Epitaxial graphene on SiC without substrate interaction is viewed as one of the most promising two-dimensional (2D) materials in the microelectronics field. In this study, quasi-free-standing bilayer epitaxial graphene (QFSBEG) on SiC was fabricated by H2 intercalation under different time periods, and the temperature-dependent Raman spectra were recorded to evaluate the intrinsic structural difference generated by H2 time duration. The G peak thermal lineshift rates dω/dT showed that the H2 intercalation significantly weakened the pinning effect in epitaxial graphene. Furthermore, the G peak dω/dT value showed a perspicuous pinning effect disparity of QFSBEG samples. Additionally, the anharmonic phonon effect was investigated from the Raman lineshift of peaks. The physical mechanism responsible for dominating the G-mode temperature-dependent behavior among samples with different substrate coupling effects was elucidated. The phonon decay process of different samples was compared as the temperature increased. The evolution from in situ grown graphene to QFSBEG was determined. This study will expand the understanding of QFSBEG and pave a new way for its fabrication.
