This paper
investigated the possibility that aerosol particles are scavenged during the
first and fast diffusional growth of small ice crystals. After ice phase
formation, riming, scavenging and aggregation may lead to the collection of
additional aerosol particles. Therefore, particles left after ice evaporation
in hydrometeors, called ice residuals, may not currently be identical to ice
nucleating particles. To overcome this problem, the largest ice crystals are
removed during sampling in clouds and only crystals in the initial phase of
growth, with diameters lower than 20 - 30 μm, are usually
considered. Published papers assume that no aerosol scavenging takes place
during the initial phase of growth of small ice crystals. The aim of this paper
was to ascertain if this assumption is valid. Experiments were performed in a
cold laboratory by considering ice crystals growing in the presence of
supercooled droplets. Results showed that crystals can scavenge aerosol even in
the first stage of growth. Theoretical considerations show that aerosol
scavenging cannot be explained by Brownian
diffusion, inertial impaction or interception processes. We suggest that
the presence of aerosol in the pristine ice crystals may be due to
diffusiophoretic force. During diffusive crystal growth, a flow called Stefan’s
flow exists near the hydrometeor surface, driving the nearby aerosol particles
towards the surface of the growing hydrometeors.
Field, P.R., Lawson, R.P., Brown, P.R.A., Lloyd, G., Westbrook, C., Moisseev, D., Miltenberger, A., Nenes, A., Blyth, A., Choularton, T., et al. (2017) Secondary Ice Production: Current State of the Science and Recommendations for the Future. Meteorological Monographs, 58, 7.1-7.20.
Heymsfield, A. and Miloshevich, L.M. (1993) Homogeneous Ice Nucleation and Supercooled Liquid Water in Orographic Wave Clouds. Journal of Atmospheric Sciences, 50, 2335-2353. https://doi.org/10.1175/1520-0469(1993)050<2335:HINASL>2.0.CO;2
Cziczo, D.J., Ladino. L., Boose, Y., Kanji, A., Kupiszewski, P., Lance, S., Mertes, S. and Wex, H. (2017) Measurements of Ice Nucleating Particles and Ice Residuals. Meteorological Monographs, 58, 8.1-8.13.
Karcher, B. and Basko, M.M. (2004) Trapping of Trace Gases in Growing Ice Crystals. Journal of Geophysical Research, 109, D22204. https://doi.org/10.1029/2004JD005254
Marécal, V., Pirre, M., Rivière, E.D., Pouvesle, N., Crowley, J.N., Freitas, S.R. and Longo, K.M. (2010). Modelling the Reversible Uptake of Chemical Species in the Gas Phase by Ice Particles Formed in a Convective Cloud. Atmospheric Chemistry and Physics, 10, 4977-5000. https://doi.org/10.5194/acp-10-4977-2010
Kupiszewski, P., Weingartner, E, Vochezer, P., Schnaiter, M., Bigi, A., Gysel, M., Rosati, B., Toprak, E., Mertes, S. and Baltensperger, U. (2015) The Ice Selective Inlet: A Novel Technique for Exclusive Extraction of Pristine Ice Crystals in Mixed-Phase Clouds. Atmospheric Measurement Techniques, 8, 3087-3106. https://doi.org/10.5194/amt-8-3087-2015
Isono, K. (1955) On Ice-Crystal Nuclei and Other Substances Found in Snow Crystals. Journal of Meteorology, 12, 456-462. https://doi.org/10.1175/1520-0469(1955)012<0456:OICNAO>2.0.CO;2
Kumai, M. (1951) Electron-Microscope Study of Snow-Crystal Nuclei. Journal of Meteorology, 8, 151-156. https://doi.org/10.1175/1520-0469(1951)008<0151:EMSOSC>2.0.CO;2
Mertes, S., Verheggen, B., Walter, S., Connolly, P., Ebert, M., Schneider, J., Bower, K.N., Cozic, J., Weinbruch, S., Baltensperger, U. and Weingartner, E. (2007) Counterflow Virtual Impactor Based Collection of Small Ice Particles in Mixed-Phase Clouds for the Physico-Chemical Characterization of Tropospheric Ice Nuclei: Sampler Description and First Case Study. Aerosol Science and Technology, 41, 848-864. https://doi.org/10.1080/02786820701501881
Cziczo, D.J., Murphy, D.M., Hudson, P.K. and Thomson, D.S. (2004) Single Particle Measurements of the Chemical Composition of Cirrus Ice Residue during CRYSTAL-FACE. Journal of Geophysical Research, 109, D04201. https://doi.org/10.1029/2003JD004032
Prenni, A.J., De Mott, P.J., Rogers, D.C., Kreidenweiss, S.M., Mcfarquhar, G.M., Zhang, G. and Poellot, M.R. (2009) Ice Nuclei Characteristics from M-PACE and Their Relation to Ice Formation in Clouds. Tellus, 61B, 436-448. https://doi.org/10.1111/j.1600-0889.2009.00415.x
Froyd, K.D., Murphy, D.M., Lawson, P., Baumgardner, D. and Herman, R.L. (2010) Aerosols That Form Subvisiblecirrus at the Tropical Tropopause. Atmospheric Chemistry and Physics, 10, 209-218. https://doi.org/10.5194/acp-10-209-2010
Santachiara, G., Belosi, F. and Prodi, F. (2014) The Mystery of Ice Crystal Multiplication in a Laboratory Experiment. Journal of Atmospheric Sciences, 71, 89-97. https://doi.org/10.1175/JAS-D-13-0117.1
Griggs, D.J. and Jayaratne, E.R. (1986) The Replication of Ice Crystals Using Formvar: Techniques and Precautions. Journal of Atmospheric and Oceanic Technology, 3, 547-551. https://doi.org/10.1175/1520-0426(1986)003<0547:TROICU>2.0.CO;2
Beresnev, S., Chernyak, V. and Starikov, S. (1999) Diffusiophoresis of Aerosol Particles in a Binary Gas Mixture. Journal of Aerosol Science, 30, S761-S762. https://doi.org/10.1016/S0021-8502(99)80391-7
Prodi, F., Santachiara, G. and Cornetti, C. (2002) Measurements of Diffusiophoretic Velocities of Aerosol Particles in the Transition Region. Journal of Aerosol Science, 33, 181-188. https://doi.org/10.1016/S0021-8502(01)00164-1
Kuroda, T. (1984) Rate Determining Processes of Growth of Ice Crystals from the Vapour Phase. Part I: Theoretical Consideration. Journal of the Meteorological Society of Japan, 62, 552-562. https://doi.org/10.2151/jmsj1965.62.3_552
Goldsmith, P. and May, F.G. (1966) Diffusiophoresis and Thermophoresis in Water Vapour Systems. In: Davies, C.N., Ed., Aerosol Science, Academic Press, New York, 163-194.
Fukuta, N. and Takahashi, T. (1999) The Growth of Atmospheric Ice Crystals: A Summary of Findings in Vertical Supercooled Cloud Tunnel Studies. Journal of Atmospheric Sciences, 56, 1963-1979. https://doi.org/10.1175/1520-0469(1999)056<1963:TGOAIC>2.0.CO;2
DeMott, P.J., Prenni, A.J., Liu, X., Kreidenweis, S.M., Petters, M.D., Twohy, C.H., Richardson, M.S., Eidhammer, T. and Rogers, D.C. (2010) Predicting Global Atmospheric Ice Nuclei Distributions and Their Impacts on Climate. Proceedings of the National Academy of Sciences, 107, 11217-11222. https://doi.org/10.1073/pnas.0910818107
Kupiszewski, P., Zanatta, M., Mertes, S., Vochezer, P., Lloyd, G., Schneider, J., Schenk, L., Schnaiter, M., Baltensperger, U., Weingartner, E. and Gysel, M. (2016) Ice Residual Properties in Mixed-Phase Clouds at the High-Alpine Jungfraujoch Site. Journal of Geophysical Research, 121, 12343-12362.
Schmidt, S., Schneider, J., Klimach, T., Mertes, S., Schenk, L.P., Kupiszewski, P., Curtius, J. and Borrmann, S. (2017) Online Single Particle Analysis of Ice Particle Residuals from Mountain-Top Mixed-Phase Cloud Using Laboratory Derived Particle Type Assignment. Atmospheric Chemistry and Physics, 17, 575-594. https://doi.org/10.5194/acp-17-575-2017
Ohtake, T. (1976) Ice Crystals in the Antarctic Atmosphere. Proceedings of Ninth International Conference on Cloud Physics, Boulder, 26-30 July 1976, 484-487.
Kumai, M. (1976) Identification of Nuclei and Concentrations of Chemical Species in Snow Crystals Sampled at the South Pole. Journal of Atmospheric Sciences, 33, 833-841. https://doi.org/10.1175/1520-0469(1976)033<0833:IONACO>2.0.CO;2
Prodi, F. and Oraltay, R.G. (1991) Scavenging of Aerosol Particles by Growing and Evaporating Ice Crystals, Assessing the Role of Competitive Processes. Proceedings of the 5th International Conference on Precipitation Scavenging and Atmosphere-Surface Exchange Processes, Richland, 15-19 July 1991, 75-86.
Santachiara, G., Belosi, F. and Prodi, F. (2016) Ice Crystal Precipitation at Dome C Site (East Antarctica). Atmospheric Research, 167, 108-117. https://doi.org/10.1016/j.atmosres.2015.08.006
Ebert, M., Worringen, A., Benker, N., Mertes, S., Weingartner, E. and Weinbruch, S. (2011) Chemical Composition and Mixing-State of Ice Residuals Sampled within Mixed Phase Clouds. Atmospheric Chemistry and Physics, 11, 2805-2816. https://doi.org/10.5194/acp-11-2805-2011
Zobrist, B., Marcolli, C., Peter, T. and Koop, T. (2008) Heterogeneous Ice Nucleation in Aqueous Solutions: The Role of Water Activity. The Journal of Physical Chemistry A, 112, 3965-3975. https://doi.org/10.1021/jp7112208
Welti, A., Lüond, F., Stetzer, O. and Lohmann, U. (2009) Influence of Particle Size on the Ice Nucleating Ability of Mineral Dusts. Atmospheric Chemistry and Physics, 9, 6705-6715. https://doi.org/10.5194/acp-9-6705-2009
Targino, A.C., Krejci, R., Noone, K.J. and Glantz P. (2006) Single Particle Analysis of Ice Crystal Residuals Observed in Orographic Wave Clouds over Scandinavia during INTACC Experiment. Atmospheric Chemistry and Physics, 6, 1977-1990. https://doi.org/10.5194/acp-6-1977-2006
Kamphus, M., Ettner-Mahl, M., Klimach, T., Drewnick, F., Keller, L., Cziczo, D.J., Mertes, S., Borrmann, S. and Curtius, J. (2010) Chemical Composition of Ambient Aerosol, Ice Residues and Cloud Droplet Residues in Mixed-Phase Clouds: Single Particle Analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6). Atmospheric Chemistry and Physics, 10, 8077-8095. https://doi.org/10.5194/acp-10-8077-2010
Worringen, A., Kandler, K., Benker, N., Dirsch, T., Mertes, S., Schenk, L., Kastner, U., Frank, F., Nillius, B. and Bunke, U. (2015) Single-Particle Characterization of Ice-Nucleating Particles and Ice Particle Residuals Sampled by Three Different Techniques. Atmospheric Chemistry and Physics, 15, 4161-4178. https://doi.org/10.5194/acp-15-4161-2015
Seifer, M., Strom, J., Kreici, R., Minikin, A., Petzold, A., Gayet, J.-F. and Schumann, U. (2003) In Situ Observations of Aerosol Particles Remaining from Evaporated Cirrus Crystals: Comparing Clean and Polluted Air Masses. Atmospheric Chemistry and Physics, 3, 1037-1049. https://doi.org/10.5194/acp-3-1037-2003
Baumgardner, D., Subramanian, R., Twohy, C., Stith, J. and Kok, G. (2008) Scavenging of Black Carbon by Ice Crystals over the Northern Pacific. Geophysical Research Letters, 35, L22815. https://doi.org/10.1029/2008GL035764
