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Atmospheric ice nucleation

Nature Reviews Physics volume 5, pages 203–217 (2023)Cite this article

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Abstract

Atmospheric ice nucleation is crucial for global precipitation and affects the structure, lifetime and reflectivity of clouds, thereby impacting climate. Ice nucleates in various ways from aerosol particles, termed ice-nucleating particles, over an extensive temperature and humidity range. Quantifying the kinetic and thermodynamic regimes of nucleation is necessary to relate fundamental physics to theoretically based predictions of ice formation for implementation in cloud and climate models. We review how the molecular picture of ice nucleation has advanced in recent years and consequential impacts on the interpretation and parameterization of ice nucleation. Advances include the role of interfacial free energy and pressure on ice nucleation rates, mobility regions of water that generate the critical ice nucleus, classical and non-classical pathways of nucleation, the type of ice polymorph that forms, the impact of solutes on freezing and the role of nanopores as surface features promoting ice nucleation. We also introduce currently debated and evaluated freezing parameterizations for application in model environments. Finally, we outline what we believe are the current needs for improving predictive understanding of ice nucleation.

Key points

  • Homogeneous ice nucleation is affected by pressure, temperature and solute strength and is predictable using water activity. However, research into the dynamics of water molecules and ice germ physicochemical properties is needed to better constrain nucleation parameters.

  • Heterogeneous ice nucleation from nano-sized confinements can lead to the formation of cubic ice or stacking disordered ice. Which ice phase forms impacts nucleation rate derivations owing to differences in the free energy of formation of the critical ice nucleus.

  • The water activity criterion is a thermodynamic predictor of kinetic ice nucleation for both homogeneous and heterogeneous ice nucleation. It can be applied to describe immersion freezing and reveals a direct relationship to the water structure at the ice-nucleating particle surface or the contact angle, allowing for interpretation of the interaction between the ice-nucleating particle and the critical ice nucleus.

  • Water in nanometre-sized confinements at the surface of aerosol particles can serve as the origin of ice formation. Pore condensation freezing in nanometre-sized pores can explain ice formation by particles in the absence of a coverage of liquid water.

  • Although nucleation is a stochastically driven process, an unambiguous evaluation of the underlying physical processes from experimental data is challenging. This is because it is difficult to obtain nanoscale control of the physicochemical properties of the nucleating substrate while observing a significant number of ice nucleation events.

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Fig. 1: Homogeneous and heterogeneous ice nucleation pathways superimposed on the ice–water phase diagram as a function of temperature, relative humidity and water activity.
Fig. 2: Homogeneous ice nucleation rate coefficients compared with nucleation rate expressions as a function of degree of supercooling.
Fig. 3: The kinetic pathways of heterogeneous ice nucleation.
Fig. 4: Heterogeneous nucleation of cubic ice on substrates and in nanopores.
Fig. 5: Contact angle between the critical ice nucleus and a biological ice-nucleating surface, as a function of the water activity criterion.
Fig. 6: The role of substrate surface features such as pores and cavities in heterogeneous ice nucleation.
Fig. 7: Determination of immersion freezing kinetics.

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Acknowledgements

This study was supported by the Atmospheric System Research Program and Atmospheric Radiation Measurement Program sponsored by the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, Climate and Environmental Sciences Division, grant DE-SC0021034. The authors are grateful to J. Aller for careful proofreading of the initial manuscript.

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  1. School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY, USA

    Daniel A. Knopf

  2. Paul Scherrer Institute, Laboratory for Environmental Chemistry, Villigen, Switzerland

    Peter A. Alpert

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Knopf, D.A., Alpert, P.A. Atmospheric ice nucleation. Nat Rev Phys 5, 203–217 (2023). https://doi.org/10.1038/s42254-023-00570-7

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