Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces

Qi, Xin; Zhou, Ya; Fichthorn, Kristen A.

doi:10.1063/1.4967521

Title: Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces

Journal Article · Mon Nov 21 00:00:00 EST 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4967521· OSTI ID:1465671

Qi, Xin ^[1]; Zhou, Ya ^[1]; Fichthorn, Kristen A. ^[2]

Pennsylvania State Univ., University Park, PA (United States). Dept. of Chemical Engineering
Pennsylvania State Univ., University Park, PA (United States). Dept. of Chemical Engineering. Dept. of Physics

The solid-liquid interfacial free energy γ_sl is an important quantity in wetting, nucleation, and crystal growth. Although various methods have been developed to calculate γ_sl with atomic-scale simulations, such calculations still remain challenging for multi-component interfaces between molecular fluids and solids. In this paper, we present a multi-scheme thermodynamic integration method that is inspired by the “cleaving-wall” method and aimed at obtaining γ_sl for such systems using open-source simulation packages. This method advances two aspects of its predecessor methods. First, we incorporate separate schemes to resolve difficulties when manipulating periodic boundary conditions of the supercell using open-source simulation packages. Second, we introduce a numerical approximation to obtain thermodynamic integrands for complex force fields when an analytical differentiation is not readily available. To demonstrate this method, we obtain γ_sl for interfaces between Ag(100) and Ag(111) and ethylene glycol (EG). These interfacial free energies mirror interfacial potential energies for each facet. We also estimate entropies of interface formation and these are consistent with theoretical predictions in signs and trends. For the Ag-EG systems, we find that the largest contribution to γ_sl is the free energy to create the bare metal surfaces. The second-largest contribution to γ_sl is from the liquid-solid interaction. Finally, this user-friendly method will accelerate investigation in a broad range of research topics, such as the thermodynamic effect of structure-directing agents in solution-phase shape-controlled nanocrystal syntheses.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

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

Grant/Contract Number:: FG02-07ER46414; OCI-1053575

OSTI ID:: 1465671

Alternate ID(s):: OSTI ID: 1333016

Journal Information:: Journal of Chemical Physics, Vol. 145, Issue 19; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 24 works

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Title: Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces

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