Local structure and dynamics of lithium garnet ionic conductors: tetragonal and cubic Li7La3Zr2O7

Matthew Klenk, Wei Lai

    Research output: Contribution to journalArticle

    • 11 Citations

    Abstract

    To better understand the ionic conduction in lithium garnet oxides, we employed molecular dynamics simulation to investigate the local structure and dynamics of a model material Li7La3Zr2O12 and origin of its tetragonal to cubic phase transition. Our simulations were able to produce lattice parameter, neutron scattering, and conductivity data close to those gathered using experimental techniques, which allows us to study atomic-scale details of this complex material. First, it was found that lithium atoms primarily perform oscillation and "structured diffusion" dynamics in the tetragonal and cubic phase, respectively. Second, we believe that the tetragonal to cubic phase transition is an entropy-driven one that involves redistribution of lithium atoms among all tetrahedral sites. The transition is likely to initiate on the tetrahedral 8a site but needs the cooperation of neighboring octahedral 32g Li as relay atoms. Finally, it was found that a few types of lithium clusters dominate in both phases of Li7La3Zr2O12, which leads to highly correlated motion of lithium atoms. The local symmetry of these clusters dictates a "center-pass" mechanism as lithium goes through the bottleneck. This journal is

    Original languageEnglish (US)
    Pages (from-to)8758-8768
    Number of pages11
    JournalPhysical Chemistry Chemical Physics
    Volume17
    Issue number14
    DOIs
    StatePublished - Apr 14 2015

    Profile

    lithium
    atoms
    Atoms
    Spontaneous Fractures
    garnets
    simulation
    Traffic Accidents
    Garnets
    Phase transitions
    relay
    lattice parameters
    neutron scattering
    conductors
    entropy
    molecular dynamics
    conduction
    conductivity
    oscillations
    oxides
    symmetry

    ASJC Scopus subject areas

    • Physics and Astronomy(all)
    • Physical and Theoretical Chemistry

    Cite this

    Local structure and dynamics of lithium garnet ionic conductors : tetragonal and cubic Li7La3Zr2O7. / Klenk, Matthew; Lai, Wei.

    In: Physical Chemistry Chemical Physics, Vol. 17, No. 14, 14.04.2015, p. 8758-8768.

    Research output: Contribution to journalArticle

    Klenk, Matthew; Lai, Wei / Local structure and dynamics of lithium garnet ionic conductors : tetragonal and cubic Li7La3Zr2O7.

    In: Physical Chemistry Chemical Physics, Vol. 17, No. 14, 14.04.2015, p. 8758-8768.

    Research output: Contribution to journalArticle

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