Large Heterogeneity Observed in Single Molecule Measurements of Intramolecular Electron Transfer Rates through DNA

Large Heterogeneity Observed in Single Molecule Measurements of Intramolecular Electron Transfer Rates through DNA
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DOI:
10.1246/bcsj.20220220
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发表时间:
2022-12-01
影响因子:
4
通讯作者:
Kawai, Kiyohiko
Kawai, Kiyohiko
中科院分区:
化学3区
文献类型:
--
作者:
Fan, Shuya;Takada, Tadao;Kawai, Kiyohiko

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目前对电子转移(ET)动力学的理解主要是基于模糊了潜在的单分子行为的系综测量。我们以前报道了系统的距离依赖性单分子ET测量,显示出很大的异质性。在这里,我们研究和讨论这种异质性更详细,并提出这是一个相当基本的现象,是很难解释的DNA构象的分布单独。这种异质性可能来自每个分子的独特性,或者它可能反映了ET动力学的不确定性。
Current understanding of electron transfer (ET) kinetics is largely based on ensemble measurements that obscure the underlying single-molecule behavior. We previously reported systematic distance-dependent single molecule ET measure-ments that show a large heterogeneity. Here we study and dis-cuss this heterogeneity in more detail and suggest that it is a rather fundamental phenomenon that is difficult to explain solely by the distribution of DNA conformations. This hetero-geneity may arise from the uniqueness of each molecule, or it may reflect the uncertainty of ET kinetics.