Pressure Tunable van Hove Singularities of Twisted Bilayer Graphene

The giant light–matter interaction induced by van Hove singularities (vHSs) of twisted bilayer graphene (tBLG) is responsible for enhanced optical absorption and strong photoresponse. Here, we investigated the evolution of vHSs in tBLG under pressure by using Raman spectroscopy. Pressure not only induces a blue shift of the G/R band but also tunes the intensity of the G/R band. The blue shift of the G/R band is due to the reduction of the in-plane lattice constant, and the variation of the G/R band intensity is due to the vHSs’ shift of tBLG. Moreover, the main band in the absorption spectrum of tBLG is attributed to multiple transitions from valence to conduction bands. Because the ratio of R to G band intensity increases under pressure and the origins of R and G bands are different, we claim that pressure enhances intervalley electron scattering. This study paves the way for pressure engineering of vHS and the corresponding photon–electron–phonon interaction in tBLG.