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RESEARCH PAPER · Journal of the American Chemical Society · 2020

Designing a Deep-UV Nonlinear Optical Fluorooxosilicophosphate

Qingran Ding, Xiaomeng Liu, Sangen Zhao, Yusong Wang, Yanqiang Li, Lina Li, Shuai Liu, Zheshuai Lin, Maochun Hong, Junhua Luo

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Designing a Deep-UV Nonlinear Optical FluorooxosilicophosphateOriginalK 4 (PO 2 F 2 ) 2 (S 2 O 7 ): first fluorooxophosphorsulfate with mixed-anion [S 2 O 7 ] 2− and [PO 2 F 2 ] − groups14Second-order nonlinear optical materials with a benzene-like conjugated π system49Multimodal Structure Solution with 19F NMR Crystallography of Spin Singlet Molybdenum Oxyfluorides14Exploring impurity phases derived from the introduction of vanadium ions in yttrium gallium garnet3Pb 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 Properties29Cs3B3O3F6 with a Deep-Ultraviolet Cutoff Edge and a Suitable Birefringence as the Potential Zero-Order Waveplate Material31From silicates to oxonitridosilicates: improving optical anisotropy for phase-matching as ultraviolet nonlinear optical materials47Ba 3 [Al(PO 4 ) 3 ]: rational design of a promising deep-UV transparent SHG crystal with balanced overall performance originating from the condensation of quartz-type [Al(PO 4 ) 4 ] 9− units16Competing hydrogen-bonding interactions in a high- T c organic molecular-ionic crystal with evident nonlinear optical response2Computationally assisted multistage design and prediction driving the discovery of deep-ultraviolet nonlinear optical materials41From centrosymmetric to noncentrosymmetric: effect of the cation on the crystal structures and birefringence values of (NH 4 ) n−2 AE(PO 2 F 2 ) n (AE = Mg, Sr and Ba; n = 2, 3 and 4)9From thiophosphate to chalcohalide: mixed-anion AgS x Cl y ligands concurrently enhancing nonlinear optical effects and laser-damage threshold10Li 5 Cs(SO 4 ) 3 : a potential zero-order wave plate material with short deep-ultraviolet cutoff edge20M 6 PS 5 X (M = Ag, Cu; X = Cl, Br) chalcohalides exhibiting strong nonlinear optical responses and high laser damage resistances9Na 4 SnS 4 and Na 4 SnSe 4 exhibiting multifunctional physicochemical performances as potential infrared nonlinear optical crystals and sodium ion conductors27Recent advances of oxyfluorides for nonlinear optical applications69The Balance of Deep-Ultraviolet Transparency and Large Second Harmonic Generation Response in a Silicate Crystal0To improve the key properties of nonlinear optical crystals assembled with tetrahedral functional building units46M(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 Birefringence27Prediction 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 Deep‐UV Nonlinear Optical Borosulfate with Incommensurate Modulations71A Deep‐UV Nonlinear Optical Borosulfate with Incommensurate Modulations13Te(CS(NH2)2)4SO4·2H2O: A Three-in-One Semiorganic Nonlinear Optical Crystal with an Unusual Quadrilateral (TeS4)6– Chromophore14Steric Group Design for Enhancement of Optical Nonlinearity in Isoxazolone-Based Crystals and Terahertz-Wave Generation19Unique Unilateral-Chelated Mode-Induced d–p−π Interaction Enhances Second-Harmonic Generation Response in New Ln3LiMS7 Family41Insights into varying dimension structures for deep-UV optical crystals NaBa2Al(P2O7)2 and NaBaAl(PO4)2 constructed separately from unique [Al(P2O7)2] chains and [Al(PO4)2] layers6Exploring Deep-UV Nonlinear Optical Materials with Enhanced Second Harmonic Generation Response and Birefringence in Fluoroaluminoborate Crystals69Heterobimetallic Cluster‐Based Coordination Polymers: Assembly, Structures and Third‐Order Nonlinear Optical Properties4Tetrafluoroborate-Monofluorophosphate (NH4)3[PO3F][BF4]: First Member of Oxyfluoride with B–F and P–F Bonds16Non-π-Conjugated Deep-Ultraviolet Nonlinear Optical Crystal K2Zn3(SO4)(HSO4)2F4372D van der Waals Layered [C(NH2)3]2SO3S Exhibits Desirable UV Nonlinear-Optical Trade-Off47La 3 Ga 3 Ge 2 S 3 O 10 : An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap Engineering63La3Ga3Ge2S3O10: An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap Engineering18Cd3(PO4)(TePO6): A Novel Cadmium Tellurite‐Phosphate featuring a {[TePO6]3−}∞ Chain15A New Nonlinear Optical Material with N(CN)2− Anion2Two molybdenyl carbonates with different dimensional structures exhibiting huge differences in band gaps7Complex coordinated functional groups: A great genes for nonlinear optical materials64Pushing KTiOPO4-like Nonlinear Optical Sulfates into the Deep-Ultraviolet Spectral Region19Recent Development of Non-π-Conjugated Deep Ultraviolet Nonlinear Optical Materials106(C 3 N 6 H 7 ) 2 SiF 6 ·H 2 O: an ultraviolet birefringent crystal exceeding the intrinsic energy gap of an organic reagent38(N 2 H 6 )[HPO 3 F] 2 : maximizing the optical anisotropy of deep-ultraviolet fluorophosphates33[C 3 N 6 H 7 ] 2 [B 3 O 3 F 4 (OH)]: a new hybrid birefringent crystal with strong optical anisotropy induced by mixed functional units85[C(NH 2 ) 3 ] 2 S 2 O 8 : combining delocalized and localized π-conjugate units to achieve strong optical anisotropy21Hexameric poly-fluoroberyllophosphate Na 4 Be 2 PO 4 F 5 with moderate birefringence and deep-ultraviolet transmission as a potential zero-order-waveplate crystal17KLi 2 CO 3 F: a beryllium-free KBBF-type deep-UV carbonate with an enhanced interlayer interaction and large birefringence20Large optical anisotropy differentiation induced by the anion-directed regulation of structures29Two host–guest grown ether supramolecules show switchable phase transition, dielectric and second-harmonic generation effect11Variable dimensionality of the anion framework in four new borophosphates and fluoroborophosphates with short cutoff edges13Review of Heteroleptic Tetrahedra as Birefringent or Nonlinear Optical Motifs17White‐Light Emission and Circularly Polarized Luminescence from a Chiral Copper(I) Coordination Polymer through Symmetry‐Breaking Crystallization13White‐Light Emission and Circularly Polarized Luminescence from a Chiral Copper(I) Coordination Polymer through Symmetry‐Breaking Crystallization77A crystalline photochromic metalloviologen compound with a chiral ligand: Synthetic strategy and SHG-photoswitching property1Balance of Deep-Ultraviolet Transparency and Large Second Harmonic Generation Response in a Silicate Crystal9Noncentrosymmetric Rare-Earth Borate Fluoride La2B5O9F3: A New Ultraviolet Nonlinear Optical Crystal with Enhanced Linear and Nonlinear Performance48Designing a deep-UV nonlinear optical monofluorophosphate22[C(NH2)3]2MoO2F4·H2O: Unique Chinese-Knot Structure Revealing Superior Nonlinear-Optical Properties19Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24Isoreticular Design of KTiOPO 4 -Like Deep-Ultraviolet Transparent Materials Exhibiting Strong Second-Harmonic Generation68SbHPO3F: 2D van der Waals Layered Phosphite Exhibiting Large Birefringence32Ag[SC(NH2)2]2F: A Laser Damage-Tolerant Infrared Nonlinear Optical Material9Local Polarity-Induced Assembly of Second-Order Nonlinear Optical Materials128LiRE(SO 4 ) 2 (RE = Y, Gd, Eu): noncentrosymmetric chiral rare-earth sulfates with very large band gaps21Rb 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 regulation13M(NH2SO3)2·xH2O (M = Ca, Pb, x = 0, 1, 4): Effect of Hydrogen Bonding on Structural Transformations and Second Harmonic Generation of Metal Sulfamates26Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25A lithium–scandium sulfate with second-harmonic generation response and deep-ultraviolet transparency7Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181Modulating optical performance by phase transition in a nonlinear optical material β-Li 2 RbBi(PO 4 ) 28Recent advances of inorganic phosphates with UV/DUV cutoff edge and large second harmonic response7Design Principles for Noncentrosymmetric Materials23Beyond π–π Stacking: Understanding Inversion Symmetry Breaking in Crystalline Racemates26Deep-ultraviolet (DUV) nonlinear optical (NLO) crystals: An application in photonic technologies29Enlargement of Bandgap and Birefringence in Nonlinear Optical Alkali‐Metal Sulfate Crystals by the Substitution of Asymmetrical Non‐π‐Conjugated Cation8(SO3CF3)−: A Non‐π‐Conjugated Motif for Nonlinear Optical Crystals Transparent into the Deep‐Ultraviolet Region23Stereochemically Active Lone-Pair Containing Metal Substitution in Polar Axis toward a Giant Phase-Matchable Optical Nonlinear Silicate Crystal Li 3 (OH)PbSiO 463Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction33Ultrashort Phase‐Matching Wavelength and Strong Second‐Harmonic Generation in Deep‐UV‐Transparent Oxyfluorides by Covalency Reduction3Na 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 Materials11Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence11Deep‐Ultraviolet Transparent Mixed Metal Sulfamates with Enhanced Nonlinear Optical Properties and Birefringence75Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals15Fluorination Strategy Towards Symmetry Breaking of Boron‐centered Tetrahedron for Poly‐fluorinated Optical Crystals70Fluorination strategy toward chemical and functional modification65Chemical perspectives on heteroanionic compounds: a potential playground for multiferroics7Designing excellent UV birefringent materials through the synergistic interaction of two highly distorted functional groups23Hydrated and fluorinated potassium scandium phosphates: topology symmetry analysis and structure prediction1Li 3 Na 7 B 4 P 6 O 26 : a new ultraviolet transparent congruently melting non-linear optical crystal3Strategically designed metal-free deep-ultraviolet birefringent crystals with superior optical properties18AX·(H2SeO3)n (A = K, Cs; X = Cl, Br; n = 1, 2): A Series of Ionic Cocrystals as Promising UV Birefringent Materials with Large Birefringence and Wide Band Gap20Centrosymmetric CaBaMF8 and Noncentrosymmetric Li2CaMF8 (M = Zr, Hf): Dimension Variation and Nonlinear Optical Activity Resulting from an Isovalent Cation Substitution-Oriented Design17Hg16O12(NO3)6F2(H2O): A Mercury-Rich Nitrate Oxyfluoride with Diverse Triple-Coordinated Mercury-Based Units That Exhibits an Unparalleled [(Hg16O12F2(H2O))6+]∞ Cationic Framework and a Large Birefringence12Combining rigid and deformable groups to construct a robust birefringent crystal for compact polarization components25Fluorine-driven materials design of novel deep-ultraviolet nonlinear optical crystal materials: Research progress and challenges6Ultraviolet Nonlinear Optical Single Crystals of A Three‐Dimensional Chiral Covalent Framework Containing Te−O−B−O Bonds3Ultraviolet Nonlinear Optical Single Crystals of A Three‐Dimensional Chiral Covalent Framework Containing Te−O−B−O Bonds19(C5H12N2S)Hg(NO3)2: A Mercury Nitrate Nonlinear Optical Crystal Motivated by Heteroatom Coordination Strategy9Screening Strategy Identifies an Overlooked Deep‐Ultraviolet Transparent Nonlinear Optical Crystal3Screening Strategy Identifies an Overlooked Deep‐Ultraviolet Transparent Nonlinear Optical Crystal45Promising Functional Structural Building Unit Trisulfimide (SO2N)33– and Its Contributions to Second Harmonic Generation and Birefringence1Two α‐SiO 2 ‐Related Deep‐Ultraviolet Phase‐Matchable Optical Nonlinear Beryllium Silicate Crystals Na 2 BeSiO 4 and Li 2 BeSiO 4 with Enhanced SHG Effect10From β-KB3O4F2 to α-KB3O4F2: Phase Transition-Directed Great Changes in Structure and Optical Anisotropy4Deep‐Ultraviolet Transparent Nonlinear Optical Phosphates: A New Alternative to Conventional Borates9Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances17Anionic modulation induces molecular polarity in a three-component crown ether system3Coordinated assembly of alkali and alkaline earth metals with the perfluorinated [AlF 6 ] group to design deep-ultraviolet zero-order waveplate materials2A HTO‐Type Nonlinear Optical Fluorophosphate with Ultrawide Bandgap16SnHPO4: A Layered Tin(II) Phosphate with Enhanced Birefringence51Polar [ NH ( CH2SO3 )2]2− Dimers Enable the First Promising Iminodimethanesulfonate with Nonlinear Optical Properties and Wide UV Transparency19Review of KBe2BO3F2-like second-order nonlinear optical materials and their structure-performance relationships13Promising UV/DUV nonlinear optical materials with X-membered (X = multiples of 6) rings in anhydrous inorganic borates20KF·[SO 2 (NH 2 ) 2 ]: the First Deep‐Ultraviolet Transparent Sulfonamide Fluoride Nonlinear Optical Crystal with Novel Cairo Pentagonal Structure13KF·[SO 2 (NH 2 ) 2 ]: the First Deep‐Ultraviolet Transparent Sulfonamide Fluoride Nonlinear Optical Crystal with Novel Cairo Pentagonal Structure5Ag(Te2O3)(PO4): The first Ag-containing phosphate-tellurite nonlinear optical crystal featuring novel zigzag layered structure0A[N(SO 2 NH 2 ) 2 ] (A = Na, K, Rb, and Cs): enhancing birefringence of non π-conjugated deep-ultraviolet crystals via novel dimeric disulfonamide [N(SO 2 NH 2 ) 2 ] − groups0Series of phosphate nonlinear optical materials containing active metal ions with short cut-off edges0From [C(NH2)3]2[Sn2(C2O4)3]·2H2O to [C(NH2)3]4[Sn(C2O4)2]2·H2O: Uneven-substitution-activated polar stannous oxalate with balanced bandgap and birefringence0Dimensionality Engineering of Fluorozirconium Phosphates for Deep-UV-Transparent Crystals with Enhanced Second-Harmonic Generation and Birefringence10Cation‐Dominated Second‐Order Nonlinear Optical Response Enabled by π‐Conjugated Guanidinium Derivatives5Cation‐Dominated Second‐Order Nonlinear Optical Response Enabled by π‐Conjugated Guanidinium Derivatives0Halogen-Substitution-Modulated Lone-Pair Orientation in Sb(H 2 PO 2 ) 2 X (X = Cl, F) for Enhanced UV Birefringence1Anion-Stabilized Incommensurate Modulation Enables Nonlinear Optical Response in Eu2SiO3.89N0.110Multidimensional Cation Modulation toward Phase-Matchable Nonlinear Optical Fluorides with Short UV Cutoff Edges0Borophosphate-based second-order nonlinear optical materials: Advances in structural diversity and optical performance0

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  1. K 4 (PO 2 F 2 ) 2 (S 2 O 7 ): first fluorooxophosphorsulfate with mixed-anion [S 2 O 7 ] 2− and [PO 2 F 2 ] − groups

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  2. Second-order nonlinear optical materials with a benzene-like conjugated π system

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  3. Multimodal Structure Solution with 19F NMR Crystallography of Spin Singlet Molybdenum Oxyfluorides

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  4. Exploring impurity phases derived from the introduction of vanadium ions in yttrium gallium garnet

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

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  7. Cs3B3O3F6 with a Deep-Ultraviolet Cutoff Edge and a Suitable Birefringence as the Potential Zero-Order Waveplate Material

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  8. From silicates to oxonitridosilicates: improving optical anisotropy for phase-matching as ultraviolet nonlinear optical materials

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  9. Ba 3 [Al(PO 4 ) 3 ]: rational design of a promising deep-UV transparent SHG crystal with balanced overall performance originating from the condensation of quartz-type [Al(PO 4 ) 4 ] 9− units

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  10. Competing hydrogen-bonding interactions in a high- T c organic molecular-ionic crystal with evident nonlinear optical response

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  11. Computationally assisted multistage design and prediction driving the discovery of deep-ultraviolet nonlinear optical materials

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  12. From centrosymmetric to noncentrosymmetric: effect of the cation on the crystal structures and birefringence values of (NH 4 ) n−2 AE(PO 2 F 2 ) n (AE = Mg, Sr and Ba; n = 2, 3 and 4)

    Dalton Transactions · 2021-01-01

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  13. From thiophosphate to chalcohalide: mixed-anion AgS x Cl y ligands concurrently enhancing nonlinear optical effects and laser-damage threshold

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  14. Li 5 Cs(SO 4 ) 3 : a potential zero-order wave plate material with short deep-ultraviolet cutoff edge

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  15. M 6 PS 5 X (M = Ag, Cu; X = Cl, Br) chalcohalides exhibiting strong nonlinear optical responses and high laser damage resistances

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  16. Na 4 SnS 4 and Na 4 SnSe 4 exhibiting multifunctional physicochemical performances as potential infrared nonlinear optical crystals and sodium ion conductors

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  17. Recent advances of oxyfluorides for nonlinear optical applications

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  18. The Balance of Deep-Ultraviolet Transparency and Large Second Harmonic Generation Response in a Silicate Crystal

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  19. To improve the key properties of nonlinear optical crystals assembled with tetrahedral functional building units

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  20. M(NH 2 SO 3 ) 2 (M=Sr, Ba): Two Deep‐Ultraviolet Transparent Sulfamates Exhibiting Strong Second Harmonic Generation Responses and Moderate Birefringence

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  21. M(NH 2 SO 3 ) 2 (M=Sr, Ba): Two Deep‐Ultraviolet Transparent Sulfamates Exhibiting Strong Second Harmonic Generation Responses and Moderate Birefringence

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  24. A Deep‐UV Nonlinear Optical Borosulfate with Incommensurate Modulations

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  26. Te(CS(NH2)2)4SO4·2H2O: A Three-in-One Semiorganic Nonlinear Optical Crystal with an Unusual Quadrilateral (TeS4)6– Chromophore

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  29. Insights into varying dimension structures for deep-UV optical crystals NaBa2Al(P2O7)2 and NaBaAl(PO4)2 constructed separately from unique [Al(P2O7)2] chains and [Al(PO4)2] layers

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  30. Exploring Deep-UV Nonlinear Optical Materials with Enhanced Second Harmonic Generation Response and Birefringence in Fluoroaluminoborate Crystals

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  31. Heterobimetallic Cluster‐Based Coordination Polymers: Assembly, Structures and Third‐Order Nonlinear Optical Properties

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  32. Tetrafluoroborate-Monofluorophosphate (NH4)3[PO3F][BF4]: First Member of Oxyfluoride with B–F and P–F Bonds

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  33. Non-π-Conjugated Deep-Ultraviolet Nonlinear Optical Crystal K2Zn3(SO4)(HSO4)2F4

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  34. 2D van der Waals Layered [C(NH2)3]2SO3S Exhibits Desirable UV Nonlinear-Optical Trade-Off

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  35. La 3 Ga 3 Ge 2 S 3 O 10 : An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap Engineering

    Angewandte Chemie International Edition · 2021-10-09

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  36. La3Ga3Ge2S3O10: An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap Engineering

    Angewandte Chemie · 2021-10-09

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  37. Cd3(PO4)(TePO6): A Novel Cadmium Tellurite‐Phosphate featuring a {[TePO6]3−}∞ Chain

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  38. A New Nonlinear Optical Material with N(CN)2− Anion

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  39. Two molybdenyl carbonates with different dimensional structures exhibiting huge differences in band gaps

    Inorganic Chemistry Frontiers · 2021-11-26

    Yunqiao Guo, Yalan Deng, Ting Zheng, Ling Huang, Daojiang Gao, Jian Bi, Guohong Zou

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

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    Weikang Wang, Dajiang Mei, Shaoguo Wen, Jian Wang, Yuandong Wu

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  41. Pushing KTiOPO4-like Nonlinear Optical Sulfates into the Deep-Ultraviolet Spectral Region

    Inorganic Chemistry · 2021-12-09

    Zhou Yang, Xiaomeng Liu, Zheshuai Lin, Yanqiang Li, Qingran Ding, Youchao Liu, Yangxin Chen, Sangen Zhao, Maochun Hong, Junhua Luo

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  42. Recent Development of Non-π-Conjugated Deep Ultraviolet Nonlinear Optical Materials

    Chemistry of Materials · 2021-12-29

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  43. (C 3 N 6 H 7 ) 2 SiF 6 ·H 2 O: an ultraviolet birefringent crystal exceeding the intrinsic energy gap of an organic reagent

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  44. (N 2 H 6 )[HPO 3 F] 2 : maximizing the optical anisotropy of deep-ultraviolet fluorophosphates

    Chemical Communications · 2022-01-01

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