All‐solid‐state thin film lithium batteries (TFBs) are proposed as the ideal power sources for microelectronic devices. However, the high‐temperature (>500 °C) annealing process of cathode films, such as LiCoO2 and LiMn2O4, restricts the on‐chip integration and potential applications of TFBs. Herein, tunnel structured LixMnO2 nanosheet arrays are fabricated as 3D cathode for TFBs by a facile electrolyte Li+ ion infusion method at very low temperature of 180 °C. Featuring an interesting tunnel intergrowth structure consisting of alternating 1 × 3 and 1 × 2 tunnels, the LixMnO2 cathode shows high specific capacity with good structural stability between 2.0 and 4.3 V (vs. Li+/Li). By utilizing the 3D LixMnO2 cathode, all‐solid‐state LixMnO2/LiPON/Li TFB (3DLMO‐TFB) has been successfully constructed with prominent advantages of greatly enriched cathode/electrolyte interface and shortened Li+ diffusion length in the 3D structure. Consequently, the 3DLMO‐TFB device exhibits large specific capacity (185 mAh g−1 at 50 mA g−1), good rate performance, and excellent cycle performance (81.3% capacity retention after 1000 cycles), outperforming the TFBs using spinel LiMn2O4 thin film cathodes fabricated at high temperature. Importantly, the low‐temperature preparation of high‐performance cathode film enables the fabrication of TFBs on various rigid and flexible substrates, which could greatly expand their potential applications in microelectronics.

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Recently, a solid electrolyte material LiTa 2 PO 8 (LTPO) with a high room-temperature ionic conductivity (1.6 mS/cm) has been reported in experiment. To understand its Li transport mechanism and find its theoretical performance limit, we systematically investigate the properties of LTPO using density functional theory and ab initio molecular dynamic (AIMD) simulations. Our results show that LTPO is electrochemically stable with a wide electrochemical window. AIMD simulations indicate that Ta, P, and O are immobile during Li diffusion, indicating a high stability of the material. The Liion diffusion channels form a quasi-two-dimensional honeycomb framework. The intrinsic ionic conductivity of LTPO is predicted to be as high as 35.3 mS/cm at room temperature. The diffusion activation energy is only 0.16 eV, consisting of a low-energy barrier obtained from the minimum-energy path calculations. These results encourage further experimental studies on this promising solid-state electrolyte material.

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