AbstractRaman spectra excited at two laser wavelengths are used to study the damage in self‐implanted silicon. Depending on the implantation conditions, a three‐layer structure can be constructed: a damaged surface crystalline layer (dsc‐Si), an amorphous layer (a‐Si) and a damaged interior crystalline layer (dic‐Si). Raman spectra can provide the structural details of these layers, together with the Rutherford backscattering–chanelling technique. Examination of the scattering intensities shows that the contribution to the Raman signals from different layers can be distinguished and separated. Further analysis of the Raman data reveals a defect‐activated low‐frequency band in the dsc‐Si layer which is sensitive to the damage and may be used for the characterization of dsc‐Si. For totally amorphlzed samples the two Raman spectra excited at 457.9 and 647.1 nm show different scattering intensity ratios for the optical‐ and acoustic‐like phonons. This novel result may indicate a depth‐dependent variation of the disordering in the amorphous layer. Quantitative comparison between the calculated and measured Raman scattering intensities provides the scattering efficiency ratios of dsc‐Si and a‐Si in samples compris