AHgSnQ4 (A = Sr, Ba; Q = S, Se): A Series of Hg-Based Infrared Nonlinear-Optical Materials with Strong Second-Harmonic-Generation Response and Good Phase Matchability

Yangwu Guo; Fei Liang; Zhuang Li; Wenhao Xing; Zhe-Shuai Lin; Jiyong Yao; Arthur Mar; Yicheng Wu

doi:10.1021/acs.inorgchem.9b01572

AHgSnQ₄ (A = Sr, Ba; Q = S, Se): A Series of Hg-Based Infrared Nonlinear-Optical Materials with Strong Second-Harmonic-Generation Response and Good Phase Matchability

Inorg Chem. 2019 Aug 5;58(15):10390-10398. doi: 10.1021/acs.inorgchem.9b01572. Epub 2019 Jul 25.

Authors

Yangwu Guo^{1

2

3}, Fei Liang^{1

3}, Zhuang Li^{1

2

3}, Wenhao Xing^{1

2

3}, Zhe-Shuai Lin¹, Jiyong Yao^{1

2}, Arthur Mar⁴, Yicheng Wu^{1

5}

Affiliations

¹ Center for Crystal Research and Development, Key Laboratory of Functional Crystals and Laser Technology, Technical Institute of Physics and Chemistry , Chinese Academy of Sciences , Beijing 100190 , People's Republic of China.
² Center of Materials Science and Optoelectronics Engineering , University of Chinese Academy of Sciences , Beijing 100049 , People's Republic of China.
³ University of Chinese Academy of Sciences , Beijing 100190 , People's Republic of China.
⁴ Department of Chemistry , University of Alberta , Edmonton , Alberta T6G 2G2 , Canada.
⁵ Institute of Functional Crystal Materials , Tianjin University of Technology , Tianjin 300384 , People's Republic of China.

PMID: 31342744
DOI: 10.1021/acs.inorgchem.9b01572

Abstract

Four Hg-based IR nonlinear-optical materials, AHgSnQ₄ (A = Sr, Ba; Q = S, Se), were discovered and investigated systematically. Their structures are built of two-dimensional [HgSnQ₄]^2- layers, which are assembled alternately by distorted (HgQ₄ and SnQ₄) tetrahedra and separated by eight-coordinated A²⁺ cations. The two sulfides AHgSnS₄ (A = Ba, Sr) exhibit large second-harmonic-generation (SHG) responses (2.8 and 1.9 × AgGaS₂ at 2.09 μm), as well as large band gaps (2.77 and 2.72 eV). The two selenides AHgSnSe₄ (A = Ba, Sr) show even stronger SHG responses, about 5 times that of AgGaS₂. Furthermore, all four compounds show phase-matching behavior, and the results of first-principles calculation elucidate the key role of the HgQ₄ group in the enhanced SHG effect in β-BaHgSnS₄ and BaHgSnSe₄.