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All-solid-state lithium batteries incorporating oxide-based solid electrolytes have attracted much attention as a promising battery system for enabling highly reversible Li metal anodes. However, the cycling stability of Li plating/stripping reactions at higher charging/discharging rates on garnet-type solid-state electrolytes must be improved to realize a practical Li metal anode for solid-state batteries. Here, we report that a short acid etching procedure performed in ambient air significantly activates the Ta-doped Li7La3Zr2O12 (LLZT) surface compared to polishing under inert gas atmosphere such as dry Ar. It has been believed that Li7La3Zr2O12 (LLZ) and related doped LLZ solid electrolyte surfaces need to be mechanically polished in dry Ar before the cell fabrication to remove Li2CO3 and LiOH that are present on the surface. However, a commonly used mechanical polishing procedure is found to form a thin electrochemically inactive layer on the LLZT surface, whereas a short acid etching procedure (e.g., HCl) removes the inactive layer, and the acid-etched LLZT exhibits excellent cycling stability.

Thin-film epitaxy is critical for investigating the original properties of materials. To obtain epitaxial films, careful consideration of the external conditions, i.e. single-crystal substrate, temperature, deposition pressure and fabrication method, is significantly important. In particular, selection of the single-crystal substrate is the first step towards fabrication of a high-quality film. Sapphire (single-crystalline α-Al2O3) is commonly used in industry as a thin-film crystal-growth substrate, and functional thin-film materials deposited on sapphire substrates have found industrial applications. However, while sapphire is a single crystal, two types of atomic planes exist in accordance with step height. Here we discuss the need to consider the lattice mismatch for each of the sapphire atomic layers. Furthermore, through cross-sectional transmission electron microscopy analysis, we demonstrate the uniepitaxial growth of cubic crystalline thin films on bistepped sapphire (0001) substrates.

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