“…Enabling the Li metal anode in a solid-state battery (SSB) promises to attain specific cell energy densities above 400 Wh/kg and 1200 Wh/L. − However, significant materials and processing challenges are disrupting the materialization of working SSBs at present. , A major challenge in bridging this gap lies in the development of practical and feasible thin, dense, solid electrolyte (SE) membranes that can be processed at scale. − Additionally, it is widely understood in the SSB research that the pathways for processing solid electrolytes dictate the local microstructures, pore distributions, grain sizes, and lattice stress, , all of which play a critical role in their performance. There is a large body of work that conclusively shows that the stochasticity of microstructure and phases within the bulk solid electrolyte strongly contribute to the failure modes of the solid-state batteries. − Thus, it is imperative to achieve a high degree of control over the microstructure of solid electrolytes to nullify this failure mode in solid electrolytes.…”