Pursuing nanometer-scale nonlinear converters based on second harmonic generation (SHG) is a stimulating strategy for bio-sensing, on-chip optical circuits, and quantum information processing, but the light-conversion efficiency is still poor in such ultra-small dimensional nanostructures. Herein, we demonstrate a highly enhanced broadband frequency converter through a hybrid plasmonic–dielectric coupler, a ZnTe/ZnO single core–shell nanowire (NW) integrated with silver (Ag) nanoparticles (NPs). The NW dimension has been optimized to allow the engineering of dielectric resonances at both fundamental wave and second harmonic frequencies. Meanwhile, the localized surface plasmon resonances are excited in the regime between the Ag NPs and ZnTe/ZnO dielectric NW, as evidenced by plasmon-enhanced Raman scattering and resonant absorption. These two contributors remarkably enhance local fields and consequently support the strong broadband SHG outputs in this hybrid nanostructure by releasing stringent phase-matching conditions. The proposed nanoscale nonlinear optical converter enables the manipulation of nonlinear light–matter interactions toward the development of on-chip nanophotonic systems.

Mechanical exfoliation (ME) and chemical vapor deposition (CVD) MoS₂ monolayers have been extensively studied, but the large differences of nonlinear optical performance between them have never been clarified. Here, we prepared MoS₂ monolayers using ME and CVD methods and investigated the two-photon absorption (TPA) response and its saturation. We found that the TPA coefficient of the ME monolayer was about (1.88 ± 0.21) × 10³ cm/GW, nearly two times that of the CVD one at (1.04 ± 0.15) × 10³ cm/GW. Furthermore, we simulated and compared the TPA-induced optical pulse modulation in multilayer cascaded structures, which is instructive and meaningful for the design of optical devices such as a beam shaper and optical limiter.