Nishiuchi Tomohiko, Sotome Hikaru, Shimizu Kazuto, Miyasaka Hiroshi, Kubo Takashi
Department of Chemistry, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka, 560-0043, Japan.
Division of Frontier Materials Science and Center for, Advanced Interdisciplinary Research, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka, 560-8531, Japan.
Chemistry. 2022 Jan 24;28(5):e202104245. doi: 10.1002/chem.202104245. Epub 2022 Jan 3.
We report the Negishi coupling based synthesis of 1,2,3-tri(9-anthryl)benzene derivatives containing three radially arranged anthracenes in a π-cluster. In the crystalline state of the unsubstituted derivative, intermolecular π-π and CH-π interactions between the anthracene units drive the formation of the two-dimensional packing structure. Owing to though-space π-conjugation between anthracene units, the substances have unique electronic properties. The excited-state dynamic behavior occurring between the three anthracene moieties, such as exciton localization/delocalization, was elucidated by means of transient absorption measurements and quantum chemical calculations. Interestingly, even though the three anthracenes are closely oriented with approximately 3.0 Å between their C-9 positions, exciton localization on two anthracene units is energetically favorable because of the flexible nature of the radially arranged aromatic rings.
我们报道了基于根岸偶联反应合成的1,2,3-三(9-蒽基)苯衍生物,其在一个π簇中含有三个呈放射状排列的蒽。在未取代衍生物的晶体状态下,蒽单元之间的分子间π-π和CH-π相互作用驱动了二维堆积结构的形成。由于蒽单元之间的穿越空间π共轭,这些物质具有独特的电子性质。通过瞬态吸收测量和量子化学计算阐明了三个蒽部分之间发生的激发态动力学行为,如激子定位/离域。有趣的是,尽管三个蒽在其C-9位置之间以约3.0 Å的距离紧密排列,但由于呈放射状排列的芳环具有柔性,激子在两个蒽单元上的定位在能量上是有利的。