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RESEARCH PAPER · Coordination Chemistry Reviews · 2021

Transition-metal-based chalcogenides: A rich source of infrared nonlinear optical materials

Hong Chen, Wenbo Wei, Hua Lin, Xintao Wu

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Transition-metal-based chalcogenides: A rich source of infrared nonlinear optical materialsOriginalAliovalent-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 6 PS 5 X (M = Ag, Cu; X = Cl, Br) chalcohalides exhibiting strong nonlinear optical responses and high laser damage resistances9The Rise of Infrared Nonlinear Optical Pnictides: Advances and Outlooks36CsCu 3 SbS 4 : rational design of a two-dimensional layered material with giant birefringence derived from Cu 3 SbS 442Cs 3 CuAs 4 Q 8 (Q = S, Se): unique two-dimensional layered inorganic thioarsenates with the lowest Cu-to-As ratio and remarkable photocurrent responses17A 6 Mo 2 P 4 O 19 (A = Rb, Cs) and Rb 2 MoP 2 O 9 : new molybdophosphates with distinct polyanionic configurations5Phase Matchability Transformation in the Infrared Nonlinear Optical Materials with Diamond‐Like Frameworks63AAg 2 PS 4 (A = K, Na/K): the first-type of noncentrosymmetric alkali metal Ag-based thiophosphates exhibiting excellent second-order nonlinear optical performances21Alkali metal partial substitution-induced improved second-harmonic generation and enhanced laser-induced damage threshold for Ag-based sulfides21Band gap modulation and nonlinear optical properties of quaternary tellurates Li 2 GeTeO 613From oxides to oxysulfides: the mixed-anion GeS 3 O unit induces huge improvement in the nonlinear optical effect and optical anisotropy for potential nonlinear optical materials19HgBrI: a possible tecton for NLO molecular materials?4Homovalent Cation Substitutions Leading to New Lithium-Containing La3cusis7 Family Members Having Chiral, Uniaxial Structures and Exhibiting Second- and Third-Harmonic Generation7Interesting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy22KNa 0.78 Eu 0.27 In 3.80 B 12 S 12 : a novel hexanary thioborate featuring a B 12 S 12 cluster and diverse InS x ( x = 4, 5, 6) units9Methylpiperazine based 0D chiral hybrid lead halides for second harmonic generation21Phase 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 properties68Sulfur-source-dependent phase-selective preparation of Cu 3 NiInSnS 6 nanocrystals and their optical and magnetic properties1Tellurate polymorphs with high-performance nonlinear optical switch property and wide mid-IR transparency19Quaternary Noncentrosymmetric Rare-Earth Sulfides Ba4RE2Cd3S10 (RE = Sm, Gd, or Tb): A Joint Experimental and Theoretical Investigation17From 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 Properties12Infrared nonlinear optical performances of a new sulfide β-PbGa2S415Phosphogermanate Crystal: A New Ultraviolet–Infrared Nonlinear Optical Crystal with Excellent Optical Performances16Controllable Synthesis of Centrosymmetric/Noncentrosymmetric Phases for the Family of Halogen-Based Photonic Coordination Polymers to Enhance the Phase-Matching Second-Harmonic-Generation Response19NaGa3Se5: An Infrared Nonlinear Optical Material with Balanced Performance Contributed by Complex {[Ga3Se5]−}∞ Anionic Network14Enhanced Second-Harmonic-Generation Efficiency and Birefringence in Melillite Oxychalcogenides Sr2MGe2OS6 (M = Mn, Zn, and Cd)97The Combination of Structure Prediction and Experiment for the Exploration of Alkali‐Earth Metal‐Contained Chalcopyrite‐Like IR Nonlinear Optical Material104Second-Harmonic Generation-Positive Na 2 Ga 2 SiS 6 with a Broad Band Gap and a High Laser Damage Threshold14Pressure induced superconductivity in nonlinear optical crystal ZnGeP2 and its capture at ambient pressure6The Kurtz-Perry powder technique revisited: A case study on the importance of reference quality and broadband nonlinear optical measurements using LiInSe232Cation Regulation to Investigate the Chalcogenide Borate RE6Nb2MgSB8O26 (RE = La–Nd) Family12Li2Mg2Si2S6 and Li2Mg2Ge2S6: Two nonlinear optical sulfides featuring a unique, polar trigonal structure incorporating ethane‐like anions5Eu 2 P 2 S 6 : The First Rare‐Earth Chalcogenophosphate Exhibiting Large Second‐Harmonic Generation Response and High Laser‐Induced Damage Threshold143Eu2P2S6: The First Rare‐Earth Chalcogenophosphate Exhibiting Large Second‐Harmonic Generation Response and High Laser‐Induced Damage Threshold7AgGaSe2-Inspired Nonlinear Optical Materials: Tetrel Selenides of Alkali Metals and Mercury34First Investigation of Nonlinear Optical Oxychalcogenide with Three‐Dimensional Anionic Framework and Special Windmill‐Like Functional Motifs †28(Na0.74Ag1.26)BaSnS4: A New AgGaS2‐Type Nonlinear Optical Sulfide with a Wide Band Gap and High Laser Induced Damage Threshold14Mixed-Anion-Oriented Design of LnMGa3S6O (Ln = La, Pr, and Nd; M = Ca and Sr) Nonlinear Optical Oxysulfides with Targeted Property Balance56Synthesis and Characterization of New Multinary Selenides A10B18Se37 (A=Sn/Pb; B=In/Sb/Bi)3Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24Growth and Characterization of a Nonlinear Optical Crystal Cd3Te2WO10 Decorated by WO4 Tetrahedra Showing a Large Band Gap9Chalcohalides: A Rising Type of Second‐Order Nonlinear Optical Materials28Novel structural transformation in K3ReP2S8 thiophosphates originating from the rare-earth (Re) cation sizes induced local coordination asymmetry25Characterizations and Nonlinear-Optical Properties of Pentanary Transition-Metal Oxysulfide Sr2CoGe2OS626AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units152Syntheses, structures, and characterization of new heteroanionic chalcohalides: Na2Ba17In8Q21F18 (Q = S, Se), KBa2InQ3F2 (Q = S, Se)5Characteristics of structure, thermal stability and optical properties for a novel NLO crystal (C5H12NO)H2PO48Nouveaux oxysulfures fonctionnels métastables obtenus par désintercalation topochimique du soufre0Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25Structural features of Li0.55Ag0.45InSe2 and Li0.37Ag0.63InSe2 crystals7d6versus d10, Which Is Better for Second Harmonic Generation Susceptibility? A Case Study of K2TGe3Ch8 (T = Fe, Cd; Ch = S, Se)18[Sr 4 Cl 2 ][Si 3 S 9 ]: Ultrawide-bandgap salt-inclusion thiosilicate nonlinear optical material with unprecedented tri-polymerized [Si 3 S 9 ] clusters21A new infrared nonlinear optical material BaZnGeS 4 with a wide band gap and large nonlinear optical response34A novel bifunctional thioarsenate based on unprecedented molecular [Cd 4 As 8 Se 16 (Se 2 ) 2 ] 8− cluster anions11A unique [Sb 6 O 2 S 13 ] 12− finite chain in oxychalcogenide Ba 6 Sb 6 O 2 S 13 leading to ultra-low thermal conductivity and giant birefringence12An overview of Mg-based IR nonlinear optical materials22From 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)19KNa 2 La 2 (BO 3 ) 3 : a shortite-type lanthanide borate exhibiting strong nonlinear optical activity induced by isolated [BO 3 ] triangles and distorted [LaO 9 ] polyhedra26Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution30Recent progress on sulfide infrared nonlinear optical materials with large SHG response and wide band gap26Stereochemically active lone-pair-driven giant enhancement of birefringence from three-dimensional CsZn 4 Ga 5 Se 12 to two-dimensional CsZnAsSe 319The first quaternary rare-earth oxythiogermanate with second-harmonic generation and ferromagnetic behavior26Two pairs of chiral Yb III enantiomers presenting distinct NIR luminescence and circularly polarized luminescence performances with giant differences in second-harmonic generation responses20Two temperature-induced 1D Cu II chain enantiomeric pairs showing different magnetic properties and nonlinear optical responses14Synthesis and Characterization of Multinary Selenides A4B10Se19 (A=Sn, Pb; B=Sb, Bi)1Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance64Partial substitution induced structural transformation and enhanced nonlinear optical properties of Na2GaxIn6-xSe10 (x = 3, 3.76)23Unbiased 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 Chalcogenides48Y3Fe0.5SiSe7: A new cation-deficient quaternary mixed transition metal chalcogenide with extremely low thermal conductivity3Structure and Optical Properties of LixAg1–xGaSe2 and LixAg1–xInSe27{[In2S7]8–}∞ Chain and Isolated HgS4 Planar Unit Constructed One-Dimensional Pentanary Sulfide K2Ba7HgIn4S16 Exhibiting Nonlinear-Optical Activity10Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance56Synthesis, Crystal Structure, and Nonlinear-Optical Properties of a Diamond-Like Chalcogenide Cu 2 GeS 313Defect diamond-like tellurides as infrared nonlinear optical materials with giant second-harmonic generation tensor13Three-in-One Tetrahedral Functional Units Constructing Diamondlike Ag2In2SiS3.06Se2.94 with High-Performance Nonlinear-Optical Activity4ACd 4 Ga 5 Te 12 (A = K, Rb, Cs): Tellurides with a Strong Nonlinear Optical Response and Purple Emission24Mixed Anionic Tetrahedra Guided Design of New Infrared Nonlinear Optical Material Cs 3 Ga 8 S 13 Cl with High Laser‐Induced Damage Threshold26Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application49Rb2Sn4Q9 (Q = S and Se): Low-Dimensional Noncentrosymmetric Chalcogenides with High Laser-Induced Damage Threshold10Rational Design of a Niobium Tellurite Crystal Nb2Te3O11 Exhibiting Good Overall Infrared NLO Performance by Structural Genetic Engineering17A prediction-driven database to enable rapid discovery of nonlinear optical materials46Temperature dependent charge carrier dynamics in 2D ternary Cu2MoS4 nanoflakes: An effect of electron-phonon coupling2ZnGa 2 S 4 : an infrared nonlinear optical material with large second‐harmonic generation response and wide band gap28A Machine Learning Study on High Thermal Conductivity Assisted to Discover Chalcogenides with Balanced Infrared Nonlinear Optical Performance58Homohelical Self-Assembly of Trimer of α-Cyclodextrin and Octamolybdate10Modulation of the Band Gap and Redox Properties by Mixed Addenda in Sandwich Polyoxometalates2A I B 3 II C 2 III Q 6 VI X VII : A Thioborate Halide Family for Developing Wide Bandgap Infrared Nonlinear Materials by Coupling Planar [BS 3 ] and Polycations25Studies of reduced graphene oxide (rGO)/CuS nanocomposite for supercapacitor applications6Na 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 ] octahedra4Advances in Solid-State Nonlinear Optical Materials: From Fundamentals to Applications61K4ZnV5O15Cl: A Congruent‐Melting Mid‐Infrared Nonlinear Optical Crystal Combined with Strong Second‐Harmonic Generation and High Laser‐Induced Damage Threshold14ACu4AsS4 (A = K, Rb): Two infrared nonlinear optical crystals with strong second-harmonic generation responses originating from multiple chromophores12“Three‐in‐One”: A New Hg‐Based Selenide Hg 7 P 2 Se 12 Exhibiting Wide Infrared Transparency Range and Strong Nonlinear Optical Effect80A-site cation manipulation of exemplary second harmonic generation response and optical anisotropy in rare-earth borates18Cation and anion co-partial substitution induced centrosymmetric to noncentrosymmetric structural transformation to construct nonlinear-optical rare-earth oxythiogermanates13Hg 3 AsS 4 X (X = Cl and Br): two Hg-based chalcogenides as long-wave infrared nonlinear optical crystals with superior comprehensive performances33Multi-step cation substitution facilitating the exploration of potential infrared nonlinear optical materials6Quality Improvement of Baga 4 Se 7 Crystal by Annealing in Base Vapor Atmosphere2Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70RbPbPS 4 : a promising IR nonlinear optical material achieved by lone-pair-cation-substitution-induced structure transformation23Syntheses, crystal structures and photocurrent responses of Cs 2 Ag 2 Sb 2 S 5 and CsAgSb 4 S 7 with thiourea as a mineralizer4Two chiral Co III and Ni II complexes with identical ligands presenting different nonlinear optical responses4Two chiral Eu III and Sm III enantiomeric pairs with enantiopure N-donor ligands: showing strong third-harmonic generation and photoluminescence properties7Two chiral lanthanide Pr III and Ho III complexes: NIR luminescence and nonlinear optical properties14Ba10In2Mn11Si3O12S18: First Hexanary Oxychalcogenide Containing an Infrequent Three-Dimensional Noncentrosysmmetric Framework8Infrared nonlinear optical materials with multiple strongly ionic cations5Design 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 substitution28Quality improvement of BaGa4Se7 crystal by annealing in BaSe vapor atmosphere8The centrosymmetric to non-centrosymmetric transformation induced by alkaline-earth cations producing infrared nonlinear optical AeMn6Ga6S16 (Ae = Ca, Sr)13[Cs14Cl][Tm71Se110]: An unusual salt-inclusion chalcogenide containing different valent Tm centers and ultralow thermal conductivity10Enhanced electro-optical properties of polymer dispersed liquid crystals doped with functional nanofibers for applications of efficient smart windows and advanced anti-counterfeiting34Chiral mono- and dinuclear CoII and CuII enantiomeric pairs with distinct enantiopure N-donor ligands: Presenting highly enhanced third-harmonic generation responses6Phase-Matching Second-Harmonic Generation and Enhanced Laser-Induced Damage Threshold Induced by Cs Substitution: Cu 3 PSe 4 vs Cs 2 CuP 3 S 94Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy26K4Cd3Ge4O13: A Congruent-Melting Germanate Nonlinear Optical Crystal with a Moderate Second-Harmonic Generation Intensity and Broad Transparent Window2From [Ba3S][GeS4] to [Ba3CO3][MS4] (M = Ge, Sn): Enhancing optical anisotropy in IR birefringent crystals via functional group implantation11SbO(OH)2(IO3): The First Polar Sb5+‐Iodate with a Strong Second‐Harmonic Generation Response and a Wide Bandgap8Rare-Earth/d10 Dual-Metal Oxychalcogenides as Infrared Nonlinear-Optical Materials10Deep‐Ultraviolet Transparent Nonlinear Optical Phosphates: A New Alternative to Conventional Borates9Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22Hg4InS2Cl5: Achieving Giant Optical Anisotropy by Introducing Well‐Aligned Linear [Hg2S2] Units14Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances17Structural and thermal properties and the origin of the ultralow thermal conductivity in the defect stannite CuIn2Se42Alkali metal/mercury dual-metal sulfides as infrared nonlinear optical materials with high laser-induced damage thresholds5Cationic substitution engineering induces a new quaternary chalcogenide in the A–M IIIA –M IVA –Q system for optical crystal applications1Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units18Impact of nuclear number on SHG and THG performances: a comparative study of chiral mono- and dinuclear Tb III complexes with identical organic ligands2Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides11La 2 ZnGa 2 S 6 O: a melilite-type transition metal oxysulfide achieving a well-balanced nonlinear optical behavior5Structural diversity and photocurrent responses of multi-component chalcogenidometalates8First-Principles High-Throughput Screening and Experimental Verification of III-VIB Transition Metal Chalcogenides Nonlinear Optical Crystals15Prediction and Evaluation of Li 2 ZnS 2 Crystals as Mid‐Infrared Nonlinear Optical Material with High Thermal Conductivity7Controllable Syntheses, Structure Identifications, and Property Explorations of Self‐Intercalated 2D Transition Metal Chalcogenides3Nonlinear Optical Effects Modulated by Distinctive Monovalent Cations with Lone Electron Pairs in AGaI 4 (A = Ga + , In + )4Symmetry over Chemistry: Harmonic Generation of Low-Dimensional Alkali Chalcopnictates RbMP2S6 (M = Sb, Bi)5A new selenide semiconductor NaMn3Ga3Se8 with strong second-harmonic generation and significant luminescence property5Multifunctional chiral dinuclear DyIII enantiomeric pairs: showing single-molecule magnet behaviors with very strong third-harmonic generation responses5From Orthorhombic Cu8GeS6 to Cubic Cu6HgGeS6: Second-Harmonic Generation and Photocurrent Responses7Mild solvothermal syntheses, crystal structures, characterizations and properties of four ternary alkaline earth metal sulfides1Second-Harmonic Generation Response in Nitridophosphates MP2N4 (M = Ge, Sn, Pb) and the Role of Stereochemically Active Lone Pairs6Two Chiral EuIII Enantiomeric Pairs with Significantly Enhanced Photophysical and Third-Harmonic Generation Performances through the Coordination Roles of Enantiopure Bi- and Tridentate N-Donors8Achieving excellent nonlinear optical performance via “dimensionality elevation”-driven transformation from centrosymmetric to non-centrosymmetric structures1Magnetic Properties and Large Second-Harmonic Generation Response of a Chiral Ternary Chalcogenide: Eu 2 SiSe 48

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  34. Cation Regulation to Investigate the Chalcogenide Borate RE6Nb2MgSB8O26 (RE = La–Nd) Family

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  35. Li2Mg2Si2S6 and Li2Mg2Ge2S6: Two nonlinear optical sulfides featuring a unique, polar trigonal structure incorporating ethane‐like anions

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  36. Eu 2 P 2 S 6 : The First Rare‐Earth Chalcogenophosphate Exhibiting Large Second‐Harmonic Generation Response and High Laser‐Induced Damage Threshold

    Angewandte Chemie International Edition · 2022-06-08

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  37. Eu2P2S6: The First Rare‐Earth Chalcogenophosphate Exhibiting Large Second‐Harmonic Generation Response and High Laser‐Induced Damage Threshold

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  38. AgGaSe2-Inspired Nonlinear Optical Materials: Tetrel Selenides of Alkali Metals and Mercury

    Chemistry of Materials · 2022-06-26

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  39. First Investigation of Nonlinear Optical Oxychalcogenide with Three‐Dimensional Anionic Framework and Special Windmill‐Like Functional Motifs †

    Chinese Journal of Chemistry · 2022-07-14

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  40. (Na0.74Ag1.26)BaSnS4: A New AgGaS2‐Type Nonlinear Optical Sulfide with a Wide Band Gap and High Laser Induced Damage Threshold

    Chemistry - A European Journal · 2022-08-10

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  41. Mixed-Anion-Oriented Design of LnMGa3S6O (Ln = La, Pr, and Nd; M = Ca and Sr) Nonlinear Optical Oxysulfides with Targeted Property Balance

    ACS Applied Materials & Interfaces · 2022-08-11

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  42. Synthesis and Characterization of New Multinary Selenides A10B18Se37 (A=Sn/Pb; B=In/Sb/Bi)

    European Journal of Inorganic Chemistry · 2022-09-08

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  43. Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)

    Inorganic Chemistry · 2022-09-21

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  44. Growth and Characterization of a Nonlinear Optical Crystal Cd3Te2WO10 Decorated by WO4 Tetrahedra Showing a Large Band Gap

    Crystal Growth & Design · 2022-09-27

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  45. Chalcohalides: A Rising Type of Second‐Order Nonlinear Optical Materials

    European Journal of Inorganic Chemistry · 2022-10-05

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  46. Novel structural transformation in K3ReP2S8 thiophosphates originating from the rare-earth (Re) cation sizes induced local coordination asymmetry

    Materials Today Physics · 2022-10-17

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  47. Characterizations and Nonlinear-Optical Properties of Pentanary Transition-Metal Oxysulfide Sr2CoGe2OS6

    Inorganic Chemistry · 2022-10-20

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  48. AIB3IIC3IIIQ8VI: A New Family for the Design of Infrared Nonlinear Optical Materials by Coupling Octahedra and Tetrahedra Units

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  49. Syntheses, structures, and characterization of new heteroanionic chalcohalides: Na2Ba17In8Q21F18 (Q = S, Se), KBa2InQ3F2 (Q = S, Se)

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  50. Characteristics of structure, thermal stability and optical properties for a novel NLO crystal (C5H12NO)H2PO4

    Optical Materials · 2022-11-27

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