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RESEARCH PAPER · ACS Applied Materials & Interfaces · 2022

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

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Mixed-Anion-Oriented Design of LnMGa3S6O (Ln = La, Pr, and Nd; M = Ca and Sr) Nonlinear Optical Oxysulfides with Targeted Property BalanceOriginalThe Antiperovskite‐Type Oxychalcogenides Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se) with Large Second Harmonic Generation Responses and Wide Band Gaps68Ba5Ga2SiO4S6: 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 Groups35Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials181LaAeAl 3 S 7 (Ae = Ca, Sr): Cairo pentagonal layered thioaluminates achieving a good balance between a strong second harmonic generation response and a wide bandgap23The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]17The first quaternary rare-earth oxythiogermanate with second-harmonic generation and ferromagnetic behavior26Intense d‐p Hybridization in Nb3O15 Tripolymer Induced the Largest Second Harmonic Generation Response and Birefringence in Germanates51Intense d‐p Hybridization in Nb3O15 Tripolymer Induced the Largest Second Harmonic Generation Response and Birefringence in Germanates7Recent 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 Performance64Comprehensive review on multiple mixed-anion ligands, physicochemical performances and application prospects in metal oxysulfides32Recent progress of newly developed functional building units and corresponding nonlinear optical materials14Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance56[Ba4(S2)][ZnGa4S10]: Design of an Unprecedented Infrared Nonlinear Salt‐Inclusion Chalcogenide with Disulfide‐Bonds36Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit38Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit1Halide-Induced Band Gap Enhancement from Ba2SnSe4 to KBa2SnSe4Cl2A series of new rare-earth sulfide borates RE3S3BO3 (RE = Nd, Tb, Dy): Syntheses, structures and optical properties1Chiral and Polar Duality Design of Heteroanionic Compounds: Sr18Ge9O5S31 Based on [Sr3OGeS3]2+ and [Sr3SGeS3]2+ Groups20Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65Partial 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-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate70Polysulfide Anions [S x ] 2− ( x = 2, 3, 4, 5): Promising Functional Building Units for Infrared Nonlinear Optical Materials22Ba10In2Mn11Si3O12S18: First Hexanary Oxychalcogenide Containing an Infrequent Three-Dimensional Noncentrosysmmetric Framework8Infrared nonlinear optical materials with multiple strongly ionic cations5The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28Effects of different groups on phase-matching and SHG in “3+4” Pn materials0LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”36LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”5Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy26From [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 Materials10La 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 Performances17Isovalent 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 behavior5Hetero‐Anionic Oxychalcogenides with Structures and Properties Tuned by the O:S Ratio14Zero-Dimensional Oxyselenide Ba12[(Ga2OSe5)3(Si2O7)]: Enhanced Optical Anisotropy through Heteroanionic Engineering4Research progress and future prospect of chalcogenides with large optical anisotropy46A 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 Oxysulfides8Doubling Polarizability Anisotropy of The Tetrahedral Motifs to Achieve Phase Matching for Melilite-Type Compound2LnEuGa3OS6 (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 Ba3SnIIGe3O2S82Reactive flux assisted metal oxide–boron–sulfur routine for syntheses of CsRESiS 4 (RE = Sm, Gd–Ho): featuring nonlinear optical activity and wide band gaps5Unveiling anionic migration mechanisms governed by mixed-anion chemistry in melilite oxyfluorides2Ba 3 S[SnOS 3 ] and [Ba 2 Sn]S[Ge 2 O 7 ]: two antiperovskite oxychalcogenides with good IR nonlinear optical performances2High‐Throughput Discovery of Large Birefringence Materials in Mixed‐N Hf‐O Systems0A Homoatomic Heteroleptic Coordination Strategy for Exceptional Infrared Linear and Nonlinear Optical Properties in ANb 2 PS 4 (S 2 ) 3 (A = K,Rb,Cs)3Ba 4 Al 4 SnS 12 : balancing bandgap and nonlinear optical performance in thioaluminate via multifunctional group engineering0Ba 4 CdGa 2 S 6 F 4 : A Chalcohalide Birefringent Crystal with Large Band Gap Designed by the Cation and Anion Cosubstitution Strategy2High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification6High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification2Eu 2+ ‐Activated KGa 5 S 8 : A New Super‐Sensitive Green Emitting Phosphor for Pressure Sensing1Enhancing Quantum Efficiency of Narrow Band Green Emitting Phosphor SrGa 2 S 4 :Eu 2+ via Solid Solution Engineering for Wide Color Gamut 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  1. The Antiperovskite‐Type Oxychalcogenides Ae3Q[GeOQ3] (Ae = Ba, Sr; Q = S, Se) with Large Second Harmonic Generation Responses and Wide Band Gaps

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    Shaoxin Cui, Hongping Wu, Zhanggui Hu, Jiyang Wang, Yicheng Wu, Hongwei Yu

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  2. Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction

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    Yong‐Fang Shi, Shenghua Zhou, Bingxuan Li, Yi Liu, Xintao Wu, Hua Lin, Qi‐Long Zhu

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  3. Oxychalcogenides: A Promising Class of Materials for Nonlinear Optical Crystals with Mixed‐Anion Groups

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  4. Anisotropic structure building unit involving diverse chemical bonds: a new opportunity for high-performance second-order NLO materials

    Chemical Society Reviews · 2023-01-01

    Xin Liu, Yi‐Chang Yang, Mengyue Li, Ling Chen, Li‐Ming Wu

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  5. LaAeAl 3 S 7 (Ae = Ca, Sr): Cairo pentagonal layered thioaluminates achieving a good balance between a strong second harmonic generation response and a wide bandgap

    Inorganic Chemistry Frontiers · 2023-01-01

    Jingjing Xu, Kui Wu, Bingbing Zhang, Haohai Yu, Huaijin Zhang

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  6. The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]

    Chemical Science · 2023-01-01

    Zhixin Qiu, Zhe-Xiong Zheng, Xiao‐Ming Jiang, Bin‐Wen Liu, Guo‐Cong Guo

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  7. The first quaternary rare-earth oxythiogermanate with second-harmonic generation and ferromagnetic behavior

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    Mei Yang, Wen‐Dong Yao, Wenlong Liu, Sheng‐Ping Guo

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  8. Intense d‐p Hybridization in Nb3O15 Tripolymer Induced the Largest Second Harmonic Generation Response and Birefringence in Germanates

    Angewandte Chemie International Edition · 2023-01-05

    Kaichuang Chen, Chensheng Lin, Jindong Chen, Guangsai Yang, Haotian Tian, Min Luo, Tao Yan, Zhanggui Hu, Jiyang Wang, Yicheng Wu, Ning Ye, Guang Peng

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  9. Intense d‐p Hybridization in Nb3O15 Tripolymer Induced the Largest Second Harmonic Generation Response and Birefringence in Germanates

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  10. Recent progress in the design of IR nonlinear optical materials by partial chemical substitution: Structural evolution and performance optimization

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  11. Rational Design of a Rare‐Earth Oxychalcogenide Nd3[Ga3O3S3][Ge2O7] with Superior Infrared Nonlinear Optical Performance

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

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  12. Comprehensive review on multiple mixed-anion ligands, physicochemical performances and application prospects in metal oxysulfides

    Coordination Chemistry Reviews · 2023-04-05

    Jing Xu, Kui Wu

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  13. Recent progress of newly developed functional building units and corresponding nonlinear optical materials

    Chinese Journal of Structural Chemistry · 2023-05-11

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  14. Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance

    Materials Today Physics · 2023-05-26

    Hedi Yang, Mao‐Yin Ran, Wenbo Wei, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  15. [Ba4(S2)][ZnGa4S10]: Design of an Unprecedented Infrared Nonlinear Salt‐Inclusion Chalcogenide with Disulfide‐Bonds

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    Kaixuan Ding, Hongping Wu, Zhanggui Hu, Jiyang Wang, Yicheng Wu, Hongwei Yu

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  16. Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit

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  17. Improved Birefringence Activated by Tetrahedra Decorated with a Single Linear Unit

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  18. Halide-Induced Band Gap Enhancement from Ba2SnSe4 to KBa2SnSe4Cl

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  19. A series of new rare-earth sulfide borates RE3S3BO3 (RE = Nd, Tb, Dy): Syntheses, structures and optical properties

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  20. Chiral and Polar Duality Design of Heteroanionic Compounds: Sr18Ge9O5S31 Based on [Sr3OGeS3]2+ and [Sr3SGeS3]2+ Groups

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    Shaoxin Cui, Hongping Wu, Xinkang Dong, Zhanggui Hu, Jiyang Wang, Yicheng Wu, Kenneth Reinhard Poeppelmeier, Hongwei Yu

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  21. Ga-based IR nonlinear optical materials: Synthesis, structures, and properties

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  22. 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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  23. Rare-earth-based chalcogenides and their derivatives: an encouraging IR nonlinear optical material candidate

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  24. Polysulfide Anions [S x ] 2− ( x = 2, 3, 4, 5): Promising Functional Building Units for Infrared Nonlinear Optical Materials

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  25. Ba10In2Mn11Si3O12S18: First Hexanary Oxychalcogenide Containing an Infrequent Three-Dimensional Noncentrosysmmetric Framework

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  26. Infrared nonlinear optical materials with multiple strongly ionic cations

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  27. The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution

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  28. Effects of different groups on phase-matching and SHG in “3+4” Pn materials

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  29. LiLnGeS 4 (Ln=La−Nd): Designing High Performance Infrared Nonlinear Optical Sulfides through “Band Reformation of AGS”

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  31. Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy

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  32. From [Ba3S][GeS4] to [Ba3CO3][MS4] (M = Ge, Sn): Enhancing optical anisotropy in IR birefringent crystals via functional group implantation

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  33. Rare-Earth/d10 Dual-Metal Oxychalcogenides as Infrared Nonlinear-Optical Materials

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  34. La 3 (Ga 3 S 3 O 3 )(Si 2 O 7 ): An Oxychalcogenide Demonstrating Ultrawide Optical Bandgap and Favorable Birefringence Propelled by Divergent Anionic Groups

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  35. Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances

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  36. Isovalent cation substitution drives structural transformation and infrared nonlinear optical activity in Eu-based chalcogenides

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  37. La 2 ZnGa 2 S 6 O: a melilite-type transition metal oxysulfide achieving a well-balanced nonlinear optical behavior

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  38. Hetero‐Anionic Oxychalcogenides with Structures and Properties Tuned by the O:S Ratio

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  39. Zero-Dimensional Oxyselenide Ba12[(Ga2OSe5)3(Si2O7)]: Enhanced Optical Anisotropy through Heteroanionic Engineering

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  42. Eu(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 Oxysulfides

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  43. Doubling Polarizability Anisotropy of The Tetrahedral Motifs to Achieve Phase Matching for Melilite-Type Compound

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  44. LnEuGa3OS6 (Ln = La, Pr, Nd): three dual rare earth metal-based oxychalcogenides with good IR nonlinear optical performances

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  45. Assembly of Highly Polarizable “Linkers” with Heteroleptic Groups for Inducing Large Optical Anisotropy in Ba2SnIIGe3O8S and Ba3SnIIGe3O2S8

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  47. Unveiling anionic migration mechanisms governed by mixed-anion chemistry in melilite oxyfluorides

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  48. Ba 3 S[SnOS 3 ] and [Ba 2 Sn]S[Ge 2 O 7 ]: two antiperovskite oxychalcogenides with good IR nonlinear optical performances

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  50. A Homoatomic Heteroleptic Coordination Strategy for Exceptional Infrared Linear and Nonlinear Optical Properties in ANb 2 PS 4 (S 2 ) 3 (A = K,Rb,Cs)

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