Volume 249, 2024

The limit of macroscopic homogeneous ice nucleation at the nanoscale

Abstract

Nucleation in small volumes of water has garnered renewed interest due to the relevance of pore condensation and freezing under conditions of low partial pressures of water, such as in the upper troposphere. Molecular simulations can in principle provide insight on this process at the molecular scale that is challenging to achieve experimentally. However, there are discrepancies in the literature as to whether the rate in confined systems is enhanced or suppressed relative to bulk water at the same temperature and pressure. In this study, we investigate the extent to which the size of the critical nucleus and the rate at which it grows in thin films of water are affected by the thickness of the film. Our results suggest that nucleation remains bulk-like in films that are barely large enough accommodate a critical nucleus. This conclusion seems robust to the presence of physical confining boundaries. We also discuss the difficulties in unambiguously determining homogeneous nucleation rates in nanoscale systems, owing to the challenges in defining the volume. Our results suggest any impact on a film’s thickness on the rate is largely inconsequential for present day experiments.

Graphical abstract: The limit of macroscopic homogeneous ice nucleation at the nanoscale

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Article information

Article type
Paper
Submitted
15 mai 2023
Accepted
20 jun 2023
First published
22 jun 2023
This article is Open Access
Creative Commons BY license

Faraday Discuss., 2024,249, 210-228

The limit of macroscopic homogeneous ice nucleation at the nanoscale

J. A. Hayton, M. B. Davies, T. F. Whale, A. Michaelides and S. J. Cox, Faraday Discuss., 2024, 249, 210 DOI: 10.1039/D3FD00099K

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