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RESEARCH PAPER · Angewandte Chemie International Edition · 2020

Nonlinear Optical Oxythiophosphate Approaching the Good Balance with Wide Ultraviolet Transparency, Strong Second Harmonic Effect, and Large Birefringence

Xinyuan Zhang, Lei Kang, Pifu Gong, Zheshuai Lin, Yicheng Wu

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Nonlinear Optical Oxythiophosphate Approaching the Good Balance with Wide Ultraviolet Transparency, Strong Second Harmonic Effect, and Large BirefringenceOriginalFinding Short-Wavelength Birefringent Crystals with Large Optical Anisotropy Activated by π-Conjugated [C(NH2)3] Units45Hydrogen‐Bond‐Driven Synergistically Enhanced Hyperpolarizability: Chiral Coordination Polymers with Nonpolar Structures Exhibiting Unusually Strong Second‐Harmonic Generation87Hydrogen‐Bond‐Driven Synergistically Enhanced Hyperpolarizability: Chiral Coordination Polymers with Nonpolar Structures Exhibiting Unusually Strong Second‐Harmonic Generation19Hydroxyfluorooxoborate Na[B3O3F2(OH)2]⋅[B(OH)3]: Optimizing the Optical Anisotropy with Heteroanionic Units for Deep Ultraviolet Birefringent Crystals146Hydroxyfluorooxoborate Na[B3O3F2(OH)2]⋅[B(OH)3]: Optimizing the Optical Anisotropy with Heteroanionic Units for Deep Ultraviolet Birefringent Crystals16Mg 2 In 3 Si 2 P 7 : A Quaternary Diamond-like Phosphide Infrared Nonlinear Optical Material Derived from ZnGeP 2130Multifunctional DyIII Enantiomeric Pairs Showing Enhanced Photoluminescences and Third-Harmonic Generation Responses through the Coordination Role of Homochiral Tridentate N,N,N-Pincer Ligands322D van der Waals Layered [C(NH2)3]2SO3S Exhibits Desirable UV Nonlinear-Optical Trade-Off47Unusual ferroelectric-dependent birefringence in 2D trilayered perovskite-type ferroelectric exploited by dimensional tailoring63CsCu 3 SbS 4 : rational design of a two-dimensional layered material with giant birefringence derived from Cu 3 SbS 442K 3 V 2 O 3 F 4 (IO 3 ) 3 : a high-performance SHG crystal containing both five and six-coordinated V 5+ cations33A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency15A Lanthanum Ammonium Sulfate Double Salt with a Strong SHG Response and Wide Deep‐UV Transparency96[C(NH 2 ) 3 ] 2 S 2 O 8 : combining delocalized and localized π-conjugate units to achieve strong optical anisotropy21Nain(C2o4)(Hpo4)(H2o)5: An Ultraviolet Transparent Nonlinear Optical Oxalate-Phosphate with Large Birefringence0Lead Tellurite Crystals BaPbTe2O6 and PbVTeO5F with Large Nonlinear-/Linear-Optical Responses due to Active Lone Pairs and Distorted Octahedra20Review of Heteroleptic Tetrahedra as Birefringent or Nonlinear Optical Motifs17Uncovering a Vital Band Gap Mechanism of Pnictides49Oriented adsorption of NO2 on WSe2 monolayer16The Kurtz-Perry powder technique revisited: A case study on the importance of reference quality and broadband nonlinear optical measurements using LiInSe232Modulating Two Pairs of Chiral Dy III Enantiomers by Distinct β-Diketone Ligands to Show Giant Differences in Single-Ion Magnet Performance and Nonlinear Optical Response35Improved Polarization in the Sr6Cd2Sb6O7Se10 Oxyselenide through Design of Lateral Sublattices for Efficient Photoelectric Conversion4Improved Polarization in the Sr6Cd2Sb6O7Se10 Oxyselenide through Design of Lateral Sublattices for Efficient Photoelectric Conversion16Design of a new ultraviolet nonlinear optical material KNO3SO3NH3 exhibiting an unexpected strong second harmonic generation response44Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24A 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‐Delocalization5Effects of Counterions, Coordination Anions, and Coordination Solvent Molecules on Single-Molecule Magnetic Behaviors and Nonlinear Optical Properties of Chiral Zn2Dy Schiff Base Complexes41Local Polarity-Induced Assembly of Second-Order Nonlinear Optical Materials128Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25A 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 materials181Deep-ultraviolet nonlinear-optical crystal BaNa2[PO3(OH)]2 with large birefringence and strong second-harmonic-generation response8Ga(IO 3 ) 3 : a mid-IR nonlinear optical iodate with balanced performance between band gap and second harmonic generation response4Two temperature-induced 1D Cu II chain enantiomeric pairs showing different magnetic properties and nonlinear optical responses14Oriented adsorption and efficient sensing of NO2 on MoSe2 monolayer: a comparative study with WSe2 monolayer20Toward Large Second-Harmonic Generation and Deep-UV Transparency in Strongly Electropositive Transition Metal Sulfates112Two Chiral YbIII Enantiomeric Pairs with Distinct Enantiomerically Pure N-Donor Ligands Presenting Significant Differences in Photoluminescence, Circularly Polarized Luminescence, and Second-Harmonic Generation30Comprehensive review on multiple mixed-anion ligands, physicochemical performances and application prospects in metal oxysulfides32Machine Learning Classification Model for Screening of Infrared Nonlinear Optical Crystals6Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 422A BBO-like trithiocyanate with significantly enhanced birefringence and second-harmonic generation39Effective third harmonic generation of 355 nm ultraviolet laser based on the borate-phosphate Ba 3 (ZnB 5 O 10 )PO 4 crystal9Sr(NH2SO3)(NO3)·H2O: An Ultraviolet Nonlinear Optical Material Exhibiting Strong Second-Harmonic Generation Response and Sufficient Birefringence10Na 10 Zn(NO 3 ) 4 (SO 3 S) 4 : a nonlinear optical crystal combining inorganic π-conjugated and non-π-conjugated heteroanion groups8Birefringent Dispersion Optimization to Achieve Superior Nonlinear Optical Phase Matching in Deeper Solar‐Blind UV Band from KH 2 PO 4 to BeH 3 PO 516A Ferroelectric Nonlinear Optical Crystal for Deep‐UV Quasi‐Phase‐Matching51[Sn 3 OF]PO 4 vs. [Sn 3 F 3 ]PO 4 : enhancing birefringence by breaking the R 3 symmetry and realigning lone pairs12Chemical perspectives on heteroanionic compounds: a potential playground for multiferroics7Designing promising ultraviolet (UV) birefringent crystals with different hydrogen-bonded phosphate frameworks18Exploration of antimony( iii ) oxyhalides via single-site substitution in quest of large birefringence10Halide-driven polarity tuning and optimized SHG-bandgap balance in (C 4 H 11 N 2 )ZnX 3 (X = Cl, Br, I)34Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals9Homochiral Dy 2 single-molecule magnets with strong magneto-optical Faraday effects and strong third-harmonic generation23Pb 2 Ga 3 F 6 (SeO 3 ) 2 X 3 ·2H 2 O (X = Cl, Br): two new HTO-type members exhibiting large NLO effects mediated by ionic mixing and substitution strategies10Predictive nonlinear optical crystal formation energy regression model based on convolutional neural networks5Two chiral Co III and Ni II complexes with identical ligands presenting different nonlinear optical responses4Two chiral Eu III and Sm III enantiomeric pairs with enantiopure N-donor ligands: showing strong third-harmonic generation and photoluminescence properties7Two chiral lanthanide Pr III and Ho III complexes: NIR luminescence and nonlinear optical properties14Hierarchical van der Waals Assemblies to Boost Deep‐Ultraviolet Nonlinear‐Optical Capabilities in Boron Phosphate8Sb2O2SeO3 and Sb2O(SeO3)2: Two-Layered Antimony(III) Selenites with Enhanced Birefringence10[B3O3F4(OH)]2–: A Versatile Hydroxyfluorooxoborate Heteroanion Producing Compounds with Highly Tunable Optical Anisotropy19NaK5La2(SO4)6: Enhanced Birefringence of Multiple-Alkali Metal Sulfate Systems via Rare Earth Metal-Centered Polyhedra5Interpretable Machine Learning for Investigating the Molecular Mechanisms Governing the Transparency of Colorless Transparent Polyimide for OLED Cover Windows33Chiral mono- and dinuclear CoII and CuII enantiomeric pairs with distinct enantiopure N-donor ligands: Presenting highly enhanced third-harmonic generation responses6Ae3[TO3][SnOQ3] (Ae = Sr, Ba; T = Si, Ge; Q = S, Se) and Ba3[CO3][MQ4] (M = Ge, Sn; Q = S, Se): Design and Syntheses of a Series of Heteroanionic Antiperovskite-Type Oxychalcogenides29Unusual Triple-State Switching of Thermally Induced Birefringence in a Two-Dimensional Perovskite Ferroelectric45Effect of pressure on the structure, elasticity and optical properties of AgGaSe2 crystal3Functional assembly and modification of nonlinear optical fundamental motifs in phosphates27Cationic Coordination Modification Drives Birefringence and Nonlinear Effect Double Lifting in Sulfate4La 3 (Ga 3 S 3 O 3 )(Si 2 O 7 ): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups6A 3 Sc(PO 4 ) 2 (A = Li, Na): rare earth cations effectively regulate phosphate structures for enhanced birefringence4Impact of nuclear number on SHG and THG performances: a comparative study of chiral mono- and dinuclear Tb III complexes with identical organic ligands2La 2 ZnGa 2 S 6 O: a melilite-type transition metal oxysulfide achieving a well-balanced nonlinear optical behavior52D Chiral Ag(I) Complexes with A-π–A- and D-π–A-Type Dicarboxylic Acid Ligands: Presenting Significant Differences in Nonlinear Optical Responses5Can Low Structural Anisotropy Produce High Optical Anisotropy? Anomalous Giant Optical Birefringent Effect in PI4AlI4 in Focus11Multifunctional chiral dinuclear DyIII enantiomeric pairs: showing single-molecule magnet behaviors with very strong third-harmonic generation responses5Exploiting Rigid Inorganic π‐Conjugated Units and Deprotonatable Organic π‐Conjugated Dimers for Enhanced Linear and Nonlinear Optical Properties9All-three-in-one: Pb2(H2PO4)2(C2O4) significantly enhanced birefringence in phosphate materials4Designing High-Performance Short-Wave UV Tellurium-Based Mixed Halides Birefringent Crystals via Halogen Substitution Engineering4Eu(II) 4 Eu(III) 2 Ge 3 S 11 O 2 : a Single‐Element Mixed‐Valence Engineering Breakthrough for Strongly Enhanced Nonlinearity and Anisotropy in Rare‐Earth Oxysulfides8[HgX 2 ] Linear Group Enabled Ultraviolet Birefringent Crystal RbHg 5 Br 11 with Strong Optical Anisotropy and Wide Bandgap12(C7H10N)3Bi2I9·I2: Synergistic Cooperation of π-Conjugated Cations and Distorted [BiI6] Octahedra Enabling a Large Infrared Birefringence4Series of phosphate nonlinear optical materials containing active metal ions with short cut-off edges0Simultaneously switching both the magnetic behaviors and nonlinear optical processes in mononuclear DyIII complexes0The condensation of π-conjugated units: a new paradigm for designing high-performance optical crystals4Two hydrated ionic cocrystals of phenylphosphonate exhibiting second-harmonic generation and proton conductivity0Simultaneously switching both the magnetic behavior and nonlinear optical process in mononuclear DyIII complexes via the coordination role of enantiopure N3-pincers2(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 Conflicts13Tuning linear and nonlinear optical performances of two eight- and nine-coordinated chiral SmIII enantiomeric pairs by enantiopure N-donor ligands1Linear [ICl 2 ] Units Induced Giant Optical Anisotropy in AICl 2 (A = NH 4 , Rb): A Pathway to Advanced Birefringent Materials4Chiral dinuclear EuIII enantiomeric pairs: simultaneously showing photoluminescences, circularly polarized luminescences, second- and third-harmonic generations with enhanced performances0

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  49. Chemical perspectives on heteroanionic compounds: a potential playground for multiferroics

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  50. Designing promising ultraviolet (UV) birefringent crystals with different hydrogen-bonded phosphate frameworks

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