### 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 1.08×10^{27} cm^{−3} s^{−1} for TIP4P and 2.30×10^{27} 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.

Language | English |
---|---|

Article number | 084309 |

Number of pages | 11 |

Journal | Journal of Chemical Physics |

Volume | 146 |

Issue number | 8 |

DOIs | |

State | Published - 28 Feb 2017 |

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**Homogeneous nucleation of water in argon : nucleation rate computation from molecular simulations of TIP4P and TIP4P/2005 water model.** / Dumitrescu, Lucia R.; Smeulders, David M.J.; Dam, Jacques A.M.; Gaastra-Nedea, Silvia V.

Research output: Contribution to journal › Article › Academic › peer-review

TY - JOUR

T1 - Homogeneous nucleation of water in argon : nucleation rate computation from molecular simulations of TIP4P and TIP4P/2005 water model

AU - Dumitrescu,Lucia R.

AU - Smeulders,David M.J.

AU - Dam,Jacques A.M.

AU - Gaastra-Nedea,Silvia V.

PY - 2017/2/28

Y1 - 2017/2/28

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.

UR - http://www.scopus.com/inward/record.url?scp=85013963845&partnerID=8YFLogxK

U2 - 10.1063/1.4975623

DO - 10.1063/1.4975623

M3 - Article

VL - 146

JO - Journal of Chemical Physics

T2 - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 8

M1 - 084309

ER -