Abstract
AbstractThe strong mutual coupling of and even the opposite change in the key parameters, such as the band gap (Eg) 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, Na2Ba[(AgxNa1−x)2Sn2S7] (1, x=0; 1 series, x=0.1–0.6; Na2Ba[(Li0.58Na0.42)2Sn2S7], 1‐0.6Li); Na2Sr[Cu2Sn2S7] (2); and Na2Ba[Cu2Sn2S7] (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 Eg and SHG is realized in 1, which exhibits a large Eg 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.
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