Nature Communications 12, 2269 (2021)
J. Gu, V. Walther, L. Waldecker, D. Rhodes, A. Raja, J. C. Hone, T. F. Heinz, S. Kéna-Cohen, T. Pohl and V. M. Menon
Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe2) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ∼𝑔2𝑠𝑝𝑜𝑙−𝑝𝑜𝑙∼46.4±13.9𝜇𝑒𝑉𝜇𝑚2gpol−pol2s∼46.4±13.9μeVμm2 which is ∼4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies.