All-solid-state batteries offer great promise for safer and higher-energy-density storage compared to conventional liquid-based Li-ion batteries. However, their practical use is hindered by high resistance caused by heterogeneity of structure and chemistry at the solid-state interfaces. To overcome these challenges, atomic-scale visualization of the interfaces and a detailed understanding of the correlation between interfacial structure, chemistry and processing conditions is critical. In this work, we use a combination of first-principles simulation and high-resolution scanning transmission electron microscopy with spatially-resolved electron energy loss spectroscopy to probe complex interfacial structures and chemistry in all-solid-state lithium batteries. We will further address how the processing conditions to prepare the interfaces will affects their structures, local chemistries and Li-ion conductivity through these interfaces.

This work of was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.