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

Abstract

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,more »« less

Authors:

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

Publication Date:: Mon Nov 21 00:00:00 EST 2016

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:: Journal Article: 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.

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                    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

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                    Qi, Xin, Zhou, Ya, and Fichthorn, Kristen A. 2016.  
        "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.

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@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},

  url          = {https://www.osti.gov/biblio/1465671},
  journal      = {Journal of Chemical Physics},

  issn         = {0021-9606},

  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}

}

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Works referencing / citing this record:

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

Abstract

Citation Formats

Nucleation and growth of micellar polycrystals under time-dependent volume fraction conditions journal, March 2013

Broken-bond rule for the surface energies of noble metals journal, June 2002

Test-area simulation method for the direct determination of the interfacial tension of systems with continuous or discontinuous potentials journal, October 2005

Quantitative Analysis of the Role Played by Poly(vinylpyrrolidone) in Seed-Mediated Growth of Ag Nanocrystals journal, January 2012

Crystal nucleation and the solid–liquid interfacial free energy journal, February 2012

Density-Functional Theory with Screened van der Waals Interactions for the Modeling of Hybrid Inorganic-Organic Systems journal, April 2012

A new Monte Carlo method for calculating surface tension journal, January 1976

Method for Computing the Anisotropy of the Solid-Liquid Interfacial Free Energy journal, June 2001

An embedded-atom potential for the Cu–Ag system journal, May 2006

Adsorption of Polyvinylpyrrolidone on Ag Surfaces: Insight into a Structure-Directing Agent journal, January 2012

How Structure-Directing Agents Control Nanocrystal Shape: Polyvinylpyrrolidone-Mediated Growth of Ag Nanocubes journal, October 2015

Applicability of the broken-bond rule to the surface energy of the fcc metals journal, June 2002

Direct calculation of the crystal–melt interfacial free energies for continuous potentials: Application to the Lennard-Jones system journal, January 2003

The ensemble switch method for computing interfacial tensions journal, April 2015

The mold integration method for the calculation of the crystal-fluid interfacial free energy from simulations journal, October 2014

Nucleation barriers for the liquid-to-crystal transition in simple metals: Experiment vs. simulation journal, February 2014

Fast Parallel Algorithms for Short-Range Molecular Dynamics journal, March 1995

Single crystal growth and anisotropic crystal-fluid interfacial free energy in soft colloidal systems journal, July 2011

Comparison of the Binding of Polyvinylpyrrolidone and Polyethylene Oxide to Ag Surfaces: Elements of a Successful Structure-Directing Agent journal, May 2013

Topology of Electronic Charge Density and Energetics of Planar Faults in fcc Metals journal, March 2002

Binding of Polyvinylpyrrolidone to Ag Surfaces: Insight into a Structure-Directing Agent from Dispersion-Corrected Density Functional Theory journal, January 2013

A simple empirical N -body potential for transition metals journal, July 1984

Predicting kinetic nanocrystal shapes through multi-scale theory and simulation: Polyvinylpyrrolidone-mediated growth of Ag nanocrystals journal, October 2016

Vibrational thermodynamics of materials journal, May 2010

The Entropy of Surface Formation journal, March 1941

The surface energy of metals journal, August 1998

Crystal-liquid interfacial free energy via thermodynamic integration journal, July 2014

The Surface Tension of Solids journal, May 1950

Surface Tensions in NaCl−Water−Air Systems from MD Simulations journal, October 2007

A Force Field for Describing the Polyvinylpyrrolidone-Mediated Solution-Phase Synthesis of Shape-Selective Ag Nanoparticles journal, January 2014

Interfacial excess energy, excess stress and excess strain in elastic solids: Planar interfaces journal, May 2008

A unified formulation of the constant temperature molecular dynamics methods journal, July 1984

Ab initio study of step formation and self-diffusion on Ag(100) journal, May 1997

A Theory for Estimation of Surface and Interfacial Energies. iii. Estimation of Surface Energies of Solids from Contact Angle data journal, May 1960

Solid-liquid surface free energy of Lennard-Jones liquid on smooth and rough surfaces computed by molecular dynamics using the phantom-wall method journal, July 2010

Multi-scale theory and simulation of shape-selective nanocrystal growth journal, January 2016

Shape-Controlled Synthesis of Metal Nanocrystals: Simple Chemistry Meets Complex Physics? journal, December 2008

Nosé–Hoover chains: The canonical ensemble via continuous dynamics journal, August 1992

Perturbation theory of solid-liquid interfacial free energies of bcc metals journal, September 2012

Molecular dynamics investigation of the crystal–fluid interface. VI. Excess surface free energies of crystal–liquid systems journal, May 1986

Molecular dynamics with coupling to an external bath journal, October 1984

Interfacial Excess Free Energies of Solid-Liquid Interfaces by Molecular Dynamics Simulation and Thermodynamic Integration journal, May 2009

Surface energy calculation of the fcc metals by using the MAEAM journal, October 2007

Evaluation of harmonic methods for calculating the free energy of defects in solids journal, June 1994

Estimation of the surface free energy of polymers journal, August 1969

The crystal-fluid interfacial free energy and nucleation rate of NaCl from different simulation methods journal, May 2015

The Statistical Mechanical Theory of Surface Tension journal, March 1949

Measurement of the average surface stress of gold as a function of temperature in the temperature range 50-985.deg. journal, November 1968

Canonical dynamics: Equilibrium phase-space distributions journal, March 1985

Local pressure components and interfacial tension at a liquid-solid interface obtained by the perturbative method in the Lennard-Jones system journal, July 2014

Semiempirical GGA-type density functional constructed with a long-range dispersion correction journal, January 2006

Computation of interfacial properties via grand canonical transition matrix Monte Carlo simulation journal, January 2008

A molecular dynamics study to determine the solid-liquid interfacial tension using test area simulation method (TASM) journal, August 2012

The anisotropic free energy of the Lennard-Jones crystal-melt interface journal, August 2003

Crystallization kinetics of colloidal model suspensions: recent achievements and new perspectives journal, July 2014

Atomic-Scale Theory and Simulations for Colloidal Metal Nanocrystal Growth journal, May 2014

Crystal-liquid interfacial free energy of hard spheres via a thermodynamic integration scheme journal, March 2015

Monte Carlo Simulations book, September 2002

Theory of the thermodynamic influence of solution-phase additives in shape-controlled nanocrystal synthesis journal, January 2017

Characterizing surface wetting and interfacial properties using enhanced sampling (SWIPES) journal, January 2019

Efficient scheme for calculating work of adhesion between a liquid and polymer-grafted substrate journal, August 2018

Characterizing Surface Wetting and Interfacial Properties using Enhanced Sampling (SWIPES) preprint, January 2018

Nucleation and growth of micellar polycrystals under time-dependent volume fraction conditions
journal, March 2013

Broken-bond rule for the surface energies of noble metals
journal, June 2002

Test-area simulation method for the direct determination of the interfacial tension of systems with continuous or discontinuous potentials
journal, October 2005

Quantitative Analysis of the Role Played by Poly(vinylpyrrolidone) in Seed-Mediated Growth of Ag Nanocrystals
journal, January 2012

Crystal nucleation and the solid–liquid interfacial free energy
journal, February 2012

Density-Functional Theory with Screened van der Waals Interactions for the Modeling of Hybrid Inorganic-Organic Systems
journal, April 2012

A new Monte Carlo method for calculating surface tension
journal, January 1976

Method for Computing the Anisotropy of the Solid-Liquid Interfacial Free Energy
journal, June 2001

An embedded-atom potential for the Cu–Ag system
journal, May 2006

Adsorption of Polyvinylpyrrolidone on Ag Surfaces: Insight into a Structure-Directing Agent
journal, January 2012

How Structure-Directing Agents Control Nanocrystal Shape: Polyvinylpyrrolidone-Mediated Growth of Ag Nanocubes
journal, October 2015

Applicability of the broken-bond rule to the surface energy of the fcc metals
journal, June 2002

Direct calculation of the crystal–melt interfacial free energies for continuous potentials: Application to the Lennard-Jones system
journal, January 2003

The ensemble switch method for computing interfacial tensions
journal, April 2015

The mold integration method for the calculation of the crystal-fluid interfacial free energy from simulations
journal, October 2014

Nucleation barriers for the liquid-to-crystal transition in simple metals: Experiment vs. simulation
journal, February 2014

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Single crystal growth and anisotropic crystal-fluid interfacial free energy in soft colloidal systems
journal, July 2011

Comparison of the Binding of Polyvinylpyrrolidone and Polyethylene Oxide to Ag Surfaces: Elements of a Successful Structure-Directing Agent
journal, May 2013

Topology of Electronic Charge Density and Energetics of Planar Faults in fcc Metals
journal, March 2002

Binding of Polyvinylpyrrolidone to Ag Surfaces: Insight into a Structure-Directing Agent from Dispersion-Corrected Density Functional Theory
journal, January 2013

A simple empirical N -body potential for transition metals
journal, July 1984

Predicting kinetic nanocrystal shapes through multi-scale theory and simulation: Polyvinylpyrrolidone-mediated growth of Ag nanocrystals
journal, October 2016

Vibrational thermodynamics of materials
journal, May 2010

The Entropy of Surface Formation
journal, March 1941

The surface energy of metals
journal, August 1998

Crystal-liquid interfacial free energy via thermodynamic integration
journal, July 2014

The Surface Tension of Solids
journal, May 1950

Surface Tensions in NaCl−Water−Air Systems from MD Simulations
journal, October 2007

A Force Field for Describing the Polyvinylpyrrolidone-Mediated Solution-Phase Synthesis of Shape-Selective Ag Nanoparticles
journal, January 2014

Interfacial excess energy, excess stress and excess strain in elastic solids: Planar interfaces
journal, May 2008

A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984

Ab initio study of step formation and self-diffusion on Ag(100)
journal, May 1997

A Theory for Estimation of Surface and Interfacial Energies. iii. Estimation of Surface Energies of Solids from Contact Angle data
journal, May 1960

Solid-liquid surface free energy of Lennard-Jones liquid on smooth and rough surfaces computed by molecular dynamics using the phantom-wall method
journal, July 2010

Multi-scale theory and simulation of shape-selective nanocrystal growth
journal, January 2016

Shape-Controlled Synthesis of Metal Nanocrystals: Simple Chemistry Meets Complex Physics?
journal, December 2008

Nosé–Hoover chains: The canonical ensemble via continuous dynamics
journal, August 1992

Perturbation theory of solid-liquid interfacial free energies of bcc metals
journal, September 2012

Molecular dynamics investigation of the crystal–fluid interface. VI. Excess surface free energies of crystal–liquid systems
journal, May 1986

Molecular dynamics with coupling to an external bath
journal, October 1984

Interfacial Excess Free Energies of Solid-Liquid Interfaces by Molecular Dynamics Simulation and Thermodynamic Integration
journal, May 2009

Surface energy calculation of the fcc metals by using the MAEAM
journal, October 2007

Evaluation of harmonic methods for calculating the free energy of defects in solids
journal, June 1994

Estimation of the surface free energy of polymers
journal, August 1969

The crystal-fluid interfacial free energy and nucleation rate of NaCl from different simulation methods
journal, May 2015

The Statistical Mechanical Theory of Surface Tension
journal, March 1949

Measurement of the average surface stress of gold as a function of temperature in the temperature range 50-985.deg.
journal, November 1968

Canonical dynamics: Equilibrium phase-space distributions
journal, March 1985

Local pressure components and interfacial tension at a liquid-solid interface obtained by the perturbative method in the Lennard-Jones system
journal, July 2014

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

Computation of interfacial properties via grand canonical transition matrix Monte Carlo simulation
journal, January 2008

A molecular dynamics study to determine the solid-liquid interfacial tension using test area simulation method (TASM)
journal, August 2012

The anisotropic free energy of the Lennard-Jones crystal-melt interface
journal, August 2003

Crystallization kinetics of colloidal model suspensions: recent achievements and new perspectives
journal, July 2014

Atomic-Scale Theory and Simulations for Colloidal Metal Nanocrystal Growth
journal, May 2014

Crystal-liquid interfacial free energy of hard spheres via a thermodynamic integration scheme
journal, March 2015

Monte Carlo Simulations
book, September 2002

Theory of the thermodynamic influence of solution-phase additives in shape-controlled nanocrystal synthesis
journal, January 2017

Characterizing surface wetting and interfacial properties using enhanced sampling (SWIPES)
journal, January 2019

Efficient scheme for calculating work of adhesion between a liquid and polymer-grafted substrate
journal, August 2018

Characterizing Surface Wetting and Interfacial Properties using Enhanced Sampling (SWIPES)
preprint, January 2018