Journal
PHYSICAL REVIEW LETTERS
Volume 116, Issue 13, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.116.135901
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Funding
- French National Research Agency (Labex STORE-EX) [ANR-10-LABX-0076]
- OCCIGEN (CINES) [x2015097321]
- Royal Society [UF130329]
- EoCoE - European Union [H2020-EINFRA-2015-1-676629]
- Engineering and Physical Sciences Research Council [EP/K016288/1] Funding Source: researchfish
- EPSRC [EP/K016288/1] Funding Source: UKRI
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We have performed long time scale molecular dynamics simulations of the cubic and tetragonal phases of the solid lithium-ion electrolyte Li7La3Zr2O12 (LLZO), using a first-principles parametrized interatomic potential. Collective lithium transport was analyzed by identifying dynamical excitations: persistent ion displacements over distances comparable to the separation between lithium sites, and stringlike clusters of ions that undergo cooperative motion. We find that dynamical excitations in c-LLZO (cubic) are frequent, with participating lithium numbers following an exponential distribution, mirroring the dynamics of fragile glasses. In contrast, excitations in t-LLZO (tetragonal) are both temporally and spatially sparse, consisting preferentially of highly concerted lithium motion around closed loops. This qualitative difference is explained as a consequence of lithium ordering in t-LLZO and provides a mechanistic basis for the much lower ionic conductivity of t-LLZO compared to c-LLZO.
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