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RESEARCH PAPER · Chemistry of Materials · 2022

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

Mao‐Yin Ran, Shenghua Zhou, Bingxuan Li, Wenbo Wei, Xintao Wu, Hua Lin, Qi‐Long Zhu

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Enhanced Second-Harmonic-Generation Efficiency and Birefringence in Melillite Oxychalcogenides Sr2MGe2OS6 (M = Mn, Zn, and Cd)OriginalAAg 3 Ga 8 Se 14 (A = Rb, Cs): second-harmonic generation responses realized through the parallel arrangement of AgSe 4 and GaSe 4 tetrahedrons5Ba 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 318Hg 2 (SeO 3 )(SO 4 ): the first sulfate selenite with large birefringence explored from d 10 transition metal compounds36Interesting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy22Phase 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 properties69First Investigation of Nonlinear Optical Oxychalcogenide with Three‐Dimensional Anionic Framework and Special Windmill‐Like Functional Motifs †28Mixed-Anion-Oriented Design of LnMGa3S6O (Ln = La, Pr, and Nd; M = Ca and Sr) Nonlinear Optical Oxysulfides with Targeted Property Balance56Recent developments on Bi-based oxychalcogenide materials with thermoelectric and optoelectronic applications: an overview33Oxychalcogenides 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 performance29Characterizations and Nonlinear-Optical Properties of Pentanary Transition-Metal Oxysulfide Sr2CoGe2OS626AeMg6Ga6S16 (Ae = Ca, Sr, Ba): The First Double Alkaline‐Earth Metal Chalcogenides with Excellent Performances29The Antiperovskite‐Type Oxychalcogenides Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se) with Large Second Harmonic Generation Responses and Wide Band Gaps68Nouveaux oxysulfures fonctionnels métastables obtenus par désintercalation topochimique du soufre0Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25Oxychalcogenides: A Promising Class of Materials for Nonlinear Optical Crystals with Mixed‐Anion Groups35A 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 materials23Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181Heteroanion-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 substitution30A New Year and 35 Years of Chemistry of Materials0Fluorooxoborates: A precious treasure of deep-ultraviolet nonlinear optical materials24Recent 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 Performance64Sr6Ge3OSe11: A Rationally Designed Noncentrosymmetric Oxyselenide with Polar [GeOSe3] Building Blocks16Comprehensive review on multiple mixed-anion ligands, physicochemical performances and application prospects in metal oxysulfides32Theoretical Prediction‐Assisted Synthesis and Characterization of Infrared Nonlinear Optical Material NaSrBS324Recent progress of newly developed functional building units and corresponding nonlinear optical materials14First-principles study on AgBi(CrO4)2:An effective infrared nonlinear optical compound3Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance57Three-in-One Tetrahedral Functional Units Constructing Diamondlike Ag2In2SiS3.06Se2.94 with High-Performance Nonlinear-Optical Activity4A survey of stereoactive oxysalts for linear and nonlinear optical applications40Two Noncentrosymmetric Bismuth Phosphates: Rational Design Synthesis and Optical Properties4Mixed Anionic Tetrahedra Guided Design of New Infrared Nonlinear Optical Material Cs 3 Ga 8 S 13 Cl with High Laser‐Induced Damage Threshold26Eu 2 MGe 2 OS 6 (M = Mn, Fe, Co): Three Melilite-Type Rare-Earth Oxythiogermanates Exhibiting Balanced Nonlinear-Optical Behaviors21Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application49Na6Ge2S6O-ionic conductor: Synthesis, structure and ionic transportation1AGe2O4Q (A = Ba, Sr; Q = S, Se): A series of heteroanionic oxychalcogenides with large birefringence9Chiral and Polar Duality Design of Heteroanionic Compounds: Sr18Ge9O5S31 Based on [Sr3OGeS3]2+ and [Sr3SGeS3]2+ Groups20K4ZnV5O15Cl: A Congruent‐Melting Mid‐Infrared Nonlinear Optical Crystal Combined with Strong Second‐Harmonic Generation and High Laser‐Induced Damage Threshold14Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy26Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65A UV non-hydrogen pure selenite nonlinear optical material for achieving balanced properties through framework-optimized structural transformation41Ba 2 GeF 2 Q 3 (Q = S, Se) and Ba 3 GeF 2 Se 4 : new F-based chalcohalides with enhanced birefringence9Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals9New nonlinear optical oxyfluoride K 2 NbO 2 F 3 with strong pseudo-centrosymmetry, obtained by mild hydrothermal synthesis0Partial 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)17Rare-earth oxychalcogenide Eu 2 ZnGe 2 OS 6 : a phase-matching infrared nonlinear optical material with [GeOS 3 ] units7Rare-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 transformation23Salt-inclusion chalcogenides with d-orbital components: unveiling remarkable nonlinear optical properties and dual-band photoluminescence10Salt-inclusion sulfides [K 4 Cl][M II 11 In 9 S 26 ] (M II = Zn, Cd) displaying robust nonlinear optical activity4A comprehensive review on synthesis, properties, and applications of quaternary transition metal oxychalcogenides19Ba10In2Mn11Si3O12S18: First Hexanary Oxychalcogenide Containing an Infrequent Three-Dimensional Noncentrosysmmetric Framework8Anhydrous Aluminum Iodate: Strong Second Harmonic Generation Effect Contributed by Unbonded and Antibonding Orbitals3Pentanary Oxythiogermanates Ba3MGe3O2S8 (M = Ca, Zn) Featuring [Ge3O2S8]8– Trimers and {[MGe3O2S8]6–}∞ Chains: Structural Chemistry and Physical Properties4The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28Sr2HgGe2OS6: A Hg-Based Oxychalcogenide Infrared Nonlinear Optical Material Exhibiting Favorable Balance between a Large Band Gap and Strong Second Harmonic Generation Response10Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals66Breaking Boundaries: Giant Ultraviolet Birefringence in Dimension‐Reduced Zn‐Based Crystals8Ag 2 GeS 3 : A Diamond‐Like Chalcogenide as an IR Nonlinear Optical Material with Outstanding Second‐Harmonic Generation Response28La3Ga5M0.5Sn0.5O14, (M = Ge, Si): Design and Synthesis of Two Langasite Nonlinear Optical Materials with Large Second Harmonic Generation and Birefringence Induced by Distorted (Sn/M)O6 Octahedra4Promising Functional Structural Building Unit Trisulfimide (SO2N)33– and Its Contributions to Second Harmonic Generation and Birefringence1Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy26ACuGa 6 S 10 (A = Rb, Cs): Design and Synthesis of Two New Cavity‐Chalcopyrite Chalcogenides Based on “Iterative Substitution” Strategy4From [Ba3S][GeS4] to [Ba3CO3][MS4] (M = Ge, Sn): Enhancing optical anisotropy in IR birefringent crystals via functional group implantation11Rare-Earth/d10 Dual-Metal Oxychalcogenides as Infrared Nonlinear-Optical Materials10Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22La 3 (Ga 3 S 3 O 3 )(Si 2 O 7 ): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups6Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances18La 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 chalcogenidometalates8Hetero‐Anionic Oxychalcogenides with Structures and Properties Tuned by the O:S Ratio15Discovering Pseudo-Supertetrahedral Functional Units in Salt-Inclusion Nonlinear Optical Material [Ba22(SO4)5][Zn14Ga18S58]14Oxygen‐Substitution Induced High‐Performance Nonlinear Optical Properties: Witnessed by the First Quaternary Oxythiostannate12Zero-Dimensional Oxyselenide Ba12[(Ga2OSe5)3(Si2O7)]: Enhanced Optical Anisotropy through Heteroanionic Engineering4Recent progress in structural design strategies of high-birefringence optical crystals55Research progress and future prospect of chalcogenides with large optical anisotropy46From Centrosymmetric Ca3Ge2O3S4 to Noncentrosymmetric Ca3Ge2O4Se3: A Nonlinear Optical Ca-Based Oxyselenide5Eu(II) 4 Eu(III) 2 Ge 3 S 11 O 2 : a Single‐Element Mixed‐Valence Engineering Breakthrough for Strongly Enhanced Nonlinearity and Anisotropy in Rare‐Earth Oxysulfides8Doubling Polarizability Anisotropy of The Tetrahedral Motifs to Achieve Phase Matching for Melilite-Type Compound2Synergistic Enhancement of Band Gap and Optical Anisotropy via Functional-Site Cosubstitution in Antiperovskite-Type Chalcohalides [Ba2K][X][MS4] (M = Ge, Si; X = Cl, Br)2Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29LnEuGa3OS6 (Ln = La, Pr, Nd): three dual rare earth metal-based oxychalcogenides with good IR nonlinear optical performances1Assembly of Highly Polarizable “Linkers” with Heteroleptic Groups for Inducing Large Optical Anisotropy in Ba2SnIIGe3O8S and Ba3SnIIGe3O2S82A high-performance IR nonlinear optical material Sr 3 MnGe 2 S 8 achieved via partial cation substitution-induced structural transformation2Maximizing the second-harmonic generation response via coordination-induced localization of nonbonding electrons12[Ba2K][Br][SiS4]: An antiperovskite-type chalcohalide with simultaneously enhanced birefringence and band gap via cation-anion co-substitution0Heterometallic Ge–O–Sn-Bridged Oxychalcogenides Sr3GeSnO4Q3 (Q = S, Se) with Wide Band Gaps and Moderate Infrared Nonlinear Optical Responses0Mineral‐Inspired and Computation‐Assisted Rational Design of Polar Gittinsite‐Type Thiophosphates With Exceptional Nonlinear Optical Performance4Cation-substitution-driven electronic, nonlinear optical, elastic, and thermal transport properties of layered AeHgGeSe4 (Ae = Ba, Sr): A first-principles study0The Multi‐Scale Paradigm: An Integrated Design Logic for Nonlinear Optical Crystals1The Multi‐Scale Paradigm: An Integrated Design Logic for Nonlinear Optical Crystals0Domino‐Effect Amplification via Covalent‐Chain Engineering for Giant Birefringence in NaAsQ 2 (Q = S, Se) Crystals0

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  3. Bridging oxygen atoms in trigonal prism units driven strong second-harmonic-generation efficiency in Sr 3 Ge 2 O 4 Te 3

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  5. Interesting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy

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  6. Phase matching achieved by isomorphous substitution in IR nonlinear optical material Ba 2 SnSSi 2 O 7 with an undiscovered [SnO 4 S] functional motif

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  7. Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties

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

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

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  12. Simple yet extraordinary: Super-polyhedra-built 3D chalcogenide framework of Cs5Ga9S16 with excellent infrared nonlinear optical performance

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

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  16. Nouveaux oxysulfures fonctionnels métastables obtenus par désintercalation topochimique du soufre

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  19. A 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 birefringence

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  43. K4ZnV5O15Cl: A Congruent‐Melting Mid‐Infrared Nonlinear Optical Crystal Combined with Strong Second‐Harmonic Generation and High Laser‐Induced Damage Threshold

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  44. Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy

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  47. Ba 2 GeF 2 Q 3 (Q = S, Se) and Ba 3 GeF 2 Se 4 : new F-based chalcohalides with enhanced birefringence

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  48. Heteroanionic [VO x S 4− x ] groups: tetrahedral units with large birefringence for mid-infrared nonlinear optical crystals

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  49. New nonlinear optical oxyfluoride K 2 NbO 2 F 3 with strong pseudo-centrosymmetry, obtained by mild hydrothermal synthesis

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  50. Partial 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)

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