Nonequilibrium DMFT approach to time-resolved Raman spectroscopy

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.

References in corpus (15)

• Inelastic Light Scattering From Correlated Electrons
• Theoretical description of time-resolved photoemission spectroscopy: application to pump-probe experiments
• Correlated electron systems periodically driven out of equilibrium: Floquet + DMFT formalism
• Nonequilibrium Steady State of Photoexcited Correlated Electrons in the Presence of Dissipation
• Interaction quench in the Holstein model: Thermalization crossover from electron- to phonon-dominated relaxation
• Femtosecond x-ray absorption spectroscopy of spin and orbital angular momentum in photoexcited Ni films during ultrafast demagnetization
• Theory of time-resolved optical spectroscopy on correlated electron systems
• Field-induced polaron formation in the Holstein-Hubbard model
• Novel Electron-Phonon Relaxation Pathway in Graphite Revealed by Time-Resolved Raman Scattering and Angle-Resolved Photoemission Spectroscopy
• Theory for Time-Resolved Resonant Inelastic X-ray Scattering
• Electronic Raman scattering in correlated materials: exact treatment of nonresonant, mixed, and resonant scattering with dynamical mean field theory
• The interplay of local electron correlations and ultrafast spin dynamics in fcc Ni
• Simulation of time-dependent resonant inelastic X-ray scattering using non-equilibrium dynamical mean-field theory
• Time-resolved photoemission and RIXS study of a site-selective Mott insulator
• Resonant Raman scattering effects in a nesting driven charge-density-wave insulator: exact analysis of the spinless Falicov-Kimball model with dynamical mean-field theory