Communication

Sr₆Cd₂Sb₆O₇S₁₀: Strong SHG Response Activated by Highly Polarizable Sb/O/S Groups

State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 P. R. China

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Dr. Fei Liang

Beijing Center for Crystal Research and Development, Key Lab of Functional Crystals and Laser Technology, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China

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Dr. Fakun Wang

State Key Laboratory of Material Processing and Die and Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074 P. R. China

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Yangwu Guo

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Dr. Xian Zhang

Corresponding Author

E-mail address: zhangxian@qxslab.cn

http://orcid.org/0000-0003-0681-8201

Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, Beijing, 100094 P. R. China

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Yi Xiao

State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 P. R. China

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Dr. Kejun Bu

CAS Key Laboratory of Materials for Energy Conversion and State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050 P. R. China

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Prof. Zheshuai Lin

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Jiyong Yao

Corresponding Author

E-mail address: jyao@pku.edu.cn

http://orcid.org/0000-0002-4802-5093

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Prof. Tianyou Zhai

Corresponding Author

E-mail address: zhaity@hust.edu.cn

http://orcid.org/0000-0003-0985-4806

State Key Laboratory of Material Processing and Die and Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074 P. R. China

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Prof. Fuqiang Huang

Corresponding Author

E-mail address: huangfq@pku.edu.cn

http://orcid.org/0000-0003-0526-5473

State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 P. R. China

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Dr. Ruiqi Wang

State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 P. R. China

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Dr. Fei Liang

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Dr. Fakun Wang

State Key Laboratory of Material Processing and Die and Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074 P. R. China

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Yangwu Guo

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Dr. Xian Zhang

Corresponding Author

E-mail address: zhangxian@qxslab.cn

http://orcid.org/0000-0003-0681-8201

Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, Beijing, 100094 P. R. China

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Yi Xiao

State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 P. R. China

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Dr. Kejun Bu

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Prof. Zheshuai Lin

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Jiyong Yao

Corresponding Author

E-mail address: jyao@pku.edu.cn

http://orcid.org/0000-0002-4802-5093

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Prof. Tianyou Zhai

Corresponding Author

E-mail address: zhaity@hust.edu.cn

http://orcid.org/0000-0003-0985-4806

State Key Laboratory of Material Processing and Die and Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074 P. R. China

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Prof. Fuqiang Huang

Corresponding Author

E-mail address: huangfq@pku.edu.cn

http://orcid.org/0000-0003-0526-5473

State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 P. R. China

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First published: 15 April 2019

https://doi.org/10.1002/anie.201902806

Citations: 12

Abstract

A new nonlinear optical (NLO) oxysulfide, Sr₆Cd₂Sb₆O₇S₁₀, which contains the functional groups [SbO_xS_5−x]⁷⁻ (x =0, 1) with a 5s² electron configuration, is synthesized by a solid‐state reaction. This compound displays a phase‐matchable second harmonic generation (SHG) response four times stronger than AgGaS₂ (AGS) under laser irradiation at 2.09 μm. Single‐crystal‐based optical measurements reveal a SHG intensity that can be tuned by temperature and novel photoluminescence properties. Theoretical analyses demonstrate that tetragonal [SbOS₄]⁷⁻ and [SbS₅]⁷⁻ pyramids make the predominant contribution to the enhanced SHG effect. Among those, the [SbOS₄]⁷⁻ units with mixed anions make a larger contribution. This work proposes that oxysulfide groups with an n s² electron configuration can serve as new functional building units in NLO materials and opens a new avenue for the design of other optoelectronic materials.