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RESEARCH PAPER · Angewandte Chemie International Edition · 2022

A Hybrid Antiperovskite with Strong Linear and Second‐Order Nonlinear Optical Responses

Minjuan Li, Xu Zhang, Zheyao Xiong, Yanqiang Li, Zhou Yang, Xin Chen, Yipeng Song, Maochun Hong, Junhua Luo, Sangen Zhao

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A Hybrid Antiperovskite with Strong Linear and Second‐Order Nonlinear Optical ResponsesOriginalA UV solar-blind nonlinear optical crystal with confined π-conjugated groups13Accurate design and synthesis of nonlinear optical crystals employing KBe2BO3F2 as structural template55Design and synthesis of anisotropic crystals with π -conjugated rings toward giant birefringence36LaAeAl 3 S 7 (Ae = Ca, Sr): Cairo pentagonal layered thioaluminates achieving a good balance between a strong second harmonic generation response and a wide bandgap23Linear π-conjugated units of the D ∞h point group as superior ultraviolet birefringent units1Second harmonic generation from symmetry breaking stimulated by mixed organic cations in zero-dimensional hybrid metal halides7Spectroscopic characterization of a mononuclear oxovanadium (IV) Schiff base complex. Oxidation catalysis applications and antibacterial activities18α-BBO-like π-Conjugated Crystal with Large Birefringence16Recent advances in non-π-conjugated nonlinear optical sulfates with deep-UV absorption edge53Flux growth of nonlinear optical crystal K3B6O10Br with high optical quality and its electro-optical property8A BBO-like trithiocyanate with significantly enhanced birefringence and second-harmonic generation39Cs 2 Mg(H 2 C 3 N 3 S 3 ) 4 ·8H 2 O: An Excellent Birefringent Material with Giant Optical Anisotropy in π-Conjugated Trithiocyanurate19Recent progress of newly developed functional building units and corresponding nonlinear optical materials14Superior ferroelectricity and nonlinear optical response in a hybrid germanium iodide hexagonal perovskite133Quartz‐Like Structure, Optical Activity, and High Stability in the First Chiral Cation‐Coordinated Perovskite Semiconductor11α- and β-(C4H5N2O)(IO3)·HIO3: Two SHG Materials Based on Organic–Inorganic Hybrid Iodates14Designing a Dimension Reduced Hybrid Perovskite with Robust Large Birefringence by Expanding Cationic π‐Delocation40A Two‐Dimensional Hybrid Perovskite With Heat Switching Birefringence47A Two‐Dimensional Hybrid Perovskite With Heat Switching Birefringence7Enlargement of Bandgap and Birefringence in Nonlinear Optical Alkali‐Metal Sulfate Crystals by the Substitution of Asymmetrical Non‐π‐Conjugated Cation8A review of the relationship between the structure and nonlinear optical properties of organic-inorganic hybrid materials149Structural diversity and complexity of antiperovskites38Solid‐State Electrolytes and Electrode/Electrolyte Interfaces in Rechargeable Batteries41Designing a Hybrid Perovskite with Enlarged Birefringence and Bandgap for Modulation of Light Polarization32Plasmon-modulated bistable second-harmonic generation in a nonlinear microcavity coupled to a metallic nanoparticle2H/F Substitution Achieved Enantiomeric Organic Inorganic Hybrid Perovskites and Trigonal Structure [DMFP] 3 (CdBr 3 )(CdBr 4 )15Achieving strong second harmonic generation effects induced via dimensional increase of PbX 6 octahedra and halogen substitutes in (C 10 H 11 N 3 )PbX 4 (X = Cl or Br)26Homochiral hybrid hexagonal antiperovskite crystals [ R - and S -3-chloroquinuclidinium] 3 (CdCl 3 )(CdCl 4 )3Synthesis and Characterization of Metal Iso-cyamelurate K0.5In0.5(H2C6N7O3)2·9H2O with Large Birefringence8From C4H7N2Ge0.4Sn0.6Br3 to C6H11N2Ge0.4Sn0.6Br3: Effective Modulation of the Second Harmonic Generation Effect and Optical Band Gap by Planar π-Conjugated Organic Cation Size11Stereochemically Active Lone Pair Leads to Birefringence in the Vacancy Ordered Cs3Sb2Cl9 Perovskite Single Crystals13Magneto‐chiral Nonlinear Optical Effect with Large Anisotropic Response in Two‐Dimensional Halide Perovskite52Magneto‐chiral Nonlinear Optical Effect with Large Anisotropic Response in Two‐Dimensional Halide Perovskite3Combining rigid and deformable groups to construct a robust birefringent crystal for compact polarization components25Anti-perovskites for photovoltaics: materials development and challenges25Nonlinear Optical Properties of Cs2AgIn1–xBixCl6 Single Crystals9Deep-Ultraviolet Bialkali–Rare Earth Metal Anhydrous Sulfate Birefringent Crystal11Halogen Bond Unlocks Ultra‐High Birefringence73Halogen Bond Unlocks Ultra‐High Birefringence14Breaking through the ‘‘200 nm deep-ultraviolet wall’’ of phase matching region by cation structural modulation27A Robust Phosphonate‐Based Hydrogen‐Bonded Organic Framework Birefringent Crystal39[C3H7N6]3[B3O5(OH)2] and [C3H8N6]4[B12O19(OH)6]: Two Melamine Borates with Large Birefringence13Chiral Metal‐Free Anti‐Perovskite with Strong Chiroptical Nonlinearity13Chiral Metal‐Free Anti‐Perovskite with Strong Chiroptical Nonlinearity23Strategically designed anisotropic organic–inorganic metal halides (OIMHs) with superior balance between bandgap and birefringence12Above Room‐Temperature Reversible Phase Transition and Nonlinear Optical Material PO(CH2CH2CH2CF3)3 with Hirshfeld Surface Analyses0Synergistic engineering of ultraviolet metal-free crystals with exceptional birefringence via pyridine-derived dimers14From (C6H5N2)2CdCl4 to (C6H5N2)2ZnCl4, Chirality Transformation to Realize a Nonlinear Optical Organic–Inorganic Hybrid Halide with Balanced Comprehensive Performance19Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals71Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals8Ultra‐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 Groups46Thermal Evolution of Phosphates and Sulfates with Antiperovskite Structure Type (The Thermal Expansion Features and Phase Transitions)1Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8Decoupling the SHG‐Birefringence Trade‐off in UV NLO Materials via Triple‐Control Coordination Engineering: Achieving Synergistic Performance Optimization88Decoupling the SHG‐Birefringence Trade‐off in UV NLO Materials via Triple‐Control Coordination Engineering: Achieving Synergistic Performance Optimization13Syntheses, Structures, and Characterization of Alkali-Metal Molybdates, A3Cl[Mo2O7] (A = K, Rb and Cs)3All-three-in-one: Pb2(H2PO4)2(C2O4) significantly enhanced birefringence in phosphate materials4Giant Birefringence and Solar‐Blind Ultraviolet Transmission by Coordination‐Induced Assembly of π‐Conjugated Pyridine–Carboxylate8Giant Birefringence and Solar‐Blind Ultraviolet Transmission by Coordination‐Induced Assembly of π‐Conjugated Pyridine–Carboxylate24Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties35Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties6Polar Lithium l -Aspartate Monohydrate: A Semiorganic Ultraviolet Transparent Nonlinear Optical Crystal1A novel metal-free crystal demonstrating superior birefringence attributed to the synergistic interaction of dual π-conjugated units8Dual‐Sided Multidentate Coordination Strategy Enables Record Birefringence in UV‐Transparent Antimony‐Based Hybrid Crystals37Dual‐Sided Multidentate Coordination Strategy Enables Record Birefringence in UV‐Transparent Antimony‐Based Hybrid Crystals11Controlling d10 Metal in Phenylthiourea‐Based Hybrid Metal Halides to Actualize Dimensional Transformation and Significantly Improve the Birefringence11Giant Birefringence and Strong Third-Order Nonlinear Optical Response in a Hybrid Crystal Templated by a Push–Pull π-Conjugated System6(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Giant Birefringence Induced by Intermolecular Aromatic Interactions in Hydrogen‐Bonded Organic Frameworks37Regulating the coplanarity of π-conjugated units through hydrogen bonding in FAHC2O4 and FAH2C3N3S3 crystals5From (C12H9N2)2TeBr6·2H2O to (C12H9N2)2TeBr6: Dehydration-Driven Crystal Reorganization for Birefringence Optimization6(C7H10N)3Bi2I9·I2: Synergistic Cooperation of π-Conjugated Cations and Distorted [BiI6] Octahedra Enabling a Large Infrared Birefringence4Exceptional Enhancement of Optical Anisotropy Achieved via the Strategy of Combining Rigid Groups with High Symmetry and π‐Conjugated Organic Groups in Hybrid Fluorides33Organic π-conjugated units as versatile building blocks for high-performance birefringent crystals6Achieving 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) Groups3Cation-dominated second-harmonic generation in chiral tetrahydro-1-naphthylammonium halides0The condensation of π-conjugated units: a new paradigm for designing high-performance optical crystals4Truss bridge-like anhydrous stacking in hybrid crystals triggers ultra-high stability and robust birefringence0Confinement-assembled ultraviolet nonlinear optical crystal from pyridine-expanded π-systems with exhibiting strong SHG and birefringence18Unveiling the Superior Birefringence Property of a Record‐Birefringent Crystal with Unique Building Block12Halogen Anion-Mediated Substitution of Nitrate: Toward Polar Materials with Intense Second-Harmonic Generation Effects3Hydrogen Bonding Engineering Achieved Hybrid Antiperovskite Ferroelastic in ( C 3 H 8 ON ) 3 ( SnCl 6 )Cl0Polar Antiperovskite Oxides: Promising Mid-Infrared Nonlinear Optical Materials with Strong Second-Harmonic Generation2Ultrawide Bandgap and Record-High Birefringence in a Covalent Beryllium-Organic Framework7Confinement of Organic–Inorganic Hybrid Perovskites within MOF Cavities for Synergistic Regulation of Third-Order Nonlinear Optics0Lock‐and‐Key Assembly Enables Record Birefringence in Monocyclic π‐Conjugated Crystals via Spatial Confinement of Linear Polyhalide5Unlocking Structural Anisotropy by Guest-Symmetry Modulation Strategy to Achieve Giant Birefringence in Molecular Crystals0Interlayer Electronic Decoupling Unlocks Giant Birefringence in π‐Conjugated Metal‐Organic Frameworks0Halogen-Substitution-Modulated Lone-Pair Orientation in Sb(H 2 PO 2 ) 2 X (X = Cl, F) for Enhanced UV Birefringence1Anion-Stabilized Incommensurate Modulation Enables Nonlinear Optical Response in Eu2SiO3.89N0.110Lateral‐Site Unblocking Enables Bilateral π ‐Chromophore Organization for Giant Birefringence in One‐Dimensional Lead Hybrids0Record Second-Harmonic Generation and Exceptional Optical Anisotropy in High-Symmetry 1D Polar Perovskites1Steric‐Guided Coordination Engineering Enables Significantly Optimized Optical Anisotropy via Sulfur‐Driven [C 5 H 5 NS] Birefringence‐Active Groups0Chiral Supramolecular Templating Enables Tunable Second‐Harmonic Generation in Hybrid Zinc Thiocyanates0Rational Construction of Fluoride Crystals With Record Birefringence via Water‐Regulated Hydrogen‐Bond Network Reconfiguration0

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  5. Linear π-conjugated units of the D ∞h point group as superior ultraviolet birefringent units

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  17. Designing a Dimension Reduced Hybrid Perovskite with Robust Large Birefringence by Expanding Cationic π‐Delocation

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  49. Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals

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  50. Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals

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