Circularly polarized laser from three‐dimensional perovskite induced by intramolecular interaction

Materials with circularly polarized (CP) lasing, featuring optical rotatory power, are attractive for various advanced optical, sensing, biological, and medical applications. In this context, chiral perovskites attract great attention owing to their superior chiral opto‐electronic‐magnetic properties. However, the trade‐off between coherence and circularity hinders lasing in low‐dimensional perovskites. Herein, we invent a novel strategy to realize three‐dimensional perovskites with high chirality featuring CP laser. The strong intramolecular interaction between chiral acid and inorganic framework via ionic bonding leads to intense electronic interaction and orbital hybridization, resulting in higher asymmetric and efficient CP emission than most low‐dimensional perovskites and an amplified asymmetric factor of up to 0.054 at up‐threshold excitation. This pioneering advancement heralds a new era for intramolecular interaction‐based stable perovskite, as well as other low‐dimensional materials, opening avenues for unprecedented applications in stable‐perovskite/chiral optoelectronics and beyond.