In light of the percentage of Earth’s cloud coverage, heterogeneous ice nucleation in clouds is the most important global-scale pathway. More recent parameterizations of ice nucleation processes in the atmosphere are based on the concept of ice nucleation active surface site density ( n s ). It is usually assumed that n s is independent of time and aerosol size distribution, i.e. that the surface properties of aerosols of the same species do not vary with size. However, the independence of n s on aerosol size for every species has been questioned. This study presents the results of ice nucleation processes of ATD laboratory-generated aerosol (particle diameters of 0 - 3 μm). Ice nucleation in the condensation mode was performed in a Dynamic Filter Processing Cham- ber at temperatures of - 18 ° C and - 22 ° C, with a saturation ratio with respect to water of 1.02. Results show that n s increased by lowering the nucleation temperature, and was also dependent on the particle size. The n s of particles collected on the filters, after a 0.5 μm D 50 cut-off cyclone, resulted statistically higher with respect to the values obtained from the particles collected on total filters. The results obtained suggest the need for further investigation of n s dependence of same composition aerosol particles with a view to support weather and climate predictions.
KeywordsIce Activated FractionIce Nucleation Active Surface Site DensityCondensation Freezing
Murray, B.J., Broadley, S.L., Wilson, T.W., Bull, S.J., Wills, R.H., Christenson, H.K. and Murray, E.J. (2010) Kinetics of the Homogeneous Freezing of Water. Physical Chemistry Chemical Physics, 12, 10380-10387. https://doi.org/10.1039/c003297b
Riechers, B., Wittbracht, F., Hütten, A. and Koop, T. (2013) The Homogeneous Ice Nucleation Rate of Water Droplets Produced in a Microfluidic Device and the Role of Temperature Uncertainty. Physical Chemistry Chemical Physics, 15, 5873-5887. https://doi.org/10.1039/c3cp42437e
Knopf, D.A., Alpert, P.A., Zipori, A., Reicher, N. and Rudich, Y. (2020) Stochastic Nucleation Processes and Substrate Abundance Explain Time-Dependent Freezing in Supercooled Droplets. NPJ Climate and Atmospheric Science, 3, Article No. 2. https://doi.org/10.1038/s41612-020-0106-4
Vali, G. (2014) Interpretation of Freezing Nucleation Experiments: Singular and Stochastic; Sites and Surfaces. Atmospheric Chemistry and Physics, 14, 5271-5294. https://doi.org/10.5194/acp-14-5271-2014
Vali, G. (1994) Freezing Rate Due to Heterogeneous Nucleation. Journal of the Atmospheric Sciences, 51, 1843-1856. https://doi.org/10.1175/1520-0469(1994)051 2.0.CO;2
Connolly, P.J., Möhler, O., Fields, P.R., Saathoff, H., Burgess, R., Choularton, T. and Gallagher, M. (2009) Studies of Heterogeneous Freezing by Three Different Desert Dust Samples. Atmospheric Chemistry and Physics, 9, 2805-2824. https://doi.org/10.5194/acp-9-2805-2009
Murray, B.J., O’Sullivan, D.O., Atkinson, J.D. and Web, M.E. (2012) Ice Nucleation by Particles Immersed in Supercooled Cloud Droplets. Chemical Society Reviews, 41, 6519-6554. https://doi.org/10.1039/c2cs35200a
Welti, A., Lüond, F., Kanji, Z.A., Stetzer, O. and Lohmann, U. (2012) Time Dependence of Immersion Freezing: An Experimental Study on Size Selected Kaolinite Particles. Atmospheric Chemistry and Physics, 12, 9893-9907. https://doi.org/10.5194/acp-12-9893-2012
Ervens, B. and Feingold, G. (2013) Sensitivity of Immersion Freezing: Reconciling Classical Nucleation Theory and Deterministic Expressions. Geophysical Research Letters, 40, 3320-3324. https://doi.org/10.1002/grl.50580
Wright, T.P. and Petters, M.D. (2013) The Role of Time in Heterogeneous Freezing Nucleation. Journal of Geophysical Research, 118, 3731-3743. https://doi.org/10.1002/jgrd.50365
Sear, R.P. (2013) Generalisation of Levine’s Prediction for the Distribution of Freezing Temperatures of Droplets: A General Singular Model for Ice Nucleation. Atmospheric Chemistry and Physics, 13, 7215-7223. https://doi.org/10.5194/acp-13-7215-2013
Berezinski, N.A., Stepanov, G.V. and Khorguani, V.G. (1988) Ice Forming Activity of Atmospheric Aerosol Particles of Different Sizes. In: Wagner, P.E. and Vali, G., Eds., Atmospheric Aerosols and Nucleation, Lecture Notes in Physics, Vol. 309, Springer, Berlin, 709-712. https://doi.org/10.1007/3-540-50108-8_1167
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
Santachiara, G., Di Matteo, L., Prodi, F. and Belosi, F. (2010) Atmospheric Particles Acting as Ice Forming Nuclei in Different Size Ranges. Atmospheric Research, 96, 266-272. https://doi.org/10.1016/j.atmosres.2009.08.004
Mason, R.H., Si, M., Chou, C., Irish, V.E., Dickie, R., Elizondo, P., Wong, R., Brintnell, M., Elsasser, M., Lassar, W.M., Pierce, K.M., Leaitch, W.R., MacDonald, A.M., Platt, A., Toom-Sauntry, D., Sarda-Estève, R., Schiller, C.L., Suski, K.J., Hill, T.C.J., Abbatt, J.P.D., Huffman, J.A., DeMott, P.J. and Bertram, A.K. (2016) Size-Resolved Measurements of Ice-Nucleating Particles at Six Locations in North America and One in Europe. Atmospheric Chemistry and Physics, 16, 1637-1651. https://doi.org/10.5194/acp-16-1637-2016
Meyers, M.P., DeMott, P.J. and Cotton, W.R. (1992) New Primary Ice-Nucleation Parameterizations in an Explicit Cloud Model. Journal of Applied Meteorology, 31, 708-721. https://doi.org/10.1175/1520-0450(1992)031 2.0.CO;2
Fletcher, N.H. (1962) The Physics of Rainclouds. Cambridge University Press, Cambridge, 410 p.
Cotton, W.R., Tripoli, G.J., Rauber, R.M. and Mulvihill, E.A. (1986) Numerical Simulation of the Effects of Varying Ice Crystal Nucleation Rates and Aggregation Processes on Orographic Snowfall. Journal of Climate and Applied Meteorology, 25, 1658-1680. https://doi.org/10.1175/1520-0450(1986)025 2.0.CO;2
Diehl, K. and Wurzel, S. (2004) Heterogeneous Drop Freezing in the Immersion Mode: Model Calculations Considering Soluble and Insoluble Particles in the Drops. Journal of the Atmospheric Sciences, 61, 2063-2072. https://doi.org/10.1175/1520-0469(2004)061 2.0.CO;2
Kärcher, B. and Lohmann, U. (2003) A Parameterization of Cirrus Cloud Formation: Heterogeneous Freezing. Journal of Geophysical Research, 108, 4402. https://doi.org/10.1029/2002JD003220
Khvorostyanov, V.I. and Curry, J.A. (2004) The Theory of Ice Nucleation by Heterogeneous Freezing of Deliquescent Mixed CCN. Part I: Critical Radius, Energy, and Nucleation Rate. Journal of the Atmospheric Sciences, 61, 2676-2691. https://doi.org/10.1175/JAS3266.1
Liu, X. and Penner, J.E. (2005) Ice Nuclei Parameterization for Global Model. Meteorologische Zeitschrift, 14, 499-514. https://doi.org/10.1127/0941-2948/2005/0059
Phillips, V.T.J., DeMott, P.J. and Andronache, C. (2008) An Empirical Parameterization of Heterogeneous Ice Nucleation for Multiple Chemical Species of Aerosol. Journal of the Atmospheric Sciences, 65, 2757-2783. https://doi.org/10.1175/2007JAS2546.1
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 of the United States of America, 107, 11217-11222. https://doi.org/10.1073/pnas.0910818107
Maters, E.C., Dingwell, D.B., Cimarelli, C., Müller, D., Whale, T.F. and Murray, B.J. (2019) The Importance of Crystalline Phases in Ice Nucleation by Volcanic Ash. Atmospheric Chemistry and Physics, 19, 5451-5465. https://doi.org/10.5194/acp-19-5451-2019
Atkinson, J.D., Murray, B.J., Woodhouse, M.T., Whael, T.F., Baustian, K.J. and Carslaw, K.S. (2013) The Importance of Feldspar for Ice Nucleation by Mineral Dust in Mixed-Phase Clouds. Nature, 498, 355-358. https://doi.org/10.1038/nature12278
Kiselev, A., Bachmann, F., Pedevilla, P., Cox, S.J., Michaelides, A., Gerthsen, D. and Leisner, T. (2017) Active Sites in Heterogeneous Ice Nucleation—The Example of K-Rich Feldspars. Science, 355, 367-371. https://doi.org/10.1126/science.aai8034
Paramonov, M., David, R.O., Kretzschmar, R. and Kanji, Z.A. (2018) A Laboratory Investigation of the Ice Nucleation Efficiency of Three Types of Mineral and Soil Dust. Atmospheric Chemistry and Physics, 18, 16515-16536. https://doi.org/10.5194/acp-18-16515-2018
Si, M., Irish, V.E., Mason, R.H., Vergara-Temprado, J., Hanna, S.J., Ladino, L.A., Yakobi-Hancock, J.D., Schiller, C.L., Wentzell, J.J.B., Abbatt, J.P.D., Carslaw, K.S., Murray, B.J. and Bertram, A.K. (2018) Ice Nucleating Ability of Aerosol Particles and Possible Sources at Three Coastal Marine Sites. Atmospheric Chemistry and Physics, 18, 15669-15685. https://doi.org/10.5194/acp-18-15669-2018
Porter, G.C.E., Sikora, S.N.F., Adams, M.P., Proske, U., Harrison, A.D., Tarn, M.D., Brooks, I.M. and Murray, B.J. (2020) Resolving the Size of Ice-Nucleating Particles with a Balloon Deployable Aerosol Sampler: The SHARK. Atmospheric Measurement Techniques, 13, 2905-2921. https://doi.org/10.5194/amt-13-2905-2020
Reicher, N., Budke, C., Eickhoff, L., Raveh-Rubin, S., Kaplan-Ashiri, I., Koop, T. and Rudich, Y. (2019) Size-Dependent Ice Nucleation by Airborne Particles during Dust Events in the Eastern Mediterranean. Atmospheric Chemistry and Physics, 19, 11143-11158. https://doi.org/10.5194/acp-19-11143-2019
Yadav, S., Venezia, R.E., Paerl, R.W. and Petters, M.D. (2019) Characterization of Ice-Nucleating Particles over Northern India. Journal of Geophysical Research, 124, 10,467-10,482. https://doi.org/10.1029/2019JD030702
Zolles, T., Burkart, J., Häusler, T., Pummer, B., Hitzenberger, R. and Grothe, H. (2015) Identification of Ice Nucleation Active Sites on Feldspar Dust Particles. The Journal of Physical Chemistry A, 119, 2692-2700. https://doi.org/10.1021/jp509839x
Hiranuma, N., Hoffmann, N., Kiselev, A., Dreyer, K., Zhang, K., Kulkarni, G., Koop, T. and Möhler, O. (2014) Influence of Surface Morphology on the Immersion Mode Ice Nucleation Efficiency of Hematite Particles. Atmospheric Chemistry and Physics, 14, 2315-2324. https://doi.org/10.5194/acp-14-2315-2014
Boose, Y., Welti, A., Atkinson, J., Ramelli, F., Danielczok, A., Bingemer, H.G., Plötze, M., Sierau, B., Kanji, Z.A. and Lohmann, U. (2016) Heterogeneous Ice Nucleation on Dust Particles Sourced from Nine Deserts Worldwide—Part 1: Immersion Freezing. Atmospheric Chemistry and Physics, 16, 15075-15095. https://doi.org/10.5194/acp-16-15075-2016
Steinke, I., Hoose, C., Möhler, O., Connolly, P. and Leisner, T. (2015) A New Temperature- and Humidity-Dependent Surface Site Density Approach for Deposition Ice Nucleation. Atmospheric Chemistry and Physics, 15, 3703-3717. https://doi.org/10.5194/acp-15-3703-2015
Hartmann, S., Wex, H., Clauss, T., Augustin-Bauditz, S., Niedermeier, D., Rosch, M. and Stratmann, F. (2016) Immersion Freezing of Kaolinite: Scaling with Particle Surface Area. Journal of the Atmospheric Sciences, 73, 263-278. https://doi.org/10.1175/JAS-D-15-0057.1
Möhler, O., Field, P.R., Connolly, P., Benz, S., Saathoff, H., Schnaiter, M., Wagner, R., Cotton, R., Krämer, M., Mangold, A. and Heymsfield, A.J. (2006) Efficiency of the Deposition Mode Ice Nucleation on Mineral Dust Particles. Atmospheric Chemistry and Physics, 6, 3007-3021. https://doi.org/10.5194/acp-6-3007-2006
DeMott, P.J., Sassen, K., Poellot, M.R., Baumgardner, D., Rogers, D.C., Brooks, S.D., Prenni, A.J. and Kreidenweis, S.M. (2003) African Dust Aerosols as Atmospheric Ice Nuclei. Geophysical Research Letters, 30, 1732. https://doi.org/10.1029/2003GL017410
Welti, A., Lüönd, F., Stetzer, O. and Lohmann, U. (2009) Influence of Particle Size on the Ice Nucleating Ability of Mineral Dust. Atmospheric Chemistry and Physics, 9, 6705-6715. https://doi.org/10.5194/acp-9-6705-2009
Kulkarni, G., Dobbie, S. and McQuaid, J.B. (2009) A New Thermal Gradient Ice Nucleation Diffusion Chamber Instrument: Design, Development and First Results Using Saharan Mineral Dust. Atmospheric Measurement Techniques, 2, 221-229. https://doi.org/10.5194/amt-2-221-2009
Kulkarni, G. and Dobbie, S. (2010) Ice Nucleation Properties of Mineral Dust Particles: Determination of Onset RHi, IN Active Fraction, Nucleation Time-Lag, and the Effect of Active Sites on Contact Angles. Atmospheric Chemistry and Physics, 10, 95-105. https://doi.org/10.5194/acp-10-95-2010
Soo, J.C., Monaghan, K., Lee, T., Kashon, M. and Harper, M. (2016) Air Sampling Filtration Media: Collection Efficiency for Respirable Size-Selective Sampling. Aerosol Science and Technology, 50, 76-87. https://doi.org/10.1080/02786826.2015.1128525
Kenny, L.C. and Gussman, R.A. (1997) Characterisation and Modelling of a Family of Cyclone Aerosol Preseparators. Journal of Aerosol Science, 28, 677-688. https://doi.org/10.1016/S0021-8502(96)00455-7
Kenny, L.C., Gussman, R. and Meyer, M. (2000) Development of a Sharp-Cut Cyclone for Ambient Aerosol Monitoring Applications. Aerosol Science and Technology, 32, 338-358. https://doi.org/10.1080/027868200303669
Stevenson, C.M. (1968) An Improved Milllipore Filter Technique for Measuring the Concentrations of Freezing Nuclei in the Atmosphere. Quarterly Journal of the Royal Meteorological Society, 94, 35-44. https://doi.org/10.1002/qj.49709439905
Bigg, E.K. (1990) Measurement of Concentrations of Natural Ice Nuclei. Atmospheric Research, 25, 397-408. https://doi.org/10.1016/0169-8095(90)90024-7
Belosi, F., Rinaldi, M., DeCesari, S., Tarozzi, A., Nicosia, A. and Santachiara, G. (2017) Ground Level Ice Nuclei Particle Measurements Including Saharan Dust Events at a Po Valley Rural Site (San Pietro Capofiume, Italy). Atmospheric Research, 186, 116-126. https://doi.org/10.1016/j.atmosres.2016.11.012
DeMott, P.J., Möhler, O., Cziczo, D.J., Hiranuma, N., Petters, M.D., Petters, S.S., H.G., Belosi, F., Bingemer, H.G., Brooks, S.D., Budke, C., et al. (2018) The Fifth International Workshop on Ice Nucleation Phase 2 (FIN-02): Laboratory Intercomparison of Ice Nucleation Measurements. Atmospheric Measurement Techniques, 11, 6231-6257. https://doi.org/10.5194/amt-11-6231-2018
Rinaldi, M., Nicosia, A., Santachiara, G., Piazza, M., Paglione, M., Gilardoni, S., Sandrini, S., Cristofanelli, P., Marinoni, A., Bonasoni, P., Facchini, M.C. and Belosi, F. (2019) Ground Level Ice Nucleating Particles Measurements at Capo Granitola, a Mediterranean Coastal Site. Atmospheric Research, 219, 57-64. https://doi.org/10.1016/j.atmosres.2018.12.022
Nicosia, A., Piazza, M., Santachiara, G. and Belosi, F. (2016) Heterogeneous Nucleation of Ice in the Atmosphere. 7th Young Researcher Meeting, Journal of Physics: Conference Series, 841, Article ID: 012028. https://doi.org/10.1088/1742-6596/841/1/012028
Mizuno, H. and Fukuta, N. (1995) Natural Ice Nucleus Measurement under High Supersaturation. Journal of the Meteorological Society of Japan, 73, 1115-1122. https://doi.org/10.2151/jmsj1965.73.6_1115
DeMott, P.J., Mohler, O., Stetzer, O., Vali, G., Levin, Z., et al. (2011) Resurgence in Ice Nuclei Measurement Research. Bulletin of the American Meteorological Society, 92, 1623-1635. https://doi.org/10.1175/2011BAMS3119.1
Kulkarni, G., Hiranuma, N., Möhler, O., Höhler, K., China, S., Cziczo, D.J. and DeMott, P.J. (2020) A New Method for Operating a Continuous-Flow Diffusion Chamber to Investigate Immersion Freezing: Assessment and Performance Study. Atmospheric Measurement Techniques, 13, 6631-6643. https://doi.org/10.5194/amt-13-6631-2020
Rinaldi, M., Santachiara, G., Nicosia, A., Piazza, M., Decesari, S.S., Gilardoni, M., Paglione, P., Cristofanelli, A., Marinoni, P., Bonasoni, F., et al. (2017) Atmospheric Ice Nucleating Particle Measurements at the High Mountain Observatory Mt. Cimone (2165 m a.s.l., Italy). Atmospheric Environment, 171, 173-180. https://doi.org/10.1016/j.atmosenv.2017.10.027
McCluskey, C.S., Ovadnevaite, J., Rinaldi, M., Atkinson, J., Belosi, F., Ceburnis, D., Marullo, S., Hill, T.C.J., Lohmann, U., Kanji, Z.A., O’Dowd, C., Kreidenweis, S.M. and DeMott, P.J. (2018) Marine and Terrestrial Organic Ice-Nucleating Particles in Pristine Marine to Continentally Influenced Northeast Atlantic Air Masses. Journal of Geophysical Research, 123, 6196-6212. https://doi.org/10.1029/2017JD028033
Lüond, F., Stetzer, O., Welti, A. and Lohmann, U. (2010) Experimental Study on the Ice Nucleation Ability of Size-Selected Kaolinite Particles in the Immersion Mode. Journal of Geophysical Research, 115, D14201. https://doi.org/10.1029/2009JD012959
David, R.O., Cascajo-Castresana, M., Brennan, K.P., Rösch, M., Els, N., Werz, J., Weichlinger, V., Boynton, L.S., Bogler, S., Borduas-Dedekind, N., Marcolli, C. and Kanji, Z.A. (2019) Pore Condensation and Freezing Is Responsible for Ice Formation below Water Saturation for Porous Particles. Proceedings of the National Academy of Sciences of the United States of America, 116, 8184-8189. https://doi.org/10.1073/pnas.1813647116
Campbell, J.M. and Christenson, H.K. (2018) Nucleation- and Emergence-Limited Growth of Ice from Pores. Physical Review Letters, 120, Article ID: 165701. https://doi.org/10.1103/PhysRevLett.120.165701