Electrical Control of Interband Resonant Nonlinear Optics in Monolayer MoS₂

Monolayer transition-metal dichalcogenides show strong optical nonlinearity with great potential for various emerging applications. Here we demonstrate the gate-tunable interband resonant four-wave mixing and sum-frequency generation in monolayer MoS2. Up to 80% modulation depth in four-wave mixing is achieved when the generated signal is resonant with the A exciton at room temperature, corresponding to an effective third-order optical nonlinearity |χ(3)eff| tuning from (∼12.0 to 5.45) × 10-18 m2/V2. The tunability of the effective second-order optical nonlinearity |χ(2)eff| at 440 nm C-exciton resonance wavelength is also demonstrated from (∼11.6 to 7.40) × 10-9 m/V with sum-frequency generation. Such a large tunability in optical nonlinearities arises from the strong excitonic charging effect in monolayer transition-metal dichalcogenides, which allows for the electrical control of the interband excitonic transitions and thus nonlinear optical responses for future on-chip nonlinear optoelectronics.