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

Yuxing Wang, Matthew Klenk, Katharine Page, Wei Lai

Research output: Contribution to journalArticle

  • 27 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
Ionic conduction
Atoms
Temperature
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: Contribution to journalArticle

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
@article{9cfc4e4edb9f4dfca8038e7e14e3deb0,
title = "Local structure and dynamics of lithium garnet ionic conductors: A model material Li5La3Ta2O12",
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).",
author = "Yuxing Wang and Matthew Klenk and Katharine Page and Wei Lai",
year = "2014",
month = "10",
day = "14",
doi = "10.1021/cm502133c",
language = "English (US)",
volume = "26",
pages = "5613--5624",
journal = "Chemistry of Materials",
issn = "0897-4756",
publisher = "American Chemical Society",
number = "19",

}

TY - JOUR

T1 - Local structure and dynamics of lithium garnet ionic conductors

T2 - Chemistry of Materials

AU - Wang,Yuxing

AU - Klenk,Matthew

AU - Page,Katharine

AU - Lai,Wei

PY - 2014/10/14

Y1 - 2014/10/14

N2 - 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).

AB - 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).

UR - http://www.scopus.com/inward/record.url?scp=84910620591&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84910620591&partnerID=8YFLogxK

U2 - 10.1021/cm502133c

DO - 10.1021/cm502133c

M3 - Article

VL - 26

SP - 5613

EP - 5624

JO - Chemistry of Materials

JF - Chemistry of Materials

SN - 0897-4756

IS - 19

ER -