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Synthesis, Crystal Structure, and Optical Properties of Noncentrosymmetric Na 2 ZnSnS 4 .
Inorganic Chemistry 2018 August 21
A new chalcogenide Na2 ZnSnS4 has been successfully synthesized by using Na2 S2 as reactive flux. Na2 ZnSnS4 crystallizes in the tetragonal system with space group of I4̅. Its cell parameters are a = 6.4835(6) Å and c = 9.134(1) Å. The structure is a derivative of AgGaS2 , in which the Ag+ ions are replaced by Na+ ions and the Ga3+ ions are replaced by Zn2+ and Sn4+ ions. All three cations are in seriously distorted tetrahedral geometry with a distortion factor (η = c/ a) of 1.4. Optical measurements show that the Na2 ZnSnS4 powder sample has a large transparent range from 0.8 to 25 μm and a wide band gap of 3.1 eV. It exhibits large second-harmonic generation intensity of 0.9 × AgGaS2 in the grain size range from 41 to 74 μm. First-principles calculation results reveal that the valence band maximum and conduction band minimum are mainly composed of S 3p, Zn 3d orbitals and Sn 5s, S 3p orbitals, respectively.
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