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Singlet Fission in Enantiomerically Pure Pentacene Dimers
ChemPhotoChem ( IF 3.7 ) Pub Date : 2020-03-30 , DOI: 10.1002/cptc.202000016
Ilias Papadopoulos 1 , Yueze Gao 2 , Constantin Hetzer 3 , Rik R. Tykwinski 2 , Dirk M. Guldi 1
Affiliation  

Singlet fission (SF), that is, producing two triplet excited states (T1+T1) from a single singlet excited state (S1S0), has the potential to surpass the thermodynamic Shockley–Queisser limit for solar cells of 33 %. Of great relevance for singlet fission is the (S1S0)‐to‐1(T1T1) transformation as it is the key step in driving the efficiency of SF. In the current study, we focus on the control over intramolecular interactions in enantiomerically pure platinum linked pentacene dimers, (S,S)‐ and (R,R)‐cis‐Pt. Despite the internal heavy‐atom effect stemming from the presence of the Pt‐centered linkers, (S,S)‐ and (R,R)‐cis‐Pt undergo quantitative and solvent dependent formation of 1(T1T1). Implicit is an enantiomer‐independent SF mediation by means of a virtual CT intermediate in a superexchange mechanism. With the help of steady‐state and time‐resolved spectroscopic techniques, a kinetic model is developed to describe the entire deactivation pathway following photoexcitation of (S,S)‐ and (R,R)‐cis‐Pt.

中文翻译:

对映体纯的并五苯二聚体中的单重态裂变

单重态裂变(SF),即从一个单重态激发态(S 1 S 0)产生两个三重态激发态(T 1 + T 1),有可能超过33个太阳能电池的热力学Shockley-Queisser极限%。与单线态裂变密切相关的是(S 1 S 0)到1(T 1 T 1)的转换,因为它是提高SF效率的关键步骤。在当前的研究中,我们着重于对映体纯铂连接的并五苯二聚体S,S)-R,R)-顺式的分子内相互作用的控制-Pt。尽管由于存在以Pt为中心的接头而产生内部重原子效应,但S,S)-R,R)-顺式-Pt仍会定量和溶剂依赖性地形成1(T 1 T 1)。隐式是通过超交换机制中的虚拟CT中间体通过非对映体进行的SF介导。借助稳态和时间分辨光谱技术,开发了动力学模型来描述光激发S,S)-R,R)--Pt后的整个失活途径
更新日期:2020-03-30
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