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Birefringent crystals could modulate the polarization of light and are widely used as polarizers, waveplates, optical isolators, etc. To date, commercial birefringent crystals have been exclusively limited to purely inorganic compounds such as α‐BaB2O4 with birefringence of about 0.12. Herein, we report a new hydrogen bonded supramolecular framework, namely, Cd(H2C6N7O3)2⋅8 H2O, which exhibits exceptionally large birefringence up to about 0.60. To the best of our knowledge, the birefringence of Cd(H2C6N7O3)2⋅8 H2O is significantly larger than those of all commercial birefringent crystals and is the largest among hydrogen bonded supramolecular framework crystals. First‐principles calculations and structural analyses reveal that the exceptional birefringence is mainly ascribed to strong covalent interactions within (H2C6N7O3)− organic ligands and the perfect coplanarity between them. Given the rich structural diversity and tunability, hydrogen bonded supramolecular frameworks would offer unprecedented opportunities beyond the traditional purely inorganic oxides for birefringent crystals. [ABSTRACT FROM AUTHOR]

Birefringent crystals could modulate the polarization of light and are widely used as polarizers, waveplates, optical isolators, etc. To date, commercial birefringent crystals have been exclusively limited to purely inorganic compounds such as α‐BaB2O4 with birefringence of about 0.12. Herein, we report a new hydrogen bonded supramolecular framework, namely, Cd(H2C6N7O3)2⋅8 H2O, which exhibits exceptionally large birefringence up to about 0.60. To the best of our knowledge, the birefringence of Cd(H2C6N7O3)2⋅8 H2O is significantly larger than those of all commercial birefringent crystals and is the largest among hydrogen bonded supramolecular framework crystals. First‐principles calculations and structural analyses reveal that the exceptional birefringence is mainly ascribed to strong covalent interactions within (H2C6N7O3)− organic ligands and the perfect coplanarity between them. Given the rich structural diversity and tunability, hydrogen bonded supramolecular frameworks would offer unprecedented opportunities beyond the traditional purely inorganic oxides for birefringent crystals. [ABSTRACT FROM AUTHOR]

Birefringent crystals that can modulate the polarization of light play a significant role in modern optical devices including polarizing microscopes, optical isolators, and achromatic quarter‐wave plates. To date, commercial birefringent crystals are exclusively limited to purely inorganic compounds. Here we report a new organic–inorganic hybrid halide, MLAPbBr4 (MLA=melamine), which features a (110)‐oriented layered perovskite structure. Although the 6s2 lone‐pair electrons of Pb2+ cations are stereochemically inert, MLAPbBr4 exhibits a birefringence of 0.322@550 nm, which exceeds those of all commercial birefringent crystals. The first‐principles calculations reveal that this birefringence should be ascribed to the highly dislocated π‐conjugation of MLA cations and high distortion of PbBr6 octahedra. This work highlights the persistently neglected great potential of hybrid halide perovskites as birefringent crystals. [ABSTRACT FROM AUTHOR]

Birefringent crystals that can modulate the polarization of light play a significant role in modern optical devices including polarizing microscopes, optical isolators, and achromatic quarter‐wave plates. To date, commercial birefringent crystals are exclusively limited to purely inorganic compounds. Here we report a new organic–inorganic hybrid halide, MLAPbBr4 (MLA=melamine), which features a (110)‐oriented layered perovskite structure. Although the 6s2 lone‐pair electrons of Pb2+ cations are stereochemically inert, MLAPbBr4 exhibits a birefringence of 0.322@550 nm, which exceeds those of all commercial birefringent crystals. The first‐principles calculations reveal that this birefringence should be ascribed to the highly dislocated π‐conjugation of MLA cations and high distortion of PbBr6 octahedra. This work highlights the persistently neglected great potential of hybrid halide perovskites as birefringent crystals. [ABSTRACT FROM AUTHOR]

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 (C2N3H4)2PbCl4 ((C2N3H4)+=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 (C2N3H4)2PbCl4, whose birefringence is switched by the change in the distortion degree of PbCl6 octahedron. This discovery may be beneficial to the further development of stimuli‐responsive polarization optical devices. [ABSTRACT FROM AUTHOR]

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 (C2N3H4)2PbCl4 ((C2N3H4)+=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 (C2N3H4)2PbCl4, whose birefringence is switched by the change in the distortion degree of PbCl6 octahedron. This discovery may be beneficial to the further development of stimuli‐responsive polarization optical devices. [ABSTRACT FROM AUTHOR]

Birefringent materials are vital materials to modulate the polarization of light, and play a key role in plorization devices such as linear optical devices, optical communication devices, and fiber optic sensors. It is still a challenge to design excellent birefringent materials. Herein, we report an organic–inorganic hybrid oxalate birefringent material, (CN4H7)SbC2O4F2(H2O)0.5, by introducing organic delocalized π-conjugated [CN4H7]+ and [C2O4]2− groups, and stereochemical active inorganic SbO4F2 polyhedra. (CN4H7)SbC2O4F2(H2O)0.5 exhibits a large birefringence (Δn = 0.126@546 nm) that is almost equal to that of the well-known birefringent material α-BaB2O4. Theoretical calculations reveal that the distinguished birefringence should stem from the synergistic arrangement of π-conjugated [CN4H7]+ and [C2O4]2− planar groups, and highly distorted SbO4F2 polyhedra with a stereochemically active lone pair. The synergistic effect of π-conjugated systems and the lone pair electrons greatly boosts the birefringence, which is helpful for the development of high-performance birefringent materials. [ABSTRACT FROM AUTHOR]

Birefringent materials, which can modulate the polarization of light, are almost exclusively limited to oxides. Peroxides have long been overlooked as birefringent materials, because they are usually not stable in air. Now, the first peroxide birefringent material Rb2VO(O2)2F is reported, the single crystals of which keep transparency after being exposed in the air for two weeks. Interestingly, Rb2VO(O2)2F does not feature an optimal anisotropic structure, but its birefringence (Δn=0.189 at 546 nm) exceeds those of the majority of oxides. According to the first‐principles calculations, this exceptional birefringence should be attributed to the strong electronic interactions between localized π orbital of O22− anions and V5+ 3d orbitals, which may be also favorable to the stability in the air for Rb2VO(O2)2F. These findings distinguish peroxides as a brand‐new class of birefringent materials that may possess birefringence superior to the traditional oxides. [ABSTRACT FROM AUTHOR]

Birefringent materials, which can modulate the polarization of light, are almost exclusively limited to oxides. Peroxides have long been overlooked as birefringent materials, because they are usually not stable in air. Now, the first peroxide birefringent material Rb2VO(O2)2F is reported, the single crystals of which keep transparency after being exposed in the air for two weeks. Interestingly, Rb2VO(O2)2F does not feature an optimal anisotropic structure, but its birefringence (Δn=0.189 at 546 nm) exceeds those of the majority of oxides. According to the first‐principles calculations, this exceptional birefringence should be attributed to the strong electronic interactions between localized π orbital of O22− anions and V5+ 3d orbitals, which may be also favorable to the stability in the air for Rb2VO(O2)2F. These findings distinguish peroxides as a brand‐new class of birefringent materials that may possess birefringence superior to the traditional oxides. [ABSTRACT FROM AUTHOR]