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Ion transport across solid solid interfaces is often slower than through thebulk of a material, impeding the charge and discharge rate of batteries.Designing highly conductive interfaces is challenging due to the need to probeion conduction at individual interfaces and correlate it with the localstructure. In this study, we address this challenge by enabling thesimultaneous measurements of local Li-dominated optical phonons and iondistributions, using high-energy and high-spatial-resolution spectroscopy in ascanning transmission electron microscope (STEM). Further, this method allowsfor a direct correlation of ion conduction with interfacial structuresidentified by STEM imaging. By examining diverse individual interfaces ofLiCoO2, we reveal the sensitivity of ion conduction to interface atomic-scalestructure and chemistry. Our method enables correlative analysis of iontransport behavior, and atomic and band structures, and can serve as a robustexperimental approach for identifying interface structures that offer highconductivity and cyclability for batteries.

Probing Lithium Ion Transport at Individual Interfaces