Publication date: 21st July 2025
The investigation of thin-film battery materials is essential for the development of future technologies capable of enabling highly miniaturized energy storage systems for critical applications, such as compact electronics, medical implants, and the Internet of Things (IoT). Thin layers also serve as exceptional model systems for gaining a fundamental understanding of diffusion phenomena within bulk materials and across interfaces. Due to their simple geometry and versatility, these thin films enable the creation of synthetic systems that can be representative of large-scale battery architectures.
In this work, we present several examples where thin films are utilized in combination with non-destructive optical techniques to provide insights into material changes during operation. Specifically, this study highlights the potential of operando spectroscopic ellipsometry and Tip-Enhanced Raman Spectroscopy for the real-time investigation of cathode materials.
Beyond their use as model systems, significant efforts over the past decades have been directed toward extending this approach to real devices. To date, one of the few commercially successful thin-film energy storage devices is the lithium solid-state battery (SSB) that incorporates a lithium phosphorus oxynitride (LiPON) electrolyte. Among alternative ceramic electrolytes, the NASICON-type superionic conductor Li₁₊ₓAlₓTi₂₋ₓ(PO₄)₃ (LATP) is particularly promising due to its high ionic conductivity (approximately 1 mS·cm⁻¹) and its stability in ambient air at elevated temperatures.
In this talk, we will discuss our recent progress in the integration of thin films into ceramic SSBs and the development of novel tools for materials research and device implementation. To achieve this, LATP[1] and various electrode materials were deposited using Large-Area Pulsed Laser Deposition. Spinel-type LiMn₂O₄[2] and Li₄Ti₅O₁₂[3], as well as olivine-type LiFePO₄, were selected due to their excellent stability, low cost, and environmental compatibility. Bi-layers consisting of LATP and these electrode materials were fabricated to investigate the structure and properties of their interfaces.
[1] V. Siller, J. C. Gonzalez-Rosillo, M. Nuñez-Eroles, M. Stchakovsky, R.Arenal, A. Morata*, A. Tarancón, Safe extended-range cycling of Li4Ti5O12-based anodes for ultra-high capacity thin-film batteries, Materials Today Energy, 25, 2022, pp.100979
[2] V. Siller, J. C. Gonzalez-Rosillo, M. Nuñez-Eroles, F. Baiutti, M. Oskar Liedke, M.Butterling, A. G. Attallah, E. Hirschmann, A. Wagner, A. Morata*, A. Tarancón, High Nanoscaled LiMn2O4 for Extended Cycling Stability in the 3 V Plateau, ACS applied materials & interfaces. 14, 2022 pp. 33438.
[3] V. Siller, J. C. Gonzalez-Rosillo, M. Nuñez-Eroles, M. Stchakovsky, R.Arenal, A. Morata*, A. Tarancón, Safe extended-range cycling of Li4Ti5O12-based anodes for ultra-high capacity thin-film batteries, Materials Today Energy, 25, 2022, pp.100979
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