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.

LanguageEnglish (US)
Pages132-136
Number of pages5
JournalComputational Materials Science
Volume134
DOIs
StatePublished - Jun 15 2017

Profile

Phase Transformation
Garnets
Conductor
Density Functional
functionals
garnets
Oxides
Density functional theory
phase transformations
conductors
Phase transitions
Ions
density functional theory
oxides
Heating
Local density approximation
ions
Simulation
heating
Generalized Gradient

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",
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T2 - Computational Materials Science

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AU - Lai,Wei

PY - 2017/6/15

Y1 - 2017/6/15

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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