Steady-state nonlinear optical response of excitons in monolayer MoSe

MS Rana, JR Hendrickson, CE Stevens… - arXiv preprint arXiv …, 2021 - arxiv.org
MS Rana, JR Hendrickson, CE Stevens, MR Koehler, DG Mandrus, T Taniguchi
arXiv preprint arXiv:2109.12160, 2021arxiv.org
Monolayer transition metal dichalcogenide (TMD) semiconductors such as MoSe $ _2 $ host
strongly bound excitons which are known to exhibit a strong resonant third-order nonlinear
response. Although there have been numerous studies of the ultrafast nonlinear response of
monolayer TMDs, a study of the steady-state nonlinear response is lacking. We report a
comprehensive study of the steady-state two-color nonlinear response of excitons in hBN-
encapsulated monolayer MoSe $ _2 $ at 7 K. We observe differential transmission (DT) …
Monolayer transition metal dichalcogenide (TMD) semiconductors such as MoSe host strongly bound excitons which are known to exhibit a strong resonant third-order nonlinear response. Although there have been numerous studies of the ultrafast nonlinear response of monolayer TMDs, a study of the steady-state nonlinear response is lacking. We report a comprehensive study of the steady-state two-color nonlinear response of excitons in hBN-encapsulated monolayer MoSe at 7 K. We observe differential transmission (DT) signals associated with the neutral and charged exciton species, which is strongly dependent on the polarization of the pump and probe. Our results are compared to a theoretical model based on a T-matrix formulation for exciton-exciton, exciton-trion, and trion-trion correlations. The parameters are chosen such that the theory accurately reproduces the experimental DT spectrum, which is found to be dominated by two-exciton correlations without strong biexciton binding, exciton-trion attractive interactions, and strong spin mixing through incoherent relaxation.
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