It has recently been shown that incident particles, neutrons, can initiate the freezing in a supercooled water volume. This new finding may have ramifications for the interpretation of both experimental data on the nucleation of laboratory samples of supercooled water and perhaps more importantly on the interpretation of ice nucleation involved in cloud physics. For example, if some fraction of the cloud nucleation previously attributed to dust, soot, or aerosols has been caused by cosmogenic neutrons, fresh consideration is required in the context of climate models. Moreover, as cosmogenic neutrons, most being muon-induced, have much greater flux at high latitudes, estimates of ice nucleates in these regions may be larger than required to accurately model cloud and condensation properties. This discrepancy has been pointed out in IPCC reports. Our paper discusses the connection between the new concept of neutrons nucleating supercooled water and the need for a new source of nucleation in high latitude clouds, ideally causing others to review current data, or to analyse future data with this idea in mind.
Szydagis, M., Levy, C., Huang, Y., Kamaha, A.C., Knight, C.C., Rischbieter, G.R.C. and Wilson, P.W. (2021) Demonstration of Neutron Radiation-Induced Nucleation of Supercooled Water. Physical Chemistry Chemical Physics , 23, 13440-13466. https://doi.org/10.1039/D1CP01083B
Szydagis, M., Levy, C., Bolotnikov, A.E., Diwan, M., Homenides, G., Kamaha, A., Martin, J., Rosero, R. and Yeh, M. (2024) A Simple Model of the Energy Threshold for Snowball Chambers. Universe , 10, Article 81. https://doi.org/10.3390/universe10020081
Koop, T. and Murray, B.J. (2016) A Physically Constrained Classical Description of the Homogeneous Nucleation of Ice in Water. The Journal of Chemical Physics , 145, Article 211915. https://doi.org/10.1063/1.4962355
Hegg, D.A. and Baker, M.B. (2009) Nucleation in the Atmosphere. Reports on Progress in Physics , 72, Article 056801. https://doi.org/10.1088/0034-4885/72/5/056801
Harrison, R.G. and Carslaw, K.S. (2003) Ion-Aerosol-Cloud Processes in the Lower Atmosphere. Reviews of Geophysics , 41, Article 1012. https://doi.org/10.1029/2002RG000114
Leisner, T., Duft, D., Möhler, O., et al. (2013) Laser-Induced Plasma Cloud Interaction and Ice Multiplication under Cirruc Cloud Conditions. Proceedings of the N a tional Academy of Sciences of the United States of America , 110, 10106-10110. https://doi.org/10.1073/pnas.1222190110
Murray, B.J., O’Sullivan, D., Atkinson J.D. and Webb, M.E. (2012) Ice Nucleation by Particles Immersed in Supercooled Cloud Droplets. Chemical Society Reviews , 41, 6519-6554. https://doi.org/10.1039/c2cs35200a
Curry, J.A. and Khvorostyanov, V.I. (2012) Assessment of Some Parameterizations of Heterogeneous Ice Nucleation in Cloud and Climate Models. Atmospheric Ch e mistry and Physics , 12, 1151-1172. https://doi.org/10.5194/acp-12-1151-2012
Heneghan, A., Wilson, P.W., Wang, G. and Haymet, A.D.J. (2001) Liquid-to-Crystal Nucleation: Automated Lag-Time Apparatus to Study Supercooled Liquids. The Journal of Chemical Physics , 115, 7599-7608. https://doi.org/10.1063/1.1407290
Herbert, R.J., Murray, B.J., Whale, T.F., Dobbie, S.J. and Atkinson, J.D. (2014) Representing Time-Dependent Freezing Behaviour in Immersion Mode Ice Nucleation. Atmospheric Chemistry and Physics , 14, 8501-8520. https://doi.org/10.5194/acp-14-8501-2014
Wilson, P.W. and Haymet, A.D.J. (2012) The Spread of Nucleation Temperatures of a Sample of Supercooled Liquid Is Independent of the Average Nucleation Temperature. The Journal of Physical Chemistry B , 116, 13472-13475. https://doi.org/10.1021/jp308177b
Stan, C.A., Schneider, G.F., Shevkoplyas, S.S., Hashimoto, M., Ibanescu, M., Wiley, B.J. and Whitesides, G.M. (2009) A Microfluidic Apparatus for the Study of Ice Nucleation in Supercooled Water Drops. Lab on a Chip , 9, 2293-2305. https://doi.org/10.1039/b906198c
Möhler, O., Adams, M., Lacher, L., et al. (2021) The Portable Ice Nucleation Experiment (PINE): A New Online Instrument for Laboratory Studies and Automated Long-Term Field Observations of Ice-Nucleating Particles. Atmospheric Measur e ment Techniques , 14, 1143-1166. https://doi.org/10.5194/amt-14-1143-2021
Hawker, R.E., Miltenberger, A.K., Wilkinson, J.M., Hill, A.A., Shipway, B.J., Cui, Z., Cotton, R.J., Carslaw, K.S., Field, P.R. and Murray, B.J. (2021) The Temperature Dependence of Ice-Nucleating Particle Concentrations Affects the Radiative Properties of Tropical Convective Cloud Systems. Atmospheric Chemistry and Physics , 21, 5439-5461. https://doi.org/10.5194/acp-21-5439-2021
Wilson, T., Ladino, L.A., Alpert, P.A., et al. (2015) A Marine Biogenic Source of Atmospheric Ice-Nucleating Particles. Nature , 525, 234-238. https://doi.org/10.1038/nature14986
Dunne, E.M., et al. (2016) Global Atmospheric Particle Formation from CERN CLOUD Measurements. Science , 354, 1119-1124. https://doi.org/10.1126/science.aaf2649
Yu, F. (2004) Formation of Large NAT Particles and Denitrification in Polar Stratosphere: Possible Role of Cosmic Rays and Effect of Solar Activity. Atmospheric Chemistry and Physics , 4, 2273-2283. https://doi.org/10.5194/acp-4-2273-2004
Seeley, L.H., Seidler G.T. and Dash, J.G. (2001) Laboratory Investigation of Possible Ice Nucleation by Ionising Radiation in Pure Water at Tropospheric Temperatures. Journal of Geophysical Research : Atmospheres , 106, 3033-3036. https://doi.org/10.1029/2000JD900670
Dilillo, L., Wrobel, F., Galliere, J.-M. and Saigné, F. (2009) Neutron Detection through an SRAM-Based Test Bench. 2009 3 rd International Workshop on Advances in sensors and Interfaces , Trani, 25-26 June 2009, 64-69. https://doi.org/10.1109/IWASI.2009.5184769
Kole, M., Chauvin, M., Fukazawa, Y., Fukuda, K., Ishizu, S., Jackson, M., Kamae, T., Kawaguchi, N., Kawano, T., Kiss, M., Mikhalev, V., Moretti, E., Pearce, M., Rydström, S., Takahashi, H. and Yanagida, T. (2015) Neutron Background Detection for a Hard X-Ray Balloon-Borne Polarimeter. Proceedings of Technology and Instr u mentation in Particle Physics 2014, Amsterdam, 2-6 June 2014, 1-8. https://doi.org/10.22323/1.213.0135
Goldhagen, P., Clem, J.M. and Wilson, J.W. (2004) The Energy Spectrum of Cosmic-Ray Induced Neutrons Measured on an Airplane over a Wide Range of Altitude and Latitude. Radiation Protection Dosimetry , 110, 387-392. https://doi.org/10.1093/rpd/nch216
Kowatari, M., Ohta, Y., Satoh, S., Nagaoka, K., Abukawa, J. and Nakamura, T. (2007) Evaluation of Geomagnetic Latitude Dependence of the Cosmic-Ray Induced Environmental Neutrons in Japan. Journal of Nuclear Science and Technology , 44, 114-120. https://doi.org/10.1080/18811248.2007.9711264
Cecchini, S. and Sioli, M. (1998) Cosmic Ray Muon Physics. Proceedings of the Fifth School on Non - Accelerator Particle Astrophysics , Trieste, 29 June-10 July 1998, 1-18.
Pittock, A.B. (1978) A Critical Look at Long-Term Sun-Weather Relationships. R e views of Geophysics , 16, 400-420. https://doi.org/10.1029/RG016i003p00400
Tinsley, B.A. and Deen, G.W. (1991) Apparent Tropospheric Response to MeV-GeV Particle Flux Variations: A Connection via Electro-Freezing of Supercooled Water in High-Level Clouds? Journal of Geophysical Research : Atmospheres , 96, 22283-22296. https://doi.org/10.1029/91JD02473
Varshneya, N.C. (1969) Detecting Radiation with a Supercooled Liquid. Nature , 223, 826-827. https://doi.org/10.1038/223826a0
Varshneya, N.C. (1971) Theory of Radiation Detection through Supercooled Liquid. Nuclear Instruments and Methods , 92, 147-150. https://doi.org/10.1016/0029-554X(71)90237-0
Detwiler, A. and Vonnegut, B. (1980) Initiation of Freezing in Supercooled Cloud Droplets by Ionising Radiation. Journal of the Atmospheric Sciences , 37, 479-780. https://doi.org/10.1175/1520-0469(1980)037 2.0.CO;2
Behnke, E., et al . (2017) Final Results of the PICASSO Dark Matter Search Experiment. Astroparticle Physics , 90, 85-92. https://doi.org/10.1016/j.astropartphys.2017.02.005
Rojdev, K., Koontz, S., Reddell, B., Atwell, W. and Boeder, P. (2015) Comparison and Validation of FLUKA and HZETRN as Tools for Investigating the Secondary Neutron Production in Large Space Vehicles. AIAA SPACE 2015 Conference and Exposition , Pasadena, California, 31 August-2 September 2015. https://doi.org/10.2514/6.2015-4601
Zanini, A., Ongaro, C., Durisi, E., Visca, L., De Agostini, S., Fasolo, F., Pelliccioni, M. and Saavedra, O. (2003) Differential Neutron Flux in Atmosphere at Various Geophysical Conditions. 28 th International Cosmic Ray Conference , Tsukuba, July 31-August 7, 2003, 4291-4294.
Leray, J.L. (2007) Effects of Atmospheric Neutrons on Devices, at Sea Level and in Avionics Embedded Systems. Microelectronics Reliability , 47, 1827-1835. https://doi.org/10.1016/j.microrel.2007.07.101
Murray, B.J., Carslaw, K.S. and Field, P.R. (2012) Opinion: Cloud-Phase Climate Feedback and the Importance of Ice-Nucleating Particles. Atmospheric Chemistry and Physics , 21, 665-679. https://doi.org/10.5194/acp-21-665-2021
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 Atmospheric Sciences , 65, 2757-2783. https://doi.org/10.1175/2007JAS2546.1
Seifert, P., et al. (2009) Saharan Dust and Heterogeneous Ice Formation: Eleven Years of Cloud Observations at a Central European EARLINET Site. Journal of Geophysical Research : Atmospheres , 115. https://doi.org/10.1029/2009JD013222
Kanji, Z.A., Ladino, L.A., Wex, H., Boose, Y., Burkert-Kohn, M., Cziczo, D.J. and Krämer, M. (2017) Overview of Ice Nucleating Particles. Meteorological Mon o graphs , 58, 1.1-1.33. https://doi.org/10.1175/AMSMONOGRAPHS-D-16-0006.1
Tabazadeh, A., Djikaev, Y.S. and Reiss, H. (2002) Surface Crystallisation of Supercooled Water in Clouds. Proceedings of the National Academy of Sciences of the United States of America , 99, 15873-15878. https://doi.org/10.1073/pnas.252640699
Hoose, C., Kristjánsson, J.E., Chen, J.-P. and Hazra, A. (2010) A Classical-Theory-Based Parameterization of Heterogeneous Ice nucleation by Mineral Dust, Soot, and Biological Particles in a Global Climate Model. Journal of the A t mospheric Sciences , 67, 2483-2503. https://doi.org/10.1175/2010JAS3425.1
Kanitz, T., Seifert, P., Ansmann, A., Engelmann, R., Althausen, D., Casiccia, C. and Rohwer, E.G. (2011) Contrasting the Impact of Aerosols at Northern and Southern Midlatitudes on Heterogeneous Ice Formation. Geophysical Research Letters , 38. https://doi.org/10.1029/2011GL048532
Burrows, S.M., Hoose, C., Pöschl, U. and Lawrence, M.G. (2013) Ice Nuclei in Marine Air: Biogenic Particles or Dust? Atmospheric Chemistry and Physics , 13, 245-267. https://doi.org/10.5194/acp-13-245-2013
Alpert, P.A., Aller, J.Y. and Knopf, D.A. (2011) Initiation of the Ice Phase by Marine Biogenic Surfaces in Supersaturated Gas and Supercooled Aqueous Phases. Physical Chemistry Chemical Physics , 13, 19882-19894. https://doi.org/10.1039/c1cp21844a
Alpert, P.A., Aller, J.Y. and Knopf, D.A. (2011) Ice Nucleation from Aqueous NaCl Droplets with and without Marine Diatoms. Atmospheric Chemistry and Physics , 11, 5539-5555. https://doi.org/10.5194/acp-11-5539-2011
Junge, K. and Swanson, B.D. (2008) High-Resolution Ice Nucleation Spectra of Sea-Ice Bacteria: Implications for Cloud Formation and Life in Frozen Environments. Biogeosciences , 5, 865-873. https://doi.org/10.5194/bg-5-865-2008
DeMott, P.J. and Prenni, A.J. (2010) New Directions: Need for Defining the Numbers and Sources of Biological Aerosols Acting as Ice Nuclei. Atmospheric Env i ronment , 44, 1944-1945. https://doi.org/10.1016/j.atmosenv.2010.02.032
DeMott, P.J., and Rogers, D.C. (1990) Freezing Nucleation Rates of Dilute Solution Droplets Measured between −30˚C and −40˚C in Laboratory Simulations of Natural Clouds. Journal of the Atmospheric Sciences , 47, 1056-1064. https://doi.org/10.1175/1520-0469(1990)047 2.0.CO;2
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, 11217-1222. https://doi.org/10.1073/pnas.0910818107
Malgin, A.S. (2017) On the Energy Spectrum of Cosmogenic Neutrons. Journal of Experimental and Theoretical Physics , 125, 728-740. https://doi.org/10.1134/S1063776117100089
Owens, M. (2021) Department of Meteorology, University of Reading, Personal Communication.
Hoyle, C.R., Luo, B.P. and Peter, T. (2005) The Origin of High Ice Crystal Number Densities in Cirrus Clouds. Journal of the Atmospheric Sciences , 62, 2568-2579. https://doi.org/10.1175/JAS3487.1
Goldhagen, P., Reginatto, M., Kniss, T., Wilson, J.W., Singleterry, R.C., Jones, I.W. and Van Steveninck, W. (2002) Measurement of the Energy Spectrum of Cosmic-Ray Induced Neutrons aboard an ER-2 High-Altitude Airplane. Nuclear Instr u ments and Methods in Physics Research Section A : Accelerators , Spectrometers , Detectors and Associated Equipment , 476, 42-51. https://doi.org/10.1016/S0168-9002(01)01386-9
Cieslak, M.J., Gamage, K.A.A. and Glover, R. (2019) Critical Review of Scintillating Crystals for Neutron Detection, Crystals , 9, Article 480. https://doi.org/10.3390/cryst9090480
Li, J., Smith, D.W., Fityus, S.G. and Sheng, D. (2003) Numerical Analysis of Neutron Moisture Prove Measurements. International Journal of Geomechanics , 3, 11-20. https://doi.org/10.1061/(ASCE)1532-3641(2003)3:1(11)