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Development of solid-state electrolyte (SSE) thin films is a key toward the fabrication of all-solid-state batteries (ASSBs). However, it is challenging for conventional deposition techniques to deposit uniform and conformal SSE thin films in a well-controlled fashion. In this study, atomic layer deposition (ALD) was used to fabricate lithium silicate thin films as a potential SSE for ASSBs. Lithium silicates thin films were deposited by combining ALD Li₂O and SiO₂ subcycles using lithium tert-butoxide, tetraethylorthosilane, and H₂O as precursors. Uniform and self-limiting growth was achieved at temperatures between 225 and 300 °C. X-ray absorption spectroscopy analysis disclosed that the as-deposited lithium silicates were composed of SiO₄ tetrahedron structure and lithium oxide as the network modifier. X-ray photoelectron spectroscopy confirmed the chemical states of Li in the thin films were the same with that in …