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We have developed a microscopic many-body theory of two-dimensional coherentspectroscopy (2DCS) for a model of polarons in one-dimensional (1D) materials.Our theory accounts for contributions from all three processes: excited-stateemission (ESE), ground-state bleaching (GSB), and excited-state absorption(ESA). While the ESE and GSB contributions can be accurately described using aChevy's ansatz with one particle-hole excitation, the ESA process requiresinformation about the many-body eigenstates involving two impurities. Tocalculate these double polaron states, we have extended the Chevy's ansatz withone particle-hole excitation. The validity of this ansatz was verified bycomparing our results with an exact calculation using Bethe's ansatz. Ournumerical results reveal that in the weak interaction limit, the ESAcontribution cancels out the total ESE and GSB contributions, resulting in lesssignificant spectral features. However, for strong interactions, the featuresof the ESA contribution and the combined ESE and GSB contributions remainobservable in the 2DCS spectra. These features provide valuable informationabout the interactions between polarons. Additionally, we have investigated themixing time dynamics, which characterize the quantum coherences of the polaronresonances. Overall, our theory provides a comprehensive framework forunderstanding and interpreting the 2DCS spectra of polarons in 1D materials,shedding light on their interactions and coherent dynamics.

Microscopic many-body theory of two-dimensional coherent spectroscopy of exciton-polarons in one-dimensional materials