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RESEARCH PAPER · Chemistry of Materials · 2017

Superpolyhedron-Built Second Harmonic Generation Materials Exhibit Large Mid-Infrared Conversion Efficiencies and High Laser-Induced Damage Thresholds

Shu‐Fang Li, Xiao‐Ming Jiang, Bin‐Wen Liu, Dong Yan, Chensheng Lin, Hui‐Yi Zeng, Guo‐Cong Guo

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Superpolyhedron-Built Second Harmonic Generation Materials Exhibit Large Mid-Infrared Conversion Efficiencies and High Laser-Induced Damage ThresholdsOriginalA series of pentanary inorganic supramolecular sulfides (A 3 X)[MB 12 (MS 4 ) 3 ] (A = K, Cs; X = Cl, Br, I; M = Ga, In, Gd) featuring B 12 S 12 clusters54Two excellent phase-matchable infrared nonlinear optical materials based on 3D diamond-like frameworks: RbGaSn 2 Se 6 and RbInSn 2 Se 639Mid-Infrared Nonlinear Optical Materials Based on Metal Chalcogenides: Structure–Property Relationship338Pb0.65Mn2.85Ga3S8 and Pb0.72Mn2.84Ga2.95Se8: Two Quaternary Metal Chalcognides with Open-Tunnel-Framework Structures Displaying Intense Second Harmonic Generation Responses and Interesting Magnetic Properties17Hg-Based Infrared Nonlinear Optical Material KHg4Ga5Se12 Exhibits Good Phase-Matchability and Exceptional Second Harmonic Generation Response101New Compressed Chalcopyrite-like Li2BaMIVQ4 (MIV = Ge, Sn; Q = S, Se): Promising Infrared Nonlinear Optical Materials245Large Second-Harmonic Generation Responses Achieved by the Dimeric [Ge2Se4(μ-Se2)]4– Functional Motif in Polar Polyselenides A4Ge4Se12 (A = Rb, Cs)49Experimental and theoretical studies on the NLO properties of two quaternary non-centrosymmetric chalcogenides: BaAg 2 GeS 4 and BaAg 2 SnS 468Na 6 Zn 3 MIII2Q 9 (M III = Ga, In; Q = S, Se): four new supertetrahedron-layered chalcogenides with unprecedented vertex-sharing T 3 -clusters and desirable photoluminescence performances31New strategy for designing promising mid-infrared nonlinear optical materials: narrowing the band gap for large nonlinear optical efficiencies and reducing the thermal effect for a high laser-induced damage threshold142Remarkable multimember-ring configurations in a new family of Na 7 M II Sb 5 S 12 (M II = Zn, Cd, Hg) exhibiting various three-dimensional tunnel structures25Strong Infrared Nonlinear Optical Efficiency and High Laser Damage Threshold Realized in Quaternary Alkali Metal Sulfides Na2Ga2MS6 (M = Ge, Sn) Containing Mixed Nonlinear Optically Active Motifs48Zn 3 P 2 S 8 : A Promising Infrared Nonlinear-Optical Material with Excellent Overall Properties70Adduct-Type IR Nonlinear-Optical Crystal SbI 3 ·(S 8 ) 3 with a Large Second-Harmonic Generation and a High Laser-Induced Damage Threshold59Second-order nonlinear optical properties of CuGa In1-Se2 (x = 0.54): Experimental and theoretical investigations4Cu2EuMQ4 (M = Si, Ge; Q = S, Se): Syntheses, structure study and physical properties determination26Recent progress on new infrared nonlinear optical materials with application prospect133BaMnSnS 4 and BaCdGeS 4 : infrared nonlinear optical sulfides containing highly distorted motifs with centers of moderate electronegativity48Li 2 ZnGeS 4 : a promising diamond-like infrared nonlinear optical material with high laser damage threshold and outstanding second-harmonic generation response43Balanced Second-Order Nonlinear Optical Properties of Adducts CHI3·(S8)3 and AsI3·(S8)3: A Systematic Survey48Large Second Harmonic Generation (SHG) Effect and High Laser‐Induced Damage Threshold (LIDT) Observed Coexisting in Gallium Selenide188Large Second Harmonic Generation (SHG) Effect and High Laser‐Induced Damage Threshold (LIDT) Observed Coexisting in Gallium Selenide48Synthesis, Structure, and Characterization of Two Mixed-Cation Quaternary Chalcogenides K2BaSnQ4 (Q = S, Se)19Mixed-Anion Inorganic Compounds: A Favorable Candidate for Infrared Nonlinear Optical Materials140Li4HgSn2Se7: The First Second-Order Nonlinear Optical-Active Selenide in the I4–II–IV2–VI7 Diamond-like Family32LiBa2MIIIQ4 (MIII = Al, Ga, In; Q = S, Se): A Series of Metal Chalcogenides with a Structural Transition12A highly distorted HgS 4 tetrahedron-induced moderate second-harmonic generation response of EuHgGeS 462Ba 6 In 6 Zn 4 Se 19 : a high performance infrared nonlinear optical crystal with [InSe 3 ] 3− trigonal planar functional motifs22Mixed-metal thiophosphate CuCd 3 PS 6 : an infrared nonlinear optical material activated by its three-in-one tetrahedra-stacking architecture33Infrared Nonlinear Optical Polymorphs α- and β-SrCu 2 SnS 4 Exhibiting Large Second Harmonic Generation Responses with Requisite Phase-Matching Behavior44Lead 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 Materials55A2SnS5: A Structural Incommensurate Modulation Exhibiting Strong Second‐Harmonic Generation and a High Laser‐Induced Damage Threshold (A=Ba, Sr)30A2SnS5: A Structural Incommensurate Modulation Exhibiting Strong Second‐Harmonic Generation and a High Laser‐Induced Damage Threshold (A=Ba, Sr)86Second-Order Nonlinear-Optical-Active Selenide Borate YSeBO2: Featuring a [YSeBO2]n Planar Belt39Inherent laws between tetrahedral arrangement pattern and optical performance in tetrahedron-based mid-infrared nonlinear optical materials131Second-order nonlinear optical-active selenide borate Zn8Se2(BO2)12: Experimental and theoretical analysis9Chalcophosphates: A Treasure House of Infrared Nonlinear Optical Materials75AMnAs3S6 (A = Cs, Rb): Phase-Matchable Infrared Nonlinear Optical Functional Motif [As3S6]3– Obtained via Surfactant–Thermal Method32Phase Matching, Strong Frequency Doubling, and Outstanding Laser-Induced Damage Threshold in the Biaxial, Quaternary Diamond-like Semiconductor Li 4 CdSn 2 S 779Investigation of the second-order nonlinear optical property of Sr6Sb6S173Cu 4 MnGe 2 S 7 and Cu 2 MnGeS 4 : two polar thiogermanates exhibiting second harmonic generation in the infrared and structures derived from hexagonal diamond22Design and synthesis of Ba 3 SiSe 5 with suitable birefringence modulated via M IV atoms in the Ba–M IV –Q (M IV = Si, Ge; Q = S, Se) system3Heterovalent cations substitution to design asymmetric chalcogenides with promising nonlinear optical performances44Synthesis, crystal structure and physical properties of a new chalcogenides Rb3Ga3Ge7S208Second-order nonlinear optical and photoelectric properties of Zn4B6O12S20A Series of Pentanary Salt-Inclusion Chalcogenoborates Containing a B12Q12 (Q = S, Se) Cluster Exhibiting a Kleinman-Forbidden Frequency-Doubling Effect25Introduction of Li into Ag-Based Noncentrosymmetric Sulfides for High-Performance Infrared Nonlinear Optical Materials40Three-in-One Strategy Constructing a Series of Hybrid Tetrahedral Motif-Based Selenides with Balanced Second-Order Nonlinear Optical Performance12Inorganic Chalcogenides: From Zero‐Dimensional Clusters to Three‐Dimensional Frameworks5AZn4Ga5Se12 (A = K, Rb, or Cs): Infrared Nonlinear Optical Materials with Simultaneous Large Second Harmonic Generation Responses and High Laser-Induced Damage Thresholds34Stepwise Li Substitution Induced Structure Evolution and Improved Nonlinear Optical Performance for Diamond-like Sulfides28SnPQ3 (Q = S, Se, S/Se): A Series of Lone-Pair Cationic Chalcogenophosphates Exhibiting Balanced NLO Activity Originating from SnQ8 Units49Helical {[HgS]} n Chain-Induced Balanced Nonlinear-Optical Performance for Trigonal Mercury Sulfide29Noncentrosymmetric chalcohalide K2Ba3Ge3S9Cl2: A new nonlinear optical material with remarkable laser-induced damage threshold17Structural Chemistry and Excellent Nonlinear Optical Properties of a Series of Ternary Selenides GaxIn2–xSe322Noncentrosymmetric (KBa0.5)In2Se4 and (K0.58Ba0.71)(Ga0.89In1.11)Se4 derived from centrosymmetric BaIn2Se4 via partial cation substitution: structural chemistry and nonlinear optical activity9Sn7Br10S2: The First Ternary Halogen‐Rich Chalcohalide Exhibiting a Chiral Structure and Pronounced Nonlinear Optical Properties24Sn7Br10S2: The First Ternary Halogen‐Rich Chalcohalide Exhibiting a Chiral Structure and Pronounced Nonlinear Optical Properties146Phase Matchability Transformation in the Infrared Nonlinear Optical Materials with Diamond‐Like Frameworks63AAg 3 Ga 8 Se 14 (A = Rb, Cs): second-harmonic generation responses realized through the parallel arrangement of AgSe 4 and GaSe 4 tetrahedrons5Symmetry breaking of A 3 M 2 X 9 -type perovskite derivatives induced by polar quaternary ammonium cations: achieving efficient nonlinear optical properties28Optimizing the Nonlinear Optical Performance of an A-N-M-Q (A: Alkali Metal; N: d10 Metal; M: Main Group Metal; Q: Chalcogen) System44Infrared nonlinear optical performances of a new sulfide β-PbGa2S415Material research from the viewpoint of functional motifs103NaGa3Se5: An Infrared Nonlinear Optical Material with Balanced Performance Contributed by Complex {[Ga3Se5]−}∞ Anionic Network14Cation Regulation to Investigate the Chalcogenide Borate RE6Nb2MgSB8O26 (RE = La–Nd) Family12First Investigation of Nonlinear Optical Oxychalcogenide with Three‐Dimensional Anionic Framework and Special Windmill‐Like Functional Motifs †28A comprehensive review on metal chalcogenides with three-dimensional frameworks for infrared nonlinear optical applications115Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance29AIn 3 Si 4 P 9 (A = Ca, Sr): quaternary phosphides with double-helix structures exhibiting high laser-induced damage thresholds19d6versus d10, Which Is Better for Second Harmonic Generation Susceptibility? A Case Study of K2TGe3Ch8 (T = Fe, Cd; Ch = S, Se)18Quasi-linear CuX 2 (X = Cl, Br) motif-built hybrid copper halides realizing encouraging nonlinear optical activities28Structure and optical property evolution in PbM(PO 4 )X (M = Zn, Sn; X = halogen): SHG effect and birefringence21LnLiSiS4 (Ln = La and Ce): Promising infrared nonlinear optical materials designed by aliovalent substitution from SrCdSiS437Glassy and crystalline sodium ternary chalcogenide materials in the Na–As–Se system: Synthesis, properties and relation to crystallization2The compatibly large nonlinear optical effect and high laser-induced damage threshold in a thiophosphate CsInP2S7 constructed with [P2S7]4- and [InS6]9-15Data driven enhancement of mid-infrared non-linear optical properties of quaternary and ternary chalcogenides6Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65“Three‐in‐One”: A New Hg‐Based Selenide Hg 7 P 2 Se 12 Exhibiting Wide Infrared Transparency Range and Strong Nonlinear Optical Effect80(C 13 N 3 H 14 ) 2 MBr 4 (M = Zn, Cd): two novel hybrid metal halides with balanced integrated nonlinear optical performance31Cation and anion co-partial substitution induced centrosymmetric to noncentrosymmetric structural transformation to construct nonlinear-optical rare-earth oxythiogermanates13A Study on the Surface Quality and Damage Properties of Single-Crystal Silicon Using Different Post-Treatment Processes5Polysubstitution Induced Centrosymmetric-to-Noncentrosymmetric Structural Transformation and Nonlinear-Optical Behavior: The Case of Na0.45Ag0.55Ga3Se52Design of Pentanary Mixed-Chalcogenides Ag2In2SiS6–xSex (x = 1, 2) Based on the Bucket Effect: Local Structural Difference and High-Performance Nonlinear-Optical Properties Realized by Partial Congener Substitution5[Rb3BaCl][In8Se14]: Compressed chalcopyrite-type selenide achieved by polycationic substitution strategy toward excellent nonlinear optical property18K2HgGe3Se8: A Quaternary Hg-Based Selenide with Nonlinear Optical Properties6Synthesis, Optical, and Magnetic Properties of the Mixed Chalcogenide Semiconductor Series Eu(II)2SiSexS4-x, Prepared via the Flux-Assisted Boron Chalcogen Mixture Method4Alkali triel chalcogenide nanocrystals: a molecular reactivity approach to ternary phase selectivity2Non-centrosymmetric structures designed rationally via a “dimensionality addition” strategy toward the promising nonlinear optical family [A–X][In–Se] (A = K/Ba and Rb/Ba; X = Cl and Br)13Expanding the Spectral Range in T2‐Supertetrahedral Nonlinear Optical Chalcogenides via Incorporating Inorganic Polycations4Expanding the Spectral Range in T2‐Supertetrahedral Nonlinear Optical Chalcogenides via Incorporating Inorganic Polycations29NbGa 2 S 4 (S 2 ): A Rare Linear [S 2 ] 2− Coordination to Niobium Resulting in Simultaneously Large SHG Effect and Giant Birefringence20NbGa 2 S 4 (S 2 ): A Rare Linear [S 2 ] 2− Coordination to Niobium Resulting in Simultaneously Large SHG Effect and Giant Birefringence6AlGaSe3: Tuning Stability via Partial Cation Substitution and Achieving a Nonlinear Optical Property Leap6Polyhedral replacement-guided design of Ce3MnGaSe7 featuring strong second-harmonic genera-tion and high laser-induced damage threshold0单晶硅光学元件缺陷检测技术研究进展综述(特邀)0Heterovalent Coexistence‐Driven Symmetry Breaking and Dimensional Evolution: Designing Polar Heart‐Shaped Channels for Exceptional MFIR Nonlinear Optics5Salt-Inclusion Rare-Earth Chalcogenides: Exploring Infrared Nonlinear Optical Crystals via a Guest-Framework Modulation Strategy0Review of defect detection technologies for single-crystal silicon optical components0AgEuPS4: Unlocking the Centrosymmetric Shackle of Rare-Earth Thiophosphates via Microscopic Distortion Cascading for Enhanced Second-Harmonic Generation Response1

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  7. Large Second-Harmonic Generation Responses Achieved by the Dimeric [Ge2Se4(μ-Se2)]4– Functional Motif in Polar Polyselenides A4Ge4Se12 (A = Rb, Cs)

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  9. Na 6 Zn 3 MIII2Q 9 (M III = Ga, In; Q = S, Se): four new supertetrahedron-layered chalcogenides with unprecedented vertex-sharing T 3 -clusters and desirable photoluminescence performances

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  15. Second-order nonlinear optical properties of CuGa In1-Se2 (x = 0.54): Experimental and theoretical investigations

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  44. Heterovalent cations substitution to design asymmetric chalcogenides with promising nonlinear optical performances

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