Homogeneous SPC/E water nucleation in large molecular dynamics simulations

• Angélil, Raymond

• Diemand, Jürg

• Tanaka, Kyoko K

• Tanaka, Hidekazu

抄録

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.

収録刊行物

• The Journal of Chemical Physics

  The Journal of Chemical Physics 143 064507-, 2015-08-11

  American Institute of Physics (AIP)

詳細情報

• CRID: 1050282813995919872
• NII論文ID: 120005667718
• HANDLE: 2115/60180
• ISSN: 00219606
• 本文言語コード: en
• 資料種別: journal article
• データソース種別:
  • IRDB
  • CiNii Articles