Nonequilibrium DMFT approach to time-resolved Raman spectroscopy

TL;DR

This paper develops a nonequilibrium dynamical mean field theory approach to simulate time-resolved Raman spectroscopy, enabling analysis of nonlinear signals and frequency mixing in strongly correlated systems after photo-excitation.

Contribution

It introduces a formalism for calculating time-dependent Raman spectra within DMFT, including hyper Raman scattering and frequency mixing, applied to the Holstein-Hubbard model.

Findings

Demonstrates hyper Raman scattering with strong probe fields.

Simulates frequency mixing signals during pump-probe experiments.

Tracks evolution of Stokes and anti-Stokes features post photo-excitation.

Abstract

Raman spectroscopy uses light scattering to extract information on low-energy excitations of solids. The Raman process is described by diagrams which are fourth order in the light-matter interaction, and in particular the resonant contribution, which involves four different space-time arguments, is difficult to evaluate. If one instead simulates explicitly the incoming (classical) light pulse, the Raman signal is given by the outgoing photon flux and can be determined from a two-point correlation function. Such a formalism can be used to compute the time-resolved Raman spectrum of non-equilibrium systems, as well as nonlinear signals which are higher order in the incoming field, such as hyper Raman scattering. Here we explain how to implement this time-dependent formalism within the dynamical mean field theory framework. The method is illustrated with applications to the Holstein-Hubbard model in the strong electron-phonon coupling regime. We demonstrate hyper Raman scattering in measurements with strong probe fields and frequency mixing signals in the presence of a pump field, and simulate the evolution of Stokes and anti-Stokes features after photo-excitations of metallic and Mott insulating systems.