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RESEARCH PAPER · Journal of the American Chemical Society · 2023

Breaking the Inherent Interarrangement of [B3O6] Clusters for Nonlinear Optics with Orbital Hybridization Enhancement

Haotian Qiu, Fuming Li, Zhi Li, Zhihua Yang, Shilie Pan, Miriding Mutailipu

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Breaking the Inherent Interarrangement of [B3O6] Clusters for Nonlinear Optics with Orbital Hybridization EnhancementOriginalHydroxyl-Driven Enhanced Birefringence in Borophosphates3Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals15Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals70Mg(C 3 O 4 H 2 )(H 2 O) 2 : A New Ultraviolet Nonlinear Optical Material Derived from KBe 2 BO 3 F 2 with High Performance and Excellent Water‐Resistance7Mg(C3O4H2)(H2O)2: A New Ultraviolet Nonlinear Optical Material Derived from KBe2BO3F2 with High Performance and Excellent Water‐Resistance43Advances in Solid-State Nonlinear Optical Materials: From Fundamentals to Applications61Multifunctional Chiral d 10 ‐Metal Coordination Polymers: Tunable Photoluminescence and Efficient Second‐Harmonic Generation with Circular Dichroic Response18Synthesis, crystal and electronic structures, linear and nonlinear optical properties, and photocurrent response of oxyhalides CeHaVIO 4 (Ha = Cl, Br; VI = Mo, W)10Achieving great optical anisotropy with the well-directed alignment of π-conjugated groups due to hydrogen bonds9Nonlinear Optical Phosphide CuInSi2P4: The Inaugural Member of Diamond-Like Family I–III–IV2–V4 Inspired by ZnGeP216“One stone two birds” design of borates featuring edge-sharing [BO 4 ] and different B–O configurations in one structure utilizing covalent tetrahedra8[(C 5 H 6 N 2 ) 2 H](Sb 4 F 13 ): a polyfluoroantimonite with a strong second harmonic generation effect60A bifunctional primitive strategy induces enhancements of large second harmonic generation and wide UV transmittance in rare-earth borates containing [B 5 O 10 ] groups22Customized structures of hydrogen-bonded organic frameworks towards photocatalysis93Discovery of a new bimetallic borate with strong optical anisotropy activated by π-conjugated [B 2 O 5 ] units3Exploration of antimony( iii ) oxyhalides via single-site substitution in quest of large birefringence10Exploring short-wavelength birefringent crystals via triggering cooperative arrangement between different π-conjugated groups8Fully tricoordinated assembly unveils a pioneering nonlinear optical crystal (SbTeO 3 )(NO 3 )25Halide-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 material32Noncentrosymmetric tellurite halides created by a depolymerization strategy: toward strong SHG intensity and wide bandgap16Optimized arrangement of non-π-conjugated PO 3 NH 3 units leads to enhanced ultraviolet optical nonlinearity in NaPO 3 NH 328Pb 6 Ba 3 Si 2 S 8 I 10 : a new thiohalide with a quasi-two-dimensional structure and wide band gap2Simple aliovalent cation substitution to induce strong optical anisotropy enhancement in a rare thioantimonate( v ) family3LiASi2O5 (A = K, Rb): Effects of cations on crystal structure and optical properties1Synthesis, structures and properties of two new nitrate optical materials: Rb3ZnNO3Cl4 and Rb5Na(NO3)4Cl24KNa 2 Lu(BO 3 ) 2 : A Rare-Earth Borate Crystal Characterized by an Enhanced Birefringence and Wide Ultraviolet Transparency Range19Synthesis, crystal structure and luminescent properties of a quinary borate-phosphate compound CsNa2Dy2(BO3)(PO4)21Rational Design of Novel Promising Infrared Nonlinear Optical Materials: Structural Chemistry and Balanced Performances156Metal Methanesulfonates with Mixed Anionic Groups with Large Band Gaps and Enhanced Birefringence50Dual-Anion Strategy Induces Dual Enhancement Toward Ultrashort Phase-Matching Wavelength in Deep-UV Transparent d0 Transition Metal Oxyfluorides21Theoretical Investigation of Structural, Electronic and Optical Properties of Cs3MoO4(HCO3) with NLO Active Functional Units2Enhanced Birefringence in Phosphates via “Two Steps in One”: d0 Transition Metal Regulation and Fluorination Synergistic Strategy7Tunable Optical Anisotropy in Rare‐Earth Borates with Flexible [BO3] Clusters7PbBeB2O5: A High-Performance Ultraviolet Nonlinear-Optical Crystal with Functional [BeB2O8]8– Group3Two polyoxovanadoborates with over 100 nuclei assembled from a {V14Co12B72} cluster13Optical nonlinear refractive index study by Z-scan technique of GOQDS dispersed in an aqueous solution2Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials24Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials1Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction11Enhanced UV Nonlinear Optical Properties in Layered Germanous Phosphites through Functional Group Sequential Construction116Old tree blossoms anew: Research progress on the structures and optical properties of ultraviolet selenites56Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units66[B3O3F4(OH)]2–: A Versatile Hydroxyfluorooxoborate Heteroanion Producing Compounds with Highly Tunable Optical Anisotropy19An innovative approach to design readily synthesizable polymers for all-polymer solar cells3A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability14(C3N2H5)B3O3F2(OH)2: Realizing Large Birefringence via a Synergistic Effect between Anion F/OH‐Ratio Optimization and Cation Activation25Na2B6SO13 with unprecedented [B6SO13]∞ double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B3O7] units19A Robust Phosphonate‐Based Hydrogen‐Bonded Organic Framework Birefringent Crystal39Hydrogen bond-derived symmetry transformation in hydroxyborates: Converting the nonlinearity from null to active7Exploiting 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 ] Groups4Constructing 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 Thiocyanates32Carbonatoperoxovanadates with Strong Second‐Harmonic Generation: Insights from First‐Principles Calculations on Anisotropic Structures and Optical Parameters0Chiral Metal Self‐Assemblies of Zirconium‐Tetrahedra and Their Second Harmonic Generation Activity6Chiral Metal Self‐Assemblies of Zirconium‐Tetrahedra and Their Second Harmonic Generation Activity0Two α‐SiO 2 ‐Related Deep‐Ultraviolet Phase‐Matchable Optical Nonlinear Beryllium Silicate Crystals Na 2 BeSiO 4 and Li 2 BeSiO 4 with Enhanced SHG Effect10From β-KB3O4F2 to α-KB3O4F2: Phase Transition-Directed Great Changes in Structure and Optical Anisotropy4Achieving strong optical nonlinearity and wide bandgap of pnictides via ionic motif–driven directed assembly of covalent groups39Hg4InS2Cl5: Achieving Giant Optical Anisotropy by Introducing Well‐Aligned Linear [Hg2S2] Units14Rational design of a series of non-centrosymmetric antiperovskite and double antiperovskite borate fluorides13La 3 (Ga 3 S 3 O 3 )(Si 2 O 7 ): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups6“Three functions in one”: multifunctional rare-earth cyamelurates with magnetism, luminescence, and giant optical nonlinearity6Ba 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 structure4Broadband laser protection and enhanced nonlinear optical response of samarium-metal–organic framework-based white/black carbon hybrids4Bulk crystal growth and optical properties of a novel organic–inorganic hybrid nonlinear optical thiocyanate: [Mn(CH 3 CONH 2 ) 2 ] [Hg(SCN) 4 ]10Cation tuning in anionic framework hydroborates: tailored deep-ultraviolet optical crystals with large birefringence1Designing rare earth borates as UV nonlinear optical crystals exhibiting strong second-harmonic generation responses15Enhancing the performance of polyoxometalate-based memristors in harsh environments based on hydrogen bonding and cooperative π-conjugation interactions10Four noncentrosymmetric molybdophosphates discovered by a chemical substitution strategy4Low thermal expansion and high lattice thermal conductivity in β-sodalite Co 4 B 6 O 13 : enhancing the local rigidity of the cationic tetrahedral cluster4Structure modulation by cationic modification of sulfates using planar CS(NH 2 ) 25Three New Chiral Schiff Base Crystals Possess an Efficient Phase-Matching Second Harmonic Generation: Experimental and Theoretical Investigations0Pb9Si8O22Cl6 and Pb3.07Ca1.93Si3O11: Two Ultraviolet Nonlinear Optical Materials Exhibit a Moderate Second Harmonic Generation Response1Soft–Rigid Structural Integration in KMgBO3: A Pathway to Negative Thermo-optic Coefficient via Positive Thermal Expansion and Negative Temperature-Dependent Optical Absorption Edge2Three Polyoxovanadoborates Constructed from “Sandwich”-Type {V10B24}, {V10B28}, and {V12B32} Clusters5Design, synthesis and characterization of two new nonlinear optical crystals based on chalcone containing furan ring: FTB and FTC5A 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 Strategy5Two nonlinear optically responsive crown ether inclusion compounds based on a sulfonimide anion assembly2From 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 Crystal28Exploring crystallinity, free volume and optical energy band gap effects on nonlinear optical properties of P(MMA-co-MA)/NiO and P(MMA-co-MA)/CuO polymer nanocomposites1Second-Harmonic Generation in Organic–Inorganic Hybrid Cadmium Thiocyanates Containing Terminal Amino Acids22A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design40A Promising Deep Ultraviolet Nonlinear Optical Crystal Activated by the Ordered Structure Design3Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence54Giant 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 Blocks32Breaking the Natural Tendency of Deep‐UV Polyborate Anion Clusters to Inducing Strong Optical Anisotropy13La2Zn3(SeO3)6: A UV Selenite Crystal with Second-Harmonic Generation and Large Birefringence13A new strategy of getting accurate refractive index dispersion curves using first-principles sum-over-states method jointed by density functional perturbation theory2Perfluorobiphenyl-Based Fluorescent Dyes and NLO-Phoric Systems: Unveiling Charge Transfer Dynamics and Nonlinear Optical Properties for Advanced Electro-Optic Applications3Designing an all-organic wide bandgap ultraviolet nonlinear optical crystal3Exceptional Second Harmonic Generation in Ultraviolet Nonlinear Optical Oxyfluoroniobate Crystals via Structural Fingerprint Optimization of Polar Chains22Exceptional Second Harmonic Generation in Ultraviolet Nonlinear Optical Oxyfluoroniobate Crystals via Structural Fingerprint Optimization of Polar Chains8Pd@PdBO x heterostructure with strong electronic interaction to promote C─H bond activation for glycerol oxidation reaction21NH4B5O7(OH)2 and CsRbB10O14(OH)4·H2O: Two Hydroxyborates Feature Significant Optical Anisotropy and Contain 1∞[B5O7(OH)2] Chains1Bromine for iodine: Unlocking short-wavelength UV phase matching in nonlinear optical metal halides6A3ZnNO3X4 (A = Rb, NH4, X = Cl, I): Regulating Cations and Halides Yields Birefringent Crystals with Significantly Enhanced Optical Anisotropy5Promising UV/DUV nonlinear optical materials with X-membered (X = multiples of 6) rings in anhydrous inorganic borates20Rational Design of a Deep-Ultraviolet Nonlinear Optical Crystal25Unveiling the NLO Potential of Transition Metalides: Stability, Electronic Structure, and Frequency‐Dependent NLO Properties1Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation3[HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap12Growth, structure and optical properties of PbBi3PO8 crystals0Low Thermal Expansion in Niobate Borate NbBO4 Enabled by Compensated Grüneisen Parameters of NbO8 Polyhedra1Unlocking Advanced UV NLO Crystals in Rare‐Earth Metal Borate Fluorides via [B 3 O 6 ]‐Mediated Structural Modulation18Effect of Multiple Hydrogen Bonding on the π-Conjugated Groups and Optical Properties in Molecular Crystals5Quantum chemical investigation of Z-shaped Diradicaloid heptazethrene derivatives towards linear and nonlinear optical polarizability2Stepwise Substitution Strategy for Beryllium-Based Selenites with Enhanced SHG Response, Moderate Birefringence, and Short UV Cutoff Edges6Unveiling the hidden potential of gallic acid: A multifaceted study of its physical and optical properties3Theoretical Insights into Alanine Maleate and Alanine Fumarate: NLO‐Active Single Crystals Stabilized by N─H Intramolecular Hydrogen Bonding0Integrating 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 Conversion2Three new chiral schiff base crystals with naphthyl groups possess second harmonic generation: Experimental and theoretical investigations1π–Conjugated B3O6 units drive directional O2 adsorption and charges separation for efficient piezoelectric H2O2 production1A multi-scale birefringence modulation strategy in DUV/UV crystals induced by organic cations1Chiral calcium thiocyanate hybrids: amino acid-enabled structural diversity and second-harmonic generation0CsB(OH) 4 (H 2 O) 2 and Na(NH 4 ) 2 B 10 O 16 OH(H 2 O): a hydroxylation modification strategy regulates the borate structures and optical properties0Synergism of [C 2 N 4 H 7 S] cations and anionic modulators: tailoring second-order nonlinear optics and birefringence in organic–inorganic crystals6Synthesis and characterization of hydrated alkali metal calcium nitrates ACa(NO 3 ) 3 ·2H 2 O (A = NH 4 , Rb, Cs) as short ultraviolet birefringent materials0Enhanced nonlinear optical characteristics of triarylmethane dye in various solvents using Z-scan and DFT method4Dimensionality Engineering of Fluorozirconium Phosphates for Deep-UV-Transparent Crystals with Enhanced Second-Harmonic Generation and Birefringence10(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 Conflicts13(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 Conflicts1Persistent 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 Halide0Anion Size‐Dependent Conformational Folding of Guanidinopropionate: Enabling Tunable Birefringence and Balanced Second‐Harmonic Generation Performance3Anion Size‐Dependent Conformational Folding of Guanidinopropionate: Enabling Tunable Birefringence and Balanced Second‐Harmonic Generation Performance0Electronegativity Adaption Approach for Solar‐Blind UV Birefringent Crystals With Ultrawide Bandgaps2Electronegativity Adaption Approach for Solar‐Blind UV Birefringent Crystals With Ultrawide Bandgaps1The Enhancement of Phase‐Matching Capability by Recombining π‐Conjugated Group in Nonlinear Optical Sulfates1Charge Compensation via Heterovalent Cation Disorder for Birefringence Modulation to Design UV Nonlinear Optical Crystal0K 3 Yb 2 (BO 3 ) 3 and Rb 3 Yb 2 (BO 3 ) 3 : Two Rare-Earth Borate Ultraviolet Nonlinear Optical Crystals1Design of deep-ultraviolet nonlinear optical BePNO2 guided by non-π-conjugated NLO-active unit0Covalent Interlayer Engineering Enables Ideal Birefringence and Strong SHG in Beryllium‐Free Deep‐UV NLO Borates2Exploring third-order NLO response of Cu-doped Ag 2 S/PMMA thin films under CW laser excitation0Intensifying Localized Polarization Piezoelectric Field via Tip Effect on Carbon Quantum Dots Modified Ca 2 B 3 O 6 Cl for H 2 O 2 Production in Pure Water0Tailoring a Solar‐Blind Ultraviolet Ferroelectric for Nonlinear Optics Through a Local Symmetry‐Breaking Cascaded Strategy1Laporte Selection Rule Induced the Suppression of d ‐ d Transitions and Vacancies Enhanced the Second Harmonic Generation in I 4¯‐MnGa 2 S 40

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