Abstract
Laboratory and field measurements have been performed in order to improve our understanding of the HCl air-snow transfer function. The solubility and diffusion of HCl in laboratory grown single crystals of ice have been measured as a function of HCl partial pressure,P HCl, between −8 and −25 °C. Measurements ofP HCl and of the mole fraction of HCl in snow,X'HCl, have been measured at Summit, Greenland. Comparison of the field and laboratory measurements show that theX'HCl values are well below equilibrium values. The major processes involved in the formation of snow crystals and in their evolution after deposition are discussed in order to attempt to understand theX'HCl values and their variations. The discussion is focussed on a few well identified snow layers. It is concluded that sublimation and recrystallization of snow probably play a major role in the evolution ofX'HCl, but that our understanding of the HCl transfer function is very incomplete. Laboratory and field measurements are suggested to improve this situation.
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References
Adamson, A. W. and Dormant, L. M., 1966, Adsorption of nitrogen on ice at 78 K,J. Amer. Chem. Soc. 88, 2055–2057.
Bergin, M. H., Jaffrezo, J. L., Davidson, C. L., Caldow, R., and Dibb, J., 1994, Fluxes of chemical species to the Greenland ice sheet at summit by fog and dry deposition,Geochim. Cosmochim. Acta 58, 3207–3215.
Borys, R. D., Del Vecchio, D., Jaffrezo, J. L., Dibb, J. E., and Mitchell, D. L., 1992, Field observation, measurements and preliminary results from a study of wet deposition processes influencing snow and ice chemistry at summit, Greenland, in S. E. Schwartz and W. G. N. Slinn (eds.),Precipitation Scavenging and Atmosphere-Surface Exchanges, Hemisphere Publ. Corp., Washington DC, pp. 1705–1718.
Buat-Ménard, P., Morelli, J., and Chesselet, R., 1974, Water-soluble elements in atmospheric particulate matter over tropical and equatorial Atlantic,J. Rech. Atmos. 8, 661–673.
Chappellaz, J., Barnola, J.-M., Raynaud, D., Korotkevich, Y. S., and Lorius, C., 1990, Ice-core record of atmospheric methane over the past 160,000 years,Nature 345, 127–131.
Chen, J.-P. and Crutzen, P. J., 1994, Solute effect on the evaporation of ice particles,J. Geophys. Res. 99, 18847–18859.
Chu, L. T., Leu, M. T., and Keyser, L. F., 1993, Uptake of HCl in water ice and nitric acid films,J. Phys. Chem. 97, 7779–7785.
Colbeck, S. C., 1989, Snow crystal growth with varying surface temperatures and radiation penetration,J. Glaciol. 35, 23–29.
Conklin, M. H. and Bales, R. C., 1993, SO2 uptake on ice spheres: liquid nature of the ice-air interface,J. Geophys. Res. 98, 16851–16855.
De Angelis, M. and Legrand, M., 1995, Preliminary investigations of post depositional effects on HCl, HNO3, and organic acids in polar firn layers, in R. J. Delmas (ed.), NATO ARWIce Core Chemistry of Global Biogeochemical Cycles, Springer-Verlag, Berlin, pp. 369–390.
Delzeit, L. A., Rowland, B., and Devlin, J. P., 1993, Infrared spectra of HCl complexed/ionized in amorphous hydrates and at ice surfaces in the 15–90 K range,J. Phys. Chem. 97, 10312–10318.
Dibb, J. E., Jaffrezo, J.-L., and Legrand, M., 1992, Initial findings of recent investigations of air-snow relationships in the summit region of the Greenland ice sheet,J. Atmos. Chem. 14, 167–180.
Dominé, F., Thibert, E., Van Landeghem, F., Silvente, E., and Wagnon, P., 1994, Diffusion and solubility of HCl in ice: preliminary results,Geophys. Res. Lett. 21, 601–604.
Fisher, J. C., 1951, Calculation of diffusion penetration curves for surface and grain boundary diffusion,J. Appl. Phys. 22, 74, 1951.
Fitzgerald, J. W., 1991, Marine aerosols: a review,Atmos. Environ. 25A, 533–545.
Fritz, J. J. and Fuget, C. R., 1956, Vapor pressure of aqueous hydrogen chloride solutions, 0° to 50 °C,Indust. Eng. Chem. 1, 10–12.
Hanson, D. and Mauersberger, K., 1988, Solubility and equilibrium vapor pressure of HCl dissolved in polar stratospheric cloud materials: ice and the trihydrate of nitric acid,Geophys. Res. Lett. 15, 1507–1510.
Haynes, D. R., Tro, N. J., and George, S. M., 1992, Condensation and evaporation of H2O on ice surfaces,J. Phys. Chem. 96, 8502–8509.
Hobbs, P. V., 1974,Ice Physics, Clarendon Press, Oxford.
Horn, A. B., Chesters, M. A., McCoustra, M. R. S., and Sodeau, J. R., Adsorption of stratospherically important molecules on thin D2O ice films using reflection absorption infrared spectroscopy,J. Chem. Soc. Faraday. Trans. 88, 1077–1078.
Iribarne, J. V. and Pyshnov, T., 1990, The effect of freezing on the composition of supercooled droplets. I — Retention of HCl, HNO3, NH3 and H2O2,Atmos. Environ. 24A, 383–390.
Jaffrezo, J.-L., Dibb, J., Bales, R., and Neftel, A., 1994a, Current atmospheric studies at Summit (Greenland) and implications for future research, in R. J. Delmas (ed.), NATO ARW:Ice Core Chemistry of Global Biogeochemical Cycles, Springer-Verlag, Berlin, pp. 435–467.
Jaffrezo, J.-L., Davidson, C. I., Legrand, M., and Dibb, J., 1994b, Sulfate and MSA in the air and snow on the Greenland ice sheet,J. Geophys. Res. 99, 1241–1253.
Johansson, C. and Granat, L., 1986, An experimental study of the dry deposition of gaseous nitric acid to snow,Atmos. Environ. 20, 1165–1170.
Kroes, G.-J. and Clary, D. C., 1992, Adsorption of HCl on ice under stratospheric conditions: a computational study,Geophys. Res. Lett. 19, 1355–1358.
Legrand, M. and Delmas, R., 1984, The ionic balance of Antarctic snow: a 10-yr detailed study,Atmos. Environ. 18, 1867–1874.
Legrand, M. and Delmas, R., 1988, Formation of HCl in the Antarctic atmosphere,J. Geophys. Res. 93, 7153–7168.
Legrand, M., De Angelis, M., Staffelbach, T., Neftel, A., and Stauffer, B., 1992, Large perturbation of ammonium and organic acids content in the Summit-Greenland ice core. Fingerprint from forest fires?Geophys. Res. Lett. 19, 473–475.
Legrand, M. and De Angelis, M., 1995, Origins and variations of light carboxylic acids in polar precipitation,J. Geophys. Res. 100, 1445–1462.
Legrand, M., 1994, Ice core chemistry: implications for our past atmosphere, in G. Moortgatet al. (eds.), NATO ASI:Low-Temperature Chemistry of the Atmosphere, Vol. 121, pp. 421–445.
Leu, M. T., 1988, Laboratory studies of sticking coefficients and heterogeneous reactions important in the Antarctic stratosphere,Geophys. Res. Lett. 15, 17–20.
Marrero, T. R. and Mason, E. A., 1972, Gaseous diffusion coefficients,J. Phys. Chem. Ref. Data 1, 3–118.
Marti, J., Mauersberger, K., and Hanson, D., 1991, HCl dissolved in solid mixtures of nitric acid and ice: implications for the polar stratosphere,Geophys. Res. Lett. 18, 1861–1864.
Marti, J. and Mauersberger, K., 1993, A survey and new measurements of ice vapor pressure at temperature between 170 and 250 K,Geophys. Res. Lett. 20, 363–366.
Mayewski, P. A. and Legrand, M., 1990, Recent increase in nitrate concentration of Antarctica,Nature 346, 258–260.
Mayewski, P. A., Spencer, M. J., Twickler, M. S., and Whitlow, S., 1990, A glaciochemical survey of the Summit region, Greenland,Ann. Glaciol. 14, 186–190.
Mayewski, P. A., Meeker, S. D., Morrison, M. C., Twickler, M. S., Whitlow, S. E., Ferland, K. K., Meese, D. A., Legrand, M., and Steffensen, J. P., 1993, Greenland ice core ‘signal’ characteristics: an expanded view of climate change,J. Geophys. Res. 98, 12839–12847.
Mosher, B. W., Winkler, P., and Jaffrezo, J.-L., 1993, Seasonal aerosol chemistry at Dye 3, Greenland,Atmos. Environ. 27A, 2761–2772.
Neftel, A., Beer, J., Oeschger, Zürcher, F., and Finkel, R. C., 1985, Sulphate and nitrate concentrations in snow from South Greenland 1895–1978,Nature 314, 611–613.
Neubauer, J. and Heumann, K. G., 1988, Nitrate trace determination in snow and firn core samples of ice shelves at the Wedell sea, Antarctica,Atmos. Environ. 22, 537–545.
Philibert, J., 1990,Diffusion et transport de matière dans les solides, Les éditions de physique, Les Ulis (France).
Pruppacher, H. R. and Klett, J. D., 1978,Microphysics of Clouds and Precipitation, D. Reidel, Dordrecht.
Rosenberg, C., Winiwater, W., Gregori, M., Pech, G., Cansensky, V., and Puxbaum, H., 1988, Determination of inorganic and organic volatile acids, NH3, particulate SO 2−4 , NO −3 and Cl− in ambient air with an annular denuder system,Fresenius Z. Anal. Chem. 331, 1–7.
Sigg, A., Staffelbach, T., and Neftel, A., 1994, Gas phase measurements of hydrogen peroxide in Greenland and their meaning for the interpretation of H2O2 records in ice cores,J. Atmos. Chem. 14, 223–232.
Silvente, E., 1993, Contribution à l'étude de la fonction de transfert air neige en régions polaires. Thèse, Université Joseph Fourier, Grenoble.
Silvente, E. and Legrand, M., 1993, Ammonium to sulphate ratio in aerosol and snow of Greenland and Antarctic regions,Geophys. Res. Lett. 20, 687–690.
Silvente, E. and Legrand, M., 1995, A preliminary study of the air-snow relationship for nitric acid in Greenland, in R. J. Delmas (ed.), NATO ARW:Ice Core Chemistry of Global Biogeochemical Cycles, Springer-Verlag, Berlin, pp. 233–248.
Staffelbach, T., Neftel, A., Stauffer, B., and Jacob, D., 1991, A record of the atmospheric methane sink from formaldehyde in polar ice cores,Nature 349, 603–605.
Steffensen, J. P., 1988, Analysis of the seasonal variations of dust, Cl−, NO −3 , and SO 2−4 in two central Greenland firn cores,Ann. Glaciol. 10, 171–177.
Valdez, M. P., Dawson, G. A., and Bales, R. C., 1989, Sulfur dioxide incorporation into ice depositing from the vapor,J. Geophys. Res. 94, 1095–1103.
Van Doren, J. N., Watson, L. R., Davidovits, P., Worsnop, D. R., Zahniser, M. S., and Kolb, C. E., 1990, Temperature dependence of the uptake coefficients of HNO3, HCl, and N2O5 by water droplets,J. Phys. Chem. 94, 3265–3269.
Vierkorn-Rudolph, B., Bächmann, K., Schwarz, B., and Meixner, F. X., 1984, Vertical profiles of hydrogen chloride in the troposphere,J. Atmos. Chem. 2, 47–63.
Wolff, E. W., Mulvaney, R., and Oates, K., 1989, Diffusion and location of hydrochloric acid in ice: implications for polar stratospheric clouds and ozone depletion,Geophys. Res. Lett. 16, 487–490.
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Dominé, F., Thibert, E., Silvente, E. et al. Determining past atmospheric HCl mixing ratios from ice core analyses. J Atmos Chem 21, 165–186 (1995). https://doi.org/10.1007/BF00696579
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DOI: https://doi.org/10.1007/BF00696579