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.

The coupling of mechanical deformation and electrical stimuli at the nanoscale has been the subject of intense investigation in the realm of materials science. Recently, twisted van der Waals (vdW) materials have emerged as a platform for exploring exotic quantum states. These states are intimately tied to the formation of moiré superlattices, which can be visualized by directly exploiting the electromechanical response. However, the origin of the response, even in twisted bilayer graphene (tBLG), remains unsettled. Here, employing lateral piezoresponse force microscopy (LPFM), we investigate the electromechanical responses of marginally twisted graphene moiré superlattices with different layer thicknesses. We observe distinct LPFM amplitudes and spatial profiles in tBLG and twisted monolayer-bilayer graphene (tMBG), exhibiting effective in-plane piezoelectric coefficients of 0.05 and 0.35 pm/V, respectively. Force tuning experiments further underscored a marked divergence in their responses. The contrasting behaviors suggest different electromechanical couplings in tBLG and tMBG. In tBLG, the response near the domain walls is attributed to the flexoelectric effect, while in tMBG, the behaviors can be comprehended within the context of the piezoelectric effect. Our results not only provide insights into electromechanical and corporative effects in twisted vdW materials with different stacking symmetries but may also offer a way to engineer them at the nanoscale.

Manipulating the flat band degeneracy and thus getting the correlated insulating phases has been an ideal thread for realizing the exotic quantum phenomenon in the moiré system. To achieve this goal, the delicately tuned twist angle and a substantial displacement field (D) are rigorously requested. Here, we report our scanning tunneling microscope (STM) work on reaching these correlated insulating states in twisted monolayer-bilayer graphene through a decorated tip. It acts as a local top gate, leading to an enhanced local D, and enables us to fully lift the 8-fold degeneracy of the flat bands. With the aid of this technique, we further expand the correlated insulating states into a more tolerant twist angle that is down to 0.92°. Moreover, the correlated insulating phases in the hole-doping regime are realized. Our tip decoration method allows us to integrate the STM study with the high displacement field for the correlated phases in the twisted moiré systems.