References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-8-1261-2008

Measuring the specific surface area of snow with X-ray tomography and gas adsorption: comparison and implications for surface smoothness

Kerbrat

² Pinzer

¹ Huthwelker

² Gäggeler

H. W.

² ³ Ammann

² Schneebeli

WSL, Swiss Federal Institute for Snow and Avalanche Research SLF, Davos, Switzerland

Paul Scherrer Institute, 5232 Villigen PSI, Switzerland

University of Berne, 3012 Bern, Switzerland

04 03 2008

8 5 1261 1275

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/8/1261/2008/acp-8-1261-2008.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/8/1261/2008/acp-8-1261-2008.pdf

Chemical and physical processes, such as heterogeneous chemical reactions, light scattering, and metamorphism occur in the natural snowpack. To model these processes in the snowpack, the specific surface area (SSA) is a key parameter. In this study, two methods, computed tomography and methane adsorption, which have intrinsically different effective resolutions – molecular and 30 μm, respectively – were used to determine the SSA of similar natural snow samples. Except for very fresh snow, the two methods give identical results, with an uncertainty of 3%. This implies that the surface of aged natural snow is smooth up to a scale of about 30 μm and that if smaller structures are present they do not contribute significantly to the overall SSA. It furthermore implies that for optical methods a voxel size of 10 μm is sufficient to capture all structural features of this type of snow; however, fresh precipitation appears to contain small features that cause an under-estimation of SSA with tomography at this resolution. The methane adsorption method is therefore superior to computed tomography for very fresh snow having high SSA. Nonetheless, in addition to SSA determination, tomography provides full geometric information about the ice matrix. It can also be advantageously used to investigate layered snow packs, as it allows measuring SSA in layers of less than 1 mm.

References 1

Adamson, A W. and Dormant, L M.: Adsorption of Nitrogen on Ice at 78 Degrees K, J. Am. Chem. Soc., 88, 2055–2057, 1966.

Adamson, A W., Dormant, L M., and Orem, M.: Physical Adsorption of Vapors on Ice. I. Nitrogen, J. Colloid Interface Sci., 25, 206–217, 1967.

Albert, M R. and Shultz, E F.: Snow and firn properties and air-snow transport processes at Summit, Greenland, Atmos. Environ., 36, 2789–2797, 2002.

Baker, M B. and Dash, J G.: Charge-Transfer in Thunderstorms and the Surface Melting of Ice, J. Cryst. Growth, 97, 770–776, 1989.

Bartels-Rausch, T., Eichler, B., Zimmermann, P., Gäggeler, H W., and Ammann, M.: The adsorption enthalpy of nitrogen oxides on crystalline ice, Atmos. Chem. Phys., 2, 235–247, 2002.

Bartels-Rausch, T., Guimbaud, C., Gäggeler, H W., and Ammann, M.: The partitioning of acetone to different types of ice and snow between 198 and 223 K, Geophys. Res. Lett., 31, L16110, doi:10.1029/2004GL020070, 2004.

Brown, D E. and George, S M.: Surface and Bulk Diffusion of H2$^18$O on Single-Crystal H2$^16$O Ice Multilayers, J. Phys. Chem., 100, 15 460–15 469, 1996.

Brunauer, S., Emmett, P H., and Teller, E.: Adsorption of gases in multimolecular layers, J. Am. Chem. Soc., 60, 309–319, 1938.

Chaix, L. and Dominé, F.: Effect of the thermal history of ice crushed at 77 K on its surface structure as determined by adsorption of CH4 at low surface coverage, J. Phys. Chem. B, 101, 6105–6108, 1997.

Chaix, L., Ocampo, J., and Dominé, F.: Adsorption of CH4 on laboratory-made crushed ice and on natural snow at 77 K. Atmospheric implications, C. R. Acad. Sci., Ser. II, 322, 609–616, 1996.

Colbeck, S., Akitaya, E., Armstrong, R., Gubler, H., Lafeuille, J., Lied, K., McClung, D., and Morris, E.: The International Classification for Seasonal Snow on the Ground, Int. Comm. On snow and Ice of the Int. Assoc. of Sci. Hydrol., Wallingford, Oxon, UK, 1990.

Colbeck, S C.: The layered character of snow covers, Rev. Geophys., 29, 81–96, 1991.

Coléou, C., Lesaffre, B., Brzoska, J B., Ludwig, W., and Boller, E.: Three-dimensional snow images by X-ray microtomography, Ann. Glaciol., 32, 75–81, 2001.

Dash, J G., Fu, H Y., and Wettlaufer, J S.: The Premelting of Ice and Its Environmental Consequences, Rep. Prog. Phys., 58, 115–167, 1995.

Dash, J G., Rempel, A W., and Wettlaufer, J S.: The physics of premelted ice and its geophysical consequences, Rev. Mod. Phys., 78, 695–741, 2006.

Dominé, F. and Shepson, P B.: Air-snow interactions and atmospheric chemistry, Science, 297, 1506–1510, 2002.

Dominé, F., Cabanes, A., Taillandier, A S., and Legagneux, L.: Specific surface area of snow samples determined by CH4 adsorption at 77 K and estimated by optical, microscopy and scanning electron microscopy, Environ. Sci. Technol., 35, 771–780, 2001.

Dominé, F., Lauzier, T., Cabanes, A., Legagneux, L., Kuhs, W F., Techmer, K., and Heinrichs, T.: Snow metamorphism as revealed by scanning electron microscopy, Microsc. Res. Tech., 62, 33–48, 2003.

Dominé, F., Albert, M., Huthwelker, T., Jacobi, H W., Kokhanovsky, A A., Lehning, M., Picard, G., and Simpson, W R.: Snow physics as relevant to snow photochemistry, Atmos. Chem. Phys., 8, 171–208, http://www.atmos-chem-phys.net/8/171/2008/, 2008a.

Dominé, F., Taillandier, A S., and Simpson, W R.: A parameterization of the specific surface area of seasonal snow for field use and for models of snowpack evolution, J. Geophys. Res., 112, F02031, doi:10.1029/2006JF000512, 2007.

Dullien, F A L.: Porous Media: Fluid Transport and Pore Structure, Academic Press Inc.,U.S., second edn., 1992.

Fassnacht, S R., Innes, J., Kouwen, N., and Soulis, E D.: The specific surface area of fresh dendritic snow crystals, Hydrol. Process., 13, 2945–2962, 1999.

Flanner, M G. and Zender, C S.: Linking snowpack microphysics and albedo evolution, J. Geophys. Res., 111, D12208, doi:10.1029/2005JD006834, 2006.

Flin, F., Brzoska, J B., Lesaffre, B., Cileou, C., and Pieritz, R A.: Full three-dimensional modelling of curvature-dependent snow metamorphism: first results and comparison with experimental tomographic data, J. Phys. D: Appl. Phys., 36, A49–A54, 2003.

Flin, F., Brzoska, J B., Lesaffre, B., Coleou, C C., and Pieritz, R A.: Three-dimensional geometric measurements of snow microstructural evolution under isothermal conditions, Ann. Glaciol., 38, 39–44, 2004.

Flin, F., Brzoska, J B., Coeurjolly, D., Pieritz, R A., Lesaffre, B., Coléou, C., Lamboley, P., Teytaud, O., Vignoles, G L., and Delesse, J F.: Adaptive estimation of normals and surface area for discrete 3-D objects: Application to snow binary data from X-ray tomography, IEEE Trans. Image Process., 14, 585–596, doi:10.1109/TIP.2005.846021, 2005.

German, R M.: Sintering Theory and Practice, John Wiley & Sons, Inc., 1996.

Granberg, H.: Distribution of grain sizes and internal surface area and their role in snow chemistry in a sub-Arctic snow cover, Ann. Glaciol., 7, 149–152, 1985.

Grannas, A M., Jones, A E., Dibb, J., Ammann, M., Anastasio, C., Beine, H J., Bergin, M., Bottenheim, J., Boxe, C S., Carver, G., Chen, G., Crawford, J H., Dominé, F., Frey, M M., Guzmán, M I., Heard, D E., Helmig, D., Hoffmann, M R., Honrath, R E., Huey, L G., Hutterli, M., Jacobi, H W., Klán, P., Lefer, B., McConnell, J., Plane, J., Sander, R., Savarino, J., Shepson, P B., Simpson, W R., Sodeau, J R., von Glasow, R., Weller, R., Wolff, E W., and Zhu, T.: An overview of snow photochemistry: evidence, mechanisms and impacts, Atmos. Chem. Phys., 7, 4329–4373, http://www.atmos-chem-phys.net/7/4329/2007/, 2007.

Gregg, S J. and Sing, K S W.: Adsorption, Surface Area and Porosity, Academic Press Limited, London, second edn., 1982.

Grenfell, T C. and Warren, S G.: Representation of a nonspherical ice particle by a collection of independent spheres for scattering and absorption of radiation, J. Geophys. Res., 104, 31 697–31 709, doi:10.1029/1999JD900496, 1999.

Henson, B F., Voss, L F., Wilson, K R., and Robinson, J M.: Thermodynamic model of quasiliquid formation on H2O ice: Comparison with experiment, J. Chem. Phys., 123, 2005.

Herbert, B M J., Halsall, C J., Jones, K C., and Kallenborn, R.: Field investigation into the diffusion of semi-volatile organic compounds into fresh and aged snow, Atmos. Environ., 40, 1385–1393, doi:10.1016/j.atmosenv.2005.10.055, 2006.

Hoff, J T., Gregor, D., Mackay, D., Wania, F., and Jia, C Q.: Measurement of the specific surface area of snow with the nitrogen adsorption technique, Environ. Sci. Technol., 32, 58–62, 1998.

Huthwelker, T.: Experimente und Modellierung der Spurengasaufnahme in Eis, Cuvillier Verlag, Göttingen, 1999.

Huthwelker, T., Ammann, M., and Peter, T.: The Uptake of Acidic Gases on Ice, Chem. Rev., 106, 1375–1444, 2006.

Jellinek, H G. and Ibrahim, S H.: Sintering of Powdered Ice, J. Colloid Interface Sci., 25, 245–254, 1967.

Jung, K H., Park, S C., Kim, J H., and Kang, H.: Vertical diffusion of water molecules near the surface of ice, J. Chem. Phys., 121, 2758–2764, 2004.

Kaempfer, T U., Schneebeli, M., and Sokratov, S A.: A microstructural approach to model heat transfer in snow, Geophys. Res. Lett., 32, L21503, doi:10.1029/2005GL023873, 2005.

Kärcher, B. and Basko, M M.: Trapping of trace gases in growing ice crystals, J. Geophys. Res., 109, D22204, doi:10.1029/2004JD005254, 2004.

Kerbrat, M., Pinzer, B., Huthwelker, T., Gäggeler, H W., Ammann, M., and Schneebeli, M.: Measuring the specific surface area of snow with X-ray tomography and gas adsorption: comparison and implications for surface smoothness, Atmos. Chem. Phys. Discuss., 7, 10 287–10 322, http://www.atmos-chem-phys-discuss.net/7/10287/2007/, 2007.

Kokhanovsky, A A. and Zege, E P.: Scattering optics of snow, Appl. Opt., 43, 1589–1602, 2004.

Legagneux, L. and Dominé, F.: A mean field model of the decrease of the specific surface area of dry snow during isothermal metamorphism, J. Geophys. Res., 110, F04011, doi:10.1029/2004JF000181, 2005.

Legagneux, L., Cabanes, A., and Dominé, F.: Measurement of the specific surface area of 176 snow samples using methane adsorption at 77 K, J. Geophys. Res., 107, 4335–4349, doi:10.1029/2001JD001016, 2002.

Legagneux, L., Taillandier, A S., and Dominé, F.: Grain growth theories and the isothermal evolution of the specific surface area of snow, J. App. Phys., 95, 6175–6184, 2004.

Libbrecht, K G.: The physics of snow crystals, Rep. Prog. Phys., 68, 855–895, 2005.

Lide, D R.: CRC Handbook of Chemistry and Physics, Taylor and Francis, Boca Raton, FL, 86th edn., 2006.

Lied, A., Dosch, H., and Bilgram, J H.: Surface Melting of Ice I$_h$ Single-Crystals Revealed by Glancing Angle X-Ray-Scattering, Phys. Rev. Lett., 72, 3554–3557, 1994.

Livingston, F E., Whipple, G C., and George, S M.: Surface and bulk diffusion of HDO on ultrathin single-crystal ice multilayers on Ru(001), J. Chem. Phys., 108, 2197–2207, 1997.

Matzl, M. and Schneebeli, M.: Measuring specific surface area of snow by near-infrared photography, J. Glaciol., 52, 558–564, 2006.

Mizuno, Y. and Hanafusa, N.: Studies of surface properties of ice using nuclear magnetic resonance, J. Phys., 48, 511–517, 1987.

Moussa, M R., Muijlwij.R, and Vandijk, H.: Vapour Pressure of Liquid Nitrogen, Physica, 32, 900–912, 1966.

Murphy, D M. and Koop, T.: Review of the vapour pressures of ice and supercooled water for atmospheric applications, Q. J. R. Meteorol. Soc., 131, 1539–1565, doi:10.1256/qj.04.94, 2005.

Narita, H.: Specific surface of deposited snow II, Low Temp. Sci., 29, 69–81, 1971.

Ohser, J. and Mücklich, F.: Statistical Analysis of Microstructures in Materials Science, John Wiley & Sons, Inc., 2000.

Painter, T H., Molotch, N P., Cassidy, M., Flanner, M., and Steffen, K.: Contact spectroscopy for determination of stratigraphy of snow optical grain size, J. Glaciol., 53, 121–127, 2007.

Pielmeier, C. and Schneebeli, M.: Stratigraphy and changes in hardness of snow measured by hand, ramsonde and snow micro penetrometer: a comparison with planar sections, Cold Reg. Sci. Technol., 34, 393–405, 2003.

Pruppacher, H R. and Klett, J D.: Microphysics of clouds and precipitation, Kluwer Academic Publishers, 1997.

Rango, A., Wergin, W P., and Erbe, E F.: Snow crystal imaging using scanning electron microscopy: I. Precipitated snow, Hydrol. Sci., 41, 219–233, 1996.

Schneebeli, M. and Sokratov, S A.: Tomography of temperature gradient metamorphism of snow and associated changes in heat conductivity, Hydrol. Process., 18, 3655–3665, 2004.

Schneebeli, M., Pielmeier, C., and Johnson, J B.: Measuring snow microstructure and hardness using a high resolution penetrometer, Cold Reg. Sci. Technol., 30, 101–114, 1999.

Schwarzenbach, R P., Gschwend, P M., and Imboden, D M.: Environmental Organic Chemistry, John Wiley & Sons, Inc., New York, 2003.

Sommerfeld, R A. and Rocchio, J E.: Permeability Measurements on New and Equitemperature Snow, Water Resour. Res., 29, 2485–2490, 1993.

Sonka, M., Hlavac, V., and Boyle, R.: Image Processing: Analysis and Machine Vision, Thomson-Engineering, second edn., 1999.

Taillandier, A S., Dominé, F., Simpson, W R., Sturm, M., and Douglas, T A.: Rate of decrease of the specific surface area of dry snow: Isothermal and temperature gradient conditions, J. Geophys. Res., 112, F03003, doi:10.1029/2006JF000514, 2007.

Wergin, W P., Rango, A., Foster, J., Erbe, E F., and Pooley, C.: Irregular snow crystals: Structural features as revealed by low temperature scanning electron microscopy, Scanning, 24, 247–256, 2002.

Wettlaufer, J S.: Impurity effects in the premelting of ice, Phys. Rev. Lett., 82, 2516–2519, 1999.

Xiao, R F. and Ming, N B.: Surface Roughening and Surface-Diffusion in Kinetic Thin-Film Deposition, Phys. Rev. E, 49, 4720–4723, 1994.