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Local crystalline structures of LiCoO 2 nanothin film cathodes in a lithium ion battery have been spectroscopically elucidated through confocal Raman imaging analysis at high spatial resolution of several hundred nanometers. A significant difference in the crystalline structure is found between the nanometric thin films and bulk powders. Thermally induced local decomposition of LiCoO 2 into an impurity phase on the films has also been revealed along with the mechanism of the temperature-triggered decomposition process. Moreover, frequency-based Raman imaging enables us to locally probe spatial separation between stoichiometric (LiCoO 2 ) and non-stoichiometric (Li 1-x CoO 2 , 0 &lt; x &lt; 1) crystal phases on the thin films. Such local crystalline analysis is a promising approach to provide new insights into the degradation mechanism of lithium-ion batteries, which would result in improving the performance of thin film-based lithium ion batteries.

Raman Imaging Analysis of Local Crystal Structures in LiCoO2 Thin Films Calcined at Different Temperatures