Properties of liquid clusters in large-scale molecular dynamics nucleation simulations
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- Raymond Angélil
- University of Zurich 1 Institute for Theoretical Physics, , 8057 Zurich, Switzerland
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- Jürg Diemand
- University of Zurich 1 Institute for Theoretical Physics, , 8057 Zurich, Switzerland
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- Kyoko K. Tanaka
- Hokkaido University 2 Institute of Low Temperature Science, , Sapporo 060-0819, Japan
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- Hidekazu Tanaka
- Hokkaido University 2 Institute of Low Temperature Science, , Sapporo 060-0819, Japan
Abstract
<jats:p>We have performed large-scale Lennard-Jones molecular dynamics simulations of homogeneous vapor-to-liquid nucleation, with 109 atoms. This large number allows us to resolve extremely low nucleation rates, and also provides excellent statistics for cluster properties over a wide range of cluster sizes. The nucleation rates, cluster growth rates, and size distributions are presented in Diemand et al. [J. Chem. Phys. 139, 74309 (2013)], while this paper analyses the properties of the clusters. We explore the cluster temperatures, density profiles, potential energies, and shapes. A thorough understanding of the properties of the clusters is crucial to the formulation of nucleation models. Significant latent heat is retained by stable clusters, by as much as ΔkT = 0.1ε for clusters with size i = 100. We find that the clusters deviate remarkably from spherical—with ellipsoidal axis ratios for critical cluster sizes typically within b/c = 0.7 ± 0.05 and a/c = 0.5 ± 0.05. We examine cluster spin angular momentum, and find that it plays a negligible role in the cluster dynamics. The interfaces of large, stable clusters are thinner than planar equilibrium interfaces by 10%−30%. At the critical cluster size, the cluster central densities are between 5% and 30% lower than the bulk liquid expectations. These lower densities imply larger-than-expected surface areas, which increase the energy cost to form a surface, which lowers nucleation rates.</jats:p>
Journal
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- The Journal of Chemical Physics
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The Journal of Chemical Physics 140 (7), 074303-, 2014-02-19
AIP Publishing
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Details 詳細情報について
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- CRID
- 1360004233910243072
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- ISSN
- 10897690
- 00219606
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- Data Source
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- Crossref
- KAKEN