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Abstract. Heterogeneous ice nucleation is thought to be the primary pathway for the formation of ice in mixed-phase clouds, with the number of active ice-nucleating particles (INPs) increasing rapidly with decreasing temperature. Here, molecular-dynamics simulations of heterogeneous ice nucleation demonstrate that the ice nucleation rate is also sensitive to pressure and that negative pressure within supercooled water shifts freezing temperatures to higher temperatures. Negative pressure, or tension, occurs naturally in water capillary bridges and pores and can also result from water agitation. Capillary bridge simulations presented in this study confirm that negative Laplace pressure within the water increases heterogeneous-freezing temperatures. The increase in freezing temperatures with negative pressure is approximately linear within the atmospherically relevant range of 1 to −1000 atm. An equation describing the slope depends on the latent heat of freezing and the molar volume difference between liquid water and ice. Results indicate that negative pressures of −500 atm, which correspond to nanometer-scale water surface curvatures, lead to a roughly 4 K increase in heterogeneous-freezing temperatures. In mixed-phase clouds, this would result in an increase of approximately 1 order of magnitude in active INP concentrations. The findings presented here indicate that any process leading to negative pressure in supercooled water may play a role in ice formation, consistent with experimental evidence of enhanced ice nucleation due to surface geometry or mechanical agitation of water droplets. This points towards the potential for dynamic processes such as contact nucleation and droplet collision or breakup to increase ice nucleation rates through pressure perturbations.
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Is Contact Nucleation Caused by Pressure Perturbation?
The reason why ice nucleation is more efficient by contact nucleation than by immersion nucleation has been elusive for over half a century. Six proposed mechanisms are summarized in this study. Among them, the pressure perturbation hypothesis, which arose from recent experiments, can qualitatively explain nearly all existing results relevant to contact nucleation. To explore the plausibility of this hypothesis in a more quantitative fashion and to guide future investigations, this study assessed the magnitude of pressure perturbation needed to cause contact nucleation and the associated spatial scales. The pressure perturbations needed were estimated using measured contact nucleation efficiencies for illite and kaolinite, obtained from previous experiments, and immersion freezing temperatures, obtained from well-established parameterizations. Pressure perturbations were obtained by assuming a constant pressure perturbation or a Gaussian distribution of the pressure perturbation. The magnitudes of the pressure perturbations needed were found to be physically reasonable, being achievable through possible mechanisms, including bubble formation and breakup, Laplace pressure arising from the distorted contact line, and shear. The pressure perturbation hypothesis provides a physically based and experimentally constrainable foundation for parameterizing contact nucleation that may be useful in future cloud-resolving models.
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- Award ID(s):
- 1639868
- PAR ID:
- 10130832
- Date Published:
- Journal Name:
- Atmosphere
- Volume:
- 11
- Issue:
- 1
- ISSN:
- 2073-4433
- Page Range / eLocation ID:
- 1
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.3390/atmos11010001
