A new chalcogenide NaZnSnS has been successfully synthesized by using NaS as reactive flux. NaZnSnS 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 AgGaS, in which the Ag ions are replaced by Na ions and the Ga ions are replaced by Zn and Sn 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 NaZnSnS 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 × AgGaS 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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