Probing Dark Excitons in Monolayer MoS2 by Nonlinear Two-Photon Spectroscopy

We report a new dark exciton in monolayer MoS2 using second harmonic generation spectroscopy. Hereby, the spectrally dependent second harmonic generation intensity splits into two branches, and an anticrossing is observed at ∼25 meV blue detuned from the bright neutral exciton. These observations are indicative of coherent quantum interference arising from strong two-photon light-matter interaction with an excitonic state that is dark for single photon interaction. The existence of the dark state is supported by engineering its relaxation to bright localized excitons, mediated by vibrational modes of a proximal nanobeam cavity. We show that two-photon light-matter interaction involving dark states has the potential to control relaxation pathways induced by nanostructuring the local environment. Moreover, our results indicate that dark excitons have significant potential for nonlinear quantum devices based on their nontrivial excitonic photophysics.