Fast charge-transfer at the self-assembled solid electrolyte interface (SEI) has been obtained in an all-solid-state ceramic lithium battery. The SEI phase was formed between a Li-AI anode and the thio-LISICON (Li_(3.25)Ge_(0.25)P_(0.75)S_4) solid electrolyte by applying current though the cell. After the spontaneous formation of the SEI phase, the interfacial resistance fluctuated and decreased to constant values during the charge-and-discharge process. The breathing interface effectively makes a close contact at the electrolyte/electrode boundary and promotes fast charge transfer at the solid-interface. The self-assembled SEI phase is a general concept of interfacial design and will play a crucial role in the development of all solid-state batteries.
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