Van Hove Singularity-Enhanced Raman Scattering and Photocurrent Generation in Twisted Monolayer–Bilayer Graphene

Twisted monolayer–bilayer graphene (TMBG) has recently emerged as an exciting platform for exploring correlated physics and topological states with rich tunability. Strong light–matter interaction was realized in twisted bilayer graphene, boosting the development of broadband graphene photodetectors from the visible to infrared spectrum with high responsivity. Extending this approach to the case of TMBG will help design advanced quantum nano-optoelectronic devices because of the reduced symmetry of the system. Here, we observe the formation of van Hove singularities (VHSs) in TMBG by monitoring the significant enhancement of the Raman intensity of the G peak and the intensity ratio of G and 2D peaks. The strong interlayer coupling also leads to the appearance of twist-angle-dependent Raman R and R′ peaks in TMBG. Furthermore, the constructed graphene photodetectors from 13.5°-TMBG show significantly enhanced photoresponsivity (∼31 folds of monolayer graphene and ∼15 folds of trilayer graphene) when the energy of incident photons matches the interval energy between the two VHSs in the conduction and valence bands. Our findings establish TMBG as a tunable platform for investigating the light–matter interaction and designing high-performance graphene photodetectors with combined high responsivity and high selectivity.