Organotetrel Chalcogenide Clusters: Between Strong Second-Harmonic and White-Light Continuum Generation.
Organotetrel Chalcogenide Clusters: Between Strong Second-Harmonic and White-Light Continuum Generation.
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DOI：
10.1021/jacs.6b10738
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发表时间：
2016-12
影响因子：
15
通讯作者：
N. Rosemann;J. Eußner;E. Dornsiepen;S. Chatterjee;S. Dehnen
中科院分区：
文献类型：
--
作者：
N. Rosemann;J. Eußner;E. Dornsiepen;S. Chatterjee;S. Dehnen
最近报道了有机锡硫化物簇[(StySn)4S6]（Sty = 对苯乙烯基）的高度定向白光产生。这种效应暂时归因于材料的无定形性质以及无反演对称性的 T/E 簇核（T = tetrel，E = 硫属元素）与允许电子密度 π 离域的配体连接的特定组合。 T 和有机配体 (R) 的系统变化（从 T = Si 到 Ge 到 Sn，以及从 R = 甲基到苯基和对苯乙烯基到 1-萘基）提供了更全面的视图。根据粉末X射线数据，在指定的组合中，只有[(PhSi)4S6]是单晶的。在这里，我们演示了非线性响应的微调能力，即从白光生成变为二次谐波生成以及控制白光特性。这些被研究为 T、R 内电子密度的 π 离域以及分子固体内的顺序的函数。
Highly directional white-light generation was recently reported for the organotin sulfide cluster [(StySn)4S6] (Sty = p-styryl). This effect was tentatively attributed to the amorphous nature of the material in combination with the specific combination of an inversion-symmetry-free T/E cluster core (T = tetrel, E = chalcogen) with the attachment of ligands that allow π delocalization of the electron density. Systematic variation of T and the organic ligand (R) that runs from T = Si through Ge to Sn and from R = methyl through phenyl and p-styryl to 1-naphthyl provides a more comprehensive view. According to powder X-ray data, only [(PhSi)4S6] is single-crystalline among the named combinations. Here we demonstrate the fine-tuneability of the nonlinear response, i.e., changing from white-light generation to second-harmonic generation as well as controlling the white-light properties. These are investigated as a function of T, π delocalization of the electron density within R, and the order within the molecular solids.