Quantum Coherence Enhances Electron Transfer Rates to Two Equivalent Electron Acceptors
Quantum Coherence Enhances Electron Transfer Rates to Two Equivalent Electron Acceptors
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DOI：
10.1021/jacs.9b06166
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发表时间：
2019-08-07
影响因子：
15
通讯作者：
Wasielewski, Michael R.
中科院分区：
文献类型：
--
作者：
Phelan, Brian T.;Zhang, Jinyuan;Wasielewski, Michael R.
当一个分子电子给体与多个电子受体相互作用时，量子相干性可以提高电子转移速率。在这里，我们报告了一对供体-受体（D-A）化合物的光驱动ET率，这些化合物将一个蒽（An）供体与一个或两个等效的1,4-苯醌（BQ）受体连接起来。从An的最低激发单重态到2个BQ的亚皮秒ET在室温下的速度约为1 BQ的2.4倍，而在低温下则快约5倍。这个因子2的增加是由于室温下从ET到两个受体之一的转变，到低温下两个受体的叠加态和相关的系统浴波动。
When a molecular electron donor interacts with multiple electron acceptors, quantum coherence can enhance the electron transfer (ET) rate. Here we report photodriven ET rates in a pair of donor-acceptor (D-A) compounds that link one anthracene (An) donor to one or two equivalent 1,4-benzoquinone (BQ) acceptors. Subpicosecond ET from the lowest excited singlet state of An to two BQs is about 2.4 times faster than ET to one BQ at room temperature, but about 5 times faster at cryogenic temperatures. This factor of 2 increase results from a transition from ET to one of two acceptors at room temperature to ET to a superposition state of the two acceptors with correlated system-bath fluctuations at low temperature.