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Atomic Defect Mediated Li-Ion Diffusion in a Lithium Lanthanum Titanate Solid-State Electrolyte.

Lithium lanthanum titanium oxide (LLTO) as a fast Li-ion conductor is a promising candidate for future all-solid-state Li batteries. Fundamental understanding of the microstructure of LLTO and its effect on the Li+ diffusion mechanism, especially across different length scales and interfaces, is a prerequisite to improving the material design and processing development of oxide-based solid electrolytes. Herein, through detailed structural analysis of LLTO ceramic pellets by aberration-corrected transmission electron microscopy, we discovered previously unreported intrinsic planar defects in LLTO single-crystal grains. These planar defects feature an antiphase boundary along specific crystal planes with a "rock-salt" structure enriched by Li within a few atomic layers. Corroborated by density-functional-theory-based calculations, we show an increased diffusion barrier across these planar defects inevitably lowers the bulk Li+ diffusivity of the oxide electrolyte.