Homogeneous nucleation of water in Argon: nucleation rate computation from molecular simulations of TIP4P and TIP4P/2005 water model

Jacques Dam, R. Dumitrescu, S.V. Gaastra-Nadea, D.M.J. Smeulders

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

Molecular dynamics (MD) simulations were conducted to study nucleation of water at 350 K in argon using TIP4P and TIP4P/2005 water models. We found that the stability of any cluster, even if large, strongly depends on the energetic interactions with its vicinity, while the stable clusters change their composition almost entirely during nucleation. Using the threshold method, direct nucleation rates are obtained. Our nucleation rates are found to be 1.08×1027 cm⁻³ s⁻¹ for TIP4P and 2.30×1027 cm⁻³ s⁻¹ for TIP4P/2005. The latter model prescribes a faster dynamics than the former, with a nucleation rate two times larger due to its higher electrostatic charges. The non-equilibrium water densities derived from simulations and state-of-art equilibrium parameters from Vega and de Miguel [J. Chem. Phys. 126, 154707 (2007)] are used for the classical nucleation theory (CNT) prediction. The CNT overestimates our results for both water models, where TIP4P/2005 shows largest discrepancy. Our results complement earlier data at high nucleation rates and supersaturations in the Hale plot [Phys. Rev. A 33, 4156 (1986)], and are consistent with MD data on the SPC/E and the TIP4P/2005 model.
Original languageEnglish
JournalJournal of chemical physics
Volume146
Issue number8
DOIs
Publication statusPublished - 2017
Externally publishedYes

Keywords

  • molecular dynamics
  • water model
  • supersaturations
  • nucleation

Cite this

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title = "Homogeneous nucleation of water in Argon: nucleation rate computation from molecular simulations of TIP4P and TIP4P/2005 water model",
abstract = "Molecular dynamics (MD) simulations were conducted to study nucleation of water at 350 K in argon using TIP4P and TIP4P/2005 water models. We found that the stability of any cluster, even if large, strongly depends on the energetic interactions with its vicinity, while the stable clusters change their composition almost entirely during nucleation. Using the threshold method, direct nucleation rates are obtained. Our nucleation rates are found to be 1.08×1027 cm⁻³ s⁻¹ for TIP4P and 2.30×1027 cm⁻³ s⁻¹ for TIP4P/2005. The latter model prescribes a faster dynamics than the former, with a nucleation rate two times larger due to its higher electrostatic charges. The non-equilibrium water densities derived from simulations and state-of-art equilibrium parameters from Vega and de Miguel [J. Chem. Phys. 126, 154707 (2007)] are used for the classical nucleation theory (CNT) prediction. The CNT overestimates our results for both water models, where TIP4P/2005 shows largest discrepancy. Our results complement earlier data at high nucleation rates and supersaturations in the Hale plot [Phys. Rev. A 33, 4156 (1986)], and are consistent with MD data on the SPC/E and the TIP4P/2005 model.",
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author = "Jacques Dam and R. Dumitrescu and S.V. Gaastra-Nadea and D.M.J. Smeulders",
year = "2017",
doi = "10.1063/1.4975623",
language = "English",
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publisher = "American Institute of Physics",
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Homogeneous nucleation of water in Argon : nucleation rate computation from molecular simulations of TIP4P and TIP4P/2005 water model . / Dam, Jacques; Dumitrescu, R.; Gaastra-Nadea, S.V.; Smeulders, D.M.J.

In: Journal of chemical physics, Vol. 146, No. 8, 2017.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Homogeneous nucleation of water in Argon

T2 - nucleation rate computation from molecular simulations of TIP4P and TIP4P/2005 water model

AU - Dam, Jacques

AU - Dumitrescu, R.

AU - Gaastra-Nadea, S.V.

AU - Smeulders, D.M.J.

PY - 2017

Y1 - 2017

N2 - Molecular dynamics (MD) simulations were conducted to study nucleation of water at 350 K in argon using TIP4P and TIP4P/2005 water models. We found that the stability of any cluster, even if large, strongly depends on the energetic interactions with its vicinity, while the stable clusters change their composition almost entirely during nucleation. Using the threshold method, direct nucleation rates are obtained. Our nucleation rates are found to be 1.08×1027 cm⁻³ s⁻¹ for TIP4P and 2.30×1027 cm⁻³ s⁻¹ for TIP4P/2005. The latter model prescribes a faster dynamics than the former, with a nucleation rate two times larger due to its higher electrostatic charges. The non-equilibrium water densities derived from simulations and state-of-art equilibrium parameters from Vega and de Miguel [J. Chem. Phys. 126, 154707 (2007)] are used for the classical nucleation theory (CNT) prediction. The CNT overestimates our results for both water models, where TIP4P/2005 shows largest discrepancy. Our results complement earlier data at high nucleation rates and supersaturations in the Hale plot [Phys. Rev. A 33, 4156 (1986)], and are consistent with MD data on the SPC/E and the TIP4P/2005 model.

AB - Molecular dynamics (MD) simulations were conducted to study nucleation of water at 350 K in argon using TIP4P and TIP4P/2005 water models. We found that the stability of any cluster, even if large, strongly depends on the energetic interactions with its vicinity, while the stable clusters change their composition almost entirely during nucleation. Using the threshold method, direct nucleation rates are obtained. Our nucleation rates are found to be 1.08×1027 cm⁻³ s⁻¹ for TIP4P and 2.30×1027 cm⁻³ s⁻¹ for TIP4P/2005. The latter model prescribes a faster dynamics than the former, with a nucleation rate two times larger due to its higher electrostatic charges. The non-equilibrium water densities derived from simulations and state-of-art equilibrium parameters from Vega and de Miguel [J. Chem. Phys. 126, 154707 (2007)] are used for the classical nucleation theory (CNT) prediction. The CNT overestimates our results for both water models, where TIP4P/2005 shows largest discrepancy. Our results complement earlier data at high nucleation rates and supersaturations in the Hale plot [Phys. Rev. A 33, 4156 (1986)], and are consistent with MD data on the SPC/E and the TIP4P/2005 model.

KW - molecular dynamics

KW - water model

KW - supersaturations

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KW - moleculaire dynamica

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