Can molecular simulations reliably compare homogeneous and heterogeneous ice nucleation?
Publication Date
2022-04-28Journal Title
Journal of Chemical Physics
ISSN
0021-9606
Publisher
American Institute of Physics
Type
Article
Metadata
Show full item recordCitation
Atherton, D., Michaelides, A., & Cox, S. J. (2022). Can molecular simulations reliably compare homogeneous and heterogeneous
ice nucleation?. Journal of Chemical Physics https://doi.org/10.1063/5.0085750
Abstract
In principle, the answer to the posed titular question is undoubtedly 'yes.'
But in practice, requisite reference data for homogeneous systems have been obtained with a treatment of intermolecular interactions that is different from that typically employed for heterogeneous systems. In this article, we assess the impact of the choice of truncation scheme when comparing water in homogeneous and inhomogeneous environments. Specifically, we use explicit free energy calculations and a simple mean field analysis to demonstrate that using the 'cut-and-shift' version of the Lennard-Jones potential (common to most simple point charge models of water) results in a systematic increase in the melting temperature of ice I$_{\rm h}$. In addition, by drawing an analogy between a change in cutoff and a change in pressure, we use existing literature data for homogeneous ice nucleation at negative pressures to suggest that
enhancements due to heterogeneous nucleation may have been overestimated by several orders of magnitude.
Relationships
Is supplemented by: https://doi.org/10.17863/CAM.80092
Sponsorship
Royal Society University Research Fellowship
Identifiers
External DOI: https://doi.org/10.1063/5.0085750
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