Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 9 20 2009 10.5194/acp-9-7679-2009 http://www.atmos-chem-phys.net/9/7679/2009/ http://www.atmos-chem-phys.net/9/7679/2009/acp-9-7679-2009.html http://www.atmos-chem-phys.net/9/7679/2009/acp-9-7679-2009.pdf 7679 7690 2009-10-16 Gas phase acetic acid and its qualitative effects on snow crystal morphology and the quasi-liquid layer T. N. Knepp T. L. Renkens P. B. Shepson pshepson@purdue.edu Department of Chemistry, Purdue University, 560 Oval Dr., West Lafayette, IN 47907, USA Department of Earth and Atmospheric Science, Purdue University, 550 Stadium Mall Dr., West Lafayette, IN 47907, USA Purdue Climate Change Research Center, Purdue University, 503 Northwestern Ave., West Lafayette, IN 47907, USA A chamber was constructed within which snow crystals were grown on a string at various temperatures, relative humidities, and acetic acid gas phase mole fractions. The temperature, relative humidity, and acid mole fraction were measured for the first time at the point of crystal growth. Snow crystal morphological transition temperature shifts were recorded as a function of acid mole fraction, and interpreted according to the calculated acid concentration in the crystal's quasi-liquid layer, which is believed to have increased in thickness as a function of acid mole fraction, thereby affecting the crystal's morphology consistent with the hypothesis of Kuroda and Lacmann. Deficiencies in the understanding of the quasi-liquid layer and its role in determining snow crystal morphology are briefly discussed. Abbatt, J. P. D.: Heterogeneous reaction of HOBr with HBr and HCl on ice surfaces at 229 K, Geophys. Res. Lett., 21, 665–668, 1994. Aloisio, S. and Francisco, J. S.: New Radical – Molecule Association Compounds, J. Am. Chem. Soc., 122, 9196–9200, 2000. Anderson, B. J., Sutkoff, J. D., and Hallett, J.: Influence of Methyl 2-Cyanoacrylate Monomer on Habit of Ice Crystals Grown from Vapor, J. Atmos. Sci., 26, 673–674, 1969. Barrie, L. A., Bottenheim, J. W., Schnell, R. C., Crutzen, P. J., and Rasmussen, R. A.: Ozone destruction and photochemical reactions at polar sunrise in the lower Arctic atmosphere, Nature, 334, 138–141, 1988. Bluhm, H., Ogletree, D. F., Fadley, C. S., Hussain, Z., and Salmeron, N.: The premelting of ice studied with photoelectron spectroscopy, J. Phys.-Condens. Mat., 14, L227–L233, 2002. Byrk, T. and Haymet, A. D. J.: Charge separation at the ice/water interface: a molecular dynamics simulation study of solute ions at the ice basal plane, J. Mol. Liq., 112, 47–50, 2004. Carignano, M. A., Shepson, P. B., and Szleifer, I.: Molecular dynamics simulations of ice growth from supercooled water, Mol. Phys., 103, 2957–2967, 2005. Carignano, M. A., Shepson, P. B., and Szleifer, I.: Ions at the ice/vapor interface, Chem. Phys. Lett., 436, 99–103, 2007. Cho, H., Shepson, P. B., Barrie, L. A., Cowin, J. P., and Zaveri, R.: NMR investigation of the quasi-brine layer in ice/brine mixtures, J. Phys. Chem. B, 106, 11226–11232, 2002. CRC: CRC Handbook of Chemistry and Physics, 87 ed., edited by: Lide, D. R., Taylor & Francis, Boca Raton, FL, 2007. De Haan, D. O., Brauers, T., Oum, K., Stutz, J., Nordmeyer, T., and Finlayson-Pitts, B. J.: Heterogeneous chemistry in the troposphere: experimental approaches and applications to the chemistry of sea salt particles, Int. Rev. Phys. Chem., 18, 343–385, 1999. Domine, F. and Rauzy, C.: Influence of the ice growth rate on the incorporation of gaseous HCl, Atmos. Chem. Phys., 4, 2513–2519, 2004. Dominé, F., Taillandier, A. S., Simpson, W. R., and Severin, K.: Specific surface area, density and microstructure of frost flowers, Geophys. Res. Lett., 32, L13502, doi:10.1029/2005GL023245, 2005. Döppenschmidt, A., Kappl, M., and Butt, H. J.: Surface properties of ice studied by atomic force microscopy, J. Phys. Chem. B, 102, 7813–7819, 1998. Döppenschmidt, A. and Butt, H. J.: Measuring the thickness of the liquid-like layer on ice surfaces with atomic force microscopy, Langmuir, 16, 6709–6714, 2000. Dosch, H., Lied, A., and Bilgram, J. H.: Glancing-Angle X-Ray-Scattering Studies of the Premelting of Ice Surfaces, Surf. Sci., 327, 145–164, 1995. Ewing, G. E.: Thin film water, J. Phys. Chem. B, 108, 15953–15961, 2004. Fan, S. M. and Jacob, D. J.: Surface Ozone Depletion in Arctic Spring Sustained by Bromine Reactions on Aerosols, Nature, 359, 522–524, 1992. Finlayson-Pitts, B. J., Livingston, F. E., and Berko, H. N.: Ozone destruction and bromine photochemistry at ground level in the Arctic spring, Nature, 343, 622–625, 1990. Finlayson-Pitts, B. J.: The tropospheric chemistry of sea salt: A molecular-level view of the chemistry of NaCl and NaBr, Chem. Rev., 103, 4801–4822, 2003. Frank, F. C.: Descartes' observations on the Amsterdam snowfalls of 4, 5, 6, and 9 February 1635, J. Glaciol., 13, 535–542, 1974. Fukuta, N.: An Origin of the Equilibrium Liquid-Like Layer on Ice, J. Phys.-Paris, 48, 503–509, 1987. Furukawa, Y., Yamamoto, M., and Kuroda, T.: Ellipsometric Study of the Transition Layer on the Surface of an Ice Crystal, J. Cryst. Growth, 82, 665–677, 1987a. Furukawa, Y., Yamamoto, M., and Kuroda, T.: Ellipsometric Study of the Ice Surface Structure Just Below the Melting Point, J. Phys.-Paris, 48, C1 495–C491 501, 1987b. Furukawa, Y.: Faszination der Schneekristalle – wie ihre bezaubernden Formen entstehen, Chem. Unserer Zeit, 31, 58–65, 1997. Furukawa, Y. and Nada, H.: Anisotropic surface melting of an ice crystal and its relationship to growth forms, J. Phys. Chem. B, 101, 6167–6170, 1997. Golecki, I. and Jaccard, C.: Intrinsic Surface Disorder in Ice near Melting-Point, J. Phys. C Solid State, 11, 4229–4237, 1978. Gopalakrishnan, S., Jungwirth, P., Tobias, D. J., and Allen, H. C.: Air-liquid interfaces of aqueous solutions containing ammonium and sulfate: Spectroscopic and molecular dynamics studies, J. Phys. Chem. B, 109, 8861–8872, 2005. Grannas, A. M., Bausch, A. R., and Mahanna, K. M.: Enhanced Aqueous Photochemical Reaction Rates after Freezing, J. Phys. Chem. A, 111, 11043-11049, 2007a. 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, 2007b. Hallett, J. and Mason, B. J.: The Influence of Temperature and Supersaturation on the Habit of Ice Crystals Grown from the Vapour, Proc. R. Soc. Lon. Ser.-A, 247, 440–453, 1958a. Hallett, J. and Mason, B. J.: The Influence of Temperature and Supersaturation on the Habit of Ice Crystals Grown from the Vapour, Proc. R. Soc. Lon. Ser.-A, 247, 440–453, 1958b. Hiramatsu, K. and Sturm, M.: A Simple, Inexpensive Chamber for Growing Snow Crystals in the Classroom, The Physics Teacher, 43, 23–25, 2005. Hönninger, G. and Platt, U.: Observations of BrO and its vertical distribution during surface ozone depletion at Alert, Atmos. Environ., 36, 2481–2489, 2002. Jones, A. E., Anderson, P. S., Wolff, E. W., Turner, J., Rankin, A. M., and Colwell, S. R.: A role for newly forming sea ice in springtime polar tropospheric ozone loss? Observational evidence from Halley station, Antarctica, J. Geophys. Res., 111, D08306, doi:10.1029/2005JD006566, 2006. Jungwirth, P. and Tobias, D. J.: Surface Effects on Aqueous Ionic Solvation: A Molecular Dynamics Simulation Study of NaCl at the Air/Water Interface from Infinite Dilution to Saturation, J. Phys. Chem. B, 104, 7702–7706, 2000. Jungwirth, P. and Tobias, D. J.: Molecular Structure of Salt Solutions: A New View of the Interface with Implications for Heterogeneous Atmospheric Chemistry, J. Phys. Chem. B, 105, 10468–10472, 2001. Jungwirth, P. and Tobias, D. J.: Ions at the Air/Water Interface, J. Phys. Chem. B, 106, 6361–6373, 2002. Jungwirth, P. and Tobias, D. J.: Specific Ion Effects at the Air/Water Interface, Chem. Rev., 106, 1259–1281, 2006. Kawamura, K., Steinberg, S., Ng, L., and Kaplan, I. R.: Wet deposition of low molecular weight mono- and di-carboxylic acids, aldehydes and inorganic species in Los Angeles, Atmos. Environ., 35, 3917–3926, 2001. Keppler, J.: Strena seu de nive sexangula, in: A New Years Gift or on the Six-Cornered Snowflake, edited by: Hardie, C., Oxford Press, 24–38, 1966. Kobayashi, T.: On the Habit of Snow Crystals Artificially Produced, J. Meteorol. Soc. Jpn., Ser. II, 36, 193–208, 1958. Kobayashi, T.: The Growth of Snow Crystals at Low Supersaturations, Philos. Mag., 6, 1363–1370, 1961. Kobayashi, T.: Vapour Growth of Ice Crystal between −40 and −90 C, J. Meteorol. Soc. Jpn., 43, 359–367, 1965. Kuroda, T. and Lacmann, R.: Growth-Kinetics of Ice from the Vapor-Phase and Its Growth Forms, J. Cryst. Growth, 56, 189–205, 1982. Libbrecht, K. G.: Designer Snowflakes: http://www.its.caltech.edu/~atomic/snowcrystals/designer1/designer1.htm, access: 19 June 2007, 1999. Libbrecht, K. G.: Morphogenesis on Ice: The Physics of Snow Crystals, Engineering & Science, 64, 10–19, 2001. Libbrecht, K. G. and Yu, H.: Crystal growth in the presence of surface melting: supersaturation dependence of the growth of columnar ice crystals, J. Cryst. Growth, 222, 822–831, 2001. Libbrecht, K. G., Crosby, T., and Swanson, M.: Electrically enhanced free dendrite growth in polar and non-polar systems, J. Cryst. Growth, 240, 241–254, 2002. Libbrecht, K. G.: California Institute of Technology, Pasadena, CA, Personal Communication, E-mail, 4 June 2005, 2005a. Libbrecht, K. G.: The physics of snow crystals, Rep. Prog. Phys., 68, 855–895, 2005b. Liu, D., Ma, G., Levering, L. M., and Allen, H. C.: Vibrational Spectroscopy of Aqueous Sodium Halide Solutions and Air-Liquid Interfaces: Observation of Increased Interfacial Depth, J. Phys. Chem. B, 108, 2252–2260, 2004. Magono, C., Higuchi, K., Orikasa, K., Takahashi, T., Kikuchi, K., Nakamura, T., Kimura, T., and Sakurai, K.: Investigation on the Growth and Distribution of Natural Snow Crystals by the Use of Observation Points Distributed Vertically, III, Journal of the Faculty Science, Hokkaido University, Japan, 1, 373–387, 1962. Makkonen, L.: Surface melting of ice, J. Phys. Chem. B, 101, 6196–6200, 1997. McNeill, V. F., Loerting, T., Geiger, F. M., Trout, B. L., and Molina, M. J.: Hydrogen chloride-induced surface disordering on ice, P. Natl. Acad. Sci. USA, 103, 9422–9427, 2006. Mucha, M., Frigato, T., Levering, L. M., Allen, H. C., Tobias, D. J., Dang, L. X., and Jungwirth, P.: Unified molecular picture of the surfaces of aqueous acid, base, and salt solutions, J. Phys. Chem. B, 109, 7617–7623, 2005. Nada, H. and Furukawa, Y.: Anisotropic growth kinetics of ice crystals from water studied by molecular dynamics simulation, J. Cryst. Growth, 169, 587–597, 1996. Nada, H. and Furukawa, Y.: Anisotropy in molecular-scaled growth kinetics at ice-water interfaces, J. Phys. Chem. B, 101, 6163–6166, 1997a. Nada, H. and Furukawa, Y.: Anisotropy in structural phase transitions at ice surfaces: a molecular dynamics study, Appl. Surf. Sci., 121, 445–447, 1997b. Nakaya, U.: Snow Crystals: Natural and Artificial, 1 ed., Harvard University Press, Cambridge, 510 pp., 1954. Orlando, J. J. and Tyndall, G. S.: Gas phase UV absorption spectra for peracetic acid, and for acetic acid monomers and dimers, J. Photoch. Photobio., 157, 161–166, 2003. Perovich, D. K. and Richter-Menge, J. A.: Surface characteristics of lead ice, J. Geophys. Res., 99, 16341–16350, 1994. Petersen, P., Saykally, R. J., Mucha, M., and Jungwirth, P.: Enhanced Concentration of Polarizable Anions at the Liquid Water Surface: SHG Spectroscopy and MD Simulations of Sodium Thiocyanide, J. Phys. Chem. B, 109, 10915–10921, 2005. Potter, A. E. and Ritter, H. L.: The Vapor Pressure of Acetic Acid and Acetic-d₃ Acid-d. The Liquid Density of Acetic-d₃ Acid-d, J. Phys. Chem., 58, 1040–1042, 1954. Rankin, A. M. and Wolff, E. W.: Frost flowers: Implications for tropospheric chemistry and ice core interpretation, J. Geophys. Res., 107, 4683–4700, 2002. Rosenberg, R.: Why is ice slippery?, Physics Today, 58, 50–55, 2005. Sadtchenko, V. and Ewing, G. E.: Interfacial melting of thin ice films: An infrared study, J. Chem. Phys., 116, 4686–4697, 2002. Sadtchenko, V., Ewing, G. E., Nutt, D. R., and Stone, A. J.: Instability of ice films, Langmuir, 18, 4632–4636, 2002. Sadtchenko, V. and Ewing, G. E.: A new approach to the study of interfacial melting of ice: infrared spectroscopy, Can. J. Phys., 81, 333–341, 2003. Shen, Y. R.: Frank Isakson prize address – Sum frequency generation for vibrational spectroscopy: Applications to water interfaces and films of water and ice, Solid State Communications, 108, 399–406, 1998. Simpson, W. R., Alvarez-Aviles, L., Douglas, T. A., and Sturm, M.: Halogens in the coastal snow pack near Barrow, Alaska: Evidence for active bromine air-snow chemistry during springtime, Geophys. Res. Lett., 32, L04811, doi:10.1029/2004GL021748, 2005. Simpson, W. R., Carlson, D., Hönninger, G., Douglas, T. A., Sturm, M., Perovich, D., and Platt, U.: First-year sea-ice contact predicts bromine monoxide (BrO) levels at Barrow, Alaska better than potential frost flower contact, Atmos. Chem. Phys., 7, 621–627, 2007. Sokolov, O. and Abbatt, J. P. D.: Adsorption to ice of n-alcohols (ethanol to 1-hexanol), acetic acid, and hexanal, J. Phys. Chem. A, 106, 775–782, 2002. Stull, D. R.: Vapor Pressure of Pure Substances: Organic Compounds, Ind. Eng. Chem., 39, 517–540, 1947. Suresh, S. J. and Naik, V. M.: Hydrogen bond thermodynamic properties of water from dielectric constant data, J. Chem. Phys., 113, 9727–9732, 2000. Takahashi, C. and Mori, M.: Growth of Snow crystals from frozen water droplets, Atmos. Res., 82, 385–290, 2006. Voss, L. F., Henson, B. F., Wilson, K. R., and Robinson, J. M.: Atmospheric impact of quasiliquid layers on ice surfaces, Geophys. Res. Lett., 32, L07807, doi:10.1029/2004GL022010, 2005. Vrbka, L. and Jungwirth, P.: Homogeneous freezing of water starts in the subsurface, J. Phys. Chem. B, 110, 18126–18129, 2006. Wei, X., Miranda, P. B., and Shen, Y. R.: Surface vibrational spectroscopic study of surface melting of ice, Phys. Rev. Lett., 86, 1554–1557, 2001. Wei, X., Miranda, P. B., Zhang, C., and Shen, Y. R.: Sum-frequency spectroscopic studies of ice interfaces, Phys. Rev. B, 66, 085401, doi:10.1103/PhysRevB.66.085401, 2002. Wei, X. and Shen, Y. R.: Vibrational spectroscopy of ice interfaces, Appl. Phys. B-Lasers O., 74, 617–620, 2002. Wettlaufer, J. S.: Impurity Effects in the Premelting of Ice, Phys. Rev. Lett., 82, 2516–2519, 1999. Wettlaufer, J. S.: Dynamics of Ice Surfaces, Interface Sci., 9, 117–129, 2001.