2006JD007073, 2006.

Pickett, H. M., Poynter, R. L., Cohen, E. A., Delitsky, M. L., Pearson, J. C., and Muller, H. S. P.: Submillimeter, millimeter, and microwave spectral line catalog, J. Quant. Spectrosc. Ra., 60, 883–890, 1998.

Pirre, M., Pisso, I., Marécal, V., Catoire, V., Mébarki, Y., and Robert, C.: Intrusion of recent air in midlatitude stratosphere revealed by in situ tracer measurements and trajectory calculations, J. Geophys. Res., 113, D11302, doi:10.1029/2007JD009188, 2008.

Renard, J.-B., Berthet, G., Brogniez, C., Catoire, V., Fussen, D., Goutail, F., Oelhaf, H., Pommereau, J.-P., Roscoe, H. K., Wetzel, G., Chartier, M., Robert, C., Balois, J.-Y., Verwaerde, C., Auriol, F., François, P., Gaubicher, B., and Wursteisen, P.: Validation of GOMOS-Envisat vertical profiles of O3, NO2, NO3, and aerosol extinction using balloon-borne instruments and analysis of the retrievals, J. Geophys. Res., 113, A02302, doi:10.1029/2007JA012345, 2008.

Rothman, L. S., Jacquemart, D., Barbe, A., Benner, D. C., Birk, M., Brown Jr., L. R., Chackerian, C., Chance, K., Coudert, L. H., Carleer, M. R., Dana, V., Devi, V. M., Flaud, J.-M., Gamache, R. R., Goldman, A., Hartmann, J.-M., Jucks, K. W., Maki, A. G., Mandin, J. Y., Massie, S. T., Orphal, J., Perrin, A., Rinsland, C. P., Smith, M. A. H., Tennyson, J., Tolchenov, R. N., Toth, R. A., Vander Auwera, J., Varanasi, P., and Wagner, G.: The HITRAN 2004 Molecular Spectroscopic Database, J. Quant. Spectrosc. Ra., 96, 139–204, doi:10.1016/j.jqsrt.2004.10.008, 2005.

Russell III, J. M., Gordley, L. L., Park, J. H., Drayson, S. R., Hesketh, W. D., Cicerone, R. J., Tuck, A. F., Frederick, J. E., Harries, J. E., and Crutzen, P. J.: The Halogen Occultation Experiment, J. Geophys. Res., 98(D6), 10777–10797, doi:10.1029/93JD00799, 1993.

Russell III, J. M., Deaver, L. E., Luo, M., Park, J. H., Gordley, L. L., Tuck, A. F., Toon, G. C., Gunson, M. R., Traub, W. A., Johnson, D. G., Jucks, K. W., Murcray, D. G., Zander, R., Nolt, I., and Webster, C. R.: Validation of Hydrogen Chloride Measurements made by HALOE from the UARS Platform, J. Geophys. Res., 101(D6), 10151–10162, 1996.

Stohl, A., Wotawa, G., Seibert, P., and Kromp-Kolb, H.: Interpolation errors in wind fields as a function of spatial and temporal resolution and their impact on different types of kinematic trajectories, J. Appl. Meteorol., 34, 2149–2165, 1995.

Toon, G. C., Blavier, J.-F., Sen, B., and Drouin, B. J.: Atmospheric COCl2 measured by solar occultation spectrometry, Geophys. Res. Lett., 28, 2835–3838, 2001.

Urban, J., Lautie, N., Flochmoen, E. L., Jimenez, C., Eriksson, P., de La Noe, J., Dupuy, E., Amraoui, L. E., Frisk, U., Jegou, F., Murtagh, D., Olberg, M., Ricaud, P., Camy-Peyret, C., Dufour, G., Payan, S., Huret, N., Pirre, M., Robinson, A. D., Harris, N. R. P., Bremer, H., Kleinbohl, A., Kullmann, K., Kunzi, K., Kuttippurath, J., Ejiri, M. K., Nakajima, H., Sasano, Y., Sugita, T., Yokota, T., Piccolo, C., Raspollini, P., and Ridolfi, M.: Odin/SMR limb observations of stratospheric trace gases: Validation of N2O, J. Geophys. Res., 110, D09301, doi:10.1029/2004JD005394, 2005a.

Wang, D. Y., Höpfner, M., Blom, C. E., Ward, W. E., Fischer, H., Blumenstock, T., Hase, F., Keim, C., Liu, G. Y., Mikuteit, S., Oelhaf, H., Wetzel, G., Cortesi, U., Mencaraglia, F., Bianchini, G., Redaelli, G., Pirre, M., Catoire, V., Huret, N., Vigouroux, C., De Mazière, M., Mahieu, E., Demoulin, P., Wood, S., Smale, D., Jones, N., Nakajima, H., Sugita, T., Urban, J., Murtagh, D., Boone, C. D., Bernath, P. F., Walker, K. A., Kuttippurath, J., Kleinböhl, A., Toon, G., and Piccolo, C.: Validation of MIPAS HNO3 operational data, Atmos. Chem. Phys., 7, 4905–4934, 2007.

Waters, J. W., Froidevaux, L., Harwood, R. S., Jarnot, R. F., Pickett, H. M., Read, W. G., Siegel, P. H., Cofield, R. E., Filipiak, M. J., Flower, D. A., Holden, J. R., Lau, G. K., Livesey, N. J., Manney, G. L., Pumphrey, H. C., Santee, M. L., Wu, D. L., Cuddy, D. T., Lay, R. R., Loo, M. S., Perun, V. S., Schwartz, M. J., Stek, P. C., Thurstans, R. P., Boyles, M. A., Chandra, K. M., Chavez, M. C., Chen, G.-S., Chudasama, B. V., Dodge, R., Fuller, R. A., Girard, M. A., Jiang, J. H., Jiang, Y., Knosp, B. W., LaBelle, R. C., Lam, J. C., Lee, K. A., Miller, D., Oswald, J. E., Patel, N. C., Pukala, D. M., Quintero, O., Scaff, D. M., Van Snyder, W., Tope, M. C., Wagner, P. A., and Walch, M. J.: The Earth Observing System Microwave Limb Sounder (EOS MLS) on the Aura satellite, IEEE T. Geosci. Remote, 44(5), 1075–1092, doi:10.1109/TGRS.2006.873771, 2006.

Waugh, D. and Polvani, L.: Climatology of Intrusions into the Tropical Upper Troposphere, Geophys. Res. Lett., 27(23), 3857–3860, 2000.

Wolff, M. A., Kerzenmacher, T., Strong, K., Walker, K. A., Toohey, M., Dupuy, E., Bernath, P. F., Boone, C. D., Brohede, S., Catoire, V., von Clarmann, T., Coffey, M., Daffer, W. H., De Mazière, M., Duchatelet, P., Glatthor, N., Griffith, D. W. T., Hannigan, J., Hase, F., Höpfner, M., Huret, N., Jones, N., Jucks, K., Kagawa, A., Kasai, Y., Kramer, I., Küllmann, H., Kuttippurath, J., Mahieu, E., Manney, G., McElroy, C. T., McLinden, C., M�barki, Y., Mikuteit, S., Murtagh, D., Piccolo, C., Raspollini, P., Ridolfi, M., Ruhnke, R., Santee, M., Senten, C., Smale, D., Tétard, C., Urban, J., and Wood, S.: Validation of HNO$_3,$ ClONO2, and N2O$_5$ from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), A tmos. Chem. Phys., 8, 3529–3562, 2008.

WMO (World Meteorological Organization), United Nations Environment Programme, Scientific Assessment of Ozone Depletion: 2006, Global Ozone Research and Monitoring Project, Report No 50, Geneva , Switzerland, 2007.