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Abstract The strong mutual coupling of and even the opposite change in the key parameters, such as the band gap ( E g ) and second‐order harmonic generation (SHG), leads to the extreme scarcity in high‐performance IR nonlinear optical (NLO) chalcogenides. Herein, we report 8 new sulfides, Na 2 Ba(Ag x Na 1− x ) 2 Sn 2 S 7 ( 1 , x =0; 1 series , x =0.1–0.6; Na 2 Ba(Li 0.58 Na 0.42 ) 2 Sn 2 S 7 , 1‐0.6Li ); Na 2 SrCu 2 Sn 2 S 7 ( 2 ); and Na 2 BaCu 2 Sn 2 S 7 ( 3 ). We use the structural tolerance factor ( ) to connect the chemical composition, crystal structure, and NLO properties. Guided by these correlations, a better balance between E g and SHG is realized in 1 , which exhibits a large E g of 3.42 eV and excellent NLO properties (SHG: 1.5×AGS; laser‐induced damage threshold: 12×AGS), representing the best performance among the known Hg‐ or As‐free sulfides to date.
Li et al. (Wed,) studied this question.