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RESEARCH PAPER · Angewandte Chemie International Edition · 2020

Pb 18 O 8 Cl 15 I 5 : A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties

Xinglong Chen, Qun Jing, Kang Min Ok

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Pb 18 O 8 Cl 15 I 5 : A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical PropertiesOriginalRecent Advances in Oxide‐based Nonlinear Optical Materials with Wide Infrared Transparency Beyond 6 μm38Bi 32 Cd 3 P 10 O 76 : a new congruently melting nonlinear optical crystal with a large SHG response and a wide transparent region24A New Nonlinear Optical Selenide Crystal AgLiGa 2 Se 4 with Good Comprehensive Performance in Mid‐Infrared Region44Chiral Template‐Driven Macroscopic Chirality Control: Structure‐Second‐Harmonic Generation Properties Relationship24Synergism of multiple functional chromophores significantly enhancing the birefringence in layered non-centrosymmetric chalcohalides20The synthesis, characterization, and theoretical analysis of (NH 4 ) 3 PbCl 52Breaking through the “3.0 eV wall” of energy band gap in mid-infrared nonlinear optical rare earth chalcogenides by charge-transfer engineering144Distinctive modulation of optical anisotropy by halogens in α/β-Cd–P–X (X = Cl, Br, and I)2Facile syntheses of silver thioantimonates exhibiting second-harmonic generation responses and large birefringence18Novel noncentrosymmetric polar coordination compounds derived from chiral histidine ligands36RbPb 8 O 4 Cl 9 : the first alkali metal lead oxyhalide with distorted [PbO 3 Cl 3 ] and [PbOCl 5 ] mixed-anion groups6Role of fluorine on the structure and second-harmonic-generation property of inorganic selenites and tellurites23Systematic centricity control using a chiral template: novel noncentrosymmetric polar niobium oxyfluorides and tantalum fluorides directed by chiral histidinium cations, [( l -hisH 2 )NbOF 5 ], [( d -hisH 2 )NbOF 5 ], [( l -hisH 2 )TaF 7 ], and [( d -hisH 2 )TaF 7 ]8Ultraviolet nonlinear optical crystals A 3 SrBi(P 2 O 7 ) 2 (A = K, Rb) with large second harmonic generation responses15Halonitrides Zn 2 NX (X=Cl,Br): Novel Mid-Infrared Nonlinear Optical Materials30Second-order nonlinear optical and photoelectric properties of Zn4B6O12S20Different mechanism of stereochemical activity and birefringence in post-transition metal halides: A first-principles investigation1Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance43Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance6A New Anhydrous Polar Rare-Earth Iodate Fluoride, Ce(IO3)2F2, Exhibiting a Large Second-Harmonic-Generation Effect and Improved Overall Performance35Hydrogen‐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 Generation19KCs2[Pb2Br5(HCOO)2]: A Polar 3D Lead‐Bromide Framework Exhibiting Strong Second‐Harmonic Generation Response10Li 4 MgGe 2 S 7 : The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap213Li4MgGe2S7: The First Alkali and Alkaline‐Earth Diamond‐Like Infrared Nonlinear Optical Material with Exceptional Large Band Gap15A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation22A Congruent‐Melting Mid‐Infrared Nonlinear Optical Vanadate Exhibiting Strong Second‐Harmonic Generation63Hg 3 P 2 S 8 : A New Promising Infrared Nonlinear Optical Material with a Large Second-Harmonic Generation and a High Laser-Induced Damage Threshold111Tourmaline with ultraviolet optical nonlinearity: Emergent material discovery from mineral5Hybrid Metal‐Halide Infrared Nonlinear Optical Crystals of (TMEDA)MI5 (M = Sb, Bi) with High Stability36A Lead Mixed Halide with Three Different Coordinated Anions and Strong Second‐Harmonic Generation Response10Ca3(TeO3)2(MO4) (M = Mo, W): Mid-Infrared Nonlinear Optical Tellurates with Ultrawide Transparency Ranges and Superhigh Laser-Induced Damage Thresholds46Polymorphic Pb14O8I12 and Pb7O4I6 oxyhalides featuring unprecedented [O8Pb14] clusters with broad IR transparency20Noncentrosymmetric chalcohalide K2Ba3Ge3S9Cl2: A new nonlinear optical material with remarkable laser-induced damage threshold17Complex coordinated functional groups: A great genes for nonlinear optical materials64Second-Harmonic-Generation-Active Oxyhalides: CuSb2O3X (X = Cl, Br)17[ASr 4 Cl][Ge 3 S 10 ] (A = Na, K) and [KBa 4 Cl][Ge 3 S 10 ]: new salt-inclusion infrared nonlinear optical crystals with zero-dimensional [Ge 3 S 9 ] clusters32An 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 polyhedra2Band gap modulation and nonlinear optical properties of quaternary tellurates Li 2 GeTeO 613Inducing large birefringence by enhancing asymmetric electron distribution of Y–O polyhedra21Metal oxyhalides: an emerging family of nonlinear optical materials124Pb 3 SBrI 3 : the first Pb-based chalcohalide with multiple halogens features a unique two-dimensional structure composed of diverse Pb-centered polyhedra12Rational design of a promising oxychalcogenide infrared nonlinear optical crystal60Tellurate polymorphs with high-performance nonlinear optical switch property and wide mid-IR transparency19Lead Tellurite Crystals BaPbTe2O6 and PbVTeO5F with Large Nonlinear-/Linear-Optical Responses due to Active Lone Pairs and Distorted Octahedra20Pb 4 SeBr 6 : A Congruently Melting Mid‐Infrared Nonlinear Optical Material with Excellent Comprehensive Performance39Infrared nonlinear optical performances of a new sulfide β-PbGa2S415Novel layered heterobimetallic fluorides with large optical band gaps3NaGa3Se5: An Infrared Nonlinear Optical Material with Balanced Performance Contributed by Complex {[Ga3Se5]−}∞ Anionic Network14SrZnGeS 4 : A Dual‐Waveband Nonlinear Optical Material with a Transparency Spanning UV/Vis and Far‐IR Spectral Regions88SrZnGeS4: A Dual‐Waveband Nonlinear Optical Material with a Transparency Spanning UV/Vis and Far‐IR Spectral Regions12Double‐Modification Oriented Design of a Deep‐UV Birefringent Crystal Functionalized by [B12O16F4(OH)4] Clusters9Double‐Modification Oriented Design of a Deep‐UV Birefringent Crystal Functionalized by [B12O16F4(OH)4] Clusters139Heteroanionic Melilite Oxysulfide: A Promising Infrared Nonlinear Optical Candidate with a Strong Second-Harmonic Generation Response, Sufficient Birefringence, and Wide Bandgap65The Kurtz-Perry powder technique revisited: A case study on the importance of reference quality and broadband nonlinear optical measurements using LiInSe232Mid-Infrared Nonlinear Optical Halides with Diamond-like Structures: A Theoretical and Experimental Study43Bi3TeBO9: A Promising Mid-Infrared Nonlinear Optical Crystal with a Large Laser Damage Threshold6Highly transparent Pb8O7I2, a novel lead oxyiodide5RbBiP2S6: A Promising IR Nonlinear Optical Material with a Giant Second-Harmonic Generation Response Designed by Aliovalent Substitution80Eu 2 P 2 S 6 : The First Rare‐Earth Chalcogenophosphate Exhibiting Large Second‐Harmonic Generation Response and High Laser‐Induced Damage Threshold143Eu2P2S6: The First Rare‐Earth Chalcogenophosphate Exhibiting Large Second‐Harmonic Generation Response and High Laser‐Induced Damage Threshold7[Ba2F2][Ge2O3S2]: An Unprecedented Heteroanionic Infrared Nonlinear Optical Material Containing Three Typical Anions47Pb5(GeO4)(Ge2O7) and Pb3.32Ca1.68(GeO4)(Ge2O7): Two Nonlinear Optical Germanates Induced by Diverse PbOx Polyhedra17Sb5O7I: Exploration of Ternary Antimony-Based Oxyhalide as a Nonlinear-Optical Material27[Cs6Cl][Ga5GeQ12] (Q = S, Se): two novel porous layered chalcohalides exhibiting two-band emission and ion exchange properties6Ag4SnGe2S7: A Noncentrosymmetric Chalcogenide in I4–II–IV2–VI7 System with Non-Diamond-Like Structure Featuring 1D ∞[SnGe2S8]6– Infinite Chain2Li x Ag 1– x GaSe 2 : Interplay Between Lithium and Silver in Mid‐Infrared Nonlinear Optical Chalcogenides33Ag[SC(NH2)2]2F: A Laser Damage-Tolerant Infrared Nonlinear Optical Material9LiAlS2: A promising infrared frequency-conversion material with ultrawide band gap and high laser-induced damage threshold19New lead-iodide formates with a strong second-harmonic generation response and suitable birefringence obtained by the substitution strategy8From Ba3Nb2O2F12(H2O)2 to Ba0.5NbO2F2(H2O): Achieving Balanced Nonlinear Optical Performance by O/F Ratio Regulation18KREP2Se6 (RE = Sm, Gd, Tb): The First Rare‐Earth Selenophosphates with Remarkable Nonlinear Optical Activities Realized by Synergistic Effect of RE‐ and P‐Based Motifs39γ-P 4 S 3 I 2 : a new metal-free infrared second-order nonlinear optical crystal designed by polymorphism strategy17From CdPb 8 (SeO 3 ) 4 Br 10 to Pb 3 (TeO 3 )Br 4 : the first tellurite bromide exhibiting an SHG response and mid-IR transparency21LaAeAl 3 S 7 (Ae = Ca, Sr): Cairo pentagonal layered thioaluminates achieving a good balance between a strong second harmonic generation response and a wide bandgap23Nitrides: a promising class of nonlinear optical material candidates9Synthesis, structure and characterization of Cd 2 TeO 3 Cl 2 with unprecedented [Cd 2 O 6 Cl 4 ] octahedral dimers5Toward Large Second-Harmonic Generation and Deep-UV Transparency in Strongly Electropositive Transition Metal Sulfates112K2(H2O)WO3F2: A new nonlinear optical material with remarkable second-harmonic generation response and enhanced laser damage threshold9NaRb 6 (B 4 O 5 (OH) 4 ) 3 (BO 2 ) Featuring Noncentrosymmetry, Chirality, and the Linear Anionic Group BO 2 –100[K2PbX][Ga7S12] (X = Cl, Br, I): The First Lead‐Containing Cationic Moieties with Ultrahigh Second‐Harmonic Generation and Band Gaps Exceeding the Criterion of 2.33 eV46Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 422Na3SiS3F: A Wide Bandgap Fluorothiosilicate with Unique [SiS3F] Unit and High Laser‐Induced Damage Threshold39First-principles study on AgBi(CrO4)2:An effective infrared nonlinear optical compound3Pb(OH)I: A lead(II)-based oxyhalide with a large birefringence5Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit38Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit1The Strategy to Improve the Phase Matching Ability in Tetrahedron‐Based Deep‐Ultraviolet Nonlinear Optical Crystals21Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75Ca2Ln(BS3)(SiS4) (Ln = La, Ce, and Gd): Mixed Metal Thioborate‐Thiosilicates as Well‐Performed Infrared Nonlinear Optical Materials29Eu 2 MGe 2 OS 6 (M = Mn, Fe, Co): Three Melilite-Type Rare-Earth Oxythiogermanates Exhibiting Balanced Nonlinear-Optical Behaviors21A new nonlinear optical crystal Li0.81Ag0.19InSe2 with balanced properties for efficient nonlinear conversion in the mid-IR region10Structural diversity and complexity of antiperovskites38A potassium lead 2-methylmalonate-iodide nonlinear optical crystal with strong second-harmonic generation response and large birefringence2Flexible Anionic Groups‐Activated Structure Dissymmetry for Strong Nonlinearity in Ln 2 Ae 3 M IV 3 S 12 Family15ZnGa 2 S 4 : an infrared nonlinear optical material with large second‐harmonic generation response and wide band gap28[RbSr 3 X][(BS 3 ) 2 ] (X = Cl, Br): two salt-inclusion thioborates with large birefringence and structure transformation from centrosymmetric to asymmetric8Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence11Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence75Positive and Negative Contribution from Lead–Oxygen Groups and Halogen Atoms to Birefringence: A First Principles Investigation4Two noncentrosymmetric alkali metal phosphates MZnPO4 (M = Rb, Cs) with honeycomb-like structures8Chiral amino acid-templated tin fluorides tailoring nonlinear optical properties, birefringence, and photoluminescence17Multifunctional Chiral d 10 ‐Metal Coordination Polymers: Tunable Photoluminescence and Efficient Second‐Harmonic Generation with Circular Dichroic Response18Rational Design of the Alkali Metal Sn‐Based Mixed Halides with Large Birefringence and Wide Transparent Range44Synthesis, crystal and electronic structures, linear and nonlinear optical properties, and photocurrent response of oxyhalides CeHaVIO 4 (Ha = Cl, Br; VI = Mo, W)10Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65Nonlinear Optical Phosphide CuInSi2P4: The Inaugural Member of Diamond-Like Family I–III–IV2–V4 Inspired by ZnGeP216Ba4Cd2Ge2Te9: A promising infrared functional crystal with large birefringent and photoluminescence properties2Chemical modulation of A I RE III C IV QVI4 family compounds for band gap and optical anisotropy enhancement16Chemical perspectives on heteroanionic compounds: a potential playground for multiferroics7Design of alkali lead oxybromides with a strong second-harmonic generation response and large birefringence1Exploration of antimony( iii ) oxyhalides via single-site substitution in quest of large birefringence10Exploring a new short-wavelength nonlinear optical fluoride material featuring unprecedented polar cis -[Zr 6 F 34 ] 10− clusters48Hydrogen bonding bolstered head-to-tail ligation of functional chromophores in a 0D SbF 3 ·glycine adduct for a short-wave ultraviolet nonlinear optical material32KBa 3 M 2 F 14 Cl (M = Zr, Hf): novel short-wavelength mixed metal halides with the largest second-harmonic generation responses contributed by mixed functional moieties37RbPbPS 4 : a promising IR nonlinear optical material achieved by lone-pair-cation-substitution-induced structure transformation23Exceptional Optical Anisotropy Enhancement Achieved Through Dual‐Ions Cosubstitution Strategy in Novel Hybrid Bismuth Halides23Rational Design of Novel Promising Infrared Nonlinear Optical Materials: Structural Chemistry and Balanced Performances156Synthesis, Structure, and Optical Properties of a 0D Hybrid Organic–Inorganic Metal Halide (C 5 N 2 H 14 Cl)GeCl 317Record Second-Harmonic Generation and Birefringence in an Ultraviolet Antimonate by Bond Engineering157[Na2PbI][Ga7S12]: Combining Diamond-Like Anionic Framework with Polycationic Chain toward Achieving Remarkable Nonlinear Optical Response21Infrared nonlinear optical materials with multiple strongly ionic cations5Mixed Anionic M(S/X)6 Polyhedra as Symmetry-Breaking Motifs to Enhance the Infrared Nonlinear Optical Response in Y–M–S–X (M = Ga, Ge; X = Cl, Br)5Edge-Sharing Tetrahedra Realizing Superior Birefringence and High Deep-Ultraviolet Transmittance in α-Be3(H2O)2(PO4)2 Crystal Synthesized by Mild Chemistry14Synthesis, Structure, and Properties of CuBiSeCl 2 : A Chalcohalide Material with Low Thermal Conductivity20An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution33An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution1A Rare Earth Chalcogenide Nonlinear Optical Crystal KLaGeS4: Achieving Good Balance among Band Gap, Second Harmonic Generation Effect, and Birefringence12Sb2O2SeO3 and Sb2O(SeO3)2: Two-Layered Antimony(III) Selenites with Enhanced Birefringence10On the Pb2HgO2Cl2 structure type: Synthesis and crystal structure of a new representative, Pb2CdO2Br2, and electronic structure and chemical bonding in the whole Pb2MO2X2 (M=Cd, Hg; X=Cl, Br) family1Pb2TeV2O10: A Lead Vanadate Tellurate with Wide Mid-IR Transparency and Large Birefringence Induced by Multiple Birefringence-Active Groups11First-principles study of three isomers of the large birefringent crystal Sb4O4F4: electronic structure and optical properties0Design of High‐Performance Infrared Nonlinear Optical PAs 3 S 3 with Perfectly Aligned Polar Molecular Cage via a Bipolar‐Axis‐Symmetry Coupling Strategy16Design of High‐Performance Infrared Nonlinear Optical PAs 3 S 3 with Perfectly Aligned Polar Molecular Cage via a Bipolar‐Axis‐Symmetry Coupling Strategy83Pb 8 O 7 I 2 ·2CsI: the salt-inclusion strategy enriches the structural chemistry in lead oxyhalides1Cd 5 Te 4 O 12 X 2 (X = Cl, Br, I): a new oxyhalide family with [CdO 4 X] mixed anionic units and adjustable optical properties4Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18M 3 MoO 4 (HCO 3 ) (M = Rb and Cs): cation-tuned synthesis of two noncentrosymmetric molybdate-carbonates with isolated [MoO 4 ] and [HCO 3 ] groups0(NH 4 ) 2 Cd 2 Cl 3 F 3 and (NH 4 ) 2 Cd 2 Br 3 F 3 : The First Fluoride‐Containing d 10 Metal Mixed Halides Exhibiting Superior Ultraviolet Nonlinear Optical Properties28Strong Second‐Harmonic Generation Responses in Salt‐Inclusion Oxychalcogenides Enabled by the Highly Distorted Polyhedra with Mixed‐Anions4Impact of Microstructural Units Configuration and Arrangement on Phase-Matching in Nonlinear Optical KGa5Se8 Crystals9Nonlinear Optical Effects Modulated by Distinctive Monovalent Cations with Lone Electron Pairs in AGaI 4 (A = Ga + , In + )4pH‐Dependent Switching Between Nonlinear‐Optical‐Active Nitrate‐Based Supramolecular Polymorphs27pH‐Dependent Switching Between Nonlinear‐Optical‐Active Nitrate‐Based Supramolecular Polymorphs2Oxygen‐Substitution Induced High‐Performance Nonlinear Optical Properties: Witnessed by the First Quaternary Oxythiostannate12Halogen-Driven Structural Engineering in Tellurium Oxyhalides: Enhanced SHG Response and Broad Optical Transparency6Synergistic Machine Learning Guided Discovery of ABa 3 (BSe 3 ) 2 X (A = Rb, Cs; X = Cl, Br, I): A Promising Family as Property‐Balanced IR Functional Materials10From AgHgI(SO4) to AgHg3I3.2Cl1.8(SO4): Symmetry Breaking of the Belousovite‐Type Topology by Mixed Halides to Achieve Strong Nonlinear Optical Effect14Recent progress in structural design strategies of high-birefringence optical crystals54

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  34. Noncentrosymmetric chalcohalide K2Ba3Ge3S9Cl2: A new nonlinear optical material with remarkable laser-induced damage threshold

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  35. Complex coordinated functional groups: A great genes for nonlinear optical materials

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  36. Second-Harmonic-Generation-Active Oxyhalides: CuSb2O3X (X = Cl, Br)

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  37. [ASr 4 Cl][Ge 3 S 10 ] (A = Na, K) and [KBa 4 Cl][Ge 3 S 10 ]: new salt-inclusion infrared nonlinear optical crystals with zero-dimensional [Ge 3 S 9 ] clusters

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  38. An 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 ] polyhedra

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  39. APb 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 polyhedra

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  40. Band gap modulation and nonlinear optical properties of quaternary tellurates Li 2 GeTeO 6

    Dalton Transactions · 2022-01-01

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  41. Inducing large birefringence by enhancing asymmetric electron distribution of Y–O polyhedra

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  42. Metal oxyhalides: an emerging family of nonlinear optical materials

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  43. Pb 3 SBrI 3 : the first Pb-based chalcohalide with multiple halogens features a unique two-dimensional structure composed of diverse Pb-centered polyhedra

    Dalton Transactions · 2022-01-01

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  44. Rational design of a promising oxychalcogenide infrared nonlinear optical crystal

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  45. Tellurate polymorphs with high-performance nonlinear optical switch property and wide mid-IR transparency

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  46. Lead Tellurite Crystals BaPbTe2O6 and PbVTeO5F with Large Nonlinear-/Linear-Optical Responses due to Active Lone Pairs and Distorted Octahedra

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  47. Pb 4 SeBr 6 : A Congruently Melting Mid‐Infrared Nonlinear Optical Material with Excellent Comprehensive Performance

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  48. Infrared nonlinear optical performances of a new sulfide β-PbGa2S4

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  49. Novel layered heterobimetallic fluorides with large optical band gaps

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  50. NaGa3Se5: An Infrared Nonlinear Optical Material with Balanced Performance Contributed by Complex {[Ga3Se5]−}∞ Anionic Network

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