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RESEARCH PAPER · Angewandte Chemie International Edition · 2025

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

Jia-Xiang Zhang, Sheng‐Hua Zhou, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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Nonbonding Electron Inversion‐Driven Structural Engineering: Synergistic Enhancement of Linear and Nonlinear Optical PropertiesOriginalSynergistic Enhancement of Band Gap and Optical Anisotropy via Functional-Site Cosubstitution in Antiperovskite-Type Chalcohalides [Ba2K][X][MS4] (M = Ge, Si; X = Cl, Br)2Glass-Forming Ionic Liquid Crystal Gold–Carbon Nanocomposites with Ultrafast Optical Nonlinearity Sign Reversal1LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance14LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance3Reactive flux assisted metal oxide–boron–sulfur routine for syntheses of CsRESiS 4 (RE = Sm, Gd–Ho): featuring nonlinear optical activity and wide band gaps5A 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 electrons12A Homoatomic Heteroleptic Coordination Strategy for Exceptional Infrared Linear and Nonlinear Optical Properties in ANb 2 PS 4 (S 2 ) 3 (A = K,Rb,Cs)3[Rb 4 Cl][Cd 11 In 9 Se 26 ]: a salt inclusion chalcogenide with a diamond-like framework for infrared nonlinear optics0A series of langasite-type compounds: size effect regulation for cation occupation and enhanced SHG response1Broadband infrared-transparent crystals enabled by heterologous isomorphic substitution0Charge-order-induced directional enhancement of non-diagonal second-order nonlinear optical tensor components2Counterion engineering in open-framework crystals: dual enhancement of birefringence and UV transparency in Cd–oxalate framework via cation substitution0Layered mixed-anion chalcohalides Pb 4 Sb 4 Q 9 Cl 2 (Q = S, Se): puckered 2D frameworks, indirect band gaps, and low thermal conductivity0SnCl 2 [SC(NH 2 ) 2 ]: lone-pair and hydrogen-bonding triggered chromophore assembling for dual optical optimization0van der Waals layered CuInP 2 S 6 as infrared nonlinear optical material1KHg 4 Ga 5 S 12 : A Diamond-like Tetrahedral Chalcogenide Exhibiting Giant Phase-Matching Second Harmonic Generation6Recent Progress in Hg-Based Oxysalt Crystals for Nonlinear Optics and Birefringence Applications5K 3 Mg 2 [K 6 MgCl 3 ][Ga 20 S 36 ]: A Diamond-like Framework Based on Mixed-Type Supertetrahedra for Excellent Nonlinear Optical Property1High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification6The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 115Heterovalent Coexistence‐Driven Symmetry Breaking and Dimensional Evolution: Designing Polar Heart‐Shaped Channels for Exceptional MFIR Nonlinear Optics5Interlayer Electronic Decoupling Unlocks Giant Birefringence in π‐Conjugated Metal‐Organic Frameworks0First‐Principles Investigation of the Structural, Electronic, Optical, Elastic, and Thermal Properties of Defect Diamond‐Like Hg 3 P 2 S 80Eu5ZnGa6S15, Eu5Zn3Ga2Sn2S15, and Pb5HgGa6S15: Crystal Chemistry and Nonlinear Optical Properties0Domino‐Effect Amplification via Covalent‐Chain Engineering for Giant Birefringence in NaAsQ 2 (Q = S, Se) Crystals0

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  1. Synergistic Enhancement of Band Gap and Optical Anisotropy via Functional-Site Cosubstitution in Antiperovskite-Type Chalcohalides [Ba2K][X][MS4] (M = Ge, Si; X = Cl, Br)

    Inorganic Chemistry · 2025-08-26

    Yong‐Fang Shi, Shenghua Zhou, Xintao Wu, Hua Lin, Qi‐Long Zhu

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  2. Glass-Forming Ionic Liquid Crystal Gold–Carbon Nanocomposites with Ultrafast Optical Nonlinearity Sign Reversal

    Journal of Composites Science · 2025-09-02

    Valentyn Rudenko, A. S. Tolochko, S. Bugaychuk, Dmytro Zhulai, Gertruda Vasylivna Klimusheva, Galina Yaremchuk, Tatyana A. Mirnaya, Yuriy A. Garbovskiy

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  3. LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance

    Angewandte Chemie International Edition · 2025-10-13

    Yuhan Hu, Ruixi Wang, Shuang Zhao, Yuzhuo Yang, Jingyu Guo, Li‐Ming Wu, Ling Chen

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  4. LiPb 3 GeS 4 Cl 3 : Quasi‐T 2 ‐Supertetrahedral 3D Framework Enabling Superior Optical Performance

    Angewandte Chemie · 2025-10-13

    Yuhan Hu, Ruixi Wang, Shuang Zhao, Yuzhuo Yang, Jingyu Guo, Li‐Ming Wu, Ling Chen

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  5. Reactive flux assisted metal oxide–boron–sulfur routine for syntheses of CsRESiS 4 (RE = Sm, Gd–Ho): featuring nonlinear optical activity and wide band gaps

    Inorganic Chemistry Frontiers · 2025-11-05

    Zhen-Cheng Wu, Fang-Xu Tian, Rui Xiao, Mao-Yin Ran, Wenlong Liu, Wen-Tong Chen, Sheng-Ping Guo

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  6. A high-performance IR nonlinear optical material Sr 3 MnGe 2 S 8 achieved via partial cation substitution-induced structural transformation

    Inorganic Chemistry Frontiers · 2025-11-14

    A-Lan Xu, Mao‐Yin Ran, Zuju Ma, Xin-Tao Wu, Hua Lin, Qi‐Long Zhu

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  7. Maximizing the second-harmonic generation response via coordination-induced localization of nonbonding electrons

    Chemical Science · 2025-11-17

    Jia-Xiang Zhang, A-Lan Xu, Yang Chi, Xin-Tao Wu, Hua Lin, Qi‐Long Zhu

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  8. 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)

    Inorganic Chemistry · 2025-12-31

    Yumiao Niu, Yan Chun Xiao, Yidan Chen, Chu Chu, Daqing Yang, Ying Wang, Bingbing Zhang

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  9. [Rb 4 Cl][Cd 11 In 9 Se 26 ]: a salt inclusion chalcogenide with a diamond-like framework for infrared nonlinear optics

    Dalton Transactions · 2026-01-01

    Pengzhi Xie, Qixian Ren, Junwei Feng, Hong Lei Du, Shuyi Mi

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  10. A series of langasite-type compounds: size effect regulation for cation occupation and enhanced SHG response

    Inorganic Chemistry Frontiers · 2026-01-01

    Zhi Deng, Nian‐Tzu Suen, Zhen‐Cheng Wu, Huizhi Gao, Sheng‐Ping Guo

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  11. Broadband infrared-transparent crystals enabled by heterologous isomorphic substitution

    Dalton Transactions · 2026-01-01

    B Yang, Ziqi Chen, Zhenjiang Lu, Juanjuan Lu

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  12. Charge-order-induced directional enhancement of non-diagonal second-order nonlinear optical tensor components

    Chemical Communications · 2026-01-01

    马祖驹, Zehui Fang, Zhenlong Xie, Jia-Xiang Zhang, Hua Lin

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  13. Counterion engineering in open-framework crystals: dual enhancement of birefringence and UV transparency in Cd–oxalate framework via cation substitution

    CrystEngComm · 2026-01-01

    Chenyuan Ma, Jingyi Xie, Zhi Fang, Meihong Duan

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  14. Layered mixed-anion chalcohalides Pb 4 Sb 4 Q 9 Cl 2 (Q = S, Se): puckered 2D frameworks, indirect band gaps, and low thermal conductivity

    Dalton Transactions · 2026-01-01

    Yen-Han Huang, Guan-Ruei Chen, Chi‐Shen Lee

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  15. SnCl 2 [SC(NH 2 ) 2 ]: lone-pair and hydrogen-bonding triggered chromophore assembling for dual optical optimization

    Dalton Transactions · 2026-01-01

    Xing-Yu Bi, Yuting Gao, Chenyuan Ma, Zhi Gang Fang, Meihong Duan

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  16. van der Waals layered CuInP 2 S 6 as infrared nonlinear optical material

    Chemical Communications · 2026-01-01

    Zheng-Tao Hu, 马祖驹, Xin‐Tao Wu, Qi‐Long Zhu, Hua Lin

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  17. KHg 4 Ga 5 S 12 : A Diamond-like Tetrahedral Chalcogenide Exhibiting Giant Phase-Matching Second Harmonic Generation

    Chemistry of Materials · 2026-02-03

    Weiping Guo, Chao Yang, Bingxuan Li, Hong‐Hua Cui, Lingyun Li, Yan Yu, Zhong‐Zhen Luo, Zhigang Zou

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  18. Recent Progress in Hg-Based Oxysalt Crystals for Nonlinear Optics and Birefringence Applications

    Inorganic Chemistry · 2026-04-15

    Peng-Fei Li, Y Wang, Naifeng Zhuang, Jiannian Yao, Yu‐Wu Zhong

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  19. K 3 Mg 2 [K 6 MgCl 3 ][Ga 20 S 36 ]: A Diamond-like Framework Based on Mixed-Type Supertetrahedra for Excellent Nonlinear Optical Property

    Chemistry of Materials · 2026-04-22

    Jun-Long Chen, Shao‐Min Pei, Xiao‐Ming Jiang, Bin‐Wen Liu, Guo-Cong Guo

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  20. High‐Performance Infrared Nonlinear Optical Crystals Discovery Guided by High‐Throughput Computation, Machine Learning, and Experimental Verification

    Angewandte Chemie International Edition · 2026-04-24

    Yan Xiao, Zhaoxi Yu, Yumiao Niu, Yidan Chen, Lin Shen, Daqing Yang, Ying Wang, Bingbing Zhang

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  21. The Power of Pnictogen Bond: As─As Linkages Drive Wide Bandgap, Strong NLO Response and Large Birefringence in SrGa 3 Si 4 As 11

    Angewandte Chemie International Edition · 2026-04-25

    Hongshan Wang, Miriding Mutailipu, Shilie Pan, Junjie Li

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  22. Heterovalent Coexistence‐Driven Symmetry Breaking and Dimensional Evolution: Designing Polar Heart‐Shaped Channels for Exceptional MFIR Nonlinear Optics

    Laser & Photonics Review · 2026-05-14

    B R Zhang, Ping Feng, Sheng‐Hua Zhou, Xin-Tao Wu, Hua Lin, Qi‐Long Zhu

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  23. Interlayer Electronic Decoupling Unlocks Giant Birefringence in π‐Conjugated Metal‐Organic Frameworks

    Advanced Materials · 2026-06-18

    Jia-Xiang Zhang, Xinyan Wu, Weishan Li, Haolin Zhong, Jinkun Guo, Qingsheng Zeng, Mao‐Yin Ran, Ze‐Fan Yao, Yu‐Qing Zheng, Qingqing Ji, Jin‐Hu Dou

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  24. First‐Principles Investigation of the Structural, Electronic, Optical, Elastic, and Thermal Properties of Defect Diamond‐Like Hg 3 P 2 S 8

    Advanced Physics Research · 2026-07-23

    Saravana Karthikeyan SKS, Sankar Ganesh Ramaraj, Ryo Watanabe, Choji Fukuhara, Chang Yi Kong

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  25. Eu5ZnGa6S15, Eu5Zn3Ga2Sn2S15, and Pb5HgGa6S15: Crystal Chemistry and Nonlinear Optical Properties

    Inorganic Chemistry · 2026-08-12

    Xu‐Bin Ni, Qiu-Yang Du, Wen‐Dong Yao, Si Yang, Wen-Rui Zhou, Wenfeng Zhou, Ru‐Ling Tang, Sheng‐Ping Guo

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  26. Domino‐Effect Amplification via Covalent‐Chain Engineering for Giant Birefringence in NaAsQ 2 (Q = S, Se) Crystals

    Laser & Photonics Review · 2026-09-24

    Bo Zhang, Weiqi Huang, Yang Chi, Xin‐Tao Wu, Hua Lin, Qi‐Long Zhu

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