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RESEARCH PAPER · Angewandte Chemie International Edition · 2021

A General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**

Lin Xiong, Li‐Ming Wu, Ling Chen

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A General Principle for DUV NLO Materials: π‐Conjugated Confinement Enlarges Band Gap**OriginalA novel 2-(aminomethyl)pyridineH 2 PO 4 crystal with second-order nonlinear optical performance8BaSc 2 (HPO 3 ) 4 (H 2 O) 2 : a new nonlinear optical phosphite exhibiting a 3D {[Sc 2 (HPO 3 ) 4 ] 2− } ∞ anionic framework and phase-matchable SHG effect32KLi 2 CO 3 F: a beryllium-free KBBF-type deep-UV carbonate with an enhanced interlayer interaction and large birefringence20KPb 3 ( o -C 5 H 4 NCOO) 2 Cl 5 : a brand-new stable lead chloride with good comprehensive nonlinear optical performance5Performance of optical materials with the derivative of planar π-conjugated groups: Recent advances and future prospects37PNO: a promising deep-UV nonlinear optical material with the largest second harmonic generation effect17Driving Nonlinear Optical Activity with Dipolar 2-Aminopyrimidinium Cations in (C4H6N3)+(H2PO3)−115The dependence of crystal structure and ultraviolet nonlinear optical property of KBe2BO3F2 by density functional theory and π-conjugate confinement2Two Indium Iodate–Nitrates with Large Birefringence Induced by Hybrid Anionic Functional Groups and Their Favorable Arrangements22Revealing Electron–Phonon Coupling Dependence on the π-Conjugated Groups in Rare-Earth Borates6Non‐Linear Optical Properties of the (RE)3CuGeS7 Family of Compounds16Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species6Promising Deep‐Ultraviolet Birefringent Materials via Rational Design and Assembly of Planar π‐Conjugated [B(OH)3] and [B3O3(OH)3] Functional Species83Enhancement of Birefringence in Borophosphate Pushing Phase-Matching into the Short-Wavelength Region150Self-Assembled Nonlinear Optical Crystals Based on an Asymmetric Fluorenone Derivative17Design of New Borates with Deep Ultraviolet Transparency Inspired by the Flexibility of Unusual Triple-Layered Frameworks3Design of a new ultraviolet nonlinear optical material KNO3SO3NH3 exhibiting an unexpected strong second harmonic generation response44Chalcohalides: A Rising Type of Second‐Order Nonlinear Optical Materials28Structural Optimization and Property Tunability by Halogen Regulation in Zero-Dimensional Zinc Halide Organic–Inorganic Hybrid Materials36Chemical Bonding Effects and Physical Properties of Noncentrosymmetric Hexagonal Fluorocarbonates ABCO3F (A: K, Rb, Cs; B: Mg, Ca, Sr, Zn, Cd)10Achieving effective balance between bandgap and birefringence by confining π-conjugation in an optically anisotropic crystal39A High‐Performance Nonlinear Optical Crystal with a Building Block Containing Expanded π‐Delocalization95A High‐Performance Nonlinear Optical Crystal with a Building Block Containing Expanded π‐Delocalization5LiRE(SO 4 ) 2 (RE = Y, Gd, Eu): noncentrosymmetric chiral rare-earth sulfates with very large band gaps21High-Tc Quadratic Nonlinear Optical and Dielectric Switchings in Fe-Based Plastic Crystalline Ferroelectric20Rb 3 B 5 O 8 F 2 and K 0.6 Rb 2.4 B 5 O 8 F 2 : two new deep-ultraviolet transparent nonlinear optical fluorooxoborates designed by cation regulation13Rb 3 B 11 P 2 O 23 : Materials Design of a New Chemically Benign Deep-Ultraviolet Nonlinear Optical Material58Aluminoborates as Nonlinear Optical Materials79Aluminoborates as Nonlinear Optical Materials142-Chloroethylamine·trifluoromethanesulfonate combined with 18-crown-6: a ferroelectric with excellent dielectric switching properties10A Cation-Driven Approach toward Deep-Ultraviolet Nonlinear Optical Materials17A UV solar-blind nonlinear optical crystal with confined π-conjugated groups13Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181C 3 N 6 H 7 SO 3 NH 2 : non-π-conjugated tetrahedra decoupling π-conjugated groups achieving large optical anisotropy and wide band gap29Co-substitution design: a new glaserite-type rare-earth phosphate K 2 RbSc(PO 4 ) 2 with high structural tolerance6KRb 2 (NO 3 ) 2 Cl: a new birefringent crystal exhibiting a perovskite-related framework and a short cutoff edge6Linear optical afterglow and nonlinear optical harmonic generation from chiral tin( iv ) halides: the role of lattice distortions37Na 7 (SeO 4 ) 3 (IO 3 ) and K 2 (SeO 4 )[IO 2 (OH)]: two new iodate-selenates with short-wave UV cutoff edge and large birefringence8Self-assembled organic nonlinear optical crystals based on pyridine derived fluorenone20Solvent-free synthesis of magnesium phosphite-oxalates that show second-harmonic generation responses5Atomic Structural Origin of Fictive Temperature Revealed by AZnP3O9 (A=K, Rb) Glasses3Atomic Structural Origin of Fictive Temperature Revealed by AZnP3O9 (A=K, Rb) Glasses2Self-assembly, physico-chemical characterization, biological, virtual screening, and computational approach of novel 2-amino pyridine derivatives13Recent advances of inorganic phosphates with UV/DUV cutoff edge and large second harmonic response7K2(H2O)WO3F2: A new nonlinear optical material with remarkable second-harmonic generation response and enhanced laser damage threshold9Recent advances in non-π-conjugated nonlinear optical sulfates with deep-UV absorption edge53A Second‐Order Nonlinear Optical Material Consisting of Two π‐Conjugated Groups10Structural Motif Cosubstitution Strategy for Designing Fluoroaluminoborate with the Sr2Be2B2O7-Type Double-Layered Structure14Two Mixed-Alkali-Metal Selenates as Short-Wave Ultraviolet Nonlinear-Optical Materials10CaB2O2F4: A Novel [BOF2]∞-Based Structural Template with a Strong Second Harmonic Generation Response and Large Band Gap2Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 422High-Symmetry Structural Phase Transition Triggers a Triple Switch Based on Dielectric, Nonlinear Optics, and Photoluminescence12Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence79Design of the Ionic Organic Nonlinear Optical Material NH 4 [LiC 3 H(CH 3 )O 4 ] with Ultrawide Band Gap and Moderate Birefringence9Host–Guest Symmetry and Charge Matching in Glycine-Templated Metal Sulfate–Oxalates Obtained by a Solvent-Free Method9External electric field driven conformation of the wing-shaped nanographene to close: enhancing and tuning nonlinear optical properties1From Monofluorophosphates A2PO3F to Difluorophosphates APO2F2 (A = alkali metal): Design of a Potential Deep-Ultraviolet Nonlinear Optical Materials System with a Shortened Phase-Matching Wavelength41The Strategy to Improve the Phase Matching Ability in Tetrahedron‐Based Deep‐Ultraviolet Nonlinear Optical Crystals21Beyond π–π Stacking: Understanding Inversion Symmetry Breaking in Crystalline Racemates26Introduction of the [B–O/F] Units Enhances the Band Gap and Birefringence from Na6Mg3B10O18F6 to K3NaB10O16F211Nonlinear optical inorganic sulfates: The improvement of the phase matching ability driven by the structural modulation41Designing a Dimension Reduced Hybrid Perovskite with Robust Large Birefringence by Expanding Cationic π‐Delocation40Sr(NH2SO3)(NO3)·H2O: An Ultraviolet Nonlinear Optical Material Exhibiting Strong Second-Harmonic Generation Response and Sufficient Birefringence10Tailored Synthesis of Two Metal Borates KSrM3B2O9 (M = Al and Ga) Exhibiting Wide Ultraviolet Transparency4Breaking the Inherent Interarrangement of [B3O6] Clusters for Nonlinear Optics with Orbital Hybridization Enhancement142New Functional Groups Design toward High Performance Ultraviolet Nonlinear Optical Materials95Na 10 Zn(NO 3 ) 4 (SO 3 S) 4 : a nonlinear optical crystal combining inorganic π-conjugated and non-π-conjugated heteroanion groups8Two van der Waals Layered Antimony(III) Phosphites as UV Optical Materials11Mg(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‐Resistance43Rb 3 MgB 5 O 10 and LiBaAl(BO 3 ) 2 : covalent tetrahedra MO 4 -containing borates with deep-ultraviolet cutoff edges9K 2 RbB 8 PO 16 : A Borophosphate with Moderate Birefringence and Deep-Ultraviolet Transmission10(C 3 N 6 H 7 )BF 4 ·H 2 O and (C 3 N 6 H 7 )SO 3 CH 3 ·H 2 O with large birefringence induced by coplanar π-conjugated [C 3 N 6 H 7 ] + groups33[Sn 3 OF]PO 4 vs. [Sn 3 F 3 ]PO 4 : enhancing birefringence by breaking the R 3 symmetry and realigning lone pairs12A bifunctional primitive strategy induces enhancements of large second harmonic generation and wide UV transmittance in rare-earth borates containing [B 5 O 10 ] groups22A nonlinear optical crystal with deep-ultraviolet transparency and appropriate birefringence achieved using π-conjugated confined [B 3 O 3 F 4 (OH)] 2−14Designing promising ultraviolet (UV) birefringent crystals with different hydrogen-bonded phosphate frameworks18From BaAlBO 3 F 2 to BaAlB 3 O 6 F 2 and BaAl 2 (B 3 O 6 ) 2 F 2 : the enhancement of birefringence and band gap by extending the π-conjugated system combined with [Al–O/F] functional groups13Large optical anisotropy in noncentrosymmetric phosphate with pseudo 2D intercalated layer16Large second harmonic generation and birefringence from extended octupolar π-conjugated structures35Noncentrosymmetric tellurite halides created by a depolymerization strategy: toward strong SHG intensity and wide bandgap16Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70Solvent-free synthesis and optical properties of two open-framework metal oxalates with zeolitic ABW and diamondoid topologies3Synergistic combination of different types of functional motif in Rb(NO 3 )(SO 3 NH 3 ) for realizing excellent ultraviolet optical nonlinearity18Toward the ultraviolet (UV) or deep-UV nonlinear optical crystals: The combination of π-conjugated planar [XY3] and tetrahedral [XY4]80KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]− Tetrahedra15Theoretical Investigation of Structural, Electronic and Optical Properties of Cs3MoO4(HCO3) with NLO Active Functional Units2Pioneering Exploration in the Na–Lu–B–O System: Na3LuB8O15 with Polyborate Structure and Short UV Cutoff Edge1Rational Combination of π‐Conjugated and Non‐π‐Conjugated Groups Achieving Strong Nonlinear Optical Response, Large Optical Anisotropy, and UV Light‐Switchable Fluorescence65A2Pb3[H2N(CH2COO)2]3Cl5 (A = K, Rb): Porous Crystals Constructed on [Pb3Cl5O6] Clusters with Comprehensive Nonlinear Optical Performance3Unleashing the potential of π-conjugated [B2O3(OH)2] to enhance birefringence in DUV crystals9Two Hydroxyfluorooxoborates Achieving Deep‐Ultraviolet Cutoff Edges and Moderate Birefringence by Assembling Multi‐Anionic Groups6A Universal Design Strategy Achieving Large Birefringence and Short Phase‐Matching Capability of Optical Materials via Dissimilating Non‐π‐Conjugated Units6Na3K6(CO3)3(NO3)2X·6H2O (X = NO3, Cl, Br): Exploring High-Performance UV Birefringent Crystals Induced by Coplanar π-Conjugated CO3 and NO3 Groups15(C 8 H 7 N 2 O 2 ) 2 [Bi 2 Br 8 ]·2H 2 O and (C 8 H 7 N 2 O 2 ) 6 [Bi 2 Cl 10 ]Cl 2 ·2H 2 O: Exploring Birefringent Crystals in Hybrid Halide Systems5[B3O3F4(OH)]2–: A Versatile Hydroxyfluorooxoborate Heteroanion Producing Compounds with Highly Tunable Optical Anisotropy19A3Sc(SO4)3 (A = K, Rb, Cs): Three Deep‐Ultraviolet Transparent Alkali‐Scandium Sulfates with Strong Second‐Harmonic Generation Response and High Thermal Stability14Ba2ScBSi2O9: A Mixed-Coordination Borosilicate with a Low B/Si Ratio Exhibiting Enhanced Second Harmonic Generation Response7A Robust Phosphonate‐Based Hydrogen‐Bonded Organic Framework Birefringent Crystal39K0.9Rb2.1B8PO16: Design and Synthesis of a Deep-Ultraviolet Nonlinear Optical Crystal with Balanced Performance Derived from π-Conjugated and Non-π-Conjugated Groups11Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy6A Giant Optically Anisotropic Phosphate Driven by Mixed Valence Mercury Units22From [Ba3S][GeS4] to [Ba3CO3][MS4] (M = Ge, Sn): Enhancing optical anisotropy in IR birefringent crystals via functional group implantation11Elucidating the Photo‐Induced Electronic Structure and Mechanisms of ZnAl‐Layered Double Hydroxide: A DFT Study0Chiral Metal Self‐Assemblies of Zirconium‐Tetrahedra and Their Second Harmonic Generation Activity6Chiral Metal Self‐Assemblies of Zirconium‐Tetrahedra and Their Second Harmonic Generation Activity0Enhanced Coplanarity and Giant Birefringence in Hydroxypyridinium Nitrate via Hydrogen Bonding between Planar Donors and Planar Acceptors15Enhanced Coplanarity and Giant Birefringence in Hydroxypyridinium Nitrate via Hydrogen Bonding between Planar Donors and Planar Acceptors53Amino substitution strategy achieves significant blue shift while preserving high optical anisotropy: A2(H3C3N4S2)2•H2O (A =NH4, K, Rb, Cs)6Achieving 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 Motifs6MgPO2F3: An Ultraviolet Nonlinear Optical System with an Extremely Short Phase-Matching Wavelength Achieved by Introducing Dual-Type Fluorine via Structure Prediction1Functional assembly and modification of nonlinear optical fundamental motifs in phosphates27The New Paradigm of Ligand Substitution-Driven Enhancement of Anisotropy from SO4 Units in Short-Wavelength Region14Rational design of a series of non-centrosymmetric antiperovskite and double antiperovskite borate fluorides13K6NaCaRe2(B5O10)3 (Re = Y, Lu): Two NLO Compounds Exhibiting a Short Absorption Edge in the A7–xA’xAeRe2(B5O10)3 (x = 0, 1) Family4“All-four-in-one”: a novel mercury tellurite–nitrate Hg 3 (TeO 3 )(Te 3 O 7 )(NO 3 ) 2 exhibiting exceptional optical anisotropy29A remarkable solar-blind ultraviolet nonlinear optical crystal with comprehensive performance and enhanced thermal stability4An excellent ultraviolet nonlinear optical crystal derived from the polar methylphosphonate unit8Structural chemistry of antimony( iii ) oxalates with lone pairs: polyhedral distortion [SbO 4 F 2 ], π-conjugation [C 2 O 4 ], and birefringence tuning1层状结构深紫外非线性光学晶体研究进展（特邀）2混合阴离子无水无机硼酸盐深紫外非线性光学晶体的研究进展（特邀）4A HTO‐Type Nonlinear Optical Fluorophosphate with Ultrawide Bandgap16Highly Polarizable Phosphorus‐Centered Tetrahedra and π‐Conjugated Carbon‐Centered Triangular Moieties Inducing Large Anisotropy and Short‐Wavelength Phase‐Matching23Ln(HCOO) 3 (Ln = Y, Gd, Ce, and La) With Triangular Configuration Exhibits Excellent UV Nonlinear Optical Performance12Unveiling the Intrinsic Superior SHG Performance of Ce 4+ Fluoride Masked by Subtle Ce 3+ Impurity and Its Effective Removal13Unveiling the Intrinsic Superior SHG Performance of Ce4+ Fluoride Masked by Subtle Ce3+ Impurity and Its Effective Removal2Prediction of New Functional Fluorooxoborates with Expected Anionic Framework: A Case of CaB3O5F4K3[HCO3]2F: a new deep-UV birefringent crystal exhibiting strong optical anisotropy17Inch‐sized K[NH2(CH2COO)2]: a High‐Performance UV Nonlinear Optical Crystal Enabled by Novel Flexible π‐Conjugated Building Units, [NH2(CH2COO)2]−13Tuning Birefringence in Supramolecular Mg-PDA Frameworks: Modulating Bonding and Layer Connectivity0Breaking the Natural Tendency of Deep‐UV Polyborate Anion Clusters to Inducing Strong Optical Anisotropy13Machine Learning Prediction on Birefringence of Nonlinear Optical Crystals and Polymorphs with Different Birefringence Activities2A Promising Short-Wave UV NLO Crystal with an Optimized KBBF-like Structure and Well-Balanced Properties Achieved via a Chemical Substitution Strategy6The riddle of α-resorcinol revisited—New perspectives on “pocket-like” structure1Reversal Enhancement of Birefringence by Stereochemically Active Lone Pairs in Sn(II)-Based Mixed Halides0The birefringence optimization by hydroxyl in organic nonlinear optical crystals3Modulation of Crystal Structure and Birefringence: Cation Size Effect in Alkali Metal Fluoroaluminoborates4La(SO3NH2)2NO3·H2O: synergistic anion engineering of the first rare-earth nitrate sulfamate defying transparency-birefringence-nonlinearity trade-offs in ultraviolet nonlinear optics8Studies on Three 3D Bimetallic Tellurates: Including a Second-Order NLO Material with d10-Zn2+ and SOJT-Effect Te4+/Mo6+ Cations2Anion-Ordered [B3O5(OH)2] Induced by Crystal Water with Deep Ultraviolet Transparency and Large Birefringence in Boron-Rich Borophosphates4PBEsol-DFT insights into anisotropic compression of diopside: chain kinking versus bond rupture4Regulating the coplanarity of π-conjugated units through hydrogen bonding in FAHC2O4 and FAH2C3N3S3 crystals5Anionic Group Trimming Strategy: Oriented Fabrication of Sulfonate UV Birefringent Crystals with High Optical Anisotropy5Growth, structure and optical properties of PbBi3PO8 crystals0Na6(SO4)2SiF6: A Stable Sulfate Fluosilicate with Wide Deep-Ultraviolet Transparency Window and Strong Second-Harmonic Generation Response4K 2 GdB 3 O 6 F 2 : A Promising Short-Wave UV Birefringent Crystal via Optimized Assembly of π-Conjugated [B 3 O 6 ] Groups8Effect of Multiple Hydrogen Bonding on the π-Conjugated Groups and Optical Properties in Molecular Crystals5Comparison of properties and performance of Eu 2+ -doped Ca 6 BaP 4 O 17 , Ca 4 Sr(PO 4 ) 3 Cl, NaSrPO 4 and Sr 3 Al 2 O 5 Cl 2 thermometric phosphors0Design and nonlinear optical properties of benzotrithiophene-based covalent organic frameworks1Effects of pressure on structural, electronic and optical properties of noncentrosymmetric monoclinic Na3Sr(PO4)(CO3) with discrete [PO4] and [CO3] units0

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  2. BaSc 2 (HPO 3 ) 4 (H 2 O) 2 : a new nonlinear optical phosphite exhibiting a 3D {[Sc 2 (HPO 3 ) 4 ] 2− } ∞ anionic framework and phase-matchable SHG effect

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  41. Atomic Structural Origin of Fictive Temperature Revealed by AZnP3O9 (A=K, Rb) Glasses

    Angewandte Chemie International Edition · 2023-02-01

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  42. Atomic Structural Origin of Fictive Temperature Revealed by AZnP3O9 (A=K, Rb) Glasses

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  43. Self-assembly, physico-chemical characterization, biological, virtual screening, and computational approach of novel 2-amino pyridine derivatives

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  44. Recent advances of inorganic phosphates with UV/DUV cutoff edge and large second harmonic response

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  46. Recent advances in non-π-conjugated nonlinear optical sulfates with deep-UV absorption edge

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  47. A Second‐Order Nonlinear Optical Material Consisting of Two π‐Conjugated Groups

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  48. Structural Motif Cosubstitution Strategy for Designing Fluoroaluminoborate with the Sr2Be2B2O7-Type Double-Layered Structure

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  49. Two Mixed-Alkali-Metal Selenates as Short-Wave Ultraviolet Nonlinear-Optical Materials

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  50. CaB2O2F4: A Novel [BOF2]∞-Based Structural Template with a Strong Second Harmonic Generation Response and Large Band Gap

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