Homogeneous SPC/E water nucleation in large molecular dynamics simulations

Raymond Angélil, Jürg Diemand, Kyoko K. Tanaka, Hidekazu Tanaka

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

We perform direct large molecular dynamics simulations of homogeneous SPC/E water nucleation, using up to ∼ 4 . 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.

Original languageEnglish
Article number064507
JournalJournal of Chemical Physics
Volume143
Issue number6
DOIs
Publication statusPublished - 2015 Aug 14

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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