Li Kaixuan, Zhang Xingyu, Chai Binqiang, Yu Hongwei, Hu Zhanggui, Wang Jiyang, Wu Yicheng, Wu Hongping
Tianjin Key Laboratory of Functional Crystal Materials, Institute of Functional Crystal, College of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
Chemistry. 2025 Jan 2;31(1):e202403515. doi: 10.1002/chem.202403515. Epub 2024 Nov 11.
Two new non-centrosymmetric chalcogenides, ACuGaS (A=Rb, Cs) have been successfully synthesized by an "iterative substitution" strategy based on chalcopyrite CuFeS structural template. Benefiting from the substitution of Fe cations by Ga cations, ACuGaS (A = Rb, Cs) exhibit wide suitable band gap of 2.48 and 2.40 eV, respectively, which is about five times higher than their structure template CuFeS, and a large second harmonic generation response (1.5 and 1.8×AgGaS). Combining theoretical calculation and structural analysis confirms that the [GaS] tetrahedra make the main contribution on their good liner and nonlinear optical (NLO) performances. The "iterative substitution" strategy expands the design idea of materials and can lead to the discovery of a large number of IR NLO compounds.
基于黄铜矿CuFeS结构模板，通过“迭代取代”策略成功合成了两种新型非中心对称硫族化物ACuGaS（A = Rb，Cs）。受益于Ga阳离子对Fe阳离子的取代，ACuGaS（A = Rb，Cs）分别表现出2.48和2.40 eV的宽合适带隙，这比其结构模板CuFeS高约五倍，并且具有大的二次谐波产生响应（1.5和1.8×AgGaS）。结合理论计算和结构分析证实，[GaS]四面体对其良好的线性和非线性光学（NLO）性能起主要作用。“迭代取代”策略扩展了材料的设计理念，并可导致发现大量红外NLO化合物。
