First-principles description of the exciton-phonon interaction: A cumulant approach

Abstract

Electron-phonon coupling leads to intriguing effects in the spectra of materials. Current approximations to calculate spectra most often describe this coupling insufficiently. Starting from basic equations of many-body perturbation theory, we derived a cumulant formulation for neutral excitation spectra that contains excitonic effects and the coupling between excitons and phonons. The cumulant approach allows us to include dynamical effects arising from the electron-phonon coupling in a simple and intuitive way. It can be implemented as a postprocessing of state-of-the-art $GW$-plus-Bethe-Salpeter calculation of excitonic states and a density functional perturbation theory calculation of phonons and electron-phonon coupling. We demonstrate that, in order to obtain a consistent treatment of exciton-phonon coupling, diagrams have to be taken into account that can be neglected when the effect of lattice vibrations is treated in a static or quasistatic approximation. From the application of this approach to a model system, we analyzed the main features of the exciton-phonon interaction and provided a general picture of their link with the properties of materials such as exciton mass and exciton Bohr radius.