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Optical anisotropic (e.g., birefringent) crystals can manipulate the polarization of light and thus are widely applied in modern optical fields. Common birefringent crystals are almost exclusively limited to inorganic oxides with small birefringence. Here, a new 1D hybrid halide perovskite PZPbCl3 (PZ = phenazine) is reported, which consists of perfectly parallel Pb–Cl chains and PZ cations. Remarkably, polarized optical observations show that even a PZPbCl3 crystal with micrometer thickness can modulate the polarized light efficiently. Furthermore, PZPbCl3 exhibits exceptional birefringence up to 0.65@546 nm, which is significantly larger than that of commercial oxide crystals. According to first‐principles calculations and polarizability anisotropy analyses, it is found that this birefringence is mainly ascribed to the linear polymerization of π‐conjugated rings in PZ cations. Due to the rich physical properties and structural diversity of hybrid perovskites, it is believed that the introduction of excellent birefringence into the hybrid perovskites will bring unprecedented opportunities to the future explorations of polarization‐dependent functional materials. [ABSTRACT FROM AUTHOR]

Birefringent crystals can manipulate the phase and polarization of light, so they are widely used as essential components in various optical devices. Common strategies to construct birefringent crystals are introducing metal cations that are either able to realize favorable coordination with functional anionic units or are susceptible to polarizability anisotropy. Herein, we report a metal-free crystal, NH 4 (H 2 C 6 N 7 O 3 )·2H 2 O, synthesized using the facile solution method. In the crystal structure of NH 4 (H 2 C 6 N 7 O 3 )·2H 2 O, (H 2 C 6 N 7 O 3 ) - functional units are assembled in an optimal manner by cooperative non-covalent interactions, i.e. , hydrogen bonding and π-π interactions. As a result, this metal-free crystal possesses exceptional birefringence up to 0.54@550 nm, which is larger than those of most metal-containing birefringent crystals. In addition, the interference color of this crystal does not change obviously from 243 K to 313 K, indicating that the birefringence is robust at different temperatures. This work will inspire useful insights into the role of non-covalent interactions in designing outstanding birefringent crystals for efficient polarized optical devices.

Birefringent crystals that can switch light polarization have important applications in optoelectronics. In the last decades, birefringence is mostly optimized by chemical strategies. Recently, switching birefringence by physical means has attracted much attention. Here, this work reports the observation of heat switching birefringence in a 2D layered hybrid halide perovskite (C 2 N 3 H 4 ) 2 PbCl 4 ((C 2 N 3 H 4 ) + =1,2,4-triazolium). This heat switching birefringence leads to a significant change in the interference color for the crystal plate under the illumination of orthogonal polarized light. Structure analyses reveal a heat dependent structure transition in (C 2 N 3 H 4 ) 2 PbCl 4 , whose birefringence is switched by the change in the distortion degree of PbCl 6 octahedron. This discovery may be beneficial to the further development of stimuli-responsive polarization optical devices., (© 2023 Wiley-VCH GmbH.)