Probing and manipulating the intriguing nonlinear optical responses in van der Waals (vdW) ferroelectrics offer opportunities for their applications in nanophotonics. Here, we report the observation of giant and tunable second-harmonic generation (SHG) in ferroelectric CuInP2S6 (CIPS) and CIPS/MoS2 heterostructures. The results show that CIPS, ranging from multilayer to bulk-like samples, all exhibit strong SHG with giant anisotropy. The SHG anisotropy is attributed to the local strain along the a-axis that naturally exists in CIPS, as evidenced by piezoresponse force microscopy measurement. We further realized the strong modulation of SHG in CIPS by interfacing with monolayer MoS2. A combination of polarization, temperature, and thickness-dependent SHG and photoluminescence analyses shows that the nonlinear optical signal control in CIPS/MoS2 heterostructures is unrelated to the polar symmetry of CIPS and MoS2 but is driven by light absorption-mediated interfacial coupling. Our study provides a material platform based on vdW ferroelectric heterostructures for achieving dynamic control of nonlinear optical responses, which shows great potential applications in modern nanophotonics.
Read full abstract