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Sr 6 Cd 2 Sb 6 O 7 S 10 : Strong SHG Response Activated by Highly Polarizable Sb/O/S Groups
Author(s) -
Wang Ruiqi,
Liang Fei,
Wang Fakun,
Guo Yangwu,
Zhang Xian,
Xiao Yi,
Bu Kejun,
Lin Zheshuai,
Yao Jiyong,
Zhai Tianyou,
Huang Fuqiang
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201902806
Subject(s) - photoluminescence , tetragonal crystal system , polarizability , second harmonic generation , materials science , nonlinear optical , crystal structure , crystallography , optoelectronics , laser , chemistry , optics , nonlinear system , physics , molecule , organic chemistry , quantum mechanics
Abstract A new nonlinear optical (NLO) oxysulfide, Sr 6 Cd 2 Sb 6 O 7 S 10 , which contains the functional groups [SbO x S 5− x ] 7− ( x =0, 1) with a 5s 2 electron configuration, is synthesized by a solid‐state reaction. This compound displays a phase‐matchable second harmonic generation (SHG) response four times stronger than AgGaS 2 (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 [SbOS 4 ] 7− and [SbS 5 ] 7− pyramids make the predominant contribution to the enhanced SHG effect. Among those, the [SbOS 4 ] 7− units with mixed anions make a larger contribution. This work proposes that oxysulfide groups with an n s 2 electron configuration can serve as new functional building units in NLO materials and opens a new avenue for the design of other optoelectronic materials.