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RESEARCH PAPER · Angewandte Chemie International Edition · 2025

Decoupling the SHG‐Birefringence Trade‐off in UV NLO Materials via Triple‐Control Coordination Engineering: Achieving Synergistic Performance Optimization

Yaolong Zhu, Jie Gou, Can Yang, Qingwen Zhu, Yi Xiong, Qi Wu

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Decoupling the SHG‐Birefringence Trade‐off in UV NLO Materials via Triple‐Control Coordination Engineering: Achieving Synergistic Performance OptimizationOriginalA strongly birefringent sulfate crystal with a wide second-harmonic generation phase-matching range4Controlling topological diversity and magnetic properties in three Tb( iii ) metal–organic frameworks through amide ligand variation3KNa 2 Y 2 B 2 O 6 F 3 : a beryllium free deep-UV nonlinear optical crystal with well-balanced properties2Pioneering Sulfophosphite Crystals: Co-Assembly of Phosphite and Sulfate Units in Novel Inorganic Architectures0Proton conduction in three molecular assemblies of bipyridyl–organodisulfonate salts1Nonlinear Optical Series A(VO2)3(SeO3)2 (A = NH4+, K+, and H3O+) with Large Birefringence Derived from High-Anisotropic VO6 Octahedra and SeO3 Pyramids8A Promising Short-Wave UV NLO Crystal with an Optimized KBBF-like Structure and Well-Balanced Properties Achieved via a Chemical Substitution Strategy6Breaking the Birefringence Barrier in B–O Crystals via B–C π-scaffolding36Synthesis and Characterization of (H7C5N2)6(V10O28)·2H2O with Edge-Sharing VO6 Octahedra Exhibiting Large Birefringence2Design and Synthesis of New Furan-Like Chalcone Crystals with Two Para-Substituents: 5MFTF and 5MFTN0Designing Hybrid Sb-Based Nonlinear Optical Crystals with Large Birefringence by Combining the Lone Pair and π-Conjugated Genes10Structural Evolution of Hybrid Bismuth-Based Halides toward Enhanced Second-Harmonic Generation Response and Birefringence through Multisite Chemical Substitution7Strongly Polar [H2PO3]− Induced π-Conjugated Group Arrangement for Balanced UV Nonlinear Optical Performance3Alkali Metal Substitution-Induced Structural Transformation for RbREP2Se6 (RE = Gd, Tb, Dy) with Second-Harmonic Generation Responses6(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Synergistic Enhancement of Band Gap and Optical Anisotropy via Functional-Site Cosubstitution in Antiperovskite-Type Chalcohalides [Ba2K][X][MS4] (M = Ge, Si; X = Cl, Br)2Pioneering sulfophosphite crystals: Co-assembly of phosphite and sulfate units in novel inorganic architectures0SrZnSiS4: Shattering the 4.0 eV Threshold toward Dual-Optimized Bandgap and Second-Harmonic Generation5Tuning the Anionic Configuration in ASc2(P2O7)2 (A = Ba, Pb) through A-Site Cationic Coordination Engineering0[HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap12LnEuGa3OS6 (Ln = La, Pr, Nd): three dual rare earth metal-based oxychalcogenides with good IR nonlinear optical performances1Modulating Nonlinear Optical Performances in α/β-SnGa2GeS6 Polymorphs via Atomic Coordination Engineering1Assembly of Highly Polarizable “Linkers” with Heteroleptic Groups for Inducing Large Optical Anisotropy in Ba2SnIIGe3O8S and Ba3SnIIGe3O2S82Exceptional Enhancement of Optical Anisotropy Achieved via the Strategy of Combining Rigid Groups with High Symmetry and π‐Conjugated Organic Groups in Hybrid Fluorides33NaAg3Ga8S14: A new diamond-like framework infrared nonlinear optical material derived from AgGaS26Hydrogen-bond-driven noncentrosymmetric structure formation in π-conjugated (C3H7N6)(IO3): achieving both strong SHG response and wide bandgap5Remarkable Birefringence Enhancement Enabled by π-Conjugated Cyanoguanidine Group Based on Anisotropic Molecule Coordination Approach8Shape‐Topology‐Driven Design of Deep Ultraviolet Nonlinear Optical Crystals: Engineering [CH 3 PO 3 ]–Metal‐Oxo Layered Frameworks for Enhanced SHG, DUV Transparency3Tunable dual-emission in a hybrid [Ph3PH]2[ZnI4] system: The role of {ZnI…HP} interactions and proton transfer in 3ILCT/3L(X + M)CT phosphorescence1Three Co 2+ /Cd 2+ -terpyridine based coordination compounds: synthesis, structures, photophysical and theoretical study0Rational design of novel mixed metal sulfates with diverse dimensional structures and short UV cutoff edges1Single‐Source Cyanurate Precursor for Making Manganese Carbodiimide and the Second Harmonic Generation Effect of the Intermediate Manganese Monohydrocyanurate Mn(HC 3 N 3 O 3 )0Cobalt-Based MOFs as an Efficient Sulfur Host for High-Performance Lithium-Sulfur Batteries0Chiral Lead-Oxyiodide Nonlinear Optical Crystals Constructed on l -Malate Groups5KCd(IO 3 ) 2 Cl: A New UV NLO Crystal with Balanced Optical Properties Engineering via Target‐Driven Multi‐Ion Substitution Strategy7Chiral-Unit-Driven Short-Wave Ultraviolet Nonlinear Optical Acetates with Balanced Overall Optical Properties3(C 4 H 8 N 5 )(PhPHO 2 )·H 2 O: a polar ionic cocrystal with strong second-harmonic generation and high birefringence0[Cd 4 P 2 ][I 3 ] and [Cd 2 P][CdCl 3 ]: two Millon's phase phosphides exhibiting wide band gaps and large birefringence0[Rb 4 Cl][Cd 11 In 9 Se 26 ]: a salt inclusion chalcogenide with a diamond-like framework for infrared nonlinear optics0A[N(SO 2 NH 2 ) 2 ] (A = Na, K, Rb, and Cs): enhancing birefringence of non π-conjugated deep-ultraviolet crystals via novel dimeric disulfonamide [N(SO 2 NH 2 ) 2 ] − groups0CaM 3 Si 4 As 11 (M = Ga, In): arsenide infrared nonlinear optical crystals enforced by novel [As 2 ] linear motifs0Covalent hybrid cadmium halides with heteroleptic tetrahedral units exhibiting a wideband nonlinear optical response0From Ba[Sn(IO 3 ) 6 ] to Ba[Sn(IO 3 ) 4 F 2 ]: fluoride-ion-driven enhancement of birefringence and band gap1Halogen-ion-driven polymorphs for high-performance nonlinear optical crystalline materials3KGdSiSe 4 and KGdGeSe 4 : two rare earth-based selenides with wide bandgaps and large nonlinear optical responses0Optical anisotropy in Mo–Te–O frameworks constructed from distorted MoO 6 and TeO 3 units0Regulating KBBF-like structures via a charge-assisted hydrogen-bonded framework to enable easily grown ultraviolet nonlinear optical crystals0Second-harmonic generation in two hybrid organic–inorganic metal chlorides based on l -thioproline ligand1Second-harmonic generation responses in low-dimensional metal bromides functionalized with l -arginine1Confinement-assembled ultraviolet nonlinear optical crystal from pyridine-expanded π-systems with exhibiting strong SHG and birefringence18The modulation of structural polarity facilitating the gradient enhancement of second harmonic generation effects in hybrid metal halides5Realizing Phase‐Matching of Nonlinear Optical [ABa 3 Br 2 ][Ga 5 Se 10 ] (A = Cs, Rb, K, Na) Through Large Anisotropic Lattice Distortion11Rare-Earth Selenophosphates Cs 2 YP 2 Se 7 and KYP 2 Se 6 Synthesized by the RFMOBQ Routine: Structural Evolution and Nonlinear Optical Activity2Strategic Oxygen‐Substitution in Perfluorinated Ce(IV) Coordination Frameworks Triggers Dual‐Wavelength Nonlinear Optical Materials With Exceptional Performances32Sn 4+ /Sn 2+ Aliovalent Substitution: A Strategy for Local Structure Engineering to Enhance Birefringence and Trigger Structural Symmetry Transition0Unlocking Strong SHG Response and Large Birefringence in Hybrid Antimony Halides via a Three-in-One Strategy7Coordination Geometry-Directed Optical Anisotropy and Phase-Matched Nonlinear Optics in Chiral Metal–Organic Frameworks2Host–guest exchange and preservation of framework chirality in Mn-based crystals0C 6 H 7 NCl·X (X = Cl, Br): Outstanding Multifunctional Nonlinear Optical and Birefringent Crystals Enabled by Incorporation of π‐Conjugated Moieties2Halogen Anion-Mediated Substitution of Nitrate: Toward Polar Materials with Intense Second-Harmonic Generation Effects3Controllable Photoluminescence Modulation of 2D Hybrid Materials Based on (DFCBA) 2 PbX 4 (X = I, Br) via Halogen Regulation2{[Ge 2 S 7 ] 6– } ∞ Chains-Mediated Framework Reorganization Triggers Dimensional Upgrade and Infrared Nonlinear Optical Response3Rational design of a quasi-0D tungsten tellurite nonlinear optical crystal with exceptionally balanced properties1An Ultraviolet Transparent Nonlinear Optical Crystal Assembled from a Polarizable Tetrahedral Unit1Dual‐Functional Ultraviolet Nonlinear Optics and Bright Luminescence Achieved in the First Fluorine‐Containing Hybrid Lone‐Pair Metal Mixed Halides8Halogen Engineering and Orbital Origins of Large Second-Harmonic Generation in Organic–Inorganic Hybrid Metal Halides2Polar Antiperovskite Oxides: Promising Mid-Infrared Nonlinear Optical Materials with Strong Second-Harmonic Generation2(C 5 H 7 N 2 ) (C 8 H 4 O 4 ) PbBr: Jahn–Teller Distortion‐Induced Tilting of π‐Conjugated Planes Resolving the Second‐Order Polarizability–Structural Anisotropy Conflicts13Quadrupolar IDIC chromophores exhibiting strong two-photon absorption beyond 1000 nm1Chirality-driven polar lattice engineering for high-performance organic nonlinear optical crystals3Strong Optical Nonlinearity in Polar Hypophosphites via Chiral Cation Assembly1Design of a High-Performance Infrared Nonlinear Optical Crystal via a Multiple Flexible-Group Synergistic Polarization Strategy10The Enhancement of Phase‐Matching Capability by Recombining π‐Conjugated Group in Nonlinear Optical Sulfates1The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 115The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 110Linear [ICl 2 ] Units Induced Giant Optical Anisotropy in AICl 2 (A = NH 4 , Rb): A Pathway to Advanced Birefringent Materials4Dual tuning of second-harmonic generation and Rashba-Dresselhaus spin-splitting in chiral hybrid perovskites via halogen-site engineering1Unlocking Nonlinear Optics and Photoluminescence with Simultaneous Enhancement of Bandgap and Birefringence in Hybrid Sb-Based Halides2A Strategy for Enhancing the Optical Anisotropy of Phosphates via Tetrahedral Unit Modification0Nonlinear Optical-Active NaAlP 2 S 6 Synthesized by the MOBQ Method: Synthesis, Structure, and Optical Properties0Covalent Interlayer Engineering Enables Ideal Birefringence and Strong SHG in Beryllium‐Free Deep‐UV NLO Borates2Potassium-Stabilized 2H-Type Indium Sulfide in the Noncentrosymmetric Crystal K0.33[Zn0.33In1.67S3] Probed by Azimuthal SHG0Simultaneous Second Harmonic Generation (SHG) and Upconversion Luminescence Enabling Fully Non‐Linear Optical Thermometry in Ferroelectric Ceramics1Record 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 Groups0A Two‐Dimensional Organic Salt With a Deep‐Ultraviolet Cutoff Edge and Strong Second‐Harmonic Generation0A Hydrogen-Bonded Molecular Crystal with Strong Optical Anisotropy and Large Second-Harmonic Generation Response0

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  1. A strongly birefringent sulfate crystal with a wide second-harmonic generation phase-matching range

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  2. Controlling topological diversity and magnetic properties in three Tb( iii ) metal–organic frameworks through amide ligand variation

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  3. KNa 2 Y 2 B 2 O 6 F 3 : a beryllium free deep-UV nonlinear optical crystal with well-balanced properties

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  4. Pioneering Sulfophosphite Crystals: Co-Assembly of Phosphite and Sulfate Units in Novel Inorganic Architectures

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  5. Proton conduction in three molecular assemblies of bipyridyl–organodisulfonate salts

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  6. Nonlinear Optical Series A(VO2)3(SeO3)2 (A = NH4+, K+, and H3O+) with Large Birefringence Derived from High-Anisotropic VO6 Octahedra and SeO3 Pyramids

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  7. A Promising Short-Wave UV NLO Crystal with an Optimized KBBF-like Structure and Well-Balanced Properties Achieved via a Chemical Substitution Strategy

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  8. Breaking the Birefringence Barrier in B–O Crystals via B–C π-scaffolding

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  9. Synthesis and Characterization of (H7C5N2)6(V10O28)·2H2O with Edge-Sharing VO6 Octahedra Exhibiting Large Birefringence

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  10. Design and Synthesis of New Furan-Like Chalcone Crystals with Two Para-Substituents: 5MFTF and 5MFTN

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  11. Designing Hybrid Sb-Based Nonlinear Optical Crystals with Large Birefringence by Combining the Lone Pair and π-Conjugated Genes

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  12. Structural Evolution of Hybrid Bismuth-Based Halides toward Enhanced Second-Harmonic Generation Response and Birefringence through Multisite Chemical Substitution

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  13. Strongly Polar [H2PO3]− Induced π-Conjugated Group Arrangement for Balanced UV Nonlinear Optical Performance

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  14. Alkali Metal Substitution-Induced Structural Transformation for RbREP2Se6 (RE = Gd, Tb, Dy) with Second-Harmonic Generation Responses

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  15. (CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment

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  16. Synergistic Enhancement of Band Gap and Optical Anisotropy via Functional-Site Cosubstitution in Antiperovskite-Type Chalcohalides [Ba2K][X][MS4] (M = Ge, Si; X = Cl, Br)

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  17. Pioneering sulfophosphite crystals: Co-assembly of phosphite and sulfate units in novel inorganic architectures

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  18. SrZnSiS4: Shattering the 4.0 eV Threshold toward Dual-Optimized Bandgap and Second-Harmonic Generation

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  19. Tuning the Anionic Configuration in ASc2(P2O7)2 (A = Ba, Pb) through A-Site Cationic Coordination Engineering

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  20. [HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap

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  23. Assembly of Highly Polarizable “Linkers” with Heteroleptic Groups for Inducing Large Optical Anisotropy in Ba2SnIIGe3O8S and Ba3SnIIGe3O2S8

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  30. Three Co 2+ /Cd 2+ -terpyridine based coordination compounds: synthesis, structures, photophysical and theoretical study

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  31. Rational design of novel mixed metal sulfates with diverse dimensional structures and short UV cutoff edges

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  32. Single‐Source Cyanurate Precursor for Making Manganese Carbodiimide and the Second Harmonic Generation Effect of the Intermediate Manganese Monohydrocyanurate Mn(HC 3 N 3 O 3 )

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  33. Cobalt-Based MOFs as an Efficient Sulfur Host for High-Performance Lithium-Sulfur Batteries

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  34. Chiral Lead-Oxyiodide Nonlinear Optical Crystals Constructed on l -Malate Groups

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  35. KCd(IO 3 ) 2 Cl: A New UV NLO Crystal with Balanced Optical Properties Engineering via Target‐Driven Multi‐Ion Substitution Strategy

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  37. (C 4 H 8 N 5 )(PhPHO 2 )·H 2 O: a polar ionic cocrystal with strong second-harmonic generation and high birefringence

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  38. [Cd 4 P 2 ][I 3 ] and [Cd 2 P][CdCl 3 ]: two Millon's phase phosphides exhibiting wide band gaps and large birefringence

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  39. [Rb 4 Cl][Cd 11 In 9 Se 26 ]: a salt inclusion chalcogenide with a diamond-like framework for infrared nonlinear optics

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  40. A[N(SO 2 NH 2 ) 2 ] (A = Na, K, Rb, and Cs): enhancing birefringence of non π-conjugated deep-ultraviolet crystals via novel dimeric disulfonamide [N(SO 2 NH 2 ) 2 ] − groups

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  41. CaM 3 Si 4 As 11 (M = Ga, In): arsenide infrared nonlinear optical crystals enforced by novel [As 2 ] linear motifs

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  42. Covalent hybrid cadmium halides with heteroleptic tetrahedral units exhibiting a wideband nonlinear optical response

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  43. From Ba[Sn(IO 3 ) 6 ] to Ba[Sn(IO 3 ) 4 F 2 ]: fluoride-ion-driven enhancement of birefringence and band gap

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  44. Halogen-ion-driven polymorphs for high-performance nonlinear optical crystalline materials

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  45. KGdSiSe 4 and KGdGeSe 4 : two rare earth-based selenides with wide bandgaps and large nonlinear optical responses

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  46. Optical anisotropy in Mo–Te–O frameworks constructed from distorted MoO 6 and TeO 3 units

    Dalton Transactions · 2026-01-01

    Cheng He, Kun Hu, Jing-Yang Zhou, Long Wu, Jian‐Han Zhang

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  47. Regulating KBBF-like structures via a charge-assisted hydrogen-bonded framework to enable easily grown ultraviolet nonlinear optical crystals

    Chemical Science · 2026-01-01

    Mingshu Zhang, Shuya Zhao, Zhen‐Cheng Wu, Yue Yin, Zheyu Zhang, Jiafeng Chen, Sheng‐Ping Guo, Yan Zhou

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  48. Second-harmonic generation in two hybrid organic–inorganic metal chlorides based on l -thioproline ligand

    CrystEngComm · 2026-01-01

    Yingjie Wang, Peiqi Qian, Xuemei Wen, Hongmei Zeng, Guohong Zou, Zhien Lin

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  49. Second-harmonic generation responses in low-dimensional metal bromides functionalized with l -arginine

    CrystEngComm · 2026-01-01

    Juan Cheng, Yingjie Wang, Qinglan Zhong, Ziyu Zhou, Hongmei Zeng, Guohong Zou, Zhien Lin

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  50. Confinement-assembled ultraviolet nonlinear optical crystal from pyridine-expanded π-systems with exhibiting strong SHG and birefringence

    Science China Chemistry · 2026-01-04

    Chunmei Huang, Xuan Pang, Fuming M. Li, Shumei Cao, Shilie Pan, Miriding Mutailipu

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