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Can molecular simulations reliably compare homogeneous and heterogeneous ice nucleation?

Published version
Peer-reviewed

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Authors

Atherton, Dominic 
Michaelides, Angelos  ORCID logo  https://orcid.org/0000-0002-9169-169X
Cox, Stephen J 

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 Ih. 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.

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Keywords

cond-mat.stat-mech, cond-mat.stat-mech

Journal Title

Journal of Chemical Physics

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Journal ISSN

0021-9606
1089-7690

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Publisher

American Institute of Physics
Sponsorship
Royal Society University Research Fellowship
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