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RESEARCH ARTICLE · Angewandte Chemie International Edition · 2024

Halogen Bond Unlocks Ultra‐High Birefringence

Jin Chen, Mingsheng Xu, Huai‐Yu Wu, Jun‐Yan Wu, Ke‐Zhao Du

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Halogen Bond Unlocks Ultra‐High BirefringenceOriginalExploring short-wavelength birefringent crystals via triggering cooperative arrangement between different π-conjugated groups8Birefringence Disparity Induced by Synergistic Effects of Stereochemically Active Lone Pairs19Exploring ultra-high optical anisotropy in polyiodides7Greatly enhancing birefringence of fluorosilicates through the synergetic effect of functional units13Hg 2 (HTe 2 O 5 )(PO 4 ): a novel phosphate crystal with enhanced birefringence enabled by the synergistic modification of multiple functional groups12Hg 2 (SeO 3 )(TeO 3 ): a novel tellurite–selenite birefringent crystal achieved by assembling multiple functional groups11Hg[CS(NH 2 ) 2 ] 4 (SiF 6 ): a fluorosilicate crystal with large birefringence achieved via multi-functional group modification6From (C6H5N2)2CdCl4 to (C6H5N2)2ZnCl4, Chirality Transformation to Realize a Nonlinear Optical Organic–Inorganic Hybrid Halide with Balanced Comprehensive Performance19Hydrogen bonding evolution and efficient blue light emission in a series of Zn-based organic–inorganic hybrid metal halide crystals14Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals71Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals8Zero-Dimensional Plastic Phase Transition Iron-Based Compounds with High T c and Switchable SHG Responses5Tuning Birefringence in Supramolecular Mg-PDA Frameworks: Modulating Bonding and Layer Connectivity0Ultra‐High Optical Anisotropy with UV Transmission Achieved by Rational Arrangement of Extended π‐Conjugated Groups5Ultra‐High Optical Anisotropy with UV Transmission Achieved by Rational Arrangement of Extended π‐Conjugated Groups46Solid‐State Photoconversion of a Discrete Mixed Iodine(I) System to a 1D Polymer1Solid‐State Photoconversion of a Discrete Mixed Iodine(I) System to a 1D Polymer0Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8Giant Birefringence Enabled by the Highly Anisotropic Linear IX 2 − (X = Cl, Br) Building Blocks6Giant Birefringence Enabled by the Highly Anisotropic Linear IX 2 − (X = Cl, Br) Building Blocks32La2Zn3(SeO3)6: A UV Selenite Crystal with Second-Harmonic Generation and Large Birefringence13Planar [HgCl 3 ] and V‑Shaped [HgCl 2 ] Units Synergistically Creating a Prominent Halide Birefringent Crystal β ‐CsHg 2 Cl 5 with Wide‐Spectrum7Distorted Molecular Conformation Enabled Supramolecular Dynamics in Elastic Organic Single Crystals5[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence18[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence4Breaking the Birefringence Barrier in B–O Crystals via B–C π-scaffolding36A novel metal-free crystal demonstrating superior birefringence attributed to the synergistic interaction of dual π-conjugated units8Synthesis and Characterization of (H7C5N2)6(V10O28)·2H2O with Edge-Sharing VO6 Octahedra Exhibiting Large Birefringence2CsICl 2 : A Record-Birefringent Inorganic Crystal with Ultrawide Infrared Transparency Enabled by Linear Interhalogen ICl 2 – Units36A Solid-State Study of the Influence of the Lewis Base on Iodine(I) 4-Trifluoromethylbenzoate Derivatives1Achieving large birefringence in oxalate crystals by a hydrogen bond-directed strategy1Anionic Group Trimming Strategy: Oriented Fabrication of Sulfonate UV Birefringent Crystals with High Optical Anisotropy5Organic Halogen Substitution-Driven Halogen Bonding Induces Polar 3D Supramolecular Framework and Second-Harmonic-Generation Response7Exceptional Enhancement of Optical Anisotropy Achieved via the Strategy of Combining Rigid Groups with High Symmetry and π‐Conjugated Organic Groups in Hybrid Fluorides33Enhanced Second Harmonic Generation Response via Rational Design of Iodinated π-Conjugated Pyridine Group5Hybrid Zinc‒Based Halides with Giant Optical Anisotropy via Protonation‒Engineered π ‒Conjugated Organic Group24Halogen-substitution-driven crystal engineering of chalcones: mechanisms and optimization for spatial ordering and nonlinear optical performance1Hydrogen‐Bond‐Driven Metal‐Free Crystal (C 6 H 7 N 2 O)(NH 2 SO 3 ) with Giant Birefringence and Solar‐Blind Ultraviolet Transmission0Achieving Ultra‐High Optical Anisotropy via Structural Regulation and Coplanar Engineering of Extended π‐Conjugated [H 2–x C 3 N 3 S 3 ] (x = 1, 2) Groups3Ligand-Directed Hydrogen Bond Symmetry Regulates Ultraviolet Absorption in Organic–Inorganic Metal Halides0Cationic‐Dual‐Modulated Linear and V‐Shaped Birefringent‐Active Unit Generates Remarkable Birefringence6Achieving record birefringence in metal-free semiorganic sulfate crystals via tetrahedral anionic group substitution0Counterion engineering in open-framework crystals: dual enhancement of birefringence and UV transparency in Cd–oxalate framework via cation substitution0Dual-tuning birefringence in hybrid crystals via Cd/Zn metal center and organic ligand isomerism0Structure–property relationships in organic framework materials: the role of linkage modes and building units1Halogen‐Bond Coupled Halogenated‐π‐Conjugation Enables Giant Birefringence in Hydrogen‐Bonded Organic Frameworks13Unit Symmetry‐Breaking and Layered Linear Ordering Enabling Superior Short‐Wave Ultraviolet Birefringent Crystal8Unit Symmetry‐Breaking and Layered Linear Ordering Enabling Superior Short‐Wave Ultraviolet Birefringent Crystal2Programmable Anisotropic in Diazapyrene Cocrystals With Birefringence Exceeding 1.27Programmable Anisotropic in Diazapyrene Cocrystals With Birefringence Exceeding 1.21V-Shaped Pseudo-Chains Coupled with Lone-Pair-Distorted [GeX 3 ] − Units Enable Large Birefringence in Ge(II) Hybrid Halides2Density-Compensated Polarizability Anisotropy for Record Birefringence in Short-Wavelength Ultraviolet Inorganic Crystals11Halogen Anion-Mediated Substitution of Nitrate: Toward Polar Materials with Intense Second-Harmonic Generation Effects3Synergistic Enhancement of Birefringence in Metal Benzoxazolium Complexes by π-Conjugated [C 9 H 10 NO] + and Triangular [HgI 3 ] − Motifs3Engineering Excited‐State Dynamics: [N···I···N] + Halogen Bonds Unlocks Efficiently Emissive Quinoline2Recent Progress in Hg-Based Oxysalt Crystals for Nonlinear Optics and Birefringence Applications5Record‐High Birefringence with Ultralow Dichroic Loss Realized by Cation‐Templated Engineering Ordered Assembly of Linear Birefringent‐Active Unit6Lock‐and‐Key Assembly Enables Record Birefringence in Monocyclic π‐Conjugated Crystals via Spatial Confinement of Linear Polyhalide5Redox‐Driven Strategy Enabling Leapfrog Enhancement of Birefringence in Layered Tin‐Based Optical Crystals1Rb 2 ZnGe 3 Se 8 : A Large-Birefringence Layered Chalcogenide Enabled by Anisotropic Electrons in Tetrahedral Units0Unlocking Structural Anisotropy by Guest-Symmetry Modulation Strategy to Achieve Giant Birefringence in Molecular Crystals0Interlayer Electronic Decoupling Unlocks Giant Birefringence in π‐Conjugated Metal‐Organic Frameworks0A Programmable Luminescent Sensing Platform via Site‐Selective Modular Installation in Metal–Organic Frameworks1Bioinspired Subnanowire‐Based Optical Devices With Programmable Polarization Irisations Through Photocuring 3D Printing0Designing Novel Solar‐Blind Ultraviolet Nonlinear Optical Crystals Based on Local Proton Distribution Complementary Effect0Steric‐Guided Coordination Engineering Enables Significantly Optimized Optical Anisotropy via Sulfur‐Driven [C 5 H 5 NS] Birefringence‐Active Groups0Local Aromatic Overlap Microregulation Enables Birefringence Enhancement in Isocompositional Hybrid Antimony Halides1Decoupling Contributions of Distinct Strategies for Enhancing Polarizability Anisotropy in Crystals Containing π-Conjugated Groups0Reversible Symmetry Switching, Giant Birefringence, and UV Second‐Harmonic Generation in Hybrid Niobium Oxyfluorides0Reversible Symmetry Switching, Giant Birefringence, and UV Second‐Harmonic Generation in Hybrid Niobium Oxyfluorides0A Dynamic Hydrogen‐Bonded Organic Framework With Giant OFF–ON Birefringence0Dual‐Role BF 3 Anchoring Enables Giant Birefringence in Short‐Wave UV‐Transparent Fluoroborates0Halogen‐Bond Dimensionality Controls π–π Packing to Unlock Ultrahigh Second‐Harmonic Generation and Giant Birefringence0

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  3. Exploring ultra-high optical anisotropy in polyiodides

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  4. Greatly enhancing birefringence of fluorosilicates through the synergetic effect of functional units

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  5. Hg 2 (HTe 2 O 5 )(PO 4 ): a novel phosphate crystal with enhanced birefringence enabled by the synergistic modification of multiple functional groups

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  6. Hg 2 (SeO 3 )(TeO 3 ): a novel tellurite–selenite birefringent crystal achieved by assembling multiple functional groups

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  7. Hg[CS(NH 2 ) 2 ] 4 (SiF 6 ): a fluorosilicate crystal with large birefringence achieved via multi-functional group modification

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  8. From (C6H5N2)2CdCl4 to (C6H5N2)2ZnCl4, Chirality Transformation to Realize a Nonlinear Optical Organic–Inorganic Hybrid Halide with Balanced Comprehensive Performance

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  9. Hydrogen bonding evolution and efficient blue light emission in a series of Zn-based organic–inorganic hybrid metal halide crystals

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  16. Solid‐State Photoconversion of a Discrete Mixed Iodine(I) System to a 1D Polymer

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  18. Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence

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  19. Giant Birefringence Enabled by the Highly Anisotropic Linear IX 2 − (X = Cl, Br) Building Blocks

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  20. Giant Birefringence Enabled by the Highly Anisotropic Linear IX 2 − (X = Cl, Br) Building Blocks

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  21. La2Zn3(SeO3)6: A UV Selenite Crystal with Second-Harmonic Generation and Large Birefringence

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  22. Planar [HgCl 3 ] and V‑Shaped [HgCl 2 ] Units Synergistically Creating a Prominent Halide Birefringent Crystal β ‐CsHg 2 Cl 5 with Wide‐Spectrum

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  48. Unit Symmetry‐Breaking and Layered Linear Ordering Enabling Superior Short‐Wave Ultraviolet Birefringent Crystal

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  49. Programmable Anisotropic in Diazapyrene Cocrystals With Birefringence Exceeding 1.2

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