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RESEARCH PAPER · Journal of the American Chemical Society · 2024

Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond Engineering

Qi Lu, Xingxing Jiang, Kaining Duanmu, Chao Wu, Zheshuai Lin, Zhipeng Huang, Mark Graeme Humphrey, Chi Zhang

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Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond EngineeringOriginal[(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect60Crystal clear: unveiling giant birefringence in organic–inorganic cocrystals33Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer16Large second harmonic generation and birefringence from extended octupolar π-conjugated structures35Reconstructing nearly isotropic microstructures to construct a one-dimensional framework causing record birefringence in thiophosphates13Research progress in optical materials with cationic organic planar π-conjugated groups containing CN bonds34Strategically designed metal-free deep-ultraviolet birefringent crystals with superior optical properties18Chiral Organic Cations and Distorted Inorganic Polyhedra Composing Metal Halide Nonlinear Optical Materials22Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals66Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals8Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units66Halogen Bond Unlocks Ultra‐High Birefringence73Halogen Bond Unlocks Ultra‐High Birefringence14Unraveling the structure–property relationship of novel thiophene and furan‐fused cyclopentadienyl chromophores for nonlinear optical applications10l -Homoproline-Directed Synthesis of Organic–Inorganic Metal Iodides for Second Harmonic Generation14C6N7(NH2)3·H3PO4: Strong Second Harmonic Generation and Giant Birefringence Benefiting from Amino Substitution Strategy24Constructing Ultraviolet Nonlinear Optical Crystals with Superior Thermal Stability Based on Organic π-Conjugated [HCOO] Groups6Toward Strong UV–Vis–NIR Second-Harmonic Generation by Dimensionality Engineering of Zinc Thiocyanates32(C10N2H10)(HI2O6)(HIO3)(IO3): A Birefringent Material Featuring Large π-Conjugated Organic Cation and Two Types of Iodate Anions2Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System7[C3H7N6]3[B3O5(OH)2] and [C3H8N6]4[B12O19(OH)6]: Two Melamine Borates with Large Birefringence13Unconventional Heterobidentate Coordination of 4‐Hydroxypyridine Leading to Remarkably Strong Second‐Harmonic Generation in Zn(C 5 H 4 NO) 267Unconventional Heterobidentate Coordination of 4‐Hydroxypyridine Leading to Remarkably Strong Second‐Harmonic Generation in Zn(C 5 H 4 NO) 221Enabling controllable time‐dependent phosphorescence in carbonized polymer dots based on chromophore excited triplet energy level modulation by ionic bonding34Enabling controllable time‐dependent phosphorescence in carbonized polymer dots based on chromophore excited triplet energy level modulation by ionic bonding5Birefringence Disparity Induced by Synergistic Effects of Stereochemically Active Lone Pairs19Designing a Heteroleptic Tetrahedral Group with an Ultrahigh Polarizability Anisotropy by Optimizing the Bonding Electrons Activity and Their Distribution14Rational Design and Controlled Synthesis of High-Performance Inorganic Short-Wave UV Nonlinear Optical Materials150Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109Strategically designed anisotropic organic–inorganic metal halides (OIMHs) with superior balance between bandgap and birefringence12Unveiling Charge Dependent Law to Enhance Birefringence in 2‐Aminopyrimidine Family21“Three functions in one”: multifunctional rare-earth cyamelurates with magnetism, luminescence, and giant optical nonlinearity6From poor-active to high performance via heteroleptic tetrahedra engineering: rational design of non-π-conjugated hybrids for phase-matchable ultraviolet nonlinear optics12Harnessing the dual role of DMSO in the synthesis of SbOCl·DMSO: an excellent nonlinear optical crystal with unique 1D spiral chain10Highly stable and reversible birefringence switching triggered by thermally stimulated phase transition1Ligand substitution in organic–inorganic hybrid zinc iodides for second-harmonic generation7Significant enhancement in the birefringence of metal phosphite halides via the introduction of π-conjugated cations17Strong second-harmonic generation response in an organic–inorganic hybrid antimony bromide1Chemical Substitution‐Driven Design of a High‐Performance Noncentrosymmetric Bismuth Molybdenum Selenite10Zwitterionic Glycine-Based Antimony Fluorides with Exceptional Ultraviolet Nonlinear Optical Properties11From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal4From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal28Enhanced Birefringence and Excellent Thermal Stability in Two Tellurium(IV) Vanadates: KTeOVO4 and Ca2TeV2O95Inch‐sized K[NH2(CH2COO)2]: a High‐Performance UV Nonlinear Optical Crystal Enabled by Novel Flexible π‐Conjugated Building Units, [NH2(CH2COO)2]−13Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals71Double Sb‐N Coordination Enables Record‐High Birefringence in UV‐Transparent Crystals8pH‐Dependent Switching Between Nonlinear‐Optical‐Active Nitrate‐Based Supramolecular Polymorphs27pH‐Dependent Switching Between Nonlinear‐Optical‐Active Nitrate‐Based Supramolecular Polymorphs2Tuning Birefringence in Supramolecular Mg-PDA Frameworks: Modulating Bonding and Layer Connectivity0Designed Metal‐Free Quasi‐1D Crystals with Giant Birefringence8Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence54Unearthing Hydrogen Bonded Metal‐Free Crystal with Remarkable Optical Anisotropy9Giant 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 Blocks32Nonbonding Electron Inversion‐Driven Structural Engineering: Synergistic Enhancement of Linear and Nonlinear Optical Properties3Nonbonding Electron Inversion‐Driven Structural Engineering: Synergistic Enhancement of Linear and Nonlinear Optical Properties26Hydrogen‐Bonded Assembly of Functional Units for Constructing Linear and Nonlinear Optical Crystals10Decoupling 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 Optimization13Giant 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–Carboxylate24La3Ga5HfO14: Rare-Earth Polyhedron Coupled with Structural Protected Octahedron for Designing Nonlinear Optical Material with Wide Bandgap and Well-Balanced Properties5[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 Birefringence4Halide Ion-Directed Symmetry Control in π-Conjugated Molecular Crystals6Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties35Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties6Enhancement of optical anisotropy from [BF4] units by ligand substitution0Breaking the Birefringence Barrier in B–O Crystals via B–C π-scaffolding36Dual‐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 Crystals11Optimizing the Hydrogen-Bond Network Drives Cadmium Ce(IV) Fluoride Hydrate with Significantly Enhanced Optical Anisotropy8Bromine for iodine: Unlocking short-wavelength UV phase matching in nonlinear optical metal halides6Structural Evolution of Hybrid Bismuth-Based Halides toward Enhanced Second-Harmonic Generation Response and Birefringence through Multisite Chemical Substitution7Achieving the birefringence-bandgap trade-off: Hydrogen-bond engineered biuret-cyanurate14Low‐Dimensional Organic–Inorganic Hybrid Metal Halide with Large Optical Anisotropy9Engineered Integration of Diverse Functional Units Induces Multifunctionality in Malonate‐Borate Hybrids44Anion-Ordered [B3O5(OH)2] Induced by Crystal Water with Deep Ultraviolet Transparency and Large Birefringence in Boron-Rich Borophosphates4Giant Birefringence Induced by Intermolecular Aromatic Interactions in Hydrogen‐Bonded Organic Frameworks37Enhanced Birefringence in Hybrid Antimony Halides via π-Conjugated Organic Cation Design10Tunable Nonlinear Optical Properties in Porphyrin–Cd II Br 2 Complexes Functionalized MXenes Featuring Different Configurations3Anionic Group Trimming Strategy: Oriented Fabrication of Sulfonate UV Birefringent Crystals with High Optical Anisotropy5Breaking the Deep‐UV Transparency/Optical Nonlinearity Trade‐Off: Three‐Parameter Optimization in Oxyfluorides by Tailoring d 0 ‐Metal Incorporation10Breaking the Deep‐UV Transparency/Optical Nonlinearity Trade‐Off: Three‐Parameter Optimization in Oxyfluorides by Tailoring d 0 ‐Metal Incorporation4Five-Membered [C 5 O 5 ] 2 – Rings as Birefringence-Active Genes for Ultrabirefringent Crystals27Organic Halogen Substitution-Driven Halogen Bonding Induces Polar 3D Supramolecular Framework and Second-Harmonic-Generation Response7From (C12H9N2)2TeBr6·2H2O to (C12H9N2)2TeBr6: Dehydration-Driven Crystal Reorganization for Birefringence Optimization6Exceptional Enhancement of Optical Anisotropy Achieved via the Strategy of Combining Rigid Groups with High Symmetry and π‐Conjugated Organic Groups in Hybrid Fluorides33[Pb(ptz)(OH)(H2O)]: A Hybrid Nonlinear Optical Crystal with Large Birefringence0Hydrogen-bond-driven noncentrosymmetric structure formation in π-conjugated (C3H7N6)(IO3): achieving both strong SHG response and wide bandgap5Enhancing birefringence and second-harmonic generation response via aliovalent metal substitution2Enhanced Second Harmonic Generation Response via Rational Design of Iodinated π-Conjugated Pyridine Group5Effect of Multiple Hydrogen Bonding on the π-Conjugated Groups and Optical Properties in Molecular Crystals5Unlocking Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Polar Organic Sulfonates through Connectivity Regulation2Unlocking Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Polar Organic Sulfonates through Connectivity Regulation6Integrating Fluorinated [BF 4 ] Anion With π‐Conjugated Six‐Membered Rings for Short‐Wavelength UV Frequency Conversion17Integrating Fluorinated [BF 4 ] Anion With π‐Conjugated Six‐Membered Rings for Short‐Wavelength UV Frequency Conversion2Chiral Lead-Oxyiodide Nonlinear Optical Crystals Constructed on l -Malate Groups5Na2(C6H4NO3)2·H2O: A promising ultraviolet nonlinear optical crystal with strong second-harmonic generation effect and large birefringence1Sb 2 (SeO 3 ) 2 SeO 4 : A Selenite–Selenate Crystal with Balanced Band Gap and Birefringence3A Homoatomic Heteroleptic Coordination Strategy for Exceptional Infrared Linear and Nonlinear Optical Properties in ANb 2 PS 4 (S 2 ) 3 (A = K,Rb,Cs)3A mercury-based selenite with wide bandgap and moderate birefringence via cation substitution and partial fluorination1A series of langasite-type compounds: size effect regulation for cation occupation and enhanced SHG response1Diamond-like Ag x Cu 3− x PS 4 ( x = 1 and 2) synthesized by the metal oxide–boron–chalcogen (MOBQ) routine: local high-entropy engineering for balanced infrared nonlinear optical performance1From centrosymmetric (C 4 H 8 N 5 )(SbF 4 ) to polar (C 4 H 7 N 4 O)(SbF 4 ): a new UV nonlinear optical material achieved by functional group modulation8Halogen-ion-driven polymorphs for high-performance nonlinear optical crystalline materials3Stable lead succinate-iodides with strong second-harmonic generation response and large birefringence0Strategically designed deep-ultraviolet optical crystals with balanced properties by small heteroatom substitution1The 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 birefringence0氢键组装的新型紫外非线性光学晶体（R/S‑DACH）Mal·H2O的设计及性能研究（特邀）0Confinement-assembled ultraviolet nonlinear optical crystal from pyridine-expanded π-systems with exhibiting strong SHG and birefringence18Realizing Phase‐Matching of Nonlinear Optical [ABa 3 Br 2 ][Ga 5 Se 10 ] (A = Cs, Rb, K, Na) Through Large Anisotropic Lattice Distortion6Realizing Phase‐Matching of Nonlinear Optical [ABa 3 Br 2 ][Ga 5 Se 10 ] (A = Cs, Rb, K, Na) Through Large Anisotropic Lattice Distortion11Hydrogen‐Bond‐Modulated Alignment of Iminodiacetic Acid Cations for Achieving Ultraviolet Second Harmonic Generation6Halogen‐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 Crystal2Zn 4 S(C 2 H 2 N 3 ) 3 (NCS) 3 : Coordination-Driven Structural Distortion Engineering Triggers Exceptional NLO Effect in Mixed-Bonding Zinc Isothiocyanate6(C 6 H 7 N 2 O)NO 3 : π-Conjugation-Driven Synergistic Enhancement of Second-Harmonic Generation and Birefringence0Unlocking Strong SHG Response and Large Birefringence in Hybrid Antimony Halides via a Three-in-One Strategy7Nonlinear Optical Responses in One-Dimensional Zinc Thiocyanates Functionalized with Natural Amino Acids8[C 3 N 2 H 5 ]B 7 O 10 F 2 : Demonstrating a New Hydrogen‐Bond‐Induced Intralayer Charge‐Balanced Structure Model with Large Birefringence3Density-Compensated Polarizability Anisotropy for Record Birefringence in Short-Wavelength Ultraviolet Inorganic Crystals11Overcoming the Bandgap‐Birefringence Trade‐Off: Proton‐Transfer Engineering of High‐Performance Ultraviolet‐Transparent Organic Crystal5Conformational Editing Drives Covalent Hybridization for Nonlinear Optical Crystals2Dual‐Functional Ultraviolet Nonlinear Optics and Bright Luminescence Achieved in the First Fluorine‐Containing Hybrid Lone‐Pair Metal Mixed Halides8Persistent Second‐Harmonic Generation Enhancement Across an Unprecedented Pressure Range in a Hybrid Antimony Halide0Persistent Second‐Harmonic Generation Enhancement Across an Unprecedented Pressure Range in a Hybrid Antimony Halide0An Ultra-Wide Bandgap Sulfonate with Two-Step Second-Harmonic Generation Switching2Recent Progress in Hg-Based Oxysalt Crystals for Nonlinear Optics and Birefringence Applications5Strong Optical Nonlinearity in Polar Hypophosphites via Chiral Cation Assembly1Ultrawide Bandgap and Record-High Birefringence in a Covalent Beryllium-Organic Framework7NaNO 3 [(NH 2 ) 2 SO 2 ] 2 : A Halogen‐Free KBBF‐Type Nitrate Crystal with Record Birefringence for Ultraviolet Applications0Enhanced Birefringence in Organic–Inorganic Hybrid Antimony Halides via Partial Halogen Substitution1Redox‐Driven Strategy Enabling Leapfrog Enhancement of Birefringence in Layered Tin‐Based Optical Crystals1Bio-inspired proton-conformation-coupled hydrogen-bond network reconfiguration for adaptive optical anisotropy0Breaking Layered Limitations via Electrostatic-to-Covalent Conversion toward Three-Dimensional T2-Cluster-Based Chalcogenides7Interlayer Electronic Decoupling Unlocks Giant Birefringence in π‐Conjugated Metal‐Organic Frameworks0Peroxide‐Assisted Solvate Engineering Enables Record‐High Birefringence in a Solar‐Blind Transparent Crystal0Peroxide‐Assisted Solvate Engineering Enables Record‐High Birefringence in a Solar‐Blind Transparent Crystal0Lateral‐Site Unblocking Enables Bilateral π ‐Chromophore Organization for Giant Birefringence in One‐Dimensional Lead Hybrids0Lateral‐Site Unblocking Enables Bilateral π ‐Chromophore Organization for Giant Birefringence in One‐Dimensional Lead Hybrids0Eu5ZnGa6S15, Eu5Zn3Ga2Sn2S15, and Pb5HgGa6S15: Crystal Chemistry and Nonlinear Optical Properties0Record Second-Harmonic Generation and Exceptional Optical Anisotropy in High-Symmetry 1D Polar Perovskites1Advances in metal selenite nonlinear optical materials: halogens directed structure modulation and property optimization0A Two‐Dimensional Organic Salt With a Deep‐Ultraviolet Cutoff Edge and Strong Second‐Harmonic Generation0A Two‐Dimensional Organic Salt With a Deep‐Ultraviolet Cutoff Edge and Strong Second‐Harmonic Generation0Coordination-Mode-Modulated Symmetry Breaking for Nonlinear Optical Crystals0The Parallel Coplanar Alignment of Planar Non‐π‐Conjugated [Pb 3 Br 3 ] Rings for a Stable Ultraviolet Nonlinear Optical Crystal0

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  1. [(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect

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  3. Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer

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  4. Large second harmonic generation and birefringence from extended octupolar π-conjugated structures

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  5. Reconstructing nearly isotropic microstructures to construct a one-dimensional framework causing record birefringence in thiophosphates

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  9. Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals

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  10. Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals

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  11. Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units

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  12. Halogen Bond Unlocks Ultra‐High Birefringence

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  13. Halogen Bond Unlocks Ultra‐High Birefringence

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  14. Unraveling the structure–property relationship of novel thiophene and furan‐fused cyclopentadienyl chromophores for nonlinear optical applications

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  16. C6N7(NH2)3·H3PO4: Strong Second Harmonic Generation and Giant Birefringence Benefiting from Amino Substitution Strategy

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  18. Toward Strong UV–Vis–NIR Second-Harmonic Generation by Dimensionality Engineering of Zinc Thiocyanates

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  19. (C10N2H10)(HI2O6)(HIO3)(IO3): A Birefringent Material Featuring Large π-Conjugated Organic Cation and Two Types of Iodate Anions

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  20. Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System

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  21. [C3H7N6]3[B3O5(OH)2] and [C3H8N6]4[B12O19(OH)6]: Two Melamine Borates with Large Birefringence

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  22. Unconventional Heterobidentate Coordination of 4‐Hydroxypyridine Leading to Remarkably Strong Second‐Harmonic Generation in Zn(C 5 H 4 NO) 2

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  23. Unconventional Heterobidentate Coordination of 4‐Hydroxypyridine Leading to Remarkably Strong Second‐Harmonic Generation in Zn(C 5 H 4 NO) 2

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  24. Enabling controllable time‐dependent phosphorescence in carbonized polymer dots based on chromophore excited triplet energy level modulation by ionic bonding

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  25. Enabling controllable time‐dependent phosphorescence in carbonized polymer dots based on chromophore excited triplet energy level modulation by ionic bonding

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  26. Birefringence Disparity Induced by Synergistic Effects of Stereochemically Active Lone Pairs

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  27. Designing a Heteroleptic Tetrahedral Group with an Ultrahigh Polarizability Anisotropy by Optimizing the Bonding Electrons Activity and Their Distribution

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  31. Unveiling Charge Dependent Law to Enhance Birefringence in 2‐Aminopyrimidine Family

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  32. “Three functions in one”: multifunctional rare-earth cyamelurates with magnetism, luminescence, and giant optical nonlinearity

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  33. From poor-active to high performance via heteroleptic tetrahedra engineering: rational design of non-π-conjugated hybrids for phase-matchable ultraviolet nonlinear optics

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  34. Harnessing the dual role of DMSO in the synthesis of SbOCl·DMSO: an excellent nonlinear optical crystal with unique 1D spiral chain

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  35. Highly stable and reversible birefringence switching triggered by thermally stimulated phase transition

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    Cheng Chen, Yunjie Bai, Qi Wu Shi, Mingye Han, Bingbing Zhang, Ying Wang

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  36. Ligand substitution in organic–inorganic hybrid zinc iodides for second-harmonic generation

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    Juan Cheng, Gangji Yi, Ying Long, Qinglan Zhong, Guohong Zou, Lindong Luan, Zhien Lin

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  37. Significant enhancement in the birefringence of metal phosphite halides via the introduction of π-conjugated cations

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    Ru‐Ling Tang, Yue Wang, Yi‐Lei Lv, Bing-Wei Miao, Wenlong Liu, Sheng‐Ping Guo

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  38. Strong second-harmonic generation response in an organic–inorganic hybrid antimony bromide

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    Xuemei Wen, Gangji Yi, Qinglan Zhong, Caihong Guo, Hongmei Zeng, Guohong Zou, Zhien Lin

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  39. Chemical Substitution‐Driven Design of a High‐Performance Noncentrosymmetric Bismuth Molybdenum Selenite

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