Second Harmonic Generation from exciton-polaritons: Strong coupling between monolayer WS2 and multilayer WSe2 metasurfaces …

The second harmonic generation (SHG) from exciton-polaritons, produced by the strong coupling between quantum emitters and cavity photons, can provide a unique insight for controlling nonlinear responses on the nanoscale. Achieving SHG generally depends on phase matching, limited by nonlinear materials and nanostructure fabrication. Here, we demonstrate a novel way to obtain tunable SHG from van der Waals metasurfaces composed of nanostructured multilayer WSe2 strong coupling with monolayer WS2. By breaking symmetry via varying the metasurface unit tilted angle and period, quasibound state in the continuum (q-BIC) mode resonances energy is tuned across the monolayer WS2 exciton resonance energy, enabling anticrossing behavior of strong coupling in both reflection spectrum and SHG spectrum, which means that SHG was successfully observed by strong coupling. Furthermore, the SHG spectrum can be tuned by changing the armchair direction of the monolayer WS2 and pump polarization direction. Moreover, the mechanism of exciton-polaritonic SHG is investigated by a coupled nonlinear oscillator model, which reveals the SHG origin from exciton-polaritons, providing a new rule for fine-tuning the SHG. Our work provides a new strategy and additional freedom in the nonlinear light-matter interaction and coherent control of the SHG in integrated photonic devices.