Microstructural impacts on ionic conductivity of oxide solid electrolytes from a combined atomistic-mesoscale approach

• DOI: 10.1038/s41524-021-00681-8
• Publication Date: 2021-12-21T23:02:22Z
• Authors: Tae Wook Heo; Andrew Grieder; Bo Wang; Marissa Wood; Tim Hsu; Sneha A. Akhade; Liwen F. Wan; Long-Qing Chen; Nicole Adelstein; Brandon C. Wood
• Keywords: Mesoscopic physics; Fast ion conductor

Abstract Although multiple oxide-based solid electrolyte materials with intrinsically high ionic conductivities have emerged, practical processing and synthesis routes introduce grain boundaries other interfaces that can perturb primary conduction channels. To directly probe these effects, we demonstrate an efficient general mesoscopic computational method capable of predicting effective conductivity through a complex polycrystalline microstructure without relying on simplified equivalent circuit description. We parameterize the framework for Li 7- x La 3 Zr 2 O 12 (LLZO) garnet by combining synthetic microstructures from phase-field simulations diffusivities molecular dynamics ordered disordered systems. Systematically designed reveal interdependence between atomistic microstructural impacts LLZO, quantified newly defined metrics characterize transport mechanism. Our results provide fundamental understanding physical origins reported variability in based extensive analysis literature data, while simultaneously outlining design guidance achieving desired properties conditions which sensitivity to features is highest. Additional implications our are discussed, including possible connection ion behavior dendrite formation.