Mg2In3Si2P7: A Quaternary Diamond-like Phosphide Infrared Nonlinear Optical Material Derived from ZnGeP2

Jindong Chen; Hongxiang Chen; Feng Xu; Liling Cao; Xiaotian Jiang; Shunda Yang; Yingshuang Sun; Xin Zhao; Chensheng Lin; Ning Ye

doi:10.1021/jacs.1c03930

Mg₂In₃Si₂P₇: A Quaternary Diamond-like Phosphide Infrared Nonlinear Optical Material Derived from ZnGeP₂

J Am Chem Soc. 2021 Jul 14;143(27):10309-10316. doi: 10.1021/jacs.1c03930. Epub 2021 Jul 1.

Authors

Jindong Chen^{1

2}, Hongxiang Chen^{3

4}, Feng Xu¹, Liling Cao^{1

2}, Xiaotian Jiang^{1

2}, Shunda Yang¹, Yingshuang Sun^{1

2}, Xin Zhao^{1

2}, Chensheng Lin¹, Ning Ye^{1

5

6}

Affiliations

¹ Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
² University of Chinese Academy of Sciences, Beijing 100049, China.
³ College of Materials, Fujian University of Technology, Fuzhou, Fujian 350108, China.
⁴ Fujian Key Laboratory of New Materials Preparation and Forming Technology, Fuzhou, Fujian 350118, China.
⁵ Tianjin Key Laboratory of Functional Crystal Materials, Institute of Functional Crystal, Tianjin University of Technology, Tianjin 300384, China.
⁶ Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, Fujian 350002, China.

PMID: 34196529
DOI: 10.1021/jacs.1c03930

Abstract

Balancing the second-harmonic generation (SHG) coefficient, band gap, and birefringence is a vital but addressable challenge for designing infrared nonlinear optical materials. By applying a "rigidity-flexibility coupling" strategy, a quaternary diamond-like phosphide, Mg₂In₃Si₂P₇, with wurtzite-type superstructure was successfully designed and synthesized. Remarkably, it achieved the rare coexistence of giant second-harmonic generation (2 × ZnGeP₂ and 7.1 × AgGaS₂), suitable band gap (2.21 eV), moderate birefringence (0.107), and wide IR transparent range (0.56-16.4 μm). First-principles calculations revealed that the giant SHG response and large birefringence can be attributed to the synergy of arrangement-aligned [InP₄] and [SiP₄] tetrahedra. This work not only opens a new avenue for designing advanced infrared nonlinear optical materials but also may spur more explorations on quaternary diamond-like pnictides.