▎ 摘　　要

To distinguish defects in defective single-layer graphene (DSLG), we developed a method combining first principles density functional theory and tight-binding that quantifies defect-induced Raman intensities. Analysis of defect potentials for defects with vacancies and/or bond rotation has shown that on-site variation dominates the scattering, and also quantified effects of oxygen adsorption. Defect potentials for DSLG were subsequently used in calculation of the electron-defect matrix elements and Raman intensities. I(D)/I(D') intensity ratios, dependent on defect topology and oxygen impurity adsorption, were elucidated for mono-vacancy, double-vacancy, Stone-Wales, and so-called 555-777 and 5555-6-7777 point defects in single-layer graphene. The results demonstrated for the first time the ability to distinguish between these defect types, also as dependent of oxygen adsorption, and were found consistent with a measured value for vacancies. Importantly, our theoretical prediction of the I(D)/I(D') Raman intensity signature metric can assist in experimental characterization of defective realistic graphene samples for any defect type. Finally, analytical analysis of the angular dependence of the electron-defect scattering matrix elements revealed a node effect in intra-valley backscattering but not in inter-valley backscattering, rationalizing the observation that the D' band intensity is mostly weaker than that of the D band. Published by Elsevier Ltd.