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RESEARCH PAPER · Angewandte Chemie International Edition · 2024

Assembly of π‐Conjugated [B3O6] Units by Mer‐Isomer [YO3F3] Octahedra to Design a UV Nonlinear Optical Material, Cs2YB3O6F2

Hongping Wu, Zhijun Wei, Zhanggui Hu, Jiyang Wang, Yicheng Wu, Hongwei Yu

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Assembly of π‐Conjugated [B3O6] Units by Mer‐Isomer [YO3F3] Octahedra to Design a UV Nonlinear Optical Material, Cs2YB3O6F2OriginalEquivalent cation-tuning to realize a new Ce( iv ) fluoride with excellent comprehensive nonlinear optical performances12Fully tricoordinated assembly unveils a pioneering nonlinear optical crystal (SbTeO 3 )(NO 3 )25Large second harmonic generation and birefringence from extended octupolar π-conjugated structures35Noncentrosymmetric tellurite halides created by a depolymerization strategy: toward strong SHG intensity and wide bandgap16Strategically designed metal-free deep-ultraviolet birefringent crystals with superior optical properties18Exploiting Deep‐Ultraviolet Nonlinear Optical Material Rb 2 ScB 3 O 6 F 2 Originated from Congruously Oriented [B 3 O 6 ] Groups61Exploiting Deep‐Ultraviolet Nonlinear Optical Material Rb 2 ScB 3 O 6 F 2 Originated from Congruously Oriented [B 3 O 6 ] Groups4[C3H7N6]3[B3O5(OH)2] and [C3H8N6]4[B12O19(OH)6]: Two Melamine Borates with Large Birefringence13Achieving Phase‐Matching in Nonlinear Optical Materials CsM 2 In 2 S 6 (M = Cd/In, Hg/In) by the Incorporation of Unprecedented Trigonal Planar MS 3 Motifs6Two l -Proline Cadmium Thiocyanates with Moderate Second-Harmonic-Generation Responses and Large Birefringences13Computer‐Aided Development of New Nonlinear Optical Materials38Computer‐Aided Development of New Nonlinear Optical Materials14K 15 La 7 (BO 3 ) 12 : A KBBF-Like Nonlinear-Optical Material with a Short Cutoff Edge and a Strong Second-Harmonic-Generation Response10Li3[AlP2O7F(OH)](H2O)0.5 and A[Al2(PO4)2F(H2O)](A = K, Rb): Counter Cation Templates Derived Three Polar Alkaline Metal Fluoroaluminophosphates6Rational design of a series of non-centrosymmetric antiperovskite and double antiperovskite borate fluorides13Rare‐Earth Substitution Induced Symmetry Breaking for The First Sc‐Based Nonlinear Optical Chalcogenide with High‐Performance30“Three functions in one”: multifunctional rare-earth cyamelurates with magnetism, luminescence, and giant optical nonlinearity6Achieving balanced UV SHG responses, optical band gaps and birefringence in rare earth compounds Ln(IO 3 )(SO 4 )·3H 2 O (Ln = Y, Gd, Er, Ho, Dy, Eu)4Ba 3 Al 2 B 12 O 24 : a beryllium-free member of the Sr 2 Be 2 B 2 O 7 family with a 2 ∞ [B 12 Al 2 O 28 ] double-layered structure4Enhancing the performance of polyoxometalate-based memristors in harsh environments based on hydrogen bonding and cooperative π-conjugation interactions10KNa 2 Y 2 B 2 O 6 F 3 : a beryllium free deep-UV nonlinear optical crystal with well-balanced properties2Non-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)13Pb 2 B 10 O 16 (OH) 2 ·B(OH) 3 ·H 2 O: significantly enhanced second harmonic generation via substituting metal cations in isostructural compounds with Pb 2+2Realizing large birefringence via S-substitution and anisotropic arrangement optimization4Significant enhancement in the birefringence of metal phosphite halides via the introduction of π-conjugated cations17Synthesising a series of promising ultraviolet nonlinear optical materials with the aid of the flexibility of isolated [B 5 O 10 ] groups3Unprecedented v-shaped [SeO2E] units stabilized in KM[Se2O5]2[SeO2] (M= Al and Ga) constructed by nanoconfinement strategy6A 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 Strategy5From (C6H5N2)2CdCl4 to (C6H5N2)2ZnCl4, Chirality Transformation to Realize a Nonlinear Optical Organic–Inorganic Hybrid Halide with Balanced Comprehensive Performance19Crystal Structures, Phase Transition, and Optical Properties of Two Rare Earth Borate Fluorides: α- and β-BaGdBO3F26A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design40A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design3LiAgCe2F10(H2O)2: Focusing on the Cation Size Effect to Reasonably Design a Nonlinear Optical Hydrated Cerium(IV) Fluoride10Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence54From AgHgI(SO4) to AgHg3I3.2Cl1.8(SO4): Symmetry Breaking of the Belousovite‐Type Topology by Mixed Halides to Achieve Strong Nonlinear Optical Effect14Ca 7 (TeO 3 ) 6 (MoO 4 ): A Promising Mid-Infrared Nonlinear Optical Crystal Activated via a Module-Oriented Dimensionality Reduction Strategy34[CON3H6BF4]: An Efficient Metal‐Free Borate with Optimized Birefringence Achieved by Structural Design Strategy15Controllable Synthesis of a Strong Ultraviolet Nonlinear Optical Crystal by Tailoring the Lead Oxychloride Polyhedron3KYSiSe 4 : A Rare-Earth Selenide Infrared Nonlinear Optical Crystal with Wide Infrared Transparency and Well-Balanced E g and SHG Response9Proton Conduction Study in 2D Layered Polyoxovanadoborate Frameworks Based on Two Types of Open-Type {V 12 B 32 } Clusters7Reversal Enhancement of Birefringence by Stereochemically Active Lone Pairs in Sn(II)-Based Mixed Halides0Cation-modulated aligned arrangement of [B3O7] units in an unprecedented 2∞[B3O5] layer with remarkable birefringence10Designing Hybrid Sb-Based Nonlinear Optical Crystals with Large Birefringence by Combining the Lone Pair and π-Conjugated Genes10Giant Birefringence and Strong Third-Order Nonlinear Optical Response in a Hybrid Crystal Templated by a Push–Pull π-Conjugated System6Modulation of Crystal Structure and Birefringence: Cation Size Effect in Alkali Metal Fluoroaluminoborates4(CN4H7)H2C3N3S3: Trithiocyanurate Exhibiting Giant Optical Anisotropy via Weak Interaction-Mediated Functional Module Alignment3Rational Design of a Deep-Ultraviolet Nonlinear Optical Crystal25K5NaZr4F22(H2O)2: A Hydrated Zirconium Fluoride with a Second-Harmonic Generation Effect and a Short Ultraviolet Cutoff Edge Induced by Cosubstitution with Heterovalent Cations6Giant Birefringence Induced by Intermolecular Aromatic Interactions in Hydrogen‐Bonded Organic Frameworks37KF·[SO 2 (NH 2 ) 2 ]: the First Deep‐Ultraviolet Transparent Sulfonamide Fluoride Nonlinear Optical Crystal with Novel Cairo Pentagonal Structure13KF·[SO 2 (NH 2 ) 2 ]: the First Deep‐Ultraviolet Transparent Sulfonamide Fluoride Nonlinear Optical Crystal with Novel Cairo Pentagonal Structure5Breaking 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 Incorporation4Organic 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 Fluorides33In Situ Tandem Synthesis of Charged Boron‐Oxo Clusters into Highly Ordered Architectures3Unlocking Advanced UV NLO Crystals in Rare‐Earth Metal Borate Fluorides via [B 3 O 6 ]‐Mediated Structural Modulation18Hydrogen-bond-driven noncentrosymmetric structure formation in π-conjugated (C3H7N6)(IO3): achieving both strong SHG response and wide bandgap5Effect of Multiple Hydrogen Bonding on the π-Conjugated Groups and Optical Properties in Molecular Crystals5Asymmetry-driven organic–inorganic hybrid strategy for constructing structures with exceptional organofunctionalized B–O units2Chiral-Unit-Driven Short-Wave Ultraviolet Nonlinear Optical Acetates with Balanced Overall Optical Properties3Synthesis, Anion Disordering and Electronic Structure of Rb2KWO3F3 Elpasolite0From 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 materials3REV 3 (BO 3 ) 4 (RE = La–Nd): a series of rare earth vanadoborates exhibit large birefringence induced by distorted V III O 6 groups2Second-harmonic generation responses in low-dimensional metal bromides functionalized with l -arginine1Series of phosphate nonlinear optical materials containing active metal ions with short cut-off edges0Two scandium borate UV NLO crystals designed through chemical element substitution1The modulation of structural polarity facilitating the gradient enhancement of second harmonic generation effects in hybrid metal halides5Constructing Deep‐Ultraviolet Nonlinear Optical Crystals via Synergistic Combination of Fluorinated Polyhedra and Polymerized BO 3 Units15Strategic Oxygen‐Substitution in Perfluorinated Ce(IV) Coordination Frameworks Triggers Dual‐Wavelength Nonlinear Optical Materials With Exceptional Performances32Rational design of a quasi-0D tungsten tellurite nonlinear optical crystal with exceptionally balanced properties1An Ultraviolet Transparent Nonlinear Optical Crystal Assembled from a Polarizable Tetrahedral Unit1CdY 2 Si 2 S 8 : A Wide Bandgap IR NLO Material with d 10 Metal-Induced Structure Transformation from CS to NCS1Dimensionality Engineering of Fluorozirconium Phosphates for Deep-UV-Transparent Crystals with Enhanced Second-Harmonic Generation and Birefringence10Boosting Ultraviolet Phase‐Matching Performance of B 3 O 7 ‐Based Systems via Synergistic Fluorination and Organic Modification Strategy1Anion Size‐Dependent Conformational Folding of Guanidinopropionate: Enabling Tunable Birefringence and Balanced Second‐Harmonic Generation Performance3Charge Compensation via Heterovalent Cation Disorder for Birefringence Modulation to Design UV Nonlinear Optical Crystal0Breaking Inversion Symmetry via Vanadium Coordination Engineering in Bismuth Vanadium Selenites0A Lithium Calcium Borate Nonlinear Optical Crystal with Deep-UV Cutoff Edge and Moderate Second-Harmonic Generation Response1Regulating B‐O Arrangement Boosts Anisotropy in a Simple Rubidium Borate, Leading to a High‐Performance UV NLO Crystal0Achieving Excellent Nonlinear Optics in α ‑Ba 2 Ge 4 S 10 via Flux‑Induced Symmetry Breaking1K 3 Yb 2 (BO 3 ) 3 and Rb 3 Yb 2 (BO 3 ) 3 : Two Rare-Earth Borate Ultraviolet Nonlinear Optical Crystals1Covalent Interlayer Engineering Enables Ideal Birefringence and Strong SHG in Beryllium‐Free Deep‐UV NLO Borates2When Octahedra Learn to Be Prisms: Unlocking a Record Deep‑UV NLO Crystal0Parallel arrangement of functional building blocks: toward performance synergy in oxalate borate ultraviolet nonlinear optical crystals0Fluorine‐Driven Chemical Scissor Effect in Scandium Borates: Structural Evolution with Retained Optically Active Motifs0Designing Novel Solar‐Blind Ultraviolet Nonlinear Optical Crystals Based on Local Proton Distribution Complementary Effect0Rational Design of a Strong Nonlinear Optical Crystal With Ultrawide Bandgap via Fine‐Tuning of Channel Structures0Decoupling Contributions of Distinct Strategies for Enhancing Polarizability Anisotropy in Crystals Containing π-Conjugated Groups0The Parallel Coplanar Alignment of Planar Non‐π‐Conjugated [Pb 3 Br 3 ] Rings for a Stable Ultraviolet Nonlinear Optical Crystal0Two Rare Earth-Based Sulfates with Enhanced Birefringence and Broad Optical Transparency Window0Potential Deep Ultraviolet Phosphate With Y‐Based: 1 [(PO 3 ) 4 ] ∞ Chains AYP 4 O 12 (A = K, NH 4 ) and the First [P 3 O 10 ] Anionic Framework KLiYP 3 O 100Three Rare‐Earth Metal Borates Synthesized via a Cation Substitution Strategy as Potential Zero‐Order Waveplate Materials0Influence of the Cation Size on Symmetry Breaking and Optical Performances in Ae2Mg3(BO3)2F4 (Ae = Sr, Ba)0Cation‐Regulated [CH 3 BO 2 F]‐Derived Borates: Synergistic Fluorination and Organic Functionalization for High‐Birefringence UV NLO Materials0

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  48. Rational Design of a Deep-Ultraviolet Nonlinear Optical Crystal

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