In situ and operando characterisation of Li metal – Solid electrolyte interfaces

The use of lithium metal as the negative electrode holds great promise for high energy density solid-state batteries (SSBs) of the future, but at the same time presents major technical challenges in their development. Li metal, with its high reactivity, soft and ductile nature, and propensity towards mechanical deformation during electrochemical cycling, is susceptible to the formation of various defects such as voids, cracks and filamentary deposits at the Li metal - solid electrolyte interface, that eventually cause rapid degradation of electrochemical cell performance. In order to gain insights into these interfacial processes and identify mechanisms for failure, in situ and operando characterisation approaches are essential. In this perspective, we present our opinions on the current state of such techniques, while highlighting the existing limitations and scope of these methods. We also endeavour to present opportunities for future research into developing and building on existing approaches to better evaluate the Li metal-solid electrolyte interface so as to guide the appropriate choice of materials to further enable efficient SSB architectures.