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RESEARCH PAPER · Angewandte Chemie International Edition · 2023

Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence

Xuefei Wang, Xudong Leng, Yunseung Kuk, Jihyun Lee, Qun Jing, Kang Min Ok

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Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and BirefringenceOriginalDesign of alkali lead oxybromides with a strong second-harmonic generation response and large birefringence1Halide-driven polarity tuning and optimized SHG-bandgap balance in (C 4 H 11 N 2 )ZnX 3 (X = Cl, Br, I)34Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material32Large second harmonic generation and birefringence from extended octupolar π-conjugated structures35New ultraviolet transparent rare-earth borates with enhanced birefringence induced by cation chemical substitution15Salt-inclusion chalcogenides with d-orbital components: unveiling remarkable nonlinear optical properties and dual-band photoluminescence10Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds31The Birefringence Modulation in Short‐Wave Ultraviolet Sulfates with Functional π‐Conjugated Cations and Polymerized Heteroleptic Tetrahedral Anions18Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation153Rational Combination of π‐Conjugated and Non‐π‐Conjugated Groups Achieving Strong Nonlinear Optical Response, Large Optical Anisotropy, and UV Light‐Switchable Fluorescence65Na3K6(CO3)3(NO3)2X·6H2O (X = NO3, Cl, Br): Exploring High-Performance UV Birefringent Crystals Induced by Coplanar π-Conjugated CO3 and NO3 Groups15A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability14Cs2Pb(CO3)2: a novel mixed-metal carbonate with rare Pb-C-O one-dimensional chain0Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering61Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering4Na2B6SO13 with unprecedented [B6SO13]∞ double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B3O7] units19Tetrahedra Modification of Phosphates for Optical Anisotropy Enhancement13Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family23Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System7The design of a non-centrosymmetric structure in sulfates by cation-induced symmetry breaking4Unconventional 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) 221The New Paradigm of Ligand Substitution-Driven Enhancement of Anisotropy from SO4 Units in Short-Wavelength Region14Designing a Heteroleptic Tetrahedral Group with an Ultrahigh Polarizability Anisotropy by Optimizing the Bonding Electrons Activity and Their Distribution14(C 6 H 5 N 2 )HgCl 3 : Discovery of a Polar Hg‐Based Hybrid Halide as Preeminent Nonlinear Optical and Birefringent Material Activated by π‐Conjugated Organic Cation Substitution38(CN 4 H 7 ) 2 SO 4 ·H 2 O: high-performance metal-free ultraviolet birefringent crystal with KBBF-like configuration5A strongly birefringent sulfate crystal with a wide second-harmonic generation phase-matching range4An excellent ultraviolet nonlinear optical crystal derived from the polar methylphosphonate unit8Deep-ultraviolet sulfamate halides with halogen-centered secondary building units for enhanced optical anisotropy4Designing a novel perovskite-type KCd(NH 2 SO 3 ) 3 with deep-ultraviolet transparency and strong second-harmonic generation response2Different p-block elements induce C 3 [111] octahedral distortion in titanium to generate an intense nonlinear effect14Highly stable and reversible birefringence switching triggered by thermally stimulated phase transition1K 2 SO 4 (NH 3 SO 3 ) 2 and Cs 2 SO 4 (NH 3 SO 3 ) 3 : two deep-UV transparent sulfamate-sulfates with moderate birefringence2Non-centrosymmetric structures designed rationally via a “dimensionality addition” strategy toward the promising nonlinear optical family [A–X][In–Se] (A = K/Ba and Rb/Ba; X = Cl and Br)13Selenoborates: a latent structure resource for infrared functional crystal materials1Designing Polar Covalent Hybrid Cadmium‐Based Chalcohalides Ultraviolet Nonlinear Optical Crystal with Strong Optical Anisotropy via Double‐Site Dual FBUs Tailoring25A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy22A Wide Band Gap Germanate with the Largest Second Harmonic Generation Response Created by Hypoxic Strategy5Reinforced Nonlinear Optical Performances Induced by P‐P Homoatomic Bond in Phosphide SrIn 3 Si 4 P 1131Reinforced Nonlinear Optical Performances Induced by P‐P Homoatomic Bond in Phosphide SrIn 3 Si 4 P 116K3[HCO3]2F: a new deep-UV birefringent crystal exhibiting strong optical anisotropy17Regulation of Refractive Index by Halogens in Two-Dimensional Layered Methylsulfonate Halides7Polar [ NH ( CH2SO3 )2]2− Dimers Enable the First Promising Iminodimethanesulfonate with Nonlinear Optical Properties and Wide UV Transparency19Synergistic Machine Learning Guided Discovery of ABa 3 (BSe 3 ) 2 X (A = Rb, Cs; X = Cl, Br, I): A Promising Family as Property‐Balanced IR Functional Materials10A strategy to achieve giant optical anisotropy via integrating linear pseudohalogen and stereochemical active lone pair cation6La(SO3NH2)2NO3·H2O: synergistic anion engineering of the first rare-earth nitrate sulfamate defying transparency-birefringence-nonlinearity trade-offs in ultraviolet nonlinear optics8Direct Deep‐UV Second‐Harmonic Generation in Disordered Χ 2 ‐Modulated Ferroelectric Crystals18Anionic 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 Incorporation4Assembly of Highly Polarizable “Linkers” with Heteroleptic Groups for Inducing Large Optical Anisotropy in Ba2SnIIGe3O8S and Ba3SnIIGe3O2S82Unlocking Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Polar Organic Sulfonates through Connectivity Regulation6Chiral Lead-Oxyiodide Nonlinear Optical Crystals Constructed on l -Malate Groups5Hydrogen‐Bond‐Driven Metal‐Free Crystal (C 6 H 7 N 2 O)(NH 2 SO 3 ) with Giant Birefringence and Solar‐Blind Ultraviolet Transmission0A Deep-Ultraviolet Transparent Nonlinear Optical Hydrogen-Bonded Organic Framework21Navigating the Landscape of Next-Generation Nonlinear Optical Materials Discovery: Opportunities and Challenges Driven by Artificial Intelligence4[Cd 4 P 2 ][I 3 ] and [Cd 2 P][CdCl 3 ]: two Millon's phase phosphides exhibiting wide band gaps and large birefringence0A[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 ] − groups0Stable lead succinate-iodides with strong second-harmonic generation response and large birefringence0Synergism of [C 2 N 4 H 7 S] cations and anionic modulators: tailoring second-order nonlinear optics and birefringence in organic–inorganic crystals6Synergistic dual-modification strategy of π-conjugated cations and tetrahedra: rational design of ultraviolet high-birefringence monofluorophosphates0Functional Unit Design of Deep‐UV NLO Crystals With Short Phase‐Matching and Large SHG Response22An Ultraviolet Transparent Nonlinear Optical Crystal Assembled from a Polarizable Tetrahedral Unit1Magnesium Methylphosphonate Ultraviolet Nonlinear Optical Crystal With Ultrawide Bandgap and Strong Second‐Harmonic Generation Response0An Ultra-Wide Bandgap Sulfonate with Two-Step Second-Harmonic Generation Switching2Synergistic Enhancement of Optical Anisotropy in Nitrate Sulfamate for UV Applications: Role of Functional Group Alignment and Hydrogen Bond Network1Anion Size‐Dependent Conformational Folding of Guanidinopropionate: Enabling Tunable Birefringence and Balanced Second‐Harmonic Generation Performance3Strong Optical Nonlinearity in Polar Hypophosphites via Chiral Cation Assembly1Regulating B‐O Arrangement Boosts Anisotropy in a Simple Rubidium Borate, Leading to a High‐Performance UV NLO Crystal0(CN 4 H 7 )(NH 2 SO 3 ): A Solar‐Blind Ultraviolet Nonlinear Optical Crystal With Short UV Cutoff Edge and Full‐Wavelength Phase‐Matching0Investigation of Conductivity Relaxation and Nonlinear Optical Activity in Pure and Cu 2+ Doped Lithium Sulphate Monohydrate Crystals0Enhancing Birefringence of Sulphates by Polarity Modification in Planar Cations0Record Second-Harmonic Generation and Exceptional Optical Anisotropy in High-Symmetry 1D Polar Perovskites1Rational Design of a Strong Nonlinear Optical Crystal With Ultrawide Bandgap via Fine‐Tuning of Channel Structures0A Hydrogen-Bonded Molecular Crystal with Strong Optical Anisotropy and Large Second-Harmonic Generation Response0

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  1. Design of alkali lead oxybromides with a strong second-harmonic generation response and large birefringence

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  2. Halide-driven polarity tuning and optimized SHG-bandgap balance in (C 4 H 11 N 2 )ZnX 3 (X = Cl, Br, I)

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  3. Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material

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    Zhiyong Bai, Jihyun Lee, Chun‐Li Hu, Guohong Zou, Kang Min Ok

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

    Chemical Science · 2024-01-01

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  5. New ultraviolet transparent rare-earth borates with enhanced birefringence induced by cation chemical substitution

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  6. Salt-inclusion chalcogenides with d-orbital components: unveiling remarkable nonlinear optical properties and dual-band photoluminescence

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  7. Wide band gap selenide infrared nonlinear optical materials A II Mg 6 Ga 6 Se 16 with strong SHG responses and high laser-induced damage thresholds

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  8. The Birefringence Modulation in Short‐Wave Ultraviolet Sulfates with Functional π‐Conjugated Cations and Polymerized Heteroleptic Tetrahedral Anions

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  9. Hg4(Te2O5)(SO4): A Giant Birefringent Sulfate Crystal Triggered by a Highly Selective Cation

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  10. Rational Combination of π‐Conjugated and Non‐π‐Conjugated Groups Achieving Strong Nonlinear Optical Response, Large Optical Anisotropy, and UV Light‐Switchable Fluorescence

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  11. Na3K6(CO3)3(NO3)2X·6H2O (X = NO3, Cl, Br): Exploring High-Performance UV Birefringent Crystals Induced by Coplanar π-Conjugated CO3 and NO3 Groups

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  12. A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability

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  13. Cs2Pb(CO3)2: a novel mixed-metal carbonate with rare Pb-C-O one-dimensional chain

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  14. Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering

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  15. Sulfate Derivatives with Heteroleptic Tetrahedra: New Deep‐Ultraviolet Birefringent Materials in which Weak Interactions Modulate Functional Module Ordering

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  16. Na2B6SO13 with unprecedented [B6SO13]∞ double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B3O7] units

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  17. Tetrahedra Modification of Phosphates for Optical Anisotropy Enhancement

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  18. Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family

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

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  20. The design of a non-centrosymmetric structure in sulfates by cation-induced symmetry breaking

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  21. 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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  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. The New Paradigm of Ligand Substitution-Driven Enhancement of Anisotropy from SO4 Units in Short-Wavelength Region

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

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  25. (C 6 H 5 N 2 )HgCl 3 : Discovery of a Polar Hg‐Based Hybrid Halide as Preeminent Nonlinear Optical and Birefringent Material Activated by π‐Conjugated Organic Cation Substitution

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  26. (CN 4 H 7 ) 2 SO 4 ·H 2 O: high-performance metal-free ultraviolet birefringent crystal with KBBF-like configuration

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  28. An excellent ultraviolet nonlinear optical crystal derived from the polar methylphosphonate unit

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  29. Deep-ultraviolet sulfamate halides with halogen-centered secondary building units for enhanced optical anisotropy

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  30. Designing a novel perovskite-type KCd(NH 2 SO 3 ) 3 with deep-ultraviolet transparency and strong second-harmonic generation response

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  31. Different p-block elements induce C 3 [111] octahedral distortion in titanium to generate an intense nonlinear effect

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

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  33. K 2 SO 4 (NH 3 SO 3 ) 2 and Cs 2 SO 4 (NH 3 SO 3 ) 3 : two deep-UV transparent sulfamate-sulfates with moderate birefringence

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  34. Non-centrosymmetric structures designed rationally via a “dimensionality addition” strategy toward the promising nonlinear optical family [A–X][In–Se] (A = K/Ba and Rb/Ba; X = Cl and Br)

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  39. Reinforced Nonlinear Optical Performances Induced by P‐P Homoatomic Bond in Phosphide SrIn 3 Si 4 P 11

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  40. Reinforced Nonlinear Optical Performances Induced by P‐P Homoatomic Bond in Phosphide SrIn 3 Si 4 P 11

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  43. Polar [ NH ( CH2SO3 )2]2− Dimers Enable the First Promising Iminodimethanesulfonate with Nonlinear Optical Properties and Wide UV Transparency

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  45. A strategy to achieve giant optical anisotropy via integrating linear pseudohalogen and stereochemical active lone pair cation

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  46. La(SO3NH2)2NO3·H2O: synergistic anion engineering of the first rare-earth nitrate sulfamate defying transparency-birefringence-nonlinearity trade-offs in ultraviolet nonlinear optics

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  47. Direct Deep‐UV Second‐Harmonic Generation in Disordered Χ 2 ‐Modulated Ferroelectric Crystals

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  48. Anionic Group Trimming Strategy: Oriented Fabrication of Sulfonate UV Birefringent Crystals with High Optical Anisotropy

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  49. Breaking the Deep‐UV Transparency/Optical Nonlinearity Trade‐Off: Three‐Parameter Optimization in Oxyfluorides by Tailoring d 0 ‐Metal Incorporation

    Angewandte Chemie International Edition · 2025-09-16

    Xiaotian Zhang, Xingxing Jiang, Hui Gao, Kaining Duanmu, Chao Wu, Zheshuai Lin, Zhipeng Huang, Mark Graeme Humphrey, Chi Zhang

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  50. Breaking the Deep‐UV Transparency/Optical Nonlinearity Trade‐Off: Three‐Parameter Optimization in Oxyfluorides by Tailoring d 0 ‐Metal Incorporation

    Angewandte Chemie · 2025-09-16

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