Sr6 Cd2 Sb6 O7 S10 : Strong SHG Response Activated by Highly Polarizable Sb/O/S Groups

Ruiqi Wang; Fei Liang; Fakun Wang; Yangwu Guo; Xian Zhang; Yi Xiao; Kejun Bu; Zheshuai Lin; Jiyong Yao; Tianyou Zhai; Fuqiang Huang

doi:10.1002/anie.201902806

Sr₆ Cd₂ Sb₆ O₇ S₁₀ : Strong SHG Response Activated by Highly Polarizable Sb/O/S Groups

Angew Chem Int Ed Engl. 2019 Jun 11;58(24):8078-8081. doi: 10.1002/anie.201902806. Epub 2019 May 8.

Authors

Ruiqi Wang¹, Fei Liang², Fakun Wang³, Yangwu Guo², Xian Zhang⁴, Yi Xiao¹, Kejun Bu⁵, Zheshuai Lin², Jiyong Yao², Tianyou Zhai³, Fuqiang Huang^{1

5}

Affiliations

¹ State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
² 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.
³ 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.
⁴ Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, Beijing, 100094, P. R. China.
⁵ 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.

PMID: 30985053
DOI: 10.1002/anie.201902806

Abstract

A new nonlinear optical (NLO) oxysulfide, Sr₆ Cd₂ Sb₆ O₇ S₁₀ , which contains the functional groups [SbO_x S_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 ns² electron configuration can serve as new functional building units in NLO materials and opens a new avenue for the design of other optoelectronic materials.

Keywords: antimony; nonlinear optical materials; oxysulfides; second-harmonic generation.