Multidimensional coherent spectroscopy of correlated lattice systems

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 electron materials, 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 the MDCS signals of prototypical correlated lattice systems. By analyzing the current induced by sequences of ultrashort laser pulses we demonstrate the usefulness of MDCS as a diagnostic tool for excitation pathways and coherent processes in correlated solids. We also show that this technique allows to extract detailed information on the nature and evolution of photo-excited nonequilibrium states. This data base provides data and the generating python script of all the figures in the publication https://doi.org/10.1038/s41524-025-01619-0.

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Publication Details

Journal
Zenodo (CERN European Organization for Nuclear Research)
Published
2025-05-09
DOI
https://doi.org/10.5281/zenodo.15880121
Primary Topic
Laser-Matter Interactions and Applications
Type
article
Field-Weighted Citation Impact
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article

Multidimensional coherent spectroscopy of correlated lattice systems

Zenodo (CERN European Organization for Nuclear Research)
Laser-Matter Interactions and Applications
article

Multidimensional coherent spectroscopy of correlated lattice systems

article en

Abstract

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 electron materials, 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 the MDCS signals of prototypical correlated lattice systems. By analyzing the current induced by sequences of ultrashort laser pulses we demonstrate the usefulness of MDCS as a diagnostic tool for excitation pathways and coherent processes in correlated solids. We also show that this technique allows to extract detailed information on the nature and evolution of photo-excited nonequilibrium states. This data base provides data and the generating python script of all the figures in the publication https://doi.org/10.1038/s41524-025-01619-0.

Zenodo (CERN European Organization for Nuclear Research)
University of Fribourg (CH)
Openalex Percentile: Top 58%
Laser-Matter Interactions and Applications
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Multidimensional coherent spectroscopy of correlated lattice systems · Zenodo (CERN European Organization for Nuclear Research) (2025) | TGRS Research Map | TGRS