Boosting classical and quantum nonlinear processes in ultrathin van der Waals materials

Abstract: Understanding and controlling nonlinear processes is crucial for engineering light-matter interaction and generating non-classical light. A significant challenge in ultra-thin nonlinear materials is the marked diminution of the nonlinear conversion efficiency due to the reduced light-matter interaction length and, in many cases, the centrosymmetric crystalline structures. Here we relax these limitations and report a giant boost of classical and quantum nonlinear processes in ultrathin van der Waals materials. Specifically, with a metal-nonlinear material heterostructure we enhance classical second-harmonic generation in h-BN flakes by two-orders of magnitude. Moreover, we have engineered a metal-SiO2-nonlinear material heterostructure resulting in a remarkable two orders of magnitude augmentation of the quantum spontaneous parametric down-conversion (SPDC) in NbOCl2 flakes. Notably, we demonstrate SPDC in a 16 nm-thick NbOCl2 flake integrated into the proposed structure. These findings simplify on-chip quantum state engineering and accelerate the use of van der Waals materials in nonlinear optoelectronics.