Thermodynamic analysis of the stability of planar interfaces between coexisting phases and its application to supercooled water

Singh, Rakesh S.; Palmer, Jeremy C.; Panagiotopoulos, Athanassios Z.; Debenedetti, Pablo G.

doi:10.1063/1.5097591

Title: Thermodynamic analysis of the stability of planar interfaces between coexisting phases and its application to supercooled water

Journal Article · Mon Jun 10 00:00:00 EDT 2019 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5097591· OSTI ID:1610631

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Princeton Univ., NJ (United States); Indian Inst. of Science Education and Research (IISER), Tirupati (India)
Univ. of Houston, TX (United States)
Princeton Univ., NJ (United States)

Two-phase simulations are commonly used to evaluate coexistence conditions, interfacial tensions, and other thermodynamic properties associated with first-order phase transitions. Calculation of these properties is often simplified when the interfaces between the two phases are flat or planar. In this paper, we derive a general thermodynamic criterion for selecting simulation cell dimensions to stabilize planar interfaces in phase-separated fluid-fluid systems with respect to homogeneous, single-phase states. The resulting expression is validated by analyzing the effects of simulation cell dimensions on the formation of planar liquid-vapor interfaces in the Lennard-Jones fluid and in the TIP4P/2005 model of water. We also perform large scale molecular dynamics simulations to study metastable liquid-liquid phase separation in the ST2 and TIP4P/2005 models of water under deeply supercooled conditions. Our simulations confirm the stability of a liquid-liquid interface in ST2, and they demonstrate that the corresponding interface for TIP4P/2005 can be stabilized by judiciously choosing the simulation cell aspect ratio in a manner consistent with the thermodynamic criterion. We posit that this sensitivity to the simulation cell aspect ratio may explain discrepancies between previous studies examining liquid-liquid separation in models of supercooled water.

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Research Organization:: Princeton Univ., NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Welch Foundation

Grant/Contract Number:: SC0002128; SC0019394; E-1882

OSTI ID:: 1610631

Alternate ID(s):: OSTI ID: 1525525

Journal Information:: Journal of Chemical Physics, Vol. 150, Issue 22; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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