In order to investigate structural changes in lithium manganese oxide during the insertion and extraction of lithium ions, Raman spectra of thin films of Li1-xMn2O4 produced by electrostatic spray deposition (ESD) were recorded in situ during a voltammetric scan in 1 M LiClO4 in propylene carbonate (PD)/ethylene carbonate (EC) solutions. Five Raman-active bands, as predicted by the theory, were observed for the Li1-xMn2O4 compound. The X-MnO2 phase has a distinct band at 592 cm(-1) and therefore can be clearly recognized from Raman spectra. The changes observed in Raman lines of Li1-xMn2O4 were ascribed to the occurrence of the phase transition of Li1-xMn2O4 electrodes. From the energy-dependence of Raman spectra, it is suggested that each value of x in Li1-xMn2O4 possesses its own electronic band structure. (C) 2003 Elsevier Science B.V. All rights reserved.