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RESEARCH PAPER · Chemistry of Materials · 2020

HgCuPS4: An Exceptional Infrared Nonlinear Optical Material with Defect Diamond-like Structure

Mengyue Li, Zuju Ma, Bingxuan Li, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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HgCuPS4: An Exceptional Infrared Nonlinear Optical Material with Defect Diamond-like StructureOriginalPartial Isovalent Anion Substitution to Access Remarkable Second-Harmonic Generation Response: A Generic and Effective Strategy for Design of Infrared Nonlinear Optical Materials114Inherent laws between tetrahedral arrangement pattern and optical performance in tetrahedron-based mid-infrared nonlinear optical materials131Salt-Inclusion Chalcogenide [Ba4Cl2][ZnGa4S10]: Rational Design of an IR Nonlinear Optical Material with Superior Comprehensive Performance Derived from AgGaS2134Chalcophosphates: A Treasure House of Infrared Nonlinear Optical Materials75Two Mixed-Anion Units of [GeOSe3] and [GeO3S] Originating from Partial Isovalent Anion Substitution and Inducing Moderate Second Harmonic Generation Response and Large Birefringence55Phase 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 novel promising infrared nonlinear optical selenide KAg 3 Ga 8 Se 14 designed from benchmark AgGaQ 2 (Q = S, Se)55A 3 Mn 2 Sb 3 S 8 (A = K and Rb): a new type of multifunctional infrared nonlinear optical material based on unique three-dimensional open frameworks53A 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 conductivities28Aliovalent-cation-substitution-induced structure transformation: a new path toward high-performance IR nonlinear optical materials47Ba 2 Ge 2 Te 5 : a ternary NLO-active telluride with unusual one-dimensional helical chains and giant second harmonic-generation tensors31M 2 As 2 Q 5 (M = Ba, Pb; Q = S, Se): a source of infrared nonlinear optical materials with excellent overall performance activated by multiple discrete arsenate anions70Lithiated Graphene Quantum Dot and its Nonlinear Optical Properties Modulated by a Single Alkali Atom: A Theoretical Perspective22Structural Modulation from Cu 3 PS 4 to Cu 5 Zn 0.5 P 2 S 8 : Single-Site Aliovalent-Substitution-Driven Second-Harmonic-Generation Enhancement28Hierarchical molecular design of high-performance infrared nonlinear Ag2HgI4 material by defect engineering strategy128AXHg3P2S8 (A = Rb, Cs; X = Cl, Br): New Excellent Infrared Nonlinear Optical Materials with Mixed‐Anion Chalcohalide Groups of Trigonal Planar [HgS2X]3− and Tetrahedral [HgS3X]5−58Mg 2 In 3 Si 2 P 7 : A Quaternary Diamond-like Phosphide Infrared Nonlinear Optical Material Derived from ZnGeP 2130A review of the structural diversity of [P x S y ] n − motifs and their potential application prospects in metal thiophosphates21Highly 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 8473D bicontinuous diamond-like morphologies in thin films of soluted block copolymers1Hg 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 Units49The Rise of Infrared Nonlinear Optical Pnictides: Advances and Outlooks36Superior Infrared Nonlinear Optical Performance Achieved by Synergetic Functional Motif and Vacancy Site Modulations48Investigation into Structural Variation from 3D to 1D and Strong Second Harmonic Generation of the AHgPS4 (A+ = Na+, K+, Rb+, Cs+) Family26Noncentrosymmetric chalcohalide K2Ba3Ge3S9Cl2: A new nonlinear optical material with remarkable laser-induced damage threshold17Synergistic Effect of π-Conjugated [C(NH 2 ) 3 ] Cation and Sb(III) Lone Pair Stereoactivity on Structural Transformation and Second Harmonic Generation58Hg-based chalcogenides: An intriguing class of infrared nonlinear optical materials129Pnictides: An emerging class of infrared nonlinear optical material candidates47AAg 2 PS 4 (A = K, Na/K): the first-type of noncentrosymmetric alkali metal Ag-based thiophosphates exhibiting excellent second-order nonlinear optical performances21AAg 3 Ga 8 Se 14 (A = Rb, Cs): second-harmonic generation responses realized through the parallel arrangement of AgSe 4 and GaSe 4 tetrahedrons5HgBrI: a possible tecton for NLO molecular materials?4KAg3Ga8S14: An Mid- and Far-infrared Nonlinear Optical Material Exhibiting High Laser-induced Damage Threshold※3Phase matching achieved by isomorphous substitution in IR nonlinear optical material Ba 2 SnSSi 2 O 7 with an undiscovered [SnO 4 S] functional motif47Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties69Structural and thermal properties of ultralow thermal conductivity Ba 3 Cu 2 Sn 3 Se 106Wide 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 performances16HgSO4: An excellent mid-infrared sulfate nonlinear optical crystal with wide band gap and strong second harmonic generation response19Quaternary Noncentrosymmetric Rare-Earth Sulfides Ba4RE2Cd3S10 (RE = Sm, Gd, or Tb): A Joint Experimental and Theoretical Investigation17Two Nonlinear Optical Thiophosphates Cu 5 Hg 0.5 P 2 S 8 and AgHg 3 PS 6 Activated by Their Tetrahedra-Stacking Architecture12From Cc to P 6 3 mc : Structural Variation in La 3 S 2 Cl 2 [SbS 3 ] and La 3 OSCl 2 [SbS 3 ] Induced by the Isovalent Anion Substitution22Ba6(CuxZy)Sn4S16 (Z = Mg, Mn, Zn, Cd, In, Bi, Sn): High Chemical Flexibility Resulting in Good Nonlinear-Optical Properties12Optimized Bridgman growth and quality improvement of LiInSe2 crystal by annealing in Li2Se vapor atmosphere12Anion-Centered Polyhedron Strategy for Strengthening Photon Emission Induced by Electron–Phonon Coupling13Application of Materials Genome Methods in Thermoelectrics15Enhanced Second-Harmonic-Generation Efficiency and Birefringence in Melillite Oxychalcogenides Sr2MGe2OS6 (M = Mn, Zn, and Cd)97The Kurtz-Perry powder technique revisited: A case study on the importance of reference quality and broadband nonlinear optical measurements using LiInSe232RbBiP2S6: A Promising IR Nonlinear Optical Material with a Giant Second-Harmonic Generation Response Designed by Aliovalent Substitution80Hg2P2S6: A layered mercury hexathiodiphosphate (IV) with large birefringence11A comprehensive review on metal chalcogenides with three-dimensional frameworks for infrared nonlinear optical applications115Fluorotrithiophosphate Abstraction from the Difluoropentathiodiphosphate Dianion: d8 and d6 Complexes of [η2-S3PF]2–6Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance29Synthesis, 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 materials90KREP2Se6 (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 strategy17Recent Advances in Infrared Nonlinear Optical Crystal7An overview of Mg-based IR nonlinear optical materials23From BPS 4 to AB 3 P 2 S 10 (A = Na, K): cations inducing dimension reduction and bandgap enlargement7Heteroanion-introduction-driven birefringence enhancement in oxychalcogenide Ba 3 M II Ge 3 O 2 S 8 (M II = Mn, Cd)19Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution30Na 6 Sn 3 P 4 S 16 : Sn( ii )-chelated PS 4 groups inspired an ultra-strong SHG response22Nitrides: a promising class of nonlinear optical material candidates9Open honeycomb frameworks of sulphides AHg 4 Ga 5 S 12 (A = Rb, Cs) exhibiting infrared nonlinear optical properties12Quaternary 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 gap26Structure, electrical and thermal properties of single-crystal BaCuGdTe 36The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]17Recent progress in the design of IR nonlinear optical materials by partial chemical substitution: Structural evolution and performance optimization133Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance64{[In2S7]8–}∞ Chain and Isolated HgS4 Planar Unit Constructed One-Dimensional Pentanary Sulfide K2Ba7HgIn4S16 Exhibiting Nonlinear-Optical Activity10HgB2S4: A d10 Metal Thioborate with Giant Birefringence and Wide Band Gap31Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance57Zn 2 HgP 2 S 8 : A Wide Bandgap Hg‐Based Infrared Nonlinear Optical Material with Large Second‐Harmonic Generation Response75The compatibly large nonlinear optical effect and high laser-induced damage threshold in a thiophosphate CsInP2S7 constructed with [P2S7]4- and [InS6]9-15Electronic and Thermal Properties of the Cation Substitution-Derived Quaternary Chalcogenide CuInSnSe 410A ll HgM IV S 4 (A ll = Sr, Ba, M IV = Si, Ge): A Series of Materials with Large Second Harmonic Generation Response and Wide Band Gaps28Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application49Na 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 Anisotropy10Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy26Ga-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 Effect80Hg 3 AsS 4 X (X = Cl and Br): two Hg-based chalcogenides as long-wave infrared nonlinear optical crystals with superior comprehensive performances33Partial 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)17RbPbPS 4 : a promising IR nonlinear optical material achieved by lone-pair-cation-substitution-induced structure transformation23Salt-inclusion chalcogenides with d-orbital components: unveiling remarkable nonlinear optical properties and dual-band photoluminescence10Unlocking the potential of coinage-based quaternary chalcogenides for thermoelectricity16Benzo‐bisimidazole based nanosheets having porphyrin like internal core with high second order nonlinear optical response: A theoretical perspective1KREP 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– } ∞ Layers8Understanding the role of symmetric/asymmetric curcuminoids in designing efficient optical, nonlinear optical and photovoltaic materials21Light correcting light with nonlinear optics28Vacancy‐Induced Extraordinary Second Harmonic Generation Response for Diamond‐Like Cu3PS49Diffusion dominant thermal transport in mixed valent Ba4Sn4Se93Design 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 Substitution5HgC4H4O6: A mercury tartrate exhibits phase matchable second harmonic generation effect1The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28Phase Matching of Infrared Nonlinear Optical Salt-Inclusion Chalcogenides Achieved by the Modulation of the Fractal Dimension of Anionic Motifs18A synergistic experimental and theoretical study elucidating the electronic and thermal properties in spinel CuInSnS46Homoatomic Polychalcogenide Nonlinear Optical Anionic Groups with Ultra-Large Optical Anisotropy31Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials24Structure‐Prediction‐Oriented Synthesis of Thiophosphates as Promising Infrared Nonlinear Optical Materials1Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units66Ag 2 GeS 3 : A Diamond‐Like Chalcogenide as an IR Nonlinear Optical Material with Outstanding Second‐Harmonic Generation Response28β-Pb3P2S8: A new optical crystal with exceptional birefringence effect12A 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 94Learning From Nature: The Rational Non‐Centrosymmetric Structural Design in the Honeycomb‐Like Gaudefroyite Family23Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22Design 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 Strategy8Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides11Structural diversity and photocurrent responses of multi-component chalcogenidometalates8新型非线性光学晶体和双折射晶体的研究进展（特邀）4A new selenide semiconductor NaMn3Ga3Se8 with strong second-harmonic generation and significant luminescence property5From Orthorhombic Cu8GeS6 to Cubic Cu6HgGeS6: Second-Harmonic Generation and Photocurrent Responses7Recent progress in structural design strategies of high-birefringence optical crystals55NbGa 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 Birefringence6Planar [HgCl 3 ] and V‑Shaped [HgCl 2 ] Units Synergistically Creating a Prominent Halide Birefringent Crystal β ‐CsHg 2 Cl 5 with Wide‐Spectrum7The Influence of Different Group Distortions on the Structure–Property Relationship of Alkali Metal Thiophosphate0[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence18[TeSeS 2 ] 2− : The First Heterotriple‐Chalcogenide Motifs Decode Giant Mid‐Far Infrared Birefringence4Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29Vacancy-driven tetrahedral distortion leading to exceptional second harmonic generation3Maximizing the second-harmonic generation response via coordination-induced localization of nonbonding electrons12ABCQ4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 performance1van der Waals layered CuInP 2 S 6 as infrared nonlinear optical material1Harnessing tetrahedral diversity: The path to superior diamond-like IR NLO crystals15KHg 4 Ga 5 S 12 : A Diamond-like Tetrahedral Chalcogenide Exhibiting Giant Phase-Matching Second Harmonic Generation6From KBa 4 Ge 3 S 10 Cl to ABa 3 EuGe 3 S 11 (A = Na, K) Synthesized by Reactive Flux Assisted Metal Oxide-Boron-Chalcogen (MOBQ) Method: Effect of Cation/Anion Cosubstitution on Crystal Structure and Nonlinear Optical Properties0Unveiling the impact of terminal structural modifications on nonlinear optical properties of push-pull pyrene derivatives1First‐Principles Investigation of the Structural, Electronic, Optical, Elastic, and Thermal Properties of Defect Diamond‐Like Hg 3 P 2 S 80Rational Design of a Strong Nonlinear Optical Crystal With Ultrawide Bandgap via Fine‐Tuning of Channel Structures0From AgGaSe2 to MIIGa2Se4 (MII = Zn, Cd): Heterovalent Substitution Creates Ordered Vacancies for Balanced IR-NLO Performance0Variation 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 Threshold0Beyond the bandgap bottleneck: structure–property design principles for infrared nonlinear optical phosphides0Vacancy-Driven Tetrahedral Distortion in Defect Diamond-Like Selenides for Exceptional Second-Order Nonlinearity0

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  2. Inherent laws between tetrahedral arrangement pattern and optical performance in tetrahedron-based mid-infrared nonlinear optical materials

    Coordination Chemistry Reviews · 2020-06-29

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  3. Salt-Inclusion Chalcogenide [Ba4Cl2][ZnGa4S10]: Rational Design of an IR Nonlinear Optical Material with Superior Comprehensive Performance Derived from AgGaS2

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

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  5. Two Mixed-Anion Units of [GeOSe3] and [GeO3S] Originating from Partial Isovalent Anion Substitution and Inducing Moderate Second Harmonic Generation Response and Large Birefringence

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

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

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  31. Hg-based chalcogenides: An intriguing class of infrared nonlinear optical materials

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  32. Pnictides: An emerging class of infrared nonlinear optical material candidates

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  33. AAg 2 PS 4 (A = K, Na/K): the first-type of noncentrosymmetric alkali metal Ag-based thiophosphates exhibiting excellent second-order nonlinear optical performances

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  34. AAg 3 Ga 8 Se 14 (A = Rb, Cs): second-harmonic generation responses realized through the parallel arrangement of AgSe 4 and GaSe 4 tetrahedrons

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  35. HgBrI: a possible tecton for NLO molecular materials?

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  44. Two Nonlinear Optical Thiophosphates Cu 5 Hg 0.5 P 2 S 8 and AgHg 3 PS 6 Activated by Their Tetrahedra-Stacking Architecture

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  45. From Cc to P 6 3 mc : Structural Variation in La 3 S 2 Cl 2 [SbS 3 ] and La 3 OSCl 2 [SbS 3 ] Induced by the Isovalent Anion Substitution

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  46. Ba6(CuxZy)Sn4S16 (Z = Mg, Mn, Zn, Cd, In, Bi, Sn): High Chemical Flexibility Resulting in Good Nonlinear-Optical Properties

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  47. Optimized Bridgman growth and quality improvement of LiInSe2 crystal by annealing in Li2Se vapor atmosphere

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  48. Anion-Centered Polyhedron Strategy for Strengthening Photon Emission Induced by Electron–Phonon Coupling

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  49. Application of Materials Genome Methods in Thermoelectrics

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  50. Enhanced Second-Harmonic-Generation Efficiency and Birefringence in Melillite Oxychalcogenides Sr2MGe2OS6 (M = Mn, Zn, and Cd)

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