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RESEARCH PAPER · Angewandte Chemie · 2018

SrB5O7F3 Functionalized with [B5O9F3]6− Chromophores: Accelerating the Rational Design of Deep‐Ultraviolet Nonlinear Optical Materials

Miriding Mutailipu, Min Zhang, Bingbing Zhang, Liying Wang, Zhihua Yang, Xin Hua Zhou, Shilie Pan

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SrB5O7F3 Functionalized with [B5O9F3]6− Chromophores: Accelerating the Rational Design of Deep‐Ultraviolet Nonlinear Optical MaterialsOriginalFrom LiB3O5 to NaRbB6O9F2: Fluorine‐Directed Evolution of Structural Chemistry33Designing Deep‐UV Birefringent Crystals by Cation Regulation57Fluorooxoborates: Ushering in a New Era of Deep Ultraviolet Nonlinear Optical Materials102Synthesis and Characterization of the First Tin Fluoride Borate Sn3[B3O7]F with Second Harmonic Generation Response28Fluoroborophosphates: a family of potential deep ultraviolet NLO materials43Lone‐Pair Enhanced Birefringence in an Alkaline‐Earth Metal Tin(II) Phosphate BaSn 2 (PO 4 ) 2130CsSbF 2 SO 4 : An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO 4 (KTP)‐type Structure87CsSbF2SO4: An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO4 (KTP)‐type Structure432[Ge2S5(S2)]4−, A NLO‐Active Unit Leading to an Asymmetric Structure Discovered in Li2Cs4Ge2S5(S2)Cl2: An Experimental and Theoretical study18RbB 11 O 16 (OH) 2 : First Hydroxyl Rubidium Borate with the B‐O 2D Layer Featuring Large Birefringence in the Rb‐B‐O‐H System5BaB 2 O 3 F 2 : A Barium Fluorooxoborate with a Unique [B 2 O 3 F] − Layer and Short Cutoff Edge38Dislocations that Decrease Size Mismatch within the Lattice Leading to Ultrawide Band Gap, Large Second‐Order Susceptibility, and High Nonlinear Optical Performance of AgGaS229Dislocations that Decrease Size Mismatch within the Lattice Leading to Ultrawide Band Gap, Large Second‐Order Susceptibility, and High Nonlinear Optical Performance of AgGaS2186β‐CsB9O14: A Triple‐Layered Borate with Edge‐Sharing BO4 Tetrahedra Exhibiting a Short Cutoff Edge and a Large Birefringence30Prediction of Fluorooxoborates with Colossal Second Harmonic Generation (SHG) Coefficients and Extremely Wide Band Gaps: Towards Modulating Properties by Tuning the BO 3 /BO 3 F Ratio in Layers99Prediction of Fluorooxoborates with Colossal Second Harmonic Generation (SHG) Coefficients and Extremely Wide Band Gaps: Towards Modulating Properties by Tuning the BO3/BO3F Ratio in Layers24K5B19O31: A Deep‐Ultraviolet Congruent Melting Compound6Sn2B5O9Cl: A Material with Large Birefringence Enhancement Activated Prepared via Alkaline‐Earth‐Metal Substitution by Tin255Sn2B5O9Cl: A Material with Large Birefringence Enhancement Activated Prepared via Alkaline‐Earth‐Metal Substitution by Tin33Giant Enhancement of Second Harmonic Generation Accompanied by the Structural Transformation of 7‐Fold to 8‐Fold Interpenetrated Metal–Organic Frameworks (MOFs)94Giant Enhancement of Second Harmonic Generation Accompanied by the Structural Transformation of 7‐Fold to 8‐Fold Interpenetrated Metal–Organic Frameworks (MOFs)35Histidinium‐Driven Chirality Control of Self‐Assembled Hybrid Molybdenum Oxyfluorides24An Uncommon Hypervalent Fluorooxosilicophosphate5Li[LiCs2Cl][Ga3S6]: A Nanoporous Framework of GaS4 Tetrahedra with Excellent Nonlinear Optical Performance172Li[LiCs2Cl][Ga3S6]: A Nanoporous Framework of GaS4 Tetrahedra with Excellent Nonlinear Optical Performance40Emergent Deep‐Ultraviolet Nonlinear Optical Candidates324Neue Kandidaten für die nichtlineare Optik im Tief‐UV‐Bereich43Selenite bromide nonlinear optical materials Pb 2 GaF 2 (SeO 3 ) 2 Br and Pb 2 NbO 2 (SeO 3 ) 2 Br: synthesis and characterization20A Promising Fluorooxoborate Framework with Flexibile Capability for Diverse Cations to Enhance the Second Harmonic Generation14Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials164Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials55Two Pyrophosphates with Large Birefringences and Second‐Harmonic Responses as Ultraviolet Nonlinear Optical Materials137Two Pyrophosphates with Large Birefringences and Second‐Harmonic Responses as Ultraviolet Nonlinear Optical Materials29K 2 Sb(P 2 O 7 )F: Cairo Pentagonal Layer with Bifunctional Genes Reveal Optical Performance297K2Sb(P2O7)F: Cairo Pentagonal Layer with Bifunctional Genes Reveal Optical Performance38Pb 18 O 8 Cl 15 I 5 : A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties165Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties29Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG Effects78Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG Effects19Recent Advances in Oxide‐based Nonlinear Optical Materials with Wide Infrared Transparency Beyond 6 μm38A2BBi2(PO4)2(P2O7) (A = K, Rb, B = Pb, Cd): the Effect of Cation Sizes on Structural Evolution10Ba3(BO3)(CO3)F: The First Borate Carbonate Fluoride Synthesized by the High‐Temperature Solution Method19Series of Crystals with Giant Optical Anisotropy: A Targeted Strategic Research19Series of Crystals with Giant Optical Anisotropy: A Targeted Strategic Research140Giant Optical Anisotropy in the UV‐Transparent 2D Nonlinear Optical Material Sc(IO 3 ) 2 (NO 3 )212Giant Optical Anisotropy in the UV‐Transparent 2D Nonlinear Optical Material Sc(IO 3 ) 2 (NO 3 )57KSnI 3 ⋅ H 2 O: A New Compound with One‐Dimensional SnI 3 Chains of Pyramidal SnI 5 Polyhedra2How Does Bridging Core Modification Alter the Photovoltaic Characteristics of Triphenylamine‐Based Hole Transport Materials? Theoretical Understanding and Prediction129A new rare-earth borate birefringent crystal with quasi-two-dimensional [BO 3 ] layers23M(NH 2 SO 3 ) 2 (M=Sr, Ba): Two Deep‐Ultraviolet Transparent Sulfamates Exhibiting Strong Second Harmonic Generation Responses and Moderate Birefringence142M(NH 2 SO 3 ) 2 (M=Sr, Ba): Two Deep‐Ultraviolet Transparent Sulfamates Exhibiting Strong Second Harmonic Generation Responses and Moderate Birefringence27New Polymorphism for Ba3Zn2(BO3)3F with Two Polymorphs Exhibiting Anomalous Phase Transition2Theoretical modification of C24 fullerene with single and multiple alkaline earth metal atoms for their potential use as NLO materials35M3B6O10NO3 (M = K, Rb): Two New Alkali Metal Borate‐Nitrates with Noncentrosymmetric Structures20A Deep‐UV Nonlinear Optical Borosulfate with Incommensurate Modulations71A Deep‐UV Nonlinear Optical Borosulfate with Incommensurate Modulations13RbMT3(BO3)2O3 (M=Ba, Sr; T=Al, Ga): New Double‐Layered Oxyborates Constructed from [BO3] Triangles and [TO4] Tetrahedra13Discovery of First Magnesium Fluorooxoborate with Stable Fluorine Terminated Framework for Deep‐UV Nonlinear Optical Application167Discovery of First Magnesium Fluorooxoborate with Stable Fluorine Terminated Framework for Deep‐UV Nonlinear Optical Application18Cs4B4O3F10: First Fluorooxoborate with [BF4] Involving Heteroanionic Units and Extremely Low Melting Point18Fluorine‐Driven Enhancement of Birefringence in the Fluorooxosulfate: A Deep Evaluation from a Joint Experimental and Computational Study139Na2Rb2SrB18O30 with [B9O19]11− fundamental building block consisting of three [B3O7]5− groups5Hydroxyfluorooxoborate 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 Crystals16Optoelectronic Evaluation, Chemical Potential Identification, Chemiparametric Oscillation Mapping, and Dielectric Efficiency Investigation of Organic NLO Crystal: 2‐Aminofluorene Using Computational Calculations1Theoretical Understanding and Role of Guest π-Bridges in Triphenylamine-Based Donor Materials for High-Performance Solar Cells67NaRbB3O4F3: A New Fluorooxoborate with a Short UV Cutoff Edge Enriching the Structural Chemistry of Borate7Sn2PO4I: An Excellent Birefringent Material with Giant Optical Anisotropy in Non π‐Conjugated Phosphate212Sn2PO4I: An Excellent Birefringent Material with Giant Optical Anisotropy in Non π‐Conjugated Phosphate22Strong SHG Responses in a Beryllium‐Free Deep‐UV‐Transparent Hydroxyborate via Covalent Bond Modification89Strong SHG Responses in a Beryllium‐Free Deep‐UV‐Transparent Hydroxyborate via Covalent Bond Modification9A New Nonlinear Optical Material with N(CN)2− Anion2From β‐Na2B6O10 to Na3AlB8O15 and Na3Al2B7O15: Structural Tuning of Anionic‐Group Architectures by Substitution of [BO4] by [AlO4] Covalent Tetrahedra10Growth of large size Triphenylphosphine Oxide 4-Nitrophenol (TP4N) single crystal by Sankaranarayanan–Ramasamy (SR) method for third order nonlinear optical applications8Na4B8O9F10: A Deep‐Ultraviolet Transparent Nonlinear Optical Fluorooxoborate with Unexpected Short Phase‐Matching Wavelength Induced by Optimized Chromatic Dispersion133Na4B8O9F10: A Deep‐Ultraviolet Transparent Nonlinear Optical Fluorooxoborate with Unexpected Short Phase‐Matching Wavelength Induced by Optimized Chromatic Dispersion13Hierarchical Modulation of Optical Anisotropy Driven by Metal Cation Polyhedra in Fluorooxoborates MIIB4O6F2 (MII=Be, Mg, Pb, Zn, Cd)6DFT study of alkali and alkaline earth metal-doped benzocryptand with remarkable NLO properties67Insights into the nonlinear optical (NLO) response of pure Aum (2 ≥ m ≤ 7) and copper-doped Au m – x Cu x clusters52KF·B(OH) 3 : a KBBF-type material with large birefringence and remarkable deep-ultraviolet transparency33Mg(H 2 O) 6 [(IO 2 (OH)) 2 (IO 3 )] 2 : a new iodate with a very large band gap and optical anisotropy13First-principles study of the influence of lone pair electrons and molecular groups on the birefringence of phosphate and fluorophosphate13Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)212Strong Nonlinearity Induced by Coaxial Alignment of Polar Chain and Dense [BO3] Units in CaZn2(BO3)2212Promising 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 Species83A Theoretical Perspective to Study the Optical Properties of Tetrafluoroborates4Double‐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] Clusters139From CsKTaF7 to CsNaTaF7: Alkali Metal Cations Regulation to Generate SHG Activity**22The electronic structures and nonlinear optical properties of Alkali and Alkali earth metal atoms doped C6H6Cl6: A density functional theoretical study0The Alkaline-earthides based parallel-stacked dimer and trimer of Janus face C6H6F6 showing extremely large nonlinear optical responses13Li2PbB2O5: A Pyroborate with Large Birefringence Induced by the Synergistic Effect of Stereochemical Active Lone Pair Cations and π-Conjugated [B2O5] Groups14Ultrafast Dynamics and Strong Two-Photon Absorption Properties of Nonplanar β-Functionalized “Push–Pull” Copper Corroles with a Mixed Substituent Pattern32Aluminoborates as Nonlinear Optical Materials79Aluminoborates as Nonlinear Optical Materials14Polar Phosphorus Chalcogenide Cage Molecules: Enhancement of Nonlinear Optical Properties in Adducts38Polar Phosphorus Chalcogenide Cage Molecules: Enhancement of Nonlinear Optical Properties in Adducts1SYNTHESIS AND CRYSTAL STRUCTURE OF TWO NEW TETRAFLUOROBORATE CRYSTALLOHYDRATES M(BF4)2·3H2O, M = Sr, Ba2Unbiased Screening of Novel Infrared Nonlinear Optical Materials with High Thermal Conductivity: Long‐neglected Nitrides and Popular Chalcogenides12Unbiased Screening of Novel Infrared Nonlinear Optical Materials with High Thermal Conductivity: Long‐neglected Nitrides and Popular Chalcogenides48Four New Sb‐based Orthophosphates: Cation Regulation to Investigate Diversified Structural Architecture1SrCl2·6H2O: An Alkaline-Earth-Metal Chloride Hexahydrate as Deep-Ultraviolet Nonlinear-Optical Crystal with the {[Sr(H2O)6]2+}∞ Cationic Framework8Heterologous Isomorphic Substitution Induces Optical Property Enhancement for Deep-UV Crystals: a Case in Rb[B3O3F2(OH)2]10Synthesis, Characterization, and DFT Study of Mono- and Di-Arylated Pyridine Derivatives4Ba 4 B 14 O 25 : A Deep Ultraviolet Transparent Nonlinear Optical Crystal with Strong Second Harmonic Generation Response Achieved by a Boron‐Rich Closed‐Loop Strategy12Halogen-assisted octet binding electrons construction of pnictogens towards wide-bandgap nonlinear optical pnictides17Ba 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 structure4Inhibiting lattice strain for highly stable and long‐life Li‐rich Mn‐based layered cathodes20Strong Second‐Harmonic Generation Responses in Salt‐Inclusion Oxychalcogenides Enabled by the Highly Distorted Polyhedra with Mixed‐Anions4An inorganic−organic hybrid KBBF-type zinc borate imidazole complex: A promising nonlinear-optical crystal4Structural Symmetry and Mixed‐anion Engineering in Halopnictides for Extraordinary Second‐Harmonic Generation6Structural Symmetry and Mixed‐anion Engineering in Halopnictides for Extraordinary Second‐Harmonic Generation3Achieving record-high birefringence in a 3D fluorozincoborate via coplanar alignment of π-conjugated [BO 3 ] units0Mechanism-driven disparities in H2S and PH3 emissions from calcium carbide hydrolysis: An atomic-scale investigation integrating DFT calculations and experimental validation0When Octahedra Learn to Be Prisms: Unlocking a Record Deep‑UV NLO Crystal0

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  1. From LiB3O5 to NaRbB6O9F2: Fluorine‐Directed Evolution of Structural Chemistry

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  2. Designing Deep‐UV Birefringent Crystals by Cation Regulation

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  3. Fluorooxoborates: Ushering in a New Era of Deep Ultraviolet Nonlinear Optical Materials

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  4. Synthesis and Characterization of the First Tin Fluoride Borate Sn3[B3O7]F with Second Harmonic Generation Response

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  5. Fluoroborophosphates: a family of potential deep ultraviolet NLO materials

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  6. Lone‐Pair Enhanced Birefringence in an Alkaline‐Earth Metal Tin(II) Phosphate BaSn 2 (PO 4 ) 2

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  7. CsSbF 2 SO 4 : An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO 4 (KTP)‐type Structure

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  8. CsSbF2SO4: An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO4 (KTP)‐type Structure

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  9. [Ge2S5(S2)]4−, A NLO‐Active Unit Leading to an Asymmetric Structure Discovered in Li2Cs4Ge2S5(S2)Cl2: An Experimental and Theoretical study

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  10. RbB 11 O 16 (OH) 2 : First Hydroxyl Rubidium Borate with the B‐O 2D Layer Featuring Large Birefringence in the Rb‐B‐O‐H System

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  11. BaB 2 O 3 F 2 : A Barium Fluorooxoborate with a Unique [B 2 O 3 F] − Layer and Short Cutoff Edge

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  12. Dislocations that Decrease Size Mismatch within the Lattice Leading to Ultrawide Band Gap, Large Second‐Order Susceptibility, and High Nonlinear Optical Performance of AgGaS2

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  13. Dislocations that Decrease Size Mismatch within the Lattice Leading to Ultrawide Band Gap, Large Second‐Order Susceptibility, and High Nonlinear Optical Performance of AgGaS2

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  14. β‐CsB9O14: A Triple‐Layered Borate with Edge‐Sharing BO4 Tetrahedra Exhibiting a Short Cutoff Edge and a Large Birefringence

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  15. Prediction of Fluorooxoborates with Colossal Second Harmonic Generation (SHG) Coefficients and Extremely Wide Band Gaps: Towards Modulating Properties by Tuning the BO 3 /BO 3 F Ratio in Layers

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  16. Prediction of Fluorooxoborates with Colossal Second Harmonic Generation (SHG) Coefficients and Extremely Wide Band Gaps: Towards Modulating Properties by Tuning the BO3/BO3F Ratio in Layers

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  17. K5B19O31: A Deep‐Ultraviolet Congruent Melting Compound

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  18. Sn2B5O9Cl: A Material with Large Birefringence Enhancement Activated Prepared via Alkaline‐Earth‐Metal Substitution by Tin

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  19. Sn2B5O9Cl: A Material with Large Birefringence Enhancement Activated Prepared via Alkaline‐Earth‐Metal Substitution by Tin

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  20. Giant Enhancement of Second Harmonic Generation Accompanied by the Structural Transformation of 7‐Fold to 8‐Fold Interpenetrated Metal–Organic Frameworks (MOFs)

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  23. An Uncommon Hypervalent Fluorooxosilicophosphate

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  24. Li[LiCs2Cl][Ga3S6]: A Nanoporous Framework of GaS4 Tetrahedra with Excellent Nonlinear Optical Performance

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  26. Emergent Deep‐Ultraviolet Nonlinear Optical Candidates

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  27. Neue Kandidaten für die nichtlineare Optik im Tief‐UV‐Bereich

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  28. Selenite bromide nonlinear optical materials Pb 2 GaF 2 (SeO 3 ) 2 Br and Pb 2 NbO 2 (SeO 3 ) 2 Br: synthesis and characterization

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  29. A Promising Fluorooxoborate Framework with Flexibile Capability for Diverse Cations to Enhance the Second Harmonic Generation

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  30. Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials

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  31. Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials

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  32. Two Pyrophosphates with Large Birefringences and Second‐Harmonic Responses as Ultraviolet Nonlinear Optical Materials

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  33. Two Pyrophosphates with Large Birefringences and Second‐Harmonic Responses as Ultraviolet Nonlinear Optical Materials

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  34. K 2 Sb(P 2 O 7 )F: Cairo Pentagonal Layer with Bifunctional Genes Reveal Optical Performance

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  35. K2Sb(P2O7)F: Cairo Pentagonal Layer with Bifunctional Genes Reveal Optical Performance

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

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  37. Pb18O8Cl15I5: A Polar Lead Mixed Oxyhalide with Unprecedented Architecture and Excellent Infrared Nonlinear Optical Properties

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  38. Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG Effects

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  39. Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG Effects

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  40. Recent Advances in Oxide‐based Nonlinear Optical Materials with Wide Infrared Transparency Beyond 6 μm

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  41. A2BBi2(PO4)2(P2O7) (A = K, Rb, B = Pb, Cd): the Effect of Cation Sizes on Structural Evolution

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  42. Ba3(BO3)(CO3)F: The First Borate Carbonate Fluoride Synthesized by the High‐Temperature Solution Method

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