Effect of exchange-correlation functionals on the density functional theory simulation of phase transformation of fast-ion conductors: A case study in the Li garnet oxide Li7La3Zr2O12

Matthew J. Klenk, Wei Lai

    Research output: Contribution to journalArticle

    Abstract

    The phase transformation of a fast-ion conductor Li7La3Zr2O12 (LLZ) upon heating was investigated using first-principle molecular dynamics by applying the local density approximation (LDA) and thirteen generalized gradient approximations (GGA) of the electron exchange and correlation (XC) energy functionals within the density-functional theory (DFT) framework. It was found that some functionals in the selected group failed to predict the phase transformation behavior while others predicted too large or small lattice volumes. Of the fourteen, three functional types, PBEsol, SOGGA, and PBE2, exhibited behaviors consistent with the tetragonal to cubic phase transformation upon heating and they were able to reproduce crystallite volumes within 1.5% of the experimental values. The correlation of XC functional forms and their accuracy in predicting materials properties was discussed.

    Original languageEnglish (US)
    Pages (from-to)132-136
    Number of pages5
    JournalComputational Materials Science
    Volume134
    DOIs
    StatePublished - Jun 15 2017

    Profile

    phase transformations
    Phase transformation
    Phase transitions
    functionals
    conductors
    density functional theory
    heating
    approximation
    ions
    Conductor
    Density functional
    Heating
    Approximation
    Density functional theory
    Ions
    garnets
    molecular dynamics
    gradients
    oxides
    electrons

    Keywords

    • Exchange-correlation functionals
    • Fast-ion conductors
    • Lithium garnet oxide
    • Phase transformation

    ASJC Scopus subject areas

    • Computer Science(all)
    • Chemistry(all)
    • Materials Science(all)
    • Mechanics of Materials
    • Physics and Astronomy(all)
    • Computational Mathematics

    Cite this

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    title = "Effect of exchange-correlation functionals on the density functional theory simulation of phase transformation of fast-ion conductors: A case study in the Li garnet oxide Li7La3Zr2O12",
    abstract = "The phase transformation of a fast-ion conductor Li7La3Zr2O12 (LLZ) upon heating was investigated using first-principle molecular dynamics by applying the local density approximation (LDA) and thirteen generalized gradient approximations (GGA) of the electron exchange and correlation (XC) energy functionals within the density-functional theory (DFT) framework. It was found that some functionals in the selected group failed to predict the phase transformation behavior while others predicted too large or small lattice volumes. Of the fourteen, three functional types, PBEsol, SOGGA, and PBE2, exhibited behaviors consistent with the tetragonal to cubic phase transformation upon heating and they were able to reproduce crystallite volumes within 1.5% of the experimental values. The correlation of XC functional forms and their accuracy in predicting materials properties was discussed.",
    keywords = "Exchange-correlation functionals, Fast-ion conductors, Lithium garnet oxide, Phase transformation",
    author = "Klenk, {Matthew J.} and Wei Lai",
    year = "2017",
    month = "6",
    doi = "10.1016/j.commatsci.2017.03.039",
    volume = "134",
    pages = "132--136",
    journal = "Computational Materials Science",
    issn = "0927-0256",
    publisher = "Elsevier",

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    TY - JOUR

    T1 - Effect of exchange-correlation functionals on the density functional theory simulation of phase transformation of fast-ion conductors

    T2 - Computational Materials Science

    AU - Klenk,Matthew J.

    AU - Lai,Wei

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    N2 - The phase transformation of a fast-ion conductor Li7La3Zr2O12 (LLZ) upon heating was investigated using first-principle molecular dynamics by applying the local density approximation (LDA) and thirteen generalized gradient approximations (GGA) of the electron exchange and correlation (XC) energy functionals within the density-functional theory (DFT) framework. It was found that some functionals in the selected group failed to predict the phase transformation behavior while others predicted too large or small lattice volumes. Of the fourteen, three functional types, PBEsol, SOGGA, and PBE2, exhibited behaviors consistent with the tetragonal to cubic phase transformation upon heating and they were able to reproduce crystallite volumes within 1.5% of the experimental values. The correlation of XC functional forms and their accuracy in predicting materials properties was discussed.

    AB - The phase transformation of a fast-ion conductor Li7La3Zr2O12 (LLZ) upon heating was investigated using first-principle molecular dynamics by applying the local density approximation (LDA) and thirteen generalized gradient approximations (GGA) of the electron exchange and correlation (XC) energy functionals within the density-functional theory (DFT) framework. It was found that some functionals in the selected group failed to predict the phase transformation behavior while others predicted too large or small lattice volumes. Of the fourteen, three functional types, PBEsol, SOGGA, and PBE2, exhibited behaviors consistent with the tetragonal to cubic phase transformation upon heating and they were able to reproduce crystallite volumes within 1.5% of the experimental values. The correlation of XC functional forms and their accuracy in predicting materials properties was discussed.

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