Local structure and dynamics of lithium garnet ionic conductors: A model material Li5La3Ta2O12

Yuxing Wang, Matthew Klenk, Katharine Page, Wei Lai

    Research output: Research - peer-reviewArticle

    • 24 Citations

    Abstract

    In this article, we combined two complementary structure/dynamics probes, i.e., total-scattering/reverse Monte Carlo (RMC) modeling and classical molecular dynamics (MD), in order to understand local lithium structure and dynamics in a model disordered garnet oxide Li5La3Ta2O12. By examining the configurations from RMC and trajectories from MD, we individually and statistically analyzed the lithium distribution and dynamics within tetrahedral (Td) cages, octahedral (Oh) cages, and triangular bottlenecks. We found that lithium atoms within either Td or Oh cages prefer to stay at the off-center positions and close to one of the triangular bottlenecks. This is likely caused by the uneven Li-Li interaction in the form of lithium clusters, and such geometrical frustration leads to the local structure instability and fast ionic conduction. Both RMC and MD studies support that the lithium conduction path goes through the triangular bottleneck in a 3D continuous network of Td/Oh cages, without a direct Oh to Oh jump. However, the conduction mechanism should not be generalized, as it is greatly influenced by the local environment or temperature. Broadly speaking, lithium atoms hop through the bottleneck from an edge-passing mechanism at low temperatures to a center-passing mechanism at higher temperatures. (Figure Presented).

    LanguageEnglish (US)
    Pages5613-5624
    Number of pages12
    JournalChemistry of Materials
    Volume26
    Issue number19
    DOIs
    StatePublished - Oct 14 2014

    Profile

    Garnets
    Lithium
    Molecular dynamics
    Temperature
    Atoms
    Ionic conduction
    Oxides
    Trajectories
    Scattering

    ASJC Scopus subject areas

    • Materials Chemistry
    • Chemical Engineering(all)
    • Chemistry(all)

    Cite this

    Local structure and dynamics of lithium garnet ionic conductors : A model material Li5La3Ta2O12. / Wang, Yuxing; Klenk, Matthew; Page, Katharine; Lai, Wei.

    In: Chemistry of Materials, Vol. 26, No. 19, 14.10.2014, p. 5613-5624.

    Research output: Research - peer-reviewArticle

    Wang, Yuxing ; Klenk, Matthew ; Page, Katharine ; Lai, Wei. / Local structure and dynamics of lithium garnet ionic conductors : A model material Li5La3Ta2O12. In: Chemistry of Materials. 2014 ; Vol. 26, No. 19. pp. 5613-5624
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