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Structures of polyimide (6051) films modified by irradiation of 2.0 MeV Si ions with different fluences are studied in detail. Variations of the functional groups in polyimide are investigated by attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and Raman spectroscopy. The results indicate that the functional groups can be destroyed gradually with the increasing ion fluence. The variations of structure and element contents are characterized by x-ray diffraction (XRD), Rutherford backscattering spectrometry (RBS) and x-ray photoelectron spectroscopy (XPS). The results indicate that the contents of N and O decrease significantly compared with the original samples, some graphite-like and carbon-rich phases are formed in the process of irradiation.