Abstract

AbstractChiral hybrid organic–inorganic metal halides (HOMHs) with intrinsic noncentrosymmetry have shown great promise for applications in second‐order nonlinear optics (NLO). However, established chiral HOMHs often suffer from their relatively small band gaps, which lead to negative impacts on transparent window and laser‐induced damage thresholds (LDT). Here, we have synthesized two chiral HOMHs based on CuI halides, namely (R‐/S‐MBA)CuBr2, which feature well‐balanced NLO performances with a highly efficient SHG response, outstanding optical transparency, and high LDT. The effective second‐order NLO coefficient of (R‐MBA)CuBr2 has been determined to be ≈24.7 pm V−1, which is two orders of magnitude higher than that of their CuII counterparts. This work shows the promising potential of CuI‐based chiral HOMHs for nonlinear photonic applications in wide wavelength regions.

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