Temperature‐Responsive Photoluminescence of 1D Chiral Lead Halide Perovskites with Highly Anisotropic Second Harmonic Generation

Comprehensive Summary Chiral perovskites provide an ideal platform for the construction of linear and nonlinear optical materials due to their diverse chemical variability, structural tunability, and intrinsic non‐centrosymmetricity which have broad application prospects for next‐generation optoelectronic devices. In this work, a pair of 1D chiral lead halide perovskites ( R / S ‐4MeOPEA)PbCl 3 (4MeOPEA = (4‐methoxyphenyl)ethylamine) were synthesized, and characterized systematically. Crystal structure analysis revealed that the one‐dimensional (1D) inorganic chain formed by face‐shared lead chloride octahedra was separated by the chiral organic spacers. The distorted octahedra endows them with broadband bluish‐white light emission centered covering the range 350—700 nm with a width of 104 nm. In addition, the highly anisotropic second‐harmonic generation (SHG) with a near unity polarization ratio was observed. This work presents a fresh example of 1D chiral perovskite with exotic linear and nonlinear optical properties, which could provide a new footstone for further optoelectronic devices.