Driving force dependence of charge separation and recombination processes in dyads of nucleotides and strongly electron-donating oligothiophenes
Driving force dependence of charge separation and recombination processes in dyads of nucleotides and strongly electron-donating oligothiophenes
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核苷酸和强给电子低聚噻吩二元组中电荷分离和重组过程的驱动力依赖性
DOI：
10.1021/jp509691f
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发表时间：
2014
期刊：
影响因子：
--
通讯作者：
and Tetsuro Majima
中科院分区：
文献类型：
--
作者：
Shih-Hsun Lin;Mamoru Fujitsuka;Mayuka Ishikawa;and Tetsuro Majima
DNA中的电荷转移由于其在生物过程中的重要性而引起了科学家的极大关注。然而，与大量关于DNA中空穴转移的研究相比，我们对DNA中过量电子转移的了解仍然有限。为了用光化学技术阐明DNA中过量电子转移的动力学，需要开发新的给电子型光敏剂。在本论文中，一个三噻吩齐聚体和两个3，4-亚乙基二氧基噻吩齐聚体作为光敏剂用于包括天然碱基为电子受体的二元体中。用飞秒激光闪光光解研究了二极体中的电荷分离和复合过程，并在Marcus理论的基础上讨论了这些速率常数的驱动力关系。通过本研究发现构象对电荷复合过程的影响。我们期望3，4-亚乙基二氧基噻吩齐聚体在研究DNA中的过量电子转移动力学方面是有用的。
Charge transfer in DNA has attracted great attention of scientists because of its importance in biological processes. However, our knowledge on excess-electron transfer in DNA still remains limited in comparison to numerous studies of hole transfer in DNA. To clarify the dynamics of excess-electron transfer in DNA by photochemical techniques, new electron-donating photosensitizers should be developed. Herein, a terthiophene and two 3,4-ethylenedioxythiophene oligomers were used as photosensitizers in dyads including natural nucleobases as electron acceptors. The charge separation and recombination processes in the dyads were investigated by femtosecond laser flash photolysis, and the driving force dependence of these rate constants was discussed on the basis of the Marcus theory. From this study, the conformation effect on charge recombination process was found. We expect that 3,4-ethylenedioxythiophene oligomers are useful in investigation of excess-electron-transfer dynamics in DNA.