Cárdenas Valdivia Abel, Lirette Frédéric, Marín-Beloqui José M, Carreras Abel, Casanova David, Boismenu-Lavoie Joël, Morin Jean-François, Casado Juan
Department of Physical Chemistry, University of Málaga, Andalucia-Tech Campus de Teatinos s/n 29071 Málaga Spain
Département de Chimie, Université Laval 1045 Ave de la Médecine Québec G1V 0A6 Canada
Chem Sci. 2024 Dec 16;16(4):1925-1931. doi: 10.1039/d4sc06442a. eCollection 2025 Jan 22.
The synthesis, electrochemical, spectroelectrochemical, photophysical and light induced electron transfer reactions in two new anthanthrene quinodimethanes have been studied and analyzed in the context of dynamic electrochemistry. Their properties are dependent on the interconversion between folded and twisted forms, which are separated by a relatively small energy range, thus allowing to explore their interconversion by variable temperature measurements. The photophysics of these molecules is mediated by a diradical excited state with a twisted structure that habilitates rapid intersystem crossing. Moreover, when codissolved with an electron acceptor compound such as PCBM, direct anthanthrene to PCBM electron transfer and back-electron transfer are also observed, resulting in the formation of charged states and, then, a raise in the population of the excited state triplet manifold upon charge recombination. Some of these properties have been interpreted with the help of quantum chemical calculations. The existence of an equilibrium between folded and twisted states upon electrochemical and photoexcitation stimuli represents a novelty in comparison with existing literature on compounds also showing dynamic electrochemical properties.
在动态电化学的背景下,对两种新型蒽醌二甲烷中的合成、电化学、光谱电化学、光物理和光诱导电子转移反应进行了研究和分析。它们的性质取决于折叠形式和扭曲形式之间的相互转化,这两种形式由相对较小的能量范围隔开,因此可以通过变温测量来探索它们的相互转化。这些分子的光物理过程由具有扭曲结构的双自由基激发态介导,这种结构有利于快速的系间窜越。此外,当与电子受体化合物如PCBM共溶解时,还观察到从蒽到PCBM的直接电子转移和回电子转移,导致形成带电状态,然后在电荷复合时激发态三重态的数量增加。其中一些性质借助量子化学计算得到了解释。与现有关于也显示动态电化学性质的化合物的文献相比,电化学和光激发刺激下折叠态和扭曲态之间平衡的存在是一个新颖之处。