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Giant anomalous exciton-multiphoton nonlinearities in layered hybrid perovskites
Yanming Xu1,2, Yi Liu3, Chao Yu4
1Fujian Key Laboratory of Quantum Information and Quantum Optics, College of Physics and Information Engineering, Fuzhou University, Fuzhou, 350108, China.
Abstract:
Directly full-color frequency-upconversion under high-order multiphoton absorption (MPA) nonlinearities in NIR-III (1550-1870 nm) and NIR-IV (2100-2300 nm) windows is highly desirable for advanced photonics and bioimaging. However, it has remained beyond the reach of current materials due to their inherently weak high-order MPA. Here, we demonstrate that, driven by Bloch oscillations of excitonic dipoles after nonlinear polarization, giant multiphoton nonlinearities can be achieved in layered hybrid perovskites to enable full-color upconversion in NIR-III/IV windows. The MPA cross-section values of the designed three Ruddlesden-Popper perovskites are found to be several orders of magnitude larger than those of the reported MPA materials. These advancements facilitate versatile applications previously inaccessible in NIR-III/IV windows, including full-color upconversion displays and multicolor information encryption. Our work highlights the prospect of efficient high-order MPA and opens avenues for investigating excitonic quantum dynamics in high-order nonlinear optics.
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