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

Strong optical nonlinearities play a central role in realizing quantum photonic technologies. In solid state systems, exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. Here, the interaction between excitons forms the basis of the polaritonic nonlinearity. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such ground state interactions is generally not sufficient to reach the regime of quantum nonlinear optics and strong single-polariton interactions. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities, as demonstrated with high-lying Rydberg states of cold atomic systems. Excitons in excited states have recently been observed in monolayer transition metal dichalcogenides. Here we demonstrate the formation of exciton-polaritons using the first excited excitonic state in monolayer tungsten diselenide (WSe2) embedded in a microcavity. Owing to the larger exciton size compared to their ground state counterpart, the realized polaritons exhibit an enhanced nonlinear response by more than an order of magnitude, as evidenced through a modification of the cavity Rabi splitting. The demonstration of excited exciton-polaritons in two-dimensional semiconductors and their enhanced nonlinear response presents the first step towards the generation of strong photon interactions in solid state systems, a necessary building block for quantum photonic technologies.