Chiral Lead‐Free Hybrid Organic‐Metal Halides for Thermally Switchable Nonlinear Optics

ABSTRACT Chiral hybrid organic–inorganic metal halides with nonlinear optics have significant application value in the field of optoelectronics. However, the existing systems contain the toxic Pb element and low laser damage thresholds, which is not friendly to the environment and has poor stability. Here, we developed a new type of lead‐free antimony‐based chiral microplates with excellent optical anisotropy by a solvent‐assisted drop‐casting strategy. These microplates not only preserve the bulk SHG activity but also exhibit excellent optical anisotropy and a remarkably high laser damage threshold exceeding 133.3 mJ cm ⁻² . In addition to the static optical properties, we further leverage the lattice phase transition characteristics to construct a proof‐of‐concept temperature‐responsive optical switch device, which realizes the dynamic regulation of micro‐nano scale nonlinear optical signals. These advances provide feasibility verification for the development of on‐chip integrated photonic devices.