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The typical chalcopyrite AgGaQ2 (Q = S, Se) are commercial infrared (IR) second‐order nonlinear optical (NLO) materials; however, they suffer from unexpected laser‐induced damage thresholds (LIDTs) primairy due to their narrow band gaps. Herein, what sets this apart from previously reported chemical substitutions is the utilization of an unusual cationic substitution strategy, represented by [[SZn...
Chalcohalides not only keep the balance between the nonlinear optical (NLO) coefficient and wide band gap, but also provide a promising solution to achieve sufficient birefringence for phase‐matching ability in NLO crystals. In this study, a novel chalcohalide, Cs4Zn5P6S18I2 (1) is successfully synthesized, by incorporating the highly electropositive Cs and the large electronegative I element into...
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