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Monolayer transition metal dichalcogenides, coupled to metal plasmonic nanocavities, have recently emerged as new platforms for strong light-matter interactions. These systems are expected to have nonlinear optical properties that will enable them to be used as entangled photon sources, compact wave-mixing devices, and other elements for classical and quantum photonic technologies. Here we report the first experimental investigation of the nonlinear properties of these strongly coupled systems, by observing second harmonic generation from a WSe2 monolayer strongly coupled to a single gold nanorod. The pump frequency dependence of the second harmonic signal displays a pronounced splitting that can be explained by a coupled oscillator model with second-order nonlinearities. Rigorous numerical simulations utilizing a nonperturbative nonlinear hydrodynamic model of conduction electrons support this interpretation and reproduce experimental results. Our study thus lays the groundwork for understanding the nonlinear properties of strongly coupled nanoscale systems.
Hyperbolic plasmonic metamaterials provide numerous opportunities for designing unusual linear and nonlinear optical properties. We show that the modal overlap of fundamental and second-harmonic light in an anisotropic plasmonic metamaterial slab res
Nano-resonator integrated with two-dimensional materials (e.g. transition metal dichalcogenides) have recently emerged as a promising nano-optoelectronic platform. Here we demonstrate resonatorenhanced second-harmonic generation (SHG) in tungsten dis
A hallmark of wave-matter duality is the emergence of quantum-interference phenomena when an electronic transition follows different trajectories. Such interference results in asymmetric absorption lines such as Fano resonances, and gives rise to sec
A new concept for second-harmonic generation (SHG) in an optical nanocircuit is proposed. We demonstrate both theoretically and experimentally that the symmetry of an optical mode alone is sufficient to allow SHG even in centro-symmetric structures m
Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic con