Title: Contact angles from Young’s equation in molecular dynamics simulations

Abstract

In this work, we propose a method to calculate the equilibrium contact angle of heterogeneous 3-phase solid/fluid/fluid systems using molecular dynamics simulations. The proposed method, which combines the phantom-wall method [F. Leroy and F. Müller-Plathe, J. Chem. Phys. 133, 044110 (2010)] and Bennett’s acceptance ratio approach [C. H. Bennett, J. Comput. Phys. 22, 245 (1976)], is able to calculate the solid/fluid surface tension relative to the solid surface energy. The calculated relative surface tensions can then be used in Young’s equation to estimate the equilibrium contact angle. A fluid droplet is not needed for the proposed method, in contrast to the situation for direct simulations of contact angles. In addition, while prior free-energy based methods for contact angles mainly focused on the wetting of fluids in coexistence with their vapor on solid surfaces, the proposed approach was designed to study the contact angles of fluid mixtures on solid surfaces above the fluid saturation pressures. Using the proposed approach, the contact angles of binary Lennard-Jones fluid mixtures on a non-polar solid substrate were calculated at various interaction parameters and the contact angle of water in equilibrium with CO₂ on a hydrophilic polar silica surface was obtained. For both non-polar and polarmore » systems, the calculated contact angles from the proposed method were in agreement with those obtained from the geometry of a cylindrical droplet. The computational cost of the proposed method was found to be comparable to that of simulations that use fluid droplets, but the new method provides a way to calculate the contact angle directly from Young’s equation without ambiguity.« less

Authors:

Jiang, Hao  ^[1];

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• Search OSTI.GOV for ORCID "0000-0002-5596-0055"
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Müller-Plathe, Florian ^[2]; Panagiotopoulos, Athanassios Z.  ^[1]

• Search OSTI.GOV for author "Panagiotopoulos, Athanassios Z."
• Search OSTI.GOV for ORCID "0000-0002-8152-6615"
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+ Show Author Affiliations

1. Princeton Univ., NJ (United States). Dept. of Chemical and Biological Engineering
2. Princeton Univ., NJ (United States). Dept. of Chemical and Biological Engineering; Technical Univ. of Darmstadt (Germany). Eduard Zintl Inst. of Inorganic and Physical Chemistry

Publication Date:

Thu Aug 31 00:00:00 EDT 2017

Research Org.:

Princeton Univ., NJ (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States); German Research Foundation (DFG)

OSTI Identifier:

1474037

Alternate Identifier(s):

OSTI ID: 1377981

Grant/Contract Number:  

SC0002128; AWD 1004131

Resource Type:

Journal Article: Accepted Manuscript

Journal Name:

Journal of Chemical Physics

Additional Journal Information:

Journal Volume: 147; Journal Issue: 8; Journal ID: ISSN 0021-9606

Publisher:

American Institute of Physics (AIP)

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 74 ATOMIC AND MOLECULAR PHYSICS; Lennard-Jones fluid; chemical compounds and components; surface energy; fluid flows; chemical elements; liquid solid interfaces; fluid systems; molecular dynamics; free energy; electrostatics