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Homogeneous SPC/E water nucleation in large molecular dynamics simulations


Angélil, Raymond; Diemand, Jürg; Tanaka, Kyoko K; Tanaka, Hidekazu (2015). Homogeneous SPC/E water nucleation in large molecular dynamics simulations. Journal of Chemical Physics, 143(6):064507.

Abstract

We perform direct large molecular dynamics simulations of homogeneous SPC/E water nucleation, using up to ˜ 4 ṡ 106 molecules. Our large system sizes allow us to measure extremely low and accurate nucleation rates, down to ˜ 1019 cm-3 s-1, helping close the gap between experimentally measured rates ˜ 1017 cm-3 s-1. We are also able to precisely measure size distributions, sticking efficiencies, cluster temperatures, and cluster internal densities. We introduce a new functional form to implement the Yasuoka-Matsumoto nucleation rate measurement technique (threshold method). Comparison to nucleation models shows that classical nucleation theory over-estimates nucleation rates by a few orders of magnitude. The semi-phenomenological nucleation model does better, under-predicting rates by at worst a factor of 24. Unlike what has been observed in Lennard-Jones simulations, post-critical clusters have temperatures consistent with the run average temperature. Also, we observe that post-critical clusters have densities very slightly higher, ˜ 5%, than bulk liquid. We re-calibrate a Hale-type J vs. S scaling relation using both experimental and simulation data, finding remarkable consistency in over 30 orders of magnitude in the nucleation rate range and 180 K in the temperature range.

Abstract

We perform direct large molecular dynamics simulations of homogeneous SPC/E water nucleation, using up to ˜ 4 ṡ 106 molecules. Our large system sizes allow us to measure extremely low and accurate nucleation rates, down to ˜ 1019 cm-3 s-1, helping close the gap between experimentally measured rates ˜ 1017 cm-3 s-1. We are also able to precisely measure size distributions, sticking efficiencies, cluster temperatures, and cluster internal densities. We introduce a new functional form to implement the Yasuoka-Matsumoto nucleation rate measurement technique (threshold method). Comparison to nucleation models shows that classical nucleation theory over-estimates nucleation rates by a few orders of magnitude. The semi-phenomenological nucleation model does better, under-predicting rates by at worst a factor of 24. Unlike what has been observed in Lennard-Jones simulations, post-critical clusters have temperatures consistent with the run average temperature. Also, we observe that post-critical clusters have densities very slightly higher, ˜ 5%, than bulk liquid. We re-calibrate a Hale-type J vs. S scaling relation using both experimental and simulation data, finding remarkable consistency in over 30 orders of magnitude in the nucleation rate range and 180 K in the temperature range.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Institute for Computational Science
Dewey Decimal Classification:530 Physics
Language:English
Date:August 2015
Deposited On:19 Feb 2016 13:41
Last Modified:08 Dec 2017 18:33
Publisher:American Institute of Physics
ISSN:0021-9606
Additional Information:Copyright 2015 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in Homogeneous SPC/E water nucleation in large molecular dynamics simulations and may be found at DOI: 10.1063/1.4928055
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1063/1.4928055

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