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Strong optical nonlinearities play a central role in realizing quantumphotonic technologies. In solid state systems, exciton-polaritons, which resultfrom the hybridization of material excitations and cavity photons, are anattractive candidate to realize such nonlinearities. Here, the interactionbetween excitons forms the basis of the polaritonic nonlinearity. While theinteraction between ground state excitons generates a notable opticalnonlinearity, the strength of such ground state interactions is generally notsufficient to reach the regime of quantum nonlinear optics and strongsingle-polariton interactions. Excited states, however, feature enhancedinteractions and therefore hold promise for accessing the quantum domain ofsingle-photon nonlinearities, as demonstrated with high-lying Rydberg states ofcold atomic systems. Excitons in excited states have recently been observed inmonolayer transition metal dichalcogenides. Here we demonstrate the formationof exciton-polaritons using the first excited excitonic state in monolayertungsten diselenide (WSe2) embedded in a microcavity. Owing to the largerexciton size compared to their ground state counterpart, the realizedpolaritons exhibit an enhanced nonlinear response by more than an order ofmagnitude, as evidenced through a modification of the cavity Rabi splitting.The demonstration of excited exciton-polaritons in two-dimensionalsemiconductors and their enhanced nonlinear response presents the first steptowards the generation of strong photon interactions in solid state systems, anecessary building block for quantum photonic technologies.

Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2