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

TL;DR

This paper explores how ultrafast phonon-assisted processes influence the transient optical response of graphene, revealing significant renormalization of electronic structure and spectral features through first-principles calculations.

Contribution

It provides a detailed first-principles analysis of electron-phonon interactions in graphene's transient optical absorption, highlighting the dominant role of phonon-assisted processes.

Findings

Phonon-assisted transitions significantly renormalize graphene's electronic structure.

Temperature and doping enhance phonon-assisted features.

Spectral changes in transient response align with experimental observations.

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 around 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 $\pi$ bands, which predominantly comes from the coupling with the zone-center $E_{2g}$ 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.