Local volume effects in the generalized pseudopotential theory

doi:10.1103/PhysRevB.99.214107

Title: Local volume effects in the generalized pseudopotential theory

Abstract

The generalized pseudopotential theory (GPT) is a compelling approach for deriving real-space transferable interatomic potentials. Using a coarse-grained electronic structure, one can explicitly determine the pair ion-ion and multi-ion interactions in simple and transition metals. While successful in determining bulk properties, in central force metals the GPT fails to describe crystal defects for which there is a significant local volume change. A previous paper [J. A. Moriarty and R. Phillips, Phys. Rev. Lett. 66, 3036 (1991)] found that by allowing the GPT total energy to depend upon some spatially averaged local electron density, the energetics of vacancies and surfaces could be calculated within experimental ranges. In this paper, we develop the formalism further by explicitly calculating the forces and stress tensor associated with this total energy. We call this scheme the adaptive GPT (aGPT) and it is capable of both molecular dynamics (MD) and molecular statics. We apply the aGPT to vacancy formation, divacancy binding, and stacking faults in hcp Mg. We also calculate the local electron density corrections to the bulk elastic constants and phonon dispersion for which there is refinement over the baseline GPT treatment. Furthermore, we demonstrate aGPT-MD simulation through the calculation of thermal expansion in magnesiummore » to 700 K.« less

Authors:

Skinner, Guy C. G. ^[1]; Paxton, Anthony T. ^[1]; Moriarty, John A. ^[2]

King's College London (United Kingdom)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Publication Date:: 2019-06-19

Research Org.:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1557065

Report Number(s):: LLNL-JRNL-761045
Journal ID: ISSN 2469-9950; PRBMDO; 949102

Grant/Contract Number:: AC52-07NA27344

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 99; Journal Issue: 21; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats


                    Skinner, Guy C.  G., Paxton, Anthony T., and Moriarty, John A. Local volume effects in the generalized pseudopotential theory.  United States: N. p., 2019. 
        Web.  doi:10.1103/PhysRevB.99.214107.

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                    Skinner, Guy C.  G., Paxton, Anthony T., & Moriarty, John A. Local volume effects in the generalized pseudopotential theory.  United States.  doi:10.1103/PhysRevB.99.214107.

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                    Skinner, Guy C.  G., Paxton, Anthony T., and Moriarty, John A. Wed .  
        "Local volume effects in the generalized pseudopotential theory".  United States.  doi:10.1103/PhysRevB.99.214107.  https://www.osti.gov/servlets/purl/1557065.

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@article{osti_1557065,

  title        = {Local volume effects in the generalized pseudopotential theory},

  author       = {Skinner, Guy C.  G. and Paxton, Anthony T. and Moriarty, John A.},

  abstractNote = {The generalized pseudopotential theory (GPT) is a compelling approach for deriving real-space transferable interatomic potentials. Using a coarse-grained electronic structure, one can explicitly determine the pair ion-ion and multi-ion interactions in simple and transition metals. While successful in determining bulk properties, in central force metals the GPT fails to describe crystal defects for which there is a significant local volume change. A previous paper [J. A. Moriarty and R. Phillips, Phys. Rev. Lett. 66, 3036 (1991)] found that by allowing the GPT total energy to depend upon some spatially averaged local electron density, the energetics of vacancies and surfaces could be calculated within experimental ranges. In this paper, we develop the formalism further by explicitly calculating the forces and stress tensor associated with this total energy. We call this scheme the adaptive GPT (aGPT) and it is capable of both molecular dynamics (MD) and molecular statics. We apply the aGPT to vacancy formation, divacancy binding, and stacking faults in hcp Mg. We also calculate the local electron density corrections to the bulk elastic constants and phonon dispersion for which there is refinement over the baseline GPT treatment. Furthermore, we demonstrate aGPT-MD simulation through the calculation of thermal expansion in magnesium to 700 K.},

  doi          = {10.1103/PhysRevB.99.214107},

  journal      = {Physical Review B},

  number       = 21,

  volume       = 99,

  place        = {United States},

  year         = {2019},

  month        = {6}

}

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Similar Records

Title: Local volume effects in the generalized pseudopotential theory

Abstract

Citation Formats

Density-functional formulation of the generalized pseudopotential theory journal, September 1977

Density-functional formulation of the generalized pseudopotential theory. II journal, August 1982

Density-functional formulation of the generalized pseudopotential theory. III. Transition-metal interatomic potentials journal, August 1988

Analytic representation of multi-ion interatomic potentials in transition metals journal, July 1990

Robust quantum-based interatomic potentials for multiscale modeling in transition metals journal, March 2006

First-principles interatomic potentials for transition-metal aluminides: Theory and trends across the 3 d series journal, October 1997

First-principles interatomic potentials for transition-metal surfaces journal, June 1991

Density-dependent pair potentials and the compressibility problem journal, March 1987

Phonons in nontransition metals [Фононы в непереходных металлах] journal, January 1974

Phonons in nontransition metals journal, February 1974

Phase diagram and thermodynamic properties of solid magnesium in the quasiharmonic approximation journal, November 1993

First-principles temperature-pressure phase diagram of magnesium journal, March 1995

Ab initio thermoelasticity of magnesium journal, February 1999

Elastic Constants of Magnesium from 4.2°K to 300°K journal, August 1957

General Theory of Pseudopotentials journal, July 1962

Analytic expression for the dielectric screening function of strongly coupled electron liquids at metallic and lower densities journal, December 1981

Accurate spin-dependent electron liquid correlation energies for local spin density calculations: a critical analysis journal, August 1980

Accurate atomistic simulation of ( a /2) 〈111〉 screw dislocations and other defects in bcc tantalum journal, May 2001

Representations of the local atomic density journal, September 1998

Forces in Molecules journal, August 1939

Three-Body Forces in the Lattice Dynamics of Beryllium journal, December 1973

Anharmonic force constants extracted from first-principles molecular dynamics: applications to heat transfer simulations journal, May 2014

High-precision sampling for Brillouin-zone integration in metals journal, August 1989

Accurate and simple analytic representation of the electron-gas correlation energy journal, June 1992

Molecular dynamics simulations at constant pressure and/or temperature journal, February 1980

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

Polymorphic transitions in single crystals: A new molecular dynamics method journal, December 1981

Ab initio study on divacancy binding energies in aluminum and magnesium journal, November 2003

The Formation Energy of Vacancies in Aluminium and Magnesium journal, June 1976

Intrinsic stacking faults in body-centred cubic crystals journal, October 1968

Comprehensive first-principles study of stable stacking faults in hcp metals journal, January 2017

Prediction of a {1122} hcp stacking fault using a modified generalized stacking-fault calculation journal, November 1997

Isothermal-isobaric molecular dynamics using stochastic velocity rescaling journal, February 2009

Anderson-Grüneisen parameter δ of some hexagonal metals and MgO from third-order elastic-constant data journal, November 1974

Breakdown of the Arrhenius Law in Describing Vacancy Formation Energies: The Importance of Local Anharmonicity Revealed by Ab initio Thermodynamics journal, February 2014

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

Density-functional formulation of the generalized pseudopotential theory
journal, September 1977

Density-functional formulation of the generalized pseudopotential theory. II
journal, August 1982

Density-functional formulation of the generalized pseudopotential theory. III. Transition-metal interatomic potentials
journal, August 1988

Analytic representation of multi-ion interatomic potentials in transition metals
journal, July 1990

Robust quantum-based interatomic potentials for multiscale modeling in transition metals
journal, March 2006

First-principles interatomic potentials for transition-metal aluminides: Theory and trends across the $3 d$ series
journal, October 1997

First-principles interatomic potentials for transition-metal surfaces
journal, June 1991

Density-dependent pair potentials and the compressibility problem
journal, March 1987

Phonons in nontransition metals [Фононы в непереходных металлах]
journal, January 1974

Phonons in nontransition metals
journal, February 1974

Phase diagram and thermodynamic properties of solid magnesium in the quasiharmonic approximation
journal, November 1993

First-principles temperature-pressure phase diagram of magnesium
journal, March 1995

Ab initio thermoelasticity of magnesium
journal, February 1999

Elastic Constants of Magnesium from 4.2°K to 300°K
journal, August 1957

General Theory of Pseudopotentials
journal, July 1962

Analytic expression for the dielectric screening function of strongly coupled electron liquids at metallic and lower densities
journal, December 1981

Accurate spin-dependent electron liquid correlation energies for local spin density calculations: a critical analysis
journal, August 1980

Accurate atomistic simulation of ( a /2) 〈111〉 screw dislocations and other defects in bcc tantalum
journal, May 2001

Representations of the local atomic density
journal, September 1998

Forces in Molecules
journal, August 1939

Three-Body Forces in the Lattice Dynamics of Beryllium
journal, December 1973

Anharmonic force constants extracted from first-principles molecular dynamics: applications to heat transfer simulations
journal, May 2014

High-precision sampling for Brillouin-zone integration in metals
journal, August 1989

Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992

Molecular dynamics simulations at constant pressure and/or temperature
journal, February 1980

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

Polymorphic transitions in single crystals: A new molecular dynamics method
journal, December 1981

Ab initio study on divacancy binding energies in aluminum and magnesium
journal, November 2003

The Formation Energy of Vacancies in Aluminium and Magnesium
journal, June 1976

Intrinsic stacking faults in body-centred cubic crystals
journal, October 1968

Comprehensive first-principles study of stable stacking faults in hcp metals
journal, January 2017

Prediction of a {1122} hcp stacking fault using a modified generalized stacking-fault calculation
journal, November 1997

Isothermal-isobaric molecular dynamics using stochastic velocity rescaling
journal, February 2009

Anderson-Grüneisen parameter $δ$ of some hexagonal metals and MgO from third-order elastic-constant data
journal, November 1974

Breakdown of the Arrhenius Law in Describing Vacancy Formation Energies: The Importance of Local Anharmonicity Revealed by Ab initio Thermodynamics
journal, February 2014

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