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RESEARCH PAPER · Angewandte Chemie International Edition · 2021

Be2(BO3)(IO3): The First Anion‐mixed Van der Waals Member in the KBe2BO3F2 Family with a Very Strong Second Harmonic Generation Response

Guang Peng, Chensheng Lin, Huixin Fan, Kaichuang Chen, Bingxuan Li, Ge Zhang, Ning Ye

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Be2(BO3)(IO3): The First Anion‐mixed Van der Waals Member in the KBe2BO3F2 Family with a Very Strong Second Harmonic Generation ResponseOriginalA Lead Mixed Halide with Three Different Coordinated Anions and Strong Second‐Harmonic Generation Response10Synergistic Effect of π-Conjugated [C(NH 2 ) 3 ] Cation and Sb(III) Lone Pair Stereoactivity on Structural Transformation and Second Harmonic Generation58AZn 2 (BO 3 )Si 2 O 5 (A = Rb, Cs): first examples of KBe 2 BO 3 F 2 structure type in the borosilicate family exhibiting a deep-ultraviolet cutoff edge25An excellent lead oxyiodide with a strong second-harmonic generation response and a large birefringence induced by the oriented arrangement of highly distorted [PbO 4 I 2 ] polyhedra13APb 2 (C 7 H 3 NO 4 ) 2 I (A = K, Rb, Cs): rare stable nonlinear optical crystals with second-harmonic generation response and highly distorted lead core coordination polyhedra2Ba 2 [WO 3 F(IO 3 )][WO 3 F 2 ]: the first polar fluorinated tungsten iodate featuring a direct W–O–I bond7CaCe(IO 3 ) 3 (IO 3 F)F: a promising nonlinear optical material containing both IO 3 − and IO 3 F 2− anions22Cd 2 (IO 3 )(PO 4 ) and Cd 1.62 Mg 0.38 (IO 3 )(PO 4 ): metal iodate-phosphates with large SHG responses and wide band gaps28Hexameric poly-fluoroberyllophosphate Na 4 Be 2 PO 4 F 5 with moderate birefringence and deep-ultraviolet transmission as a potential zero-order-waveplate crystal17KPb 3 ( o -C 5 H 4 NCOO) 2 Cl 5 : a brand-new stable lead chloride with good comprehensive nonlinear optical performance5KRE(CO 3 ) 2 (RE = Eu, Gd, Tb): new mixed metal carbonates with strong photoluminescence and large birefringence15Na 3 B 6 O 10 (HCOO): an ultraviolet nonlinear optical sodium borate-formate33Unprecedented boat-shaped [Mo 2 O 5 (IO 3 ) 4 ] 2− polyanions induced a strong second harmonic generation response31Chiral Ligand‐Driven Systematic Synthesis of Coordination Polymers with Non‐centrosymmetric Structures12New double nonlinear-optical borate Rb3SmB6O12: Synthesis, structure and spectroscopic properties26Explorations of New SHG Materials in Mercury Iodate Sulfate System**9Sr3[SnOSe3][CO3]: A Heteroanionic Nonlinear Optical Material Containing Planar π‐conjugated [CO3] and Heteroleptic [SnOSe3] Anionic Groups78Sr3[SnOSe3][CO3]: A Heteroanionic Nonlinear Optical Material Containing Planar π‐conjugated [CO3] and Heteroleptic [SnOSe3] Anionic Groups7A2BeS2O8 (A = NH4, K, Rb, Cs) Deep Ultraviolet Nonlinear Optical Crystals33Maximizing the linear and nonlinear optical responses of alkaline tricyanomelaminate28Enhanced Interlayer Interaction and Second-Harmonic-Generation Response in a KBe 2 BO 3 F 2 -Type Inorganic–Organic Hybrid Zinc Borate33General relationship between the band-gap energy and iodine-oxygen bond distance in metal iodates15Realization of Enlarged Birefringence from BaCdBe2(BO3)2F2 to NaMgBe2(BO3)2F via the Cation Size Effect as a Potential Deep-Ultraviolet Birefringent Material18A Hybrid Antiperovskite with Strong Linear and Second‐Order Nonlinear Optical Responses15A Hybrid Antiperovskite with Strong Linear and Second‐Order Nonlinear Optical Responses96Design of a new ultraviolet nonlinear optical material KNO3SO3NH3 exhibiting an unexpected strong second harmonic generation response44Dual-Ligand-Oriented Design of Noncentrosymmetric Complexes with Nonlinear-Optical Activity11ZrF2(IO3)2 and RbGaF3(IO3): Two Promising Birefringent Crystals Featuring 1D Metal-Fluoride Cationic Chains and Wide Bandgaps22Na 2 (C 4 O 4 )(H 3 BO 3 )(H 2 O) 4 ·H 3 BO 3 : the first borate-squarate with strong SHG response obtained by superior synergy11Enhanced Second-Harmonic-Generation Response in a KH2PO4-Type Calcium Nitrate Carboxylate with Unusual Three-Dimensional Inorganic and Organic Connections3(C 5 H 6.16 N 2 Cl 0.84 )(IO 2 Cl 2 ): a birefringent crystal featuring unprecedented (IO 2 Cl 2 ) − anions and π-conjugated organic cations56[M(OH) 2 ] 3 (IO 3 )(SeO 4 )·H 2 O (M = Ga and In): metal iodate–selenate nonlinear optical materials with a hexagonal tungsten oxide-type topology20Honeycomb layered topology construction for exceptional long-wave infrared nonlinear optical crystals29KRb 2 (NO 3 ) 2 Cl: a new birefringent crystal exhibiting a perovskite-related framework and a short cutoff edge6Second harmonic generation from symmetry breaking stimulated by mixed organic cations in zero-dimensional hybrid metal halides7The transformation of a zero-dimensional cluster into a one-dimensional chain structure achieving a dramatically enhanced birefringence in tin( ii )-based oxalates33C(NH2)3(I3O8)(HI3O8)(H2I2O6)(HIO3)4·3H2O: An Unprecedented Asymmetric Guanidinium Polyiodate with a Strong Second-Harmonic-Generation Response and a Wide Band Gap16Recent advances of inorganic phosphates with UV/DUV cutoff edge and large second harmonic response7CsHfF4(IO3): A Hafnium Iodate Exhibiting a Strong Second-Harmonic-Generation Effect and a Wide Band Gap Achieved by Mixed-Ligand Acentric Coordination8Two Mixed-Alkali-Metal Selenates as Short-Wave Ultraviolet Nonlinear-Optical Materials10Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 422A Polar Tetragonal Tungsten Bronze with Colossal Second‐Harmonic Generation18A BBO-like trithiocyanate with significantly enhanced birefringence and second-harmonic generation39Advances in aliovalent substitution strategy for the design and synthesis of nonlinear optical materials: d0 transition metal/gallium iodates and selenites70Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability40Single-Crystalline Li2Sn(IO3)6 Microwires: Combining Optical-Waveguiding and Frequency-Doubling Functions5Halogen Bonding Assembles Anion⋅⋅⋅Anion Architectures in Non‐centrosymmetric Iodate and Bromate Crystals24Recent Progress in Crystalline Borates with Edge-Sharing BO4 Tetrahedra21Design Principles for Noncentrosymmetric Materials23(NH 4 ) 2 (I 5 O 12 )(IO 3 ) and K 1.03 (NH 4 ) 0.97 (I 5 O 12 )(IO 3 ): Mixed‐Valent Polyiodates with Unprecedented I 5 O 12 − Unit Exhibiting Strong Second‐Harmonic Generation Responses and Giant Birefringence22Introduction of the [B–O/F] Units Enhances the Band Gap and Birefringence from Na6Mg3B10O18F6 to K3NaB10O16F211Centrosymmetric Rb2Sb(C2O4)2.5(H2O)3 and Noncentrosymmetric RbSb2(C2O4)F5: Two Antimony (III) Oxalates as UV Optical Materials20A survey of stereoactive oxysalts for linear and nonlinear optical applications40YSO4F·H2O: A Deep-Ultraviolet Birefringent Rare-Earth Sulfate Fluoride with Enhanced Birefringence Induced by Fluorinated Y-Centered Polyhedra19Ln 2 F 2 (OH 2 )(MoO 3 ) 2 (SeO 3 ) 2 : Promising Multifunctional Nonlinear Optical Materials Created by Partial Fluorination Strategy under Corrosion Resistant Supercritical Reactions25Ba 2 Ga 2 F 6 (IO 3 )(PO 4 ): the first fluoride-containing iodate-phosphate with a 1D [Ga 2 F 6 (IO 3 )(PO 4 )] 4− helix chain2Fully tricoordinated assembly unveils a pioneering nonlinear optical crystal (SbTeO 3 )(NO 3 )25Noncentrosymmetric tellurite halides created by a depolymerization strategy: toward strong SHG intensity and wide bandgap16Cs 3 In(In 4 Se 7 )(P 2 Se 6 ): A Multi‐Chromophore Chalcogenide with Excellent Nonlinear Optical Property Designed by Group Grafting55Cs3In(In4Se7)(P2Se6): A Multi‐Chromophore Chalcogenide with Excellent Nonlinear Optical Property Designed by Group Grafting2Centrosymmetric CaBaMF8 and Noncentrosymmetric Li2CaMF8 (M = Zr, Hf): Dimension Variation and Nonlinear Optical Activity Resulting from an Isovalent Cation Substitution-Oriented Design17Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond Engineering157A Noncentrosymmetric Metal‐Free Borophosphate: Achieving a Large Birefringence and Excellent Stability by Covalent‐Linkage27Designing Strong Polarity and High Configurational Entropy Flexible Units toward Excellent Ultraviolet Nonlinear Optical Materials42An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution33An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution1Second Harmonic Generation in β-K2TeW3O12: An Acentric Crystal Designed from Centric Phase via Pressure Modulation4Gradual Increase in Birefringence of Antimony Oxalates through Precise Tuning of the Sb3+/[C2O4]2– Ratio7Cu(I)‐Induced ‘Click Reaction’ Involving Coordination and Covalent Assembly of Hybrid Borates for the Electrocatalytic CO 2 Reduction4Cu(I)‐Induced ‘Click Reaction’ Involving Coordination and Covalent Assembly of Hybrid Borates for the Electrocatalytic CO 2 Reduction11Ae3[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 Oxychalcogenides29π-Lone pair synergy in (C7H4NO4)(IO3): Optimal balance among SHG, birefringence, and bandgap performance29Lanthanide Contraction Eliminates Disorder while Holding Robust Second Harmonic Generation in a Series of Polyiodates13Li2NaB3S2O12: A Deep-UV Transparent Borosulfate with Moderate Birefringence Derived from the [B3S2O12]∞ Infinite Chain Designed by the High Boron-to-Sulfur Ratio Strategy6Breaking Symmetry for SHG Response: Lanthanide Acetate Crystals via Water Molecule Regulation Strategy5LaAgSiS4: Increasing Optical Birefringence in Rare Earth Chalcogenide by Addition of Planar [AgS3] Groups5Amino substitution strategy achieves significant blue shift while preserving high optical anisotropy: A2(H3C3N4S2)2•H2O (A =NH4, K, Rb, Cs)6Unveiling Noncentrosymmetric Pyridine Carboxylates from Centrosymmetric Templates through Motif Configuration Modulation in Zero-Dimensional System7Looking Back the Nonlinear Optical Crystals in a Functionalized Unit's Perspective109Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization5Breaking Performance Barriers in KBe 2 BO 3 F 2 (KBBF) Analogs by Functional Group Self‐Polymerization48“All-four-in-one”: a novel mercury tellurite–nitrate Hg 3 (TeO 3 )(Te 3 O 7 )(NO 3 ) 2 exhibiting exceptional optical anisotropy29(C 5 N 2 H 7 )IO 2 F 2 and (C 3 N 6 H 8 )(IO 2 F 2 ) 2 : two new organic–inorganic hybrid fluoroiodate birefringent crystals7A π-conjugated organic molecule-modified strategy to achieve high-performance metal nitrate birefringent crystals9Different p-block elements induce C 3 [111] octahedral distortion in titanium to generate an intense nonlinear effect14K 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 birefringence2Synthesising a series of promising ultraviolet nonlinear optical materials with the aid of the flexibility of isolated [B 5 O 10 ] groups3Cationic Modification in Hybrid Iodates: A Pathway to Superior Performance12Lithium Borate-Squarate: An Organic–Inorganic Groups-Mixed Nonlinear Optical Crystal with Large Birefringence4From 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 Crystal28The birefringence in orthorhombic and triclinic lead-iodates and the functional basic units' contribution: A first-principles investigation3Design of rare earth borate short-wave UV nonlinear optical crystals with strengthened second harmonic generation activities via cationic modification strategy11Review of KBe2BO3F2-like second-order nonlinear optical materials and their structure-performance relationships13Na[B3IO7(OH)] and Na2[B4IO9](IO3): Explorations of Boroiodates with Strong Second Harmonic Generation Response and Large Birefringence54Hg3(TeO3)2(NO3)2 and Hg3(Te2O5)2(NO3)2: The First Two Hg‐Based Tellurite Nitrate Unit‐Mixed Crystals with Large Optical Anisotropy16[C(NH2)3]Y(HCOO)4: Constructing 3D Framework for Guanidine-Based UV Nonlinear Optical Crystals with Good Performance8Cd 7 I 12 Q·As 4 Q n (Q = S, Se; n = 3, 4): In Situ Alteration of Functional Molecules in Polar Metal Inorganic Framework Tailoring High‐Performance Infrared Nonlinear Optical Crystals9Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties35Dual Chemical Scissors Strategy Enables 1D Antimony Selenates with Ultraviolet Nonlinear Optical Properties6Cs2CdV2O6Br2: A Mid-Infrared Nonlinear Optical Vanadate Containing Both d0/d10 Transition Metal Cations and Bromine Anions5A balance in SHG response, band gap and birefringence in a series of rare-earth sulfate-iodate6Hydrogen Bond-Assisted Structural Regulation Enables Large Birefringence in Two Antimony Oxalofluoride Crystals5Strongly Polar [H2PO3]− Induced π-Conjugated Group Arrangement for Balanced UV Nonlinear Optical Performance3Lewis Acidity‐Governed Ion Exchange and Record Birefringence in A′[Ag 3 (PO 3 F) 2 ]11Lewis Acidity‐Governed Ion Exchange and Record Birefringence in A′[Ag 3 (PO 3 F) 2 ]2Borosilicates as deep-ultraviolet transparent nonlinear optical crystals: Structural motifs, performance limits and future directions9Multifactorial directed regulation of anionic units in praseodymium-contained iodates1Organic Halogen Substitution-Driven Halogen Bonding Induces Polar 3D Supramolecular Framework and Second-Harmonic-Generation Response7Na6(SO4)2SiF6: A Stable Sulfate Fluosilicate with Wide Deep-Ultraviolet Transparency Window and Strong Second-Harmonic Generation Response4Metal Chloride‐Iodate Nonlinear Optical Materials via Direct Chlorination of Centrosymmetric Metal Iodate Crystals0Ag(Te2O3)(PO4): The first Ag-containing phosphate-tellurite nonlinear optical crystal featuring novel zigzag layered structure0Hydrogen-bond-driven noncentrosymmetric structure formation in π-conjugated (C3H7N6)(IO3): achieving both strong SHG response and wide bandgap5KCd(IO 3 ) 2 Cl: A New UV NLO Crystal with Balanced Optical Properties Engineering via Target‐Driven Multi‐Ion Substitution Strategy7Isovalent cation substitution strategy for enhancing nonlinear optical properties of iodate-selenate materials0A universal synthetic strategy for noncentrosymmetric lead oxyhalide frameworks with strong second-harmonic generation0Halogen-ion-driven polymorphs for high-performance nonlinear optical crystalline materials3LiHgTeO 3 : a Hg( i )-containing tellurite crystal with typical Hg–Hg bonds0Confinement-assembled ultraviolet nonlinear optical crystal from pyridine-expanded π-systems with exhibiting strong SHG and birefringence18Zn 4 (BO 3 ) 2 (CO 2 CH 2 NH 2 ) 2 ·H 2 O: An Organic–Inorganic Hybridized KBe 2 BO 3 F 2 -like Ultraviolet Nonlinear Optical Crystal3Pyrazole‐Protected Heteronuclear Rare‐Earth Boron‐Oxo Cluster Cage With Tunable Luminescence0Rational design of a quasi-0D tungsten tellurite nonlinear optical crystal with exceptionally balanced properties1Ultrawide Bandgap and Record-High Birefringence in a Covalent Beryllium-Organic Framework7NaNO 3 [(NH 2 ) 2 SO 2 ] 2 : A Halogen‐Free KBBF‐Type Nitrate Crystal with Record Birefringence for Ultraviolet Applications0Regulating B‐O Arrangement Boosts Anisotropy in a Simple Rubidium Borate, Leading to a High‐Performance UV NLO Crystal0Breaking Layered Limitations via Electrostatic-to-Covalent Conversion toward Three-Dimensional T2-Cluster-Based Chalcogenides7K 3 Yb 2 (BO 3 ) 3 and Rb 3 Yb 2 (BO 3 ) 3 : Two Rare-Earth Borate Ultraviolet Nonlinear Optical Crystals1First‐Principles Investigation of the Structural, Electronic, Optical, Elastic, and Thermal Properties of Defect Diamond‐Like Hg 3 P 2 S 80Charge and structural flexibility of tartrate groups enable high-performance ultraviolet nonlinear optical crystals0Cation‐Regulated [CH 3 BO 2 F]‐Derived Borates: Synergistic Fluorination and Organic Functionalization for High‐Birefringence UV NLO Materials0

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  9. Hexameric poly-fluoroberyllophosphate Na 4 Be 2 PO 4 F 5 with moderate birefringence and deep-ultraviolet transmission as a potential zero-order-waveplate crystal

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  10. KPb 3 ( o -C 5 H 4 NCOO) 2 Cl 5 : a brand-new stable lead chloride with good comprehensive nonlinear optical performance

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  28. ZrF2(IO3)2 and RbGaF3(IO3): Two Promising Birefringent Crystals Featuring 1D Metal-Fluoride Cationic Chains and Wide Bandgaps

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  29. Na 2 (C 4 O 4 )(H 3 BO 3 )(H 2 O) 4 ·H 3 BO 3 : the first borate-squarate with strong SHG response obtained by superior synergy

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  30. Enhanced Second-Harmonic-Generation Response in a KH2PO4-Type Calcium Nitrate Carboxylate with Unusual Three-Dimensional Inorganic and Organic Connections

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  31. (C 5 H 6.16 N 2 Cl 0.84 )(IO 2 Cl 2 ): a birefringent crystal featuring unprecedented (IO 2 Cl 2 ) − anions and π-conjugated organic cations

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  32. [M(OH) 2 ] 3 (IO 3 )(SeO 4 )·H 2 O (M = Ga and In): metal iodate–selenate nonlinear optical materials with a hexagonal tungsten oxide-type topology

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  33. Honeycomb layered topology construction for exceptional long-wave infrared nonlinear optical crystals

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  34. KRb 2 (NO 3 ) 2 Cl: a new birefringent crystal exhibiting a perovskite-related framework and a short cutoff edge

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

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

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  41. Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 4

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  42. A Polar Tetragonal Tungsten Bronze with Colossal Second‐Harmonic Generation

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  43. A BBO-like trithiocyanate with significantly enhanced birefringence and second-harmonic generation

    Science China Materials · 2023-05-09

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  44. Advances in aliovalent substitution strategy for the design and synthesis of nonlinear optical materials: d0 transition metal/gallium iodates and selenites

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  45. Cd2Nb2Te4O15: A Novel Pseudo‐Aurivillius‐Type Tellurite with Unprecedented Nonlinear Optical Properties and Excellent Stability

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  46. Single-Crystalline Li2Sn(IO3)6 Microwires: Combining Optical-Waveguiding and Frequency-Doubling Functions

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  47. Halogen Bonding Assembles Anion⋅⋅⋅Anion Architectures in Non‐centrosymmetric Iodate and Bromate Crystals

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  48. Recent Progress in Crystalline Borates with Edge-Sharing BO4 Tetrahedra

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  49. Design Principles for Noncentrosymmetric Materials

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  50. (NH 4 ) 2 (I 5 O 12 )(IO 3 ) and K 1.03 (NH 4 ) 0.97 (I 5 O 12 )(IO 3 ): Mixed‐Valent Polyiodates with Unprecedented I 5 O 12 − Unit Exhibiting Strong Second‐Harmonic Generation Responses and Giant Birefringence

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