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RESEARCH PAPER · Angewandte Chemie International Edition · 2021

La 3 Ga 3 Ge 2 S 3 O 10 : An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap Engineering

Hong Yan, Yoshitaka Matsushita, Kazunari Yamaura, Yoshihiro Tsujimoto

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La 3 Ga 3 Ge 2 S 3 O 10 : An Ultraviolet Nonlinear Optical Oxysulfide Designed by Anion‐Directed Band Gap EngineeringOriginalNa4B8O9F10: A Deep‐Ultraviolet Transparent Nonlinear Optical Fluorooxoborate with Unexpected Short Phase‐Matching Wavelength Induced by Optimized Chromatic Dispersion133Na4B8O9F10: A Deep‐Ultraviolet Transparent Nonlinear Optical Fluorooxoborate with Unexpected Short Phase‐Matching Wavelength Induced by Optimized Chromatic Dispersion13Metal oxyhalides: an emerging family of nonlinear optical materials124Phase 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 of a promising oxychalcogenide infrared nonlinear optical crystal60Synthesis, structural evolution and optical properties of a new family of oxychalcogenides [Sr 3 VO 4 ][MQ 3 ] (M = Ga, In, Q = S, Se)10Sr3[SnOSe3][CO3]: A Heteroanionic Nonlinear Optical Material Containing Planar π‐conjugated [CO3] and Heteroleptic [SnOSe3] Anionic Groups78Sr3[SnOSe3][CO3]: A Heteroanionic Nonlinear Optical Material Containing Planar π‐conjugated [CO3] and Heteroleptic [SnOSe3] Anionic Groups7Enhanced 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 LiInSe232Improved Polarization in the Sr6Cd2Sb6O7Se10 Oxyselenide through Design of Lateral Sublattices for Efficient Photoelectric Conversion4Improved Polarization in the Sr6Cd2Sb6O7Se10 Oxyselenide through Design of Lateral Sublattices for Efficient Photoelectric Conversion16First 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 Balance56Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2(AE = Sr and Ba)24Design of novel deep-UV nonlinear optical materials with one-dimensional functional module [BO2]∞ chain and fluorine-driven short phase-matching43Characterizations and Nonlinear-Optical Properties of Pentanary Transition-Metal Oxysulfide Sr2CoGe2OS626Synthesis and Characterization of Heat-Tempered Cu2Zn0.6Ca0.4SnS4 Alloy Thin Film0Predicting Diamond-like Nitrides as Infrared Nonlinear Optical Materials with High Thermal Conductivity20A High‐Performance Nonlinear Optical Crystal with a Building Block Containing Expanded π‐Delocalization95A High‐Performance Nonlinear Optical Crystal with a Building Block Containing Expanded π‐Delocalization5Ba5Ga2SiO4S6: 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 UV solar-blind nonlinear optical crystal with confined π-conjugated groups13The first quaternary rare-earth oxythiogermanate with second-harmonic generation and ferromagnetic behavior26Recent 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 Performance64Unbiased 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 Chalcogenides48Shooting mid-infrared nonlinear optical materials with targeted balance performances in ternary d0-transition metal oxides through first-principles13An interlinked prediction-experiment paradigm discovering deep-ultraviolet fluorooxoborates with desired optical nonlinearity and birefringence76Comprehensive review on multiple mixed-anion ligands, physicochemical performances and application prospects in metal oxysulfides32Mixed Rare-Earth Chalcogenide Borate Eu9–xRExMgS2B20O41 (RE = Sm, Gd) Featuring a 3D {[B20O41]22–}∞ Framework Connected by [B6O9(O0.5)6]6– and [B7O13(O0.5)3]8– Clusters7From Monofluorophosphates A2PO3F to Difluorophosphates APO2F2 (A = alkali metal): Design of a Potential Deep-Ultraviolet Nonlinear Optical Materials System with a Shortened Phase-Matching Wavelength41Eu 2 MGe 2 OS 6 (M = Mn, Fe, Co): Three Melilite-Type Rare-Earth Oxythiogermanates Exhibiting Balanced Nonlinear-Optical Behaviors21Cation and anion co-partial substitution induced centrosymmetric to noncentrosymmetric structural transformation to construct nonlinear-optical rare-earth oxythiogermanates13Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70Ba10In2Mn11Si3O12S18: First Hexanary Oxychalcogenide Containing an Infrequent Three-Dimensional Noncentrosysmmetric Framework8LaMg6Ga6S16: a chemical stable divalent lanthanide chalcogenide70The 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 Response10Balanced 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 Groups6Flux Crystal Growth of Cation Deficient Ruddlesden-Popper Type Layered Oxysulfides: Ce2Zr2S2O5 and Nd2Zr2S2O50La 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 chalcogenidometalates8Accelerating Discovery of Infrared Nonlinear Optical Materials with High Lattice Thermal Conductivity: Combining Machine Learning and First‐Principles Calculations10Oxygen‐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 crystals54Design, Synthesis, and Improvement of Nonlinear Optical Properties from Aluminophosphite to Aluminophosphate1A Series of Pentanary Rare-Earth Oxysulfides Obtained by Heterovalent Cation and Anion Cosubstitution Exhibiting Nonlinear Optical Activity and Ultrawide Band Gaps1Eu(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 Oxysulfides8La(SO3NH2)2NO3·H2O: synergistic anion engineering of the first rare-earth nitrate sulfamate defying transparency-birefringence-nonlinearity trade-offs in ultraviolet nonlinear optics8[C(NH 2 ) 3 ] 2 PO 3 (OH): A Deep-Ultraviolet Birefringent Crystal Enabled by Synergy of π-Conjugated Cations and Heteroleptic Tetrahedra2A Homoatomic Heteroleptic Coordination Strategy for Exceptional Infrared Linear and Nonlinear Optical Properties in ANb 2 PS 4 (S 2 ) 3 (A = K,Rb,Cs)3Regulating KBBF-like structures via a charge-assisted hydrogen-bonded framework to enable easily grown ultraviolet nonlinear optical crystals0Synergistic dual-modification strategy of π-conjugated cations and tetrahedra: rational design of ultraviolet high-birefringence monofluorophosphates0Flux crystal growth of cation deficient Ruddlesden-Popper type layered oxysulfides: Ce2Zr2S2O5 and Nd2Zr2S2O50(C 5 H 7 N 2 ) (C 8 H 4 O 4 ) PbBr: Jahn–Teller Distortion‐Induced Tilting of π‐Conjugated Planes Resolving the Second‐Order Polarizability–Structural Anisotropy Conflicts13Structural Anion Geometry-Regulated Molecular Alignment in [C 10 H 8 NO 2 ]-Based Crystals for Enhancing Ultraviolet Birefringence0Symmetry Breaking Induced by Hydration-Number Tuning Enables Second-Order Nonlinear Optical Responses in Lanthanum Sulfate Hydrates0Exceptional Solar‐Blind Birefringence Engineered by Complementary Hydrogen‐Bond Ordering of π‐Conjugated Units0

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  4. 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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