Quasi-phase-matching enabled by van der Waals stacking.

Quasi-phase matching (QPM) is a technique extensively utilized in nonlinear optics for enhancing the efficiency and stability of frequency conversion processes. However, the conventional QPM relies on periodically poled ferroelectric crystals, which are limited in availability. The 3R phase of molybdenum disulfide (3R-MoS), a transition metal dichalcogenide (TMDc) with the broken inversion symmetry, stands out as a promising candidate for QPM, enabling efficient nonlinear process. Here, we experimentally demonstrate the QPM at nanoscale, utilizing van der Waals stacking of 3R-MoS layers with specific orientation to realize second harmonic generation (SHG) enhancement beyond the non QPM limit. We have also demonstrated enhanced spontaneous parametric down-conversion (SPDC) via QPM of 3R-MoS homo-structure, enabling more efficient generation of entangled photon pairs. The tunable capacity of 3R-MoS van der Waals stacking provides a platform for tuning phase-matching condition. This technique opens interesting possibilities for potential applications in nonlinear process and quantum technology.