Lithium-ion batteries (LIBs) have transformed the use of mobile electronicsand storage technologies. Alongside advances in materials, an in-depthunderstanding of the interfacial phenomena and interphase formationmechanisms in LIBs is crucial. Interphases are widely recognized as the mostimportant and the least understood components of LIBs and play a directrole in defining cell performance, cyclability, and safety. This article presentsa review of recent developments in vibrational spectroscopy techniques ofRaman, infrared, and sum-frequency generation spectroscopies to probethe fundamental aspects of interphases on the anode and cathode of LIBs.First the vibrational spectroscopy techniques and their relevant technicalconsiderations for interphase characterization are briefly introduced. In thenext step, the latest studies on the fundamental properties, composition, andstructure of interphases employing vibrational spectroscopy techniques arepresented. This review focuses on in situ/operando investigations; however,post-mortem studies are also discussed briefly.
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