Enhancing Resonant Second-Harmonic Generation in Bilayer WSe2 by Layer-Dependent Exciton-Polaron Effect

Two-dimensional (2D) materials serve as exceptional platforms for controlled second-harmonic generation (SHG). Current approaches to SHG control often depend on nonresonant conditions or symmetry breaking via single-gate control. Here, we employ dual-gate bilayer WSe₂ to demonstrate an SHG enhancement concept that leverages strong exciton resonance and a layer-dependent exciton-polaron effect. By selectively localizing injected holes within one layer, we induce exciton-polaron states in the hole-filled layer while maintaining normal exciton states in the charge-neutral layer. The distinct resonant conditions of these layers effectively break interlayer inversion symmetry, thereby promoting resonant SHG. This method achieves a remarkable 40-fold enhancement of SHG at minimal electric field, equivalent to conditions near the dielectric-breakdown threshold but using only ∼3% of the critical breakdown field. Our results highlight SHG sensitivity to carrier density and type, offering a new tool for manipulating SHG and probing quantum states in 2D excitonic systems.