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RESEARCH PAPER · Chemistry of Materials · 2020

Molecular Construction from AgGaS 2 to CuZnPS 4 : Defect-Induced Second Harmonic Generation Enhancement and Cosubstitution-Driven Band Gap Enlargement

Zhuang Li, Shengzi Zhang, Zhiwei Huang, Li‐Dong Zhao, Ece Uykur, Wenhao Xing, Zheshuai Lin, Jiyong Yao, Yicheng Wu

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Molecular Construction from AgGaS 2 to CuZnPS 4 : Defect-Induced Second Harmonic Generation Enhancement and Cosubstitution-Driven Band Gap EnlargementOriginalHgCuPS4: An Exceptional Infrared Nonlinear Optical Material with Defect Diamond-like Structure146Functional Chalcogenide Na2HgSn2Se6 and K2MnGe2Se6 Exhibiting Flexible Chain Structure and Intriguing Birefringence Tunability16Inherent laws between tetrahedral arrangement pattern and optical performance in tetrahedron-based mid-infrared nonlinear optical materials131Anionic 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 Effects19Chalcophosphates: A Treasure House of Infrared Nonlinear Optical Materials75Phase Matching, Strong Frequency Doubling, and Outstanding Laser-Induced Damage Threshold in the Biaxial, Quaternary Diamond-like Semiconductor Li 4 CdSn 2 S 779EuHgGeSe 4 and EuHgSnS 4 : Two Quaternary Eu-Based Infrared Nonlinear Optical Materials with Strong Second-Harmonic-Generation Responses55From AgGaS 2 to AgHgPS 4 : vacancy defects and highly distorted HgS 4 tetrahedra double-induced remarkable second-harmonic generation response68A series of M 3 PS 4 (M = Ag, Cu and Ag/Cu) thiophosphates with diamond-like structures exhibiting large second harmonic generation responses and moderate ion conductivities28Cu 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 diamond22Structural Modulation from Cu 3 PS 4 to Cu 5 Zn 0.5 P 2 S 8 : Single-Site Aliovalent-Substitution-Driven Second-Harmonic-Generation Enhancement28Cross‐Substitution Promoted Ultrawide Bandgap up to 4.5 eV in a 2D Semiconductor: Gallium Thiophosphate91From K[ZnBP2O8] to K[(Zn0.5Al0.5)2P2O8]: Substitution-Induced Microporous Zincoaluminophosphate with a Congruent-Melting Behavior5Mg 2 In 3 Si 2 P 7 : A Quaternary Diamond-like Phosphide Infrared Nonlinear Optical Material Derived from ZnGeP 2130Highly Distorted [HgS 4 ] Motif-Driven Structural Symmetry Degradation and Strengthened Second-Harmonic Generation Response in the Defect Diamond-Like Chalcogenide Hg 3 P 2 S 847Hg 3 P 2 S 8 : A New Promising Infrared Nonlinear Optical Material with a Large Second-Harmonic Generation and a High Laser-Induced Damage Threshold111Transition-metal-based chalcogenides: A rich source of infrared nonlinear optical materials184SnPQ3 (Q = S, Se, S/Se): A Series of Lone-Pair Cationic Chalcogenophosphates Exhibiting Balanced NLO Activity Originating from SnQ8 Units49Synthesis and Characterizations of Two Tellurides β-BaGa2Te4 and Ba5Ga2Ge3Te12 with Flexible Chain Structure16Polarimetric Image Sensor and Fermi Level Shifting Induced Multichannel Transition Based on 2D PdPS89Superior Infrared Nonlinear Optical Performance Achieved by Synergetic Functional Motif and Vacancy Site Modulations48Highly polarized [GeOTe 3 ] motif-driven structural order promotion and an enhanced second harmonic generation response in the new nonlinear optical oxytelluride Ba 3 Ge 2 O 4 Te 334Hg-based chalcogenides: An intriguing class of infrared nonlinear optical materials129Defect-induced nonlinearity in 2D nanoparticles5AAg 2 PS 4 (A = K, Na/K): the first-type of noncentrosymmetric alkali metal Ag-based thiophosphates exhibiting excellent second-order nonlinear optical performances21Ba 6 In 2 Ge 2 Te 15 : a THz birefringent material with an intriguing quasi-[Te 5 ] 4− chain possessing large optical anisotropy and an ultrawide transmission range7Bridging oxygen atoms in trigonal prism units driven strong second-harmonic-generation efficiency in Sr 3 Ge 2 O 4 Te 318Infrared nonlinear optical sulfide CsCd 4 In 5 S 12 exhibiting large second harmonic generation response16Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties69The synthesis and structure–property relation analysis of metal chalcohalide crystals Cs 2 InPS 4 X 2 (X = Cl, Br) with mixed anions6Wide band gap thiophosphates ASrPS 4 (A = Li, Na, K, Rb, Cs): cation size effect induced successive structural transformation13A new salt-inclusion chalcogenide exhibiting distinctive [Cd11In9S26]3− host framework and decent nonlinear optical performances16Two Nonlinear Optical Thiophosphates Cu 5 Hg 0.5 P 2 S 8 and AgHg 3 PS 6 Activated by Their Tetrahedra-Stacking Architecture12Two non-centrosymmetric scandium borate nonlinear optical crystals containing the B5O10 anion group26Toward the Rational Design of Mid‐Infrared Nonlinear Optical Materials with Targeted Properties via a Multi‐Level Data‐Driven Approach111Enhanced Second-Harmonic-Generation Efficiency and Birefringence in Melillite Oxychalcogenides Sr2MGe2OS6 (M = Mn, Zn, and Cd)97Second-Harmonic Generation-Positive Na 2 Ga 2 SiS 6 with a Broad Band Gap and a High Laser Damage Threshold14The Kurtz-Perry powder technique revisited: A case study on the importance of reference quality and broadband nonlinear optical measurements using LiInSe232BaSi7P10 and SrSi7P10: Two Infrared Nonlinear Optical Phosphides with T2 Supertetrahedra Exhibiting Strong Second‐Harmonic Generation Effects22Hg2P2S6: A layered mercury hexathiodiphosphate (IV) with large birefringence11Ag4SnGe2S7: A Noncentrosymmetric Chalcogenide in I4–II–IV2–VI7 System with Non-Diamond-Like Structure Featuring 1D ∞[SnGe2S8]6– Infinite Chain2Synthesis, Crystal and Electronic Structures, Nonlinear Optical Properties, and Magnetic Properties of Two Thiophosphates: KInP2S7 and KCrP2S79Ag-based chalcogenides and derivatives as promising infrared nonlinear optical materials90Breaking the bottleneck of simultaneously wide band gap and large nonlinear optical coefficient by a “pore reconstruction” strategy in a salt-inclusion chalcogenide26From BPS 4 to AB 3 P 2 S 10 (A = Na, K): cations inducing dimension reduction and bandgap enlargement7Na 6 Sn 3 P 4 S 16 : Sn( ii )-chelated PS 4 groups inspired an ultra-strong SHG response22Quaternary alkaline-earth metal thiophosphate SrAgPS 4 : syntheses, structures, and optical properties9Recent progress on sulfide infrared nonlinear optical materials with large SHG response and wide band gap26Revisiting two thiophosphate compounds constituting d 0 transition metal HfP 2 S 6 and d 10 transition metal α-Ag 4 P 2 S 6 as multifunctional materials for combining second harmonic generation response and photocurrent response12The Kurtz–Perry Powder Technique Revisited: A Study of the Effect of Reference Selection on Powder Second-Harmonic Generation Response20Phase Competition and Strong SHG Responses of the Li2MIIMIVSe4 Family: Atom Response Theory Predictions versus Experimental Results24Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance57Unravelling the regulating role of strain engineering on the phonon dispersion, mechanical behavior, and electronic transport properties of pentagonal PtTe2 monolayer19Defect diamond-like tellurides as infrared nonlinear optical materials with giant second-harmonic generation tensor14ACd 4 Ga 5 Te 12 (A = K, Rb, Cs): Tellurides with a Strong Nonlinear Optical Response and Purple Emission24AgMAsS3 (M = Cd, Hg): Double d10 Cation-Containing Thioarsenites(III) Exhibiting High Photocurrent Response and Moderate Second Harmonic Generation11The compatibly large nonlinear optical effect and high laser-induced damage threshold in a thiophosphate CsInP2S7 constructed with [P2S7]4- and [InS6]9-15Na 6 Mg 3 P 4 S 16 and RbMg 2 PS 4 Cl 2 : two Mg-based thiophosphates with ultrawide bandgaps resulting from [MgS 6 ] and [MgS x Cl 6− x ] octahedra4Noncentrosymmetric Na6Pb3P4S16 and Centrosymmetric K2MIIP2S6 (MII = Mg and Zn) Displaying Multiple Membered-Ring Configurations and Strong Optical Anisotropy10Partial substitution with a significant effect: coexistence of a wide band gap and large birefringence in the oxychalcogenide AEGe 2 O 4 Se (AE = Sr and Ba)17Second Harmonic Generation Control in 2D Layered Materials: Status and Outlook102KREP 2 S 6 (RE = Sm, Gd, Tb, Dy): A Series of Polar Rare-Earth Thiophosphates with High Laser-Induced Damage Thresholds and Moderate Nonlinear-Optical Responses Synergistically Contributed by Isolated P 2 S 6 Units and {[RE 2 S 15 ] 24– } ∞ Layers8Infrared nonlinear optical materials with multiple strongly ionic cations5Vacancy‐Induced Extraordinary Second Harmonic Generation Response for Diamond‐Like Cu3PS49Phase Matching of Infrared Nonlinear Optical Salt-Inclusion Chalcogenides Achieved by the Modulation of the Fractal Dimension of Anionic Motifs18Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials24Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials1A Congruent-Melt Infrared Nonlinear Optical Crystal Na4SrAs2S83Phase-Matching Second-Harmonic Generation and Enhanced Laser-Induced Damage Threshold Induced by Cs Substitution: Cu 3 PSe 4 vs Cs 2 CuP 3 S 94Tin chalcohalide Sn 11 (PS 4 ) 4 I 10 obtained from structural-template-oriented synthesis: exhibiting balanced infrared nonlinear optical performance6Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances18Ca 2 La(MS 4 )(BS 3 ) (M = Ge/Si and Sn/Si): high-performance infrared nonlinear optical materials designed using an atomic site co-occupancy strategy9Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18Partial congener substitution induced wide band gap witnessed in diamond-like chalcogenide ZnHg 2 P 2 S 8 and its second-order nonlinear optical properties3Phase transition engineering to break the symmetry of diamond-like chalcogenide for second-order nonlinear optics2新型非线性光学晶体和双折射晶体的研究进展（特邀）4AgGaS2 and Derivatives: Design, Synthesis, and Optical Properties10Assembly between diverse polycations and diamond-like anionic frameworks in salt-inclusion phosphides enables excellent nonlinear optical properties4Chalcophosphates: A plentiful source of infrared nonlinear optical materials42A new selenide semiconductor NaMn3Ga3Se8 with strong second-harmonic generation and significant luminescence property5Structural-disorder-induced enhancement of second-harmonic generation in bismuth-based perovskite-inspired materials7The Influence of Different Group Distortions on the Structure–Property Relationship of Alkali Metal Thiophosphate0Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation3ABCQ4型硫属化物红外非线性光学材料的构效关系（特邀）0Diamond-like Ag x Cu 3− x PS 4 ( x = 1 and 2) synthesized by the metal oxide–boron–chalcogen (MOBQ) routine: local high-entropy engineering for balanced infrared nonlinear optical performance1Inorganic Ge-based ferroelectric perovskites towards quasi-phase-matching in the infrared region0高性能硫属化物红外非线性光学材料构效关系（特邀）0Harnessing tetrahedral diversity: The path to superior diamond-like IR NLO crystals15Achieving phase matching in infrared nonlinear optical crystal Cd3ZnSiS6 via isovalent substitution from Cd4SiS60Defect Diamond‐Like d 10 Metal Indium Selenium With Strong Second‐Harmonic Generation and Enhanced Laser‐Induced Damage Threshold3Desert rose-like zinc-doped copper sulfide: a promising photoelectrode for efficient solar water splitting0First‐Principles Investigation of the Structural, Electronic, Optical, Elastic, and Thermal Properties of Defect Diamond‐Like Hg 3 P 2 S 80AVP2S7 (A = K, Rb): Dual-Optimized Infrared Nonlinear Optical Thiophosphates via Heterovalent-Substitution-Driven Symmetry Breaking and Reinforced Interlayer Interactions0Variation of Tetrahedrons and Cations Regulates LIDTs in 3D‐DL Structure MIR‐NLO Crystals0NaGa2PS6: A Noncentrosymmetric Thiophosphate with Wide Band Gap and High Laser-Induced Damage Threshold0Vacancy-Driven Tetrahedral Distortion in Defect Diamond-Like Selenides for Exceptional Second-Order Nonlinearity0

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  2. Functional Chalcogenide Na2HgSn2Se6 and K2MnGe2Se6 Exhibiting Flexible Chain Structure and Intriguing Birefringence Tunability

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  6. Chalcophosphates: A Treasure House of Infrared Nonlinear Optical Materials

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  7. Phase Matching, Strong Frequency Doubling, and Outstanding Laser-Induced Damage Threshold in the Biaxial, Quaternary Diamond-like Semiconductor Li 4 CdSn 2 S 7

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  8. EuHgGeSe 4 and EuHgSnS 4 : Two Quaternary Eu-Based Infrared Nonlinear Optical Materials with Strong Second-Harmonic-Generation Responses

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  9. From AgGaS 2 to AgHgPS 4 : vacancy defects and highly distorted HgS 4 tetrahedra double-induced remarkable second-harmonic generation response

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  10. A series of M 3 PS 4 (M = Ag, Cu and Ag/Cu) thiophosphates with diamond-like structures exhibiting large second harmonic generation responses and moderate ion conductivities

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  12. Structural Modulation from Cu 3 PS 4 to Cu 5 Zn 0.5 P 2 S 8 : Single-Site Aliovalent-Substitution-Driven Second-Harmonic-Generation Enhancement

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  13. Cross‐Substitution Promoted Ultrawide Bandgap up to 4.5 eV in a 2D Semiconductor: Gallium Thiophosphate

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  14. From K[ZnBP2O8] to K[(Zn0.5Al0.5)2P2O8]: Substitution-Induced Microporous Zincoaluminophosphate with a Congruent-Melting Behavior

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  16. Highly Distorted [HgS 4 ] Motif-Driven Structural Symmetry Degradation and Strengthened Second-Harmonic Generation Response in the Defect Diamond-Like Chalcogenide Hg 3 P 2 S 8

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  31. The synthesis and structure–property relation analysis of metal chalcohalide crystals Cs 2 InPS 4 X 2 (X = Cl, Br) with mixed anions

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  32. Wide band gap thiophosphates ASrPS 4 (A = Li, Na, K, Rb, Cs): cation size effect induced successive structural transformation

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  33. A new salt-inclusion chalcogenide exhibiting distinctive [Cd11In9S26]3− host framework and decent nonlinear optical performances

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  35. Two non-centrosymmetric scandium borate nonlinear optical crystals containing the B5O10 anion group

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  39. The Kurtz-Perry powder technique revisited: A case study on the importance of reference quality and broadband nonlinear optical measurements using LiInSe2

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  40. BaSi7P10 and SrSi7P10: Two Infrared Nonlinear Optical Phosphides with T2 Supertetrahedra Exhibiting Strong Second‐Harmonic Generation Effects

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  41. Hg2P2S6: A layered mercury hexathiodiphosphate (IV) with large birefringence

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  42. Ag4SnGe2S7: A Noncentrosymmetric Chalcogenide in I4–II–IV2–VI7 System with Non-Diamond-Like Structure Featuring 1D ∞[SnGe2S8]6– Infinite Chain

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  43. Synthesis, Crystal and Electronic Structures, Nonlinear Optical Properties, and Magnetic Properties of Two Thiophosphates: KInP2S7 and KCrP2S7

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  44. Ag-based chalcogenides and derivatives as promising infrared nonlinear optical materials

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  45. Breaking the bottleneck of simultaneously wide band gap and large nonlinear optical coefficient by a “pore reconstruction” strategy in a salt-inclusion chalcogenide

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  46. From BPS 4 to AB 3 P 2 S 10 (A = Na, K): cations inducing dimension reduction and bandgap enlargement

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  47. Na 6 Sn 3 P 4 S 16 : Sn( ii )-chelated PS 4 groups inspired an ultra-strong SHG response

    Inorganic Chemistry Frontiers · 2023-01-01

    Chenyao Zhao, Bingbing Zhang, Xinyu Tian, Guoqiang Zhou, Jingjing Xu, Kui Wu

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  48. Quaternary alkaline-earth metal thiophosphate SrAgPS 4 : syntheses, structures, and optical properties

    Dalton Transactions · 2023-01-01

    Wenhao Xing, Jian Tang, Fei Liang, Chunlan Tang, Jieyun Wu, Wenlong Yin, Bin Kang, Jianguo Deng

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  49. Recent progress on sulfide infrared nonlinear optical materials with large SHG response and wide band gap

    Chinese Journal of Structural Chemistry · 2023-01-01

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