Fachbereich Physik und Wissenschaftliches Zentrum für Materialwissenschaften (WZMW), Philipps-Universität Marburg , Renthof 5, DE-35032 Marburg, Germany.
Institute of Experimental Physics I, Justus-Liebig-University Giessen , DE-35392 Giessen, Germany.
J Am Chem Soc. 2016 Dec 21;138(50):16224-16227. doi: 10.1021/jacs.6b10738. Epub 2016 Dec 6.
Highly directional white-light generation was recently reported for the organotin sulfide cluster [(StySn)S] (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)S] 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.
最近有报道称，有机锡硫化物簇[(StySn)S]（Sty = 对乙烯基苯基）可以产生高度定向的白光。这种效应被认为是由于材料的非晶态性质与反转对称自由 T/E 簇核（T = 四族元素，E = 硫族元素）的特定组合相结合，再加上连接配体，从而允许电子密度的π离域。从 T = Si 通过 Ge 到 Sn 以及从 R = 甲基通过苯基和对乙烯基苯基到 1-萘基的 T 和有机配体（R）的系统变化提供了更全面的视角。根据粉末 X 射线数据，在所提到的组合中，只有[(PhSi)S]是单晶。在这里，我们证明了非线性响应的微调能力，即从白光产生到二次谐波产生的转变，以及对白光性质的控制。这些作为 T、R 内电子密度的π离域以及分子固体的有序性的函数进行了研究。
