High efficiency and large optical anisotropy in the high-order nonlinear processes of 2D perovskite nanosheets.

Nonlinear nanophotonic devices have brought about great advances in the fields of nano-optics, quantum science, biomedical engineering, etc. However, in order to push these nanophotonic devices out of laboratory, it is still highly necessary to improve their efficiency. Since obtaining novel nanomaterials with large nonlinearity is of crucial importance for improving the efficiency of nonlinear nanodevices, we propose the two-dimensional (2D) perovskites. Different from most previous studies which focused on the 2D perovskites in large scale (such as the bulk materials or the thick flakes), herein we studied the 2D perovskites nanosheets with thickness of ∼50 nm. The high-order nonlinear processes including multi-photon photoluminescence and third-harmonic generation (THG) have been systematically investigated, and it is found the THG process can have a high conversion efficiency up to ∼8 × 10. Also, it is observed that the nonlinear responses of 2D perovskites have large optical anisotropy, i.e., the polarization ratio for the incident polarization dependence of nonlinear response can be as high as ∼0.99, which is an impressive record in the perovskite systems. Our findings reveal the properties of high efficiency and huge optical anisotropy in the nonlinear processes of 2D perovskite nanosheets, shedding light on the design of advanced integrated nonlinear nanodevices in future.