Designing a Hybrid Perovskite with Enlarged Birefringence and Bandgap for Modulation of Light Polarization

Abstract Birefringent crystals have important applications in optoelectronics areas due to their ability to modulate and polarize light. Despite increasing discovery of the birefringence potential of new crystals, it remains a great challenge to optimize both birefringence and bandgap simultaneously. Herein, a 1D chain‐like hybrid perovskite birefringent crystal designed by 3D‐to‐1D dimensional tailoring, (GAM) 2 PbI 7 ·H 2 O (GAM = C 5 N 10 H 10 ), is presented, showing enlarged birefringence of 0.49@550 nm and enlarged optical bandgap (2.48 eV). Consequently, the birefringent quality factor of (GAM) 2 PbI 7 ·H 2 O is up to 2.8 times that of the template MAPbI 3 . In particular, the birefringence is much larger than those of commercial birefringent crystals and surpasses that of the vast majority of hybrid perovskite known to date. Theoretical calculations reveal that the strongly anisotropic arrangement of (GAM) 2.5+ π ‐conjugated cations and ordered PbI 6 octahedra contributes to the large birefringence and wide bandgap of (GAM) 2 PbI 7 ·H 2 O. It is believed that this work will provide a new pathway toward the rational design and synthesis of hybrid perovskite birefringent crystals for compact wide‐bandgap polarization dependent devices.