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The vanadium oxide thin films are prepared on zinc selenide by DC magnet sputtering method. The optical character changing of vanadium oxide thin films are tested by CO2 laser, some phenomena is observed. The components are gotten by The X-ray photoelectron spectroscopy (XPS). By utilizing the Castep program package of the Material Studio simulation tool, based on local density function approximation and pseudo-potential method, optimization for the geometric structure of vanadium dioxides is accomplished with the BFGS calculate way. Using the super soft pseudo-potential of reciprocal space lattice, the optical characteristics of crystal are calculated within the 7 μm scope. Furthermore, some trends can be concluded from the extended estimation for the optical characteristics at 10.6 μm by formula.