Multidimensional coherent spectroscopy(MDCS)has been established in quantum chemistry as a powerful tool for studying the nonlinear response and nonequilibrium dynamics of molecular systems.More recently,the technique...Multidimensional coherent spectroscopy(MDCS)has been established in quantum chemistry as a powerful tool for studying the nonlinear response and nonequilibrium dynamics of molecular systems.More recently,the technique has also been applied to correlated electronmaterials,where the interplay of localized and itinerant states makes the interpretation of the spectra more challenging.Here we use the Keldysh contour representation of effective models and nonequilibrium dynamical mean field theory to systematically study theMDCSsignals of prototypical correlated lattice systems.By analyzing the current induced by sequences of ultrashort laser pulseswe demonstrate the usefulness ofMDCS as a diagnostic tool for excitation pathways and coherent processes in correlated solids.Wealso show that this technique allows to extract detailed information on the nature and evolution of photo-excited nonequilibrium states.展开更多
基金supported by the Swiss National Science Foundation through the Research Unit QUAST of Deutsche Foschungsgemeinschaft(FOR5249)Grant No.200021-196966.The calculations were performed on the Beo05 cluster at the University of Fribourg.
文摘Multidimensional coherent spectroscopy(MDCS)has been established in quantum chemistry as a powerful tool for studying the nonlinear response and nonequilibrium dynamics of molecular systems.More recently,the technique has also been applied to correlated electronmaterials,where the interplay of localized and itinerant states makes the interpretation of the spectra more challenging.Here we use the Keldysh contour representation of effective models and nonequilibrium dynamical mean field theory to systematically study theMDCSsignals of prototypical correlated lattice systems.By analyzing the current induced by sequences of ultrashort laser pulseswe demonstrate the usefulness ofMDCS as a diagnostic tool for excitation pathways and coherent processes in correlated solids.Wealso show that this technique allows to extract detailed information on the nature and evolution of photo-excited nonequilibrium states.
