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RESEARCH PAPER · Chemical Science · 2022

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

Hedi Yang, Mao‐Yin Ran, Shenghua Zhou, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive propertiesOriginalInteresting dimensional transition through changing cations as the trigger in multinary thioarsenates displaying variable photocurrent response and optical anisotropy22Oxychalcogenides 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 performance29Ba5Ga2SiO4S6: a Phase-Matching Nonlinear Optical Oxychalcogenide Design via Structural Regulation Originated from Heteroanion Introduction25d6versus 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 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 materials23Dramatically improved optical anisotropy by realizing stereochemically active lone pairs in a sulfate system, K 2 SO 4 ·HIO 323LaAeAl 3 S 7 (Ae = Ca, Sr): Cairo pentagonal layered thioaluminates achieving a good balance between a strong second harmonic generation response and a wide bandgap23Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution30Polarization-dependent second harmonic generation in peptide crystals: effects of molecular packing5The first polyanion-substitution-driven centrosymmetric-to-noncentrosymmetric structural transformation realizing an excellent nonlinear optical supramolecule [Cd 4 P 2 ][CdBr 4 ]17LnLiSiS4 (Ln = La and Ce): Promising infrared nonlinear optical materials designed by aliovalent substitution from SrCdSiS437Recent 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 Performance64Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 423Nonlinear Optical Sulfides LiMGa8S14 (M = Rb/Ba, Cs/Ba) Created by Li+ Driven 2D Centrosymmetric to 3D Noncentrosymmetric Transformation20Na3SiS3F: A Wide Bandgap Fluorothiosilicate with Unique [SiS3F] Unit and High Laser‐Induced Damage Threshold39Recent advances in IR nonlinear optical chalcogenides with well-balanced comprehensive performance57Cs4Zn5P6S18I2: the Largest Birefringence in Chalcohalide Achieved by Highly Polarizable Nonlinear Optical Functional Motifs22Three-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 Emission24Ca2Ln(BS3)(SiS4) (Ln = La, Ce, and Gd): Mixed Metal Thioborate‐Thiosilicates as Well‐Performed Infrared Nonlinear Optical Materials29Double alkaline earth metals sulfide SrMgGeS4 with high laser-induced damage threshold and strong second-harmonic generation29Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application49Flexible Anionic Groups‐Activated Structure Dissymmetry for Strong Nonlinearity in Ln 2 Ae 3 M IV 3 S 12 Family16Chiral and Polar Duality Design of Heteroanionic Compounds: Sr18Ge9O5S31 Based on [Sr3OGeS3]2+ and [Sr3SGeS3]2+ Groups20Advances in Solid-State Nonlinear Optical Materials: From Fundamentals to Applications61Regulating the key performance parameters for Hg-based IR NLO chalcogenides via bandgap engineering strategy26Ga-based IR nonlinear optical materials: Synthesis, structures, and properties65Ba4Cd2Ge2Te9: A promising infrared functional crystal with large birefringent and photoluminescence properties2Multi-step cation substitution facilitating the exploration of potential infrared nonlinear optical materials6Rare-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 transformation23Structural strategy for advancing nonlinear optical effects in 1D-[MX 2 ] ∞ chains: internal distortion and atomic types2The first Hg-based oxychalcogenide Sr2HgGe2OS6: Achieving balanced IR nonlinear optical properties through synergistic cation and anion substitution28Old tree blossoms anew: Research progress on the structures and optical properties of ultraviolet selenites56Recent 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 Response28Realizing Excellent Infrared Nonlinear Optical Performance in Eu-Based Chalcogenides via Rational Cross Substitution Strategy26Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides22Impact of Sensitizer Yb3+ on Structural and Optical Properties of AE2SiO4 (AE = Ba, Ca, Sr) Orthosilicates3Emergent Mid‐Infrared Nonlinear Optical Candidates With Targeted Balance Performances18Exploring 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 chalcogenides11磷属红外非线性光学晶体带隙调控的可能策略（特邀）5SrZnGeSe 4 : a promising infrared nonlinear optical material with strong second harmonic generation and high laser-induced damage threshold4Nonbonding Electron Inversion‐Driven Structural Engineering: Synergistic Enhancement of Linear and Nonlinear Optical Properties3Nonbonding Electron Inversion‐Driven Structural Engineering: Synergistic Enhancement of Linear and Nonlinear Optical Properties26Research progress and future prospect of chalcogenides with large optical anisotropy46From Centrosymmetric Eu 2 Ga 2 S 5 to Noncentrosymmetric EuMg 6 Ga 6 S 16 via Introduction of Distorted MgS 6 Octahedron: Featuring Wide Bandgap and Nonlinear Optical Activity3Structure-property relationships in IR nonlinear optical chalcogenides with stereochemically active lone pairs29SrZnSiS4: Shattering the 4.0 eV Threshold toward Dual-Optimized Bandgap and Second-Harmonic Generation7SrZnGeSe4: An Infrared Nonlinear Optical Crystal Material with Wide Transmission Range and Large SHG Response7BaAl2MS6 (M = Si and Ge): the rational construction of diamond-like structures with ultrawide band gap by group-optimization approach6A high-performance IR nonlinear optical material Sr 3 MnGe 2 S 8 achieved via partial cation substitution-induced structural transformation2ABCQ4型硫属化物红外非线性光学材料的构效关系（特邀）0Effect of the cation-to-silicon ratio on structural transformation and optical performance in [NaSr 3 Cl 3 ][SiS 4 ] and [NaSr 4 SCl][Si 3 S 9 ]0van der Waals layered CuInP 2 S 6 as infrared nonlinear optical material1高性能硫属化物红外非线性光学材料构效关系（特邀）0SrMnGeS 4 : A Two-Dimensional Layered Chalcogenide with Magnetic Triangular Lattice0CdY 2 Si 2 S 8 : A Wide Bandgap IR NLO Material with d 10 Metal-Induced Structure Transformation from CS to NCS1Synergistic Distortion Engineering: Activating Nonlinear Optical Response in Quaternary Chalcogenides via Lattice‐Induced [MnS 4 ] Asymmetry2Heterovalent Coexistence‐Driven Symmetry Breaking and Dimensional Evolution: Designing Polar Heart‐Shaped Channels for Exceptional MFIR Nonlinear Optics5AgEuPS4: Unlocking the Centrosymmetric Shackle of Rare-Earth Thiophosphates via Microscopic Distortion Cascading for Enhanced Second-Harmonic Generation Response1d-f synergistic effect contributing record-high second-harmonic generation response in phase-matchable Mn-based chalcogenides0A Composition-Matched Intermediate Reveals Site-Specific Symmetry Evolution with Retained Second-Harmonic Generation in Supertetrahedral Sulfides0

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

    Inorganic Chemistry Frontiers · 2022-01-01

    Chao Zhang, Shenghua Zhou, Yu Xiao, Hua Lin, Yi Liu

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

    Inorganic Chemistry · 2022-09-21

    Hedi Yang, Shenghua Zhou, Mao‐Yin Ran, Xintao Wu, Hua Lin, Qi‐Long Zhu

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

    Chinese Chemical Letters · 2022-09-23

    Hong Chen, Mao‐Yin Ran, Shenghua Zhou, Xintao Wu, Hua Lin, Qi‐Long Zhu

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

    Inorganic Chemistry · 2022-12-16

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

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  5. d6versus d10, Which Is Better for Second Harmonic Generation Susceptibility? A Case Study of K2TGe3Ch8 (T = Fe, Cd; Ch = S, Se)

    Inorganic Chemistry · 2022-12-27

    Bingheng Ji, Fei Wang, Kui Wu, Bingbing Zhang, Jian Wang

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  6. [Sr 4 Cl 2 ][Si 3 S 9 ]: Ultrawide-bandgap salt-inclusion thiosilicate nonlinear optical material with unprecedented tri-polymerized [Si 3 S 9 ] clusters

    Journal of Materials Chemistry C · 2023-01-01

    Chenyao Zhao, Kui Wu, Yan Xiao, Bingbing Zhang, Haohai Yu, Huaijin Zhang

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  7. A new infrared nonlinear optical material BaZnGeS 4 with a wide band gap and large nonlinear optical response

    Inorganic Chemistry Frontiers · 2023-01-01

    Hongshan Wang, Xueting Pan, Wang Zhao, Yu Chu, Junjie Li

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  8. 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

    Inorganic Chemistry Frontiers · 2023-01-01

    Yong‐Fang Shi, Shenghua Zhou, Pengfei Liu, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  9. An overview of Mg-based IR nonlinear optical materials

    Inorganic Chemistry Frontiers · 2023-01-01

    Jiaxiang Zhang, Mao‐Yin Ran, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  10. Dramatically improved optical anisotropy by realizing stereochemically active lone pairs in a sulfate system, K 2 SO 4 ·HIO 3

    Inorganic Chemistry Frontiers · 2023-01-01

    Zhiyong Bai, Kang Min Ok

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  11. 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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  12. Melilite oxychalcogenide Sr 2 FeGe 2 OS 6 : a phase-matching IR nonlinear optical material realized by isomorphous substitution

    Inorganic Chemistry Frontiers · 2023-01-01

    Hedi Yang, Shenghua Zhou, Mao‐Yin Ran, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  13. Polarization-dependent second harmonic generation in peptide crystals: effects of molecular packing

    Physical Chemistry Chemical Physics · 2023-01-01

    Sujay Kumar Nandi, Samrat Roy, Bipul Pal, Debasish Haldar

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  14. 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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  15. LnLiSiS4 (Ln = La and Ce): Promising infrared nonlinear optical materials designed by aliovalent substitution from SrCdSiS4

    Materials Today Physics · 2023-01-21

    Ya‐Xiang Han, Chun‐Li Hu, Bingxuan Li, Jiang‐Gao Mao

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

    Coordination Chemistry Reviews · 2023-02-08

    Mao‐Yin Ran, A-Yang Wang, Wenbo Wei, Xintao Wu, Hua Lin, Qi‐Long Zhu

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

    Small · 2023-02-12

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

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  18. Optimal Design of Mid-Infrared Nonlinear-Optical Crystals: From SrZnSnSe 4 to SrZnSiSe 4

    Inorganic Chemistry · 2023-04-16

    Mengjie Ma, Junhui Dang, Yuandong Wu, Xiao‐Ming Jiang, Dajiang Mei

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  19. Nonlinear Optical Sulfides LiMGa8S14 (M = Rb/Ba, Cs/Ba) Created by Li+ Driven 2D Centrosymmetric to 3D Noncentrosymmetric Transformation

    Small · 2023-05-05

    Ming‐Shu Zhang, Bin‐Wen Liu, Xiao‐Ming Jiang, Guo‐Cong Guo

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  20. Na3SiS3F: A Wide Bandgap Fluorothiosilicate with Unique [SiS3F] Unit and High Laser‐Induced Damage Threshold

    Advanced Optical Materials · 2023-05-17

    Jiazheng Zhou, Linan Wang, Yu Chu, Hongshan Wang, Shilie Pan, Junjie Li

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  21. 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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  22. Cs4Zn5P6S18I2: the Largest Birefringence in Chalcohalide Achieved by Highly Polarizable Nonlinear Optical Functional Motifs

    Small · 2023-07-18

    Xian‐Dan Chai, Mingze Li, Shujuan Lin, Wen‐Fa Chen, Xiao‐Ming Jiang, Bin‐Wen Liu, Guo‐Cong Guo

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  23. Three-in-One Tetrahedral Functional Units Constructing Diamondlike Ag2In2SiS3.06Se2.94 with High-Performance Nonlinear-Optical Activity

    Inorganic Chemistry · 2023-08-10

    Jun Li, Wenfeng Zhou, Wen‐Dong Yao, Wenlong Liu, Sheng‐Ping Guo

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  24. ACd 4 Ga 5 Te 12 (A = K, Rb, Cs): Tellurides with a Strong Nonlinear Optical Response and Purple Emission

    Chemistry of Materials · 2023-08-29

    Mengran Sun, Wenhao Xing, Shyong K. Chen, Chunxiao Li, Wenhao Liu, Ming‐Hsien Lee, Jiyong Yao

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  25. Ca2Ln(BS3)(SiS4) (Ln = La, Ce, and Gd): Mixed Metal Thioborate‐Thiosilicates as Well‐Performed Infrared Nonlinear Optical Materials

    Small · 2023-09-19

    Ya‐Xiang Han, Chun‐Li Hu, Jiang‐Gao Mao

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  26. Double alkaline earth metals sulfide SrMgGeS4 with high laser-induced damage threshold and strong second-harmonic generation

    Materials Today Physics · 2023-09-29

    Hongshan Wang, Yu Chu, Xueting Pan, Zhihua Yang, Shilie Pan, Junjie Li

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  27. Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application

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

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  28. Flexible Anionic Groups‐Activated Structure Dissymmetry for Strong Nonlinearity in Ln 2 Ae 3 M IV 3 S 12 Family

    Small · 2023-10-24

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

    Advanced Science · 2023-12-08

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

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  30. Advances in Solid-State Nonlinear Optical Materials: From Fundamentals to Applications

    ACS Applied Optical Materials · 2023-12-12

    Hafiz Zohaib Aslam, Joseph T. Doane, Michael T. Yeung, Georgiy Akopov

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

    Chinese Chemical Letters · 2023-12-12

    A-Yang Wang, Shenghua Zhou, Mao‐Yin Ran, Xintao Wu, Hua Lin, Qi‐Long Zhu

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

    Coordination Chemistry Reviews · 2023-12-21

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  33. Ba4Cd2Ge2Te9: A promising infrared functional crystal with large birefringent and photoluminescence properties

    Journal of Alloys and Compounds · 2023-12-29

    Mengran Sun, Haojian Su, Wenhao Liu, Jiyong Yao

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  34. Multi-step cation substitution facilitating the exploration of potential infrared nonlinear optical materials

    Inorganic Chemistry Frontiers · 2024-01-01

    Ya‐Xiang Han, Chun‐Li Hu, Wen‐Tong Chen, Jiang‐Gao Mao

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

    Chemical Science · 2024-01-01

    Ping Feng, Jiaxiang Zhang, Mao‐Yin Ran, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  36. RbPbPS 4 : a promising IR nonlinear optical material achieved by lone-pair-cation-substitution-induced structure transformation

    Inorganic Chemistry Frontiers · 2024-01-01

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  37. Structural strategy for advancing nonlinear optical effects in 1D-[MX 2 ] ∞ chains: internal distortion and atomic types

    RSC Advances · 2024-01-01

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

    Materials Today Physics · 2024-04-17

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  39. Old tree blossoms anew: Research progress on the structures and optical properties of ultraviolet selenites

    Coordination Chemistry Reviews · 2024-06-15

    Pengfei Li, Chun‐Li Hu, Jiang‐Gao Mao, Fang Kong

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  40. Recent advances and future perspectives on rare-earth-based nonlinear optical materials with π-conjugated [XO3] (X = B, C, N) units

    Coordination Chemistry Reviews · 2024-07-03

    Bo Zhang, Mao‐Yin Ran, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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  41. Ag 2 GeS 3 : A Diamond‐Like Chalcogenide as an IR Nonlinear Optical Material with Outstanding Second‐Harmonic Generation Response

    Advanced Optical Materials · 2024-07-04

    Hong Chen, Mao‐Yin Ran, Shenghua Zhou, Xin‐Tao Wu, Hua Lin

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

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  43. Balanced IR Nonlinear Optical Performance Achieved by Cation–Anion Module Cosubstitution in V-Based Salt-Inclusion Oxychalcogenides

    Chemistry of Materials · 2024-12-03

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  44. Impact of Sensitizer Yb3+ on Structural and Optical Properties of AE2SiO4 (AE = Ba, Ca, Sr) Orthosilicates

    Journal of Fluorescence · 2024-12-19

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

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  46. Exploring new horizons in mid-to-far infrared nonlinear optical crystals: the significant potential of trigonal pyramidal [TeS 3 ] 2− functional units

    Chemical Science · 2025-01-01

    Bo Zhang, Sheng-Hua Zhou, Bingxuan Li, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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

    Inorganic Chemistry Frontiers · 2025-01-01

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  48. 磷属红外非线性光学晶体带隙调控的可能策略（特邀）

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  49. SrZnGeSe 4 : a promising infrared nonlinear optical material with strong second harmonic generation and high laser-induced damage threshold

    Optics Express · 2025-03-27

    Hongshan Wang, Ran An, Yi Du, Shilie Pan, Junjie Li

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  50. Nonbonding Electron Inversion‐Driven Structural Engineering: Synergistic Enhancement of Linear and Nonlinear Optical Properties

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