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Time‐Resolved Interception of Multiple‐Charge Accumulation in a Sensitizer–Acceptor Dyad
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2017-11-15 , DOI: 10.1002/anie.201706564
Stéphanie Mendes Marinho 1 , Minh-Huong Ha-Thi 2 , Van-Thai Pham 2, 3, 4 , Annamaria Quaranta 5 , Thomas Pino 2 , Christophe Lefumeux 2 , Thierry Chamaillé 2 , Winfried Leibl 5 , Ally Aukauloo 1, 5
Affiliation  

Biomimetic models that contain elements of photosynthesis are fundamental in the development of synthetic systems that can use sunlight to produce fuel. The critical task consists of running several rounds of light‐induced charge separation, which is required to accumulate enough redox equivalents at the catalytic sites for the target chemistry to occur. Long‐lived first charge‐separated state and distinct electronic signatures for the sequential charge accumulated species are essential features to be able to track these events on a spectroscopic ground. Herein, we use a double‐excitation nanosecond pump–pump–probe experiment to interrogate two successive rounds of photo‐induced electron transfer on a molecular dyad containing a naphthalene diimide (NDI) linked to a [Ru(bpy)3]2+ (bpy=bipyridine) chromophore by using a reversible electron donor. We report an unprecedented long‐lived two‐electron charge accumulation (t=200 μs).

中文翻译:

敏化器-受体二元组中多电荷累积的时间分辨拦截

包含光合作用元素的仿生模型是可以使用阳光产生燃料的合成系统开发的基础。关键任务包括运行几轮光诱导的电荷分离,这需要在催化部位积累足够的氧化还原当量,以进行目标化学反应。长寿命的第一个电荷分离状态和连续的电荷累积物种的独特电子签名是能够在光谱基础上跟踪这些事件的基本特征。本文中,我们使用双激发纳秒泵浦-泵浦-探针实验,对包含与[Ru(bpy)3 ] 2+连接的萘二酰亚胺(NDI)的分子二元组上的两个连续的光诱导电子转移进行询问。(bpy =联吡啶)发色团通过使用可逆电子给体。我们报道了前所未有的长寿命双电子电荷积累(t = 200μs)。
更新日期:2017-11-15
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