Phonon-assisted processes in the ultraviolet-transient optical response of graphene

Abstract

Many recent experiments investigated potential and attractive means of modifying many-body interactions in two-dimensional materials through time-resolved spectroscopy techniques. However, the role of ultrafast phonon-assisted processes in two-dimensional systems is rarely discussed in depth. Here, we investigate the role of electron–phonon interaction in the transient optical absorption of graphene by means of first-principles methods. It is shown at equilibrium that the phonon-assisted transitions renormalize significantly the electronic structure. As a result, absorption peak around the Van-Hove singularity broadens and redshifts by ~100 meV. In addition, temperature increase and chemical doping are shown to notably enhance these phonon-assisted features. In the photoinduced transient response, we obtain spectral changes in close agreement with the experiments, and we associate them to the strong renormalization of occupied and unoccupied π bands, which predominantly comes from the coupling with the zone-center E2g optical phonon. Our estimation of the Coulomb interaction effects shows that the phonon-assisted processes can have a dominant role even in the subpicosecond regime.