ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-10-7945-2010 Volume nucleation rates for homogeneous freezing in supercooled water microdroplets: results from a combined experimental and modelling approach Earle M. E. 1 2 Kuhn T. 1 3 Khalizov A. F. 1 4 Sloan J. J. 1 Department of Earth and Environmental Sciences, University of Waterloo, Waterloo, ON, Canada now at: Cloud Physics and Severe Weather Research Section, Environment Canada, Toronto, ON, Canada now at: Department of Space Science, Luleå University of Technology, Kiruna, Sweden now at: Department of Atmospheric Sciences, Texas A&M University, College Station, TX, USA 27 08 2010 10 16 7945 7961 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/10/7945/2010/acp-10-7945-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/7945/2010/acp-10-7945-2010.pdf

Temperature-dependent volume nucleation rate coefficients for supercooled water droplets, <i>J<sub>V</sub>(T</i>), are derived from infrared extinction measurements in a cryogenic laminar aerosol flow tube using a microphysical model. The model inverts water and ice aerosol size distributions retrieved from experimental extinction spectra by considering the evolution of a measured initial droplet distribution via homogeneous nucleation and the exchange of vapour-phase water along a well-defined temperature profile. Experiment and model results are reported for supercooled water droplets with mean radii of 1.0, 1.7, and 2.9 μm. Values of mass accommodation coefficients for evaporation of water droplets and vapour deposition on ice particles are also determined from the model simulations. The coefficient for ice deposition was found to be 0.031 ± 0.001, while that for water evaporation was 0.054 ± 0.012. Results are considered in terms of the applicability of classical nucleation theory to the freezing of micrometre-sized droplets in cirrus clouds, with implications for the parameterization of homogeneous ice nucleation in numerical models.

 References Anderson, R. J., Miller, R. C., Kassner, J. L., and Hagen, D. E.: A study of homogeneous condensation-freezing nucleation of small water droplets in an expansion cloud chamber, J. Atmos. Sci., 37, 2508–2520, 1980. Bohren, C. F. and Huffman, D. R.: Absorption and scattering of light by small particles, John Wiley and Sons, Inc., New York, 530~pp., 1983. Butorin, G. T. and Skripov, V. P.: Crystallization in supercooled water, Kristallografiya, 17, 379–0384, 1972. Chelf, J. H. and Martin, S. T.: Homogeneous ice nucleation in aqueous ammonium sulfate aerosol particles, J. Geophys. Res., 106, 1215–1226, 2001. Choularton, T. W. and Latham, J.: Measurements of deposition coefficient for ice, and its application to cirrus seeding, Q. J. Roy. Meteorol. Soc., 103, 307–318, 1977. Clapp, M. L., Miller, R. E., and Worsnop, D. R.: Frequency-dependent optical-constants of water ice obtained directly from aerosol extinction spectra, J. Phys. Chem., 99, 6317–6326, 1995. Cotton, R. J., Benz, S., Field, P. R., Möhler, O., and Schnaiter, M.: Technical Note: A numerical test-bed for detailed ice nucleation studies in the AIDA cloud simulation chamber, Atmos. Chem. Phys., 7, 243–256, doi:10.5194/acp-7-243-2007, 2007. Cziczo, D. J. and Abbatt, J. P. D.: Deliquescence, efflorescence, and supercooling of ammonium sulfate aerosols at low temperature: implications for cirrus cloud formation and aerosol phase in the atmosphere, J. Geophys. Res., 104, 13781–13790, 1999. DeMott, P. J. and Rogers, D. C.: Freezing nucleation rates of dilute-solution droplets measured between −30 °C and −40 °C in laboratory simulations of natural clouds, J. Atmos. Sci., 47, 1056–1064, 1990. Djikaev, Y. S., Tabazadeh, A., Hamill, P., and Reiss, H.: Thermodynamic conditions for the surface-stimulated crystallization of atmospheric droplets, J. Phys. Chem. A, 106, 10247–10253, 2002. Duft, D. and Leisner, T.: Laboratory evidence for volume-dominated nucleation of ice in supercooled water microdroplets, Atmos. Chem. Phys., 4, 1997–2000, doi:10.5194/acp-4-1997-2004, 2004. Glickman, T.: Glossary of meteorology, American Meteorological Society, Boston, 855~pp., 2000. Haynes, D. R., Tro, N. J., and George, S. M.: Condensation and evaporation of H<sub>2</sub>O on ice surfaces, J. Phys. Chem., 96, 8502–8509, 1992. Heymsfield, A. J., Miloshevich, L. M., Schmitt, C., Bansemer, A., Twohy, C., Poellot, M. R., Fridlind, A., and Gerber, H.: Homogeneous ice nucleation in subtropical and tropical convection and its influence on cirrus anvil microphysics, J. Atmos. Sci., 62, 41–64, 2005. Hinds, W. C.: Aerosol technology: properties, behavior, and measurement of airborne particles, Wiley-Interscience, Toronto, 483~pp., 1999. Houzelot, J. L. and Villermaux, J.: Mass-transfer in annular cylindrical reactors in laminar-flow, Chem. Eng. Sci., 32, 1465–1470, 1977. Hung, H. M., Malinowski, A., and Martin, S. T.: Ice nucleation kinetics of aerosols containing aqueous and solid ammonium sulfate particles, J. Phys. Chem. A, 106, 293–306, 2002. Hung, H. M. and Martin, S. T.: Apparent freezing temperatures modeled for several experimental apparatus, J. Geophys. Res.-Atmos., 106, 20379–20394, 2001. Jensen, E. J., Toon, O. B., Tabazadeh, A., Sachse, G. W., Anderson, B. E., Chan, K. R., Twohy, C. W., Gandrud, B., Aulenbach, S. M., Heymsfield, A., Hallett, J., and Gary, B.: Ice nucleation processes in upper tropospheric wave-clouds observed during SUCCESS, Geophys. Res. Lett., 25, 1363–1366, 1998. Kärcher, B. and Lohmann, U.: A parameterization of cirrus cloud formation: homogeneous freezing of supercooled aerosols, J. Geophys. Res.-Atmos., 107, 4010, doi:10.1029/2001JD000470, 2002. Khalizov, A., Earle, M. E., Johnson, W. J. W., Stubley, G. D., and Sloan, J. J.: Development and characterization of a laminar aerosol flow tube, Rev. Sci. Instrum., 77, 033102, doi:10.1063/1.2175958, 2006a. Khalizov, A. F., Earle, M. E., Johnson, W. J. W., Stubley, G. D., and Sloan, J. J.: Modeling of flow dynamics in laminar aerosol flow tubes, J. Aerosol. Sci., 37, 1174–1187, 2006b. Krämer, B., Hubner, O., Vortisch, H., Woste, L., Leisner, T., Schwell, M., Ruhl, E., and Baumgartel, H.: Homogeneous nucleation rates of supercooled water measured in single levitated microdroplets, J. Chem. Phys., 111, 6521–6527, 1999. Kuhn, T., Earle, M. E., Khalizov, A. F., and Sloan, J. J.: Size dependence of volume and surface nucleation rates for homogeneous freezing of supercooled water droplets, Atmos. Chem. Phys. Discuss., 9, 22929–22953, doi:10.5194/acpd-9-22929-2009, 2009. Lagarias, J. C., Reeds, J. A., Wright, M. H., and Wright, P. E.: Convergence properties of the Nelder-Mead simplex method in low dimensions, Siam J. Optimiz., 9, 112–147, 1998. Lawson, R. P., Baker, B. A., Pilson, B., and Mo, Q.: In situ observations of the microphysical properties of wave, cirrus, and anvil clouds – Part II: Cirrus clouds, J. Atmos. Sci., 63, 3186–3203, 2006. Li, Y. Q., Davidovits, P., Shi, Q., Jayne, J. T., Kolb, C. E., and Worsnop, D. R.: Mass and thermal accommodation coefficients of H<sub>2</sub>O(g) on liquid water as a function of temperature, J. Phys. Chem. A, 105, 10627–10634, 2001. Liou, K. N.: Influence of cirrus clouds on weather and climate processes: a global perspective, Mon. Weather Rev., 114, 1167–1199, 1986. Liu, X. and Penner, J. E.: Ice nucleation parameterization for global models, Meteorol. Z., 14, 499–514, 2005. Magee, N., Moyle, A. M., and Lamb, D.: Experimental determination of the deposition coefficient of small cirrus-like ice crystals near −50 °C, Geophys. Res. Lett., 33, L17813, doi:10.1029/2006GL026665, 2006. Prakash, A., Bapat, A. P., and Zachariah, M. R.: A simple numerical algorithm and software for solution of nucleation, surface growth, and coagulation problems, Aerosol Sci. Tech., 37, 892–898, 2003. Pratte, P., Van Den Bergh, H., and Rossi, M. J.: The kinetics of H<sub>2</sub>O vapor condensation and evaporation on different types of ice in the range 130–210 K, J. Phys. Chem. A, 110, 3042–3058, 2006. Pruppacher, H. R.: A new look at homogeneous ice nucleation in supercooled water drops, J. Atmos. Sci., 52, 1924–1933, 1995. Pruppacher, H. R. and Klett, J. D.: Microphysics of clouds and precipitation, Kluwer Academic Publishers, Boston, 954~pp., 1998. Shaw, R. A. and Lamb, D.: Experimental determination of the thermal accommodation and condensation coefficients of water, J. Chem. Phys., 111, 10659–10663, 1999. Stöckel, P., Weidinger, I. M., Baumgartel, H., and Leisner, T.: Rates of homogeneous ice nucleation in levitated H<sub>2</sub>O and D<sub>2</sub>O droplets, J. Phys. Chem. A, 109, 2540-2546, 2005. Tabazadeh, A., Djikaev, Y. S., Hamill, P., and Reiss, H.: Laboratory evidence for surface nucleation of solid polar stratospheric cloud particles, J. Phys. Chem. A, 106, 10238–10246, 2002a. Tabazadeh, A., Djikaev, Y. S., and Reiss, H.: Surface crystallization of supercooled water in clouds, P. Natl. Acad. Sci. USA, 99, 15873–15878, 2002b. Taborek, P.: Nucleation in emulsified supercooled water, Phys. Rev. B, 32, 5902–5906, 1985. Turnbull, J. and Fisher, J. C.: Rate of nucleation in condensed systems, J. Chem. Phys., 17, 71–73, 1949. Villermaux, J.: Diffusion in a cylindrical reactor, Int. J. Heat Mass Trans., 14, 1963–1981, 1971. Zasetsky, A. Y., Earle, M. E., Cosic, B., Schiwon, R., Grishin, I. A., McPhail, R., Pancescu, R. G., Najera, J., Khalizov, A. F., Cook, K. B., and Sloan, J. J.: Retrieval of aerosol physical and chemical properties from mid-infrared extinction spectra, J. Quant. Spectrosc. Radiat. Trans., 107, 294–305, 2007. Zasetsky, A. Y., Khalizov, A. F., Earle, M. E., and Sloan, J. J.: Frequency dependent complex refractive indices of supercooled liquid water and ice determined from aerosol extinction spectra, J. Phys. Chem. A, 109, 2760–2764, 2005. Zasetsky, A. Y., Khalizov, A. F., and Sloan, J. J.: Characterization of atmospheric aerosols from infrared measurements: simulations, testing, and applications, Appl. Opt., 43, 5503–5511, 2004a. Zasetsky, A. Y., Khalizov, A. F., and Sloan, J. J.: Local order and dynamics in supercooled water: a study by IR spectroscopy and molecular dynamic simulations, J. Chem. Phys., 121, 6941–6947, 2004b.