Header

UZH-Logo

Maintenance Infos

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.

Statistics

Citations

5 citations in Web of Science®
3 citations in Scopus®
Google Scholar™

Altmetrics

Downloads

35 downloads since deposited on 19 Feb 2016
13 downloads since 12 months
Detailed statistics

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:12 May 2016 10:28
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

Download

Preview Icon on Download
Preview
Content: Published Version
Filetype: PDF
Size: 2MB
View at publisher

Article Networks

TrendTerms

TrendTerms displays relevant terms of the abstract of this publication and related documents on a map. The terms and their relations were extracted from ZORA using word statistics. Their timelines are taken from ZORA as well. The bubble size of a term is proportional to the number of documents where the term occurs. Red, orange, yellow and green colors are used for terms that occur in the current document; red indicates high interlinkedness of a term with other terms, orange, yellow and green decreasing interlinkedness. Blue is used for terms that have a relation with the terms in this document, but occur in other documents.
You can navigate and zoom the map. Mouse-hovering a term displays its timeline, clicking it yields the associated documents.

Author Collaborations