Tailored synthesis of nonlinear optical quaternary chalcohalides: Ba4Ge3S9Cl2, Ba4Si3Se9Cl2and Ba4Ge3Se9Cl2.
Three novel zero-dimensional quaternary chalcohalides, Ba4Ge3S9Cl2, Ba4Si3Se9Cl2and Ba4Ge3Se9Cl2, which crystallize in the polar noncentrosymmetric space group P63(no. 173), have been rationally synthesized by a tailored approach on the basis of unique [M3Q9]6-(M = Ge, Q = S; M = Ge/Si, Q = Se) units with Ba2+cations and Cl-anions occupying the interspaces. The [M3Q9]6-units which consist of three Q-corner-sharing [MQ4]4-tetrahedra, are arranged along the 63screw axis. Remarkably, Ba4Ge3S9Cl2exhibits a strong powder second harmonic generation (SHG) response that is 2.4 times that of benchmark AgGaS2at a laser radiation of 2.05 μm in the same particle size range of 46-74 μm. Furthermore, theoretical studies based on the density functional theory helped to gain insight into the origin of the SHG.
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn and University of Chinese Academy of Sciences, Beijing 100039, People's Republic of China.
Peng-Fei
http://orcid.org/0000-0002-9170-5238
PF
Liu
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn.
Yan-Yan
YY
Li
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn and University of Chinese Academy of Sciences, Beijing 100039, People's Republic of China.
Yu-Jun
YJ
Zheng
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn and University of Chinese Academy of Sciences, Beijing 100039, People's Republic of China.
Ju-Song
JS
Yu
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn and University of Chinese Academy of Sciences, Beijing 100039, People's Republic of China.
Rui-Huan
http://orcid.org/0000-0003-4999-9735
RH
Duan
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn.
Hong
H
Chen
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn.
Hua
H
Lin
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn.
Ling
http://orcid.org/0000-0002-1195-1114
L
Chen
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China. liming_wu@fjirsm.ac.cn.
Li-Ming
http://orcid.org/0000-0002-3464-6032
LM
Wu