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The combination of graphene’s intrinsically-high nonlinear optical response with its ability to support long-lived, electrically tunable plasmons that couple strongly with light has generated great expectations for application of the atomically-thin material to nanophotonic devices. These expectations are mainly reinforced by classical analyses performed using the response derived from extended graphene, neglecting finite-size and nonlocal effects that become important when the carbon layer is structured on the nanometer scale in actual device designs. Based on a quantum-mechanical description of graphene using tight-binding electronic states combined with the random-phase approximation, we show that finite-size effects produce large contributions that increase the nonlinear response associated with plasmons in nanostructured graphene to significantly higher levels than previously thought, particularly in the case of Kerr-type optical nonlinearities. Motivated by this finding, we discuss and compare saturable absorption in extended and nanostructured graphene, with or without plasmonic enhancement, within the context of passive mode-locking for ultrafast lasers. We also explore the possibility of high-harmonic generation in doped graphene nanoribbons and nanoislands, where illumination by an infrared pulse of moderate intensity, tuned to a plasmon resonance, is predicted to generate light at harmonics of order 13 or higher, extending over the visible and UV regimes. Our atomistic description of graphene’s nonlinear optical response reveals its complex nature in both extended and nanostructured systems, while further supporting the exceptional potential of this material for nonlinear nanophotonic devices.
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