Robust and Manufacturable Lithium Lanthanum Titanate-Based Solid-State Electrolyte Thin Films Deposited in Open Air

State-of-the-art solid-state electrolytes (SSEs) are limited in their energy density and processability based on thick, brittle pellets, which are generally hot pressed in vacuum over the course of several hours. We report on a high-throughput, open-air process for printable thin-film ceramic SSEs in a remarkable one-minute time frame using a lithium lanthanum titanium oxide (LLTO)-based SSE that we refer to as robust LLTO (R-LLTO). Powder XRD analysis revealed that the main phase of R-LLTO is polycrystalline LLTO, accompanied by selectively retained crystalline precursor phases. R-LLTO is highly dense and closely matched to the stoichiometry of LLTO with some heterogeneity throughout the film. A minimal presence of lithium carbonate is identified despite processing fully in ambient conditions. The LLTO films exhibit remarkable mechanical properties, demonstrating both flexibility with a low modulus of ∼35 GPa and a high fracture toughness of >2.0 . We attribute this mechanical robustness to several factors, including grain boundary strengthening, the presence of precursor crystalline phases, and a decrease in crystallinity or ordering caused by ultrafast processing. The creation of R-LLTO-a ceramic material with elastic properties that are closer to polymers with higher fracture toughness-enables new possibilities for the design of robust solid-state batteries.