Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces
Abstract
The solid-liquid interfacial free energy γsl is an important quantity in wetting, nucleation, and crystal growth. Although various methods have been developed to calculate γsl 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 γsl 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 γsl 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 γsl is the free energy to create the bare metal surfaces. The second-largest contribution to γsl is from the liquid-solid interaction. Finally,more »
- Authors:
-
- 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
- Publication Date:
- Research Org.:
- Pennsylvania State Univ., University Park, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1465671
- Alternate Identifier(s):
- OSTI ID: 1333016
- Grant/Contract Number:
- FG02-07ER46414; OCI-1053575
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 145; Journal Issue: 19; 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; nucleation; lattice constants; crystalline solids; silver; nanocrystals; entropy; molecular dynamics; liquid solid interfaces; electron densities of states; free energy
Citation Formats
Qi, Xin, Zhou, Ya, and Fichthorn, Kristen A. Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces. United States: N. p., 2016.
Web. doi:10.1063/1.4967521.
Qi, Xin, Zhou, Ya, & Fichthorn, Kristen A. Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces. United States. https://doi.org/10.1063/1.4967521
Qi, Xin, Zhou, Ya, and Fichthorn, Kristen A. Mon .
"Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces". United States. https://doi.org/10.1063/1.4967521. https://www.osti.gov/servlets/purl/1465671.
@article{osti_1465671,
title = {Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces},
author = {Qi, Xin and Zhou, Ya and Fichthorn, Kristen A.},
abstractNote = {The solid-liquid interfacial free energy γsl is an important quantity in wetting, nucleation, and crystal growth. Although various methods have been developed to calculate γsl 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 γsl 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 γsl 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 γsl is the free energy to create the bare metal surfaces. The second-largest contribution to γsl 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.},
doi = {10.1063/1.4967521},
journal = {Journal of Chemical Physics},
number = 19,
volume = 145,
place = {United States},
year = {Mon Nov 21 00:00:00 EST 2016},
month = {Mon Nov 21 00:00:00 EST 2016}
}
Web of Science
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