Electric-Field Switchable Second-Harmonic Generation in Bilayer MoS2 by Inversion Symmetry Breaking.

We demonstrate pronounced electric-field-induced second-harmonic generation in naturally inversion symmetric 2H stacked bilayer MoS2 embedded into microcapacitor devices. By applying strong external electric field perturbations (|F| = ±2.6 MV cm-1) perpendicular to the basal plane of the crystal, we control the inversion symmetry breaking and, hereby, tune the nonlinear conversion efficiency. Strong tunability of the nonlinear response is observed throughout the energy range (Eω ∼ 1.25-1.47 eV) probed by measuring the second-harmonic response at E2ω, spectrally detuned from both the A- and B-exciton resonances. A 60-fold enhancement of the second-order nonlinear signal is obtained for emission at E2ω = 2.49 eV, energetically detuned by ΔE = E2ω - EC = -0.26 eV from the C-resonance (EC = 2.75 eV). The pronounced spectral dependence of the electric-field-induced second-harmonic generation signal reflects the bandstructure and wave function admixture and exhibits particularly strong tunability below the C-resonance, in good agreement with density functional theory calculations. Moreover, we show that the field-induced second-harmonic generation relies on the interlayer coupling in the bilayer. Our findings strongly suggest that the strong tunability of the electric-field-induced second-harmonic generation signal in bilayer transition metal dichalcogenides may find applications in miniaturized electrically switchable nonlinear devices.