Molecular dynamics simulations of nucleation from vapor to solid composed of Lennard-Jones molecules

Kyoko K. Tanaka, Hidekazu Tanaka, Tetsuo Yamamoto, Katsuyuki Kawamura

Research output: Contribution to journalArticle

28 Citations (Scopus)

Abstract

We performed molecular dynamics (MD) simulations of nucleation from vapor at temperatures below the triple point for systems consisting of 10 4-105 Lennard-Jones (L-J) type molecules in order to test nucleation theories at relatively low temperatures. Simulations are performed for a wide range of initial supersaturation ratio (S0 ≃ 10 - 108) and temperature (kT 0.2 - 0.6ε), where and k are the depth of the L-J potential and the Boltzmann constant, respectively. Clusters are nucleated as supercooled liquid droplets because of their small size. Crystallization of the supercooled liquid nuclei is observed after their growth slows. The classical nucleation theory (CNT) significantly underestimates the nucleation rates (or the number density of critical clusters) in the low-T region. The semi-phenomenological (SP) model, which corrects the CNT prediction of the formation energy of clusters using the second virial coefficient of a vapor, reproduces the nucleation rate and the cluster size distributions with good accuracy in the low-T region, as well as in the higher-T cases considered in our previous study. The sticking probability of vapor molecules onto the clusters is also obtained in the present MD simulations. Using the obtained values of sticking probability in the SP model, we can further refine the accuracy of the SP model.

Original languageEnglish
Article number204313
JournalThe Journal of Chemical Physics
Volume134
Issue number20
DOIs
Publication statusPublished - May 28 2011

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Molecular dynamics
Nucleation
Vapors
nucleation
vapors
molecular dynamics
Molecules
Computer simulation
molecules
simulation
Signal filtering and prediction
Lennard-Jones potential
Supersaturation
virial coefficients
Liquids
energy of formation
liquids
Crystallization
supersaturation
Temperature

ASJC Scopus subject areas

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

Cite this

Molecular dynamics simulations of nucleation from vapor to solid composed of Lennard-Jones molecules. / Tanaka, Kyoko K.; Tanaka, Hidekazu; Yamamoto, Tetsuo; Kawamura, Katsuyuki.

In: The Journal of Chemical Physics, Vol. 134, No. 20, 204313, 28.05.2011.

Research output: Contribution to journalArticle

Tanaka, Kyoko K. ; Tanaka, Hidekazu ; Yamamoto, Tetsuo ; Kawamura, Katsuyuki. / Molecular dynamics simulations of nucleation from vapor to solid composed of Lennard-Jones molecules. In: The Journal of Chemical Physics. 2011 ; Vol. 134, No. 20.
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