Chiral 3D Perovskite Single Crystals Realized by Lattice Expansion

This is the authors' abstract. We don't add key points for this paper.

Chiral 3D perovskites possess remarkable chiroptoelectronic properties, which exhibit potential for overcoming the intrinsic limitations of carrier/exciton dynamics in low‐dimensional chiral perovskites. However, chiral 3D perovskites face significant synthetic challenges compared to their low‐dimensional counterparts, owing to the large steric hindrance of available chiral organic ammonium cations. Here, a novel chiral 3D perovskite single crystal, [( R / S )‐3APr] 2 Pb 4 I 12 ·2H 2 O [( R / S )‐3APr = ( R / S )‐3‐aminopyrrolidine] is demonstrated. The chiral ligands along with water molecules are incorporated inside 3D inorganic frameworks with expanded crystal lattices. An electrode‐transfer device fabrication strategy is developed to construct the chiral 3D perovskite‐based circularly polarized light (CPL) photodetector. The resulting photodetector exhibits excellent performance, with a high anisotropy factor for photocurrent (g I ph ) of 0.4. Furthermore, the non‐centrosymmetry enables chiral 3D perovskites to have efficient second harmonic generation (SHG) properties and a large circular polarization sensitivity of SHG, with an optical anisotropy factor of 0.83, extending the CPL detection range to near infrared region.