Delocalization-Assisted Transport through Nucleic Acids in Molecular Junctions
Delocalization-Assisted Transport through Nucleic Acids in Molecular Junctions
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DOI：
10.1021/acs.biochem.1c00072
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发表时间：
2021-04-19
期刊：
影响因子：
2.9
通讯作者：
Waldeck, David H.
中科院分区：
文献类型：
--
作者：
Valdiviezo, Jesus;Clever, Caleb;Waldeck, David H.
通过分子的电荷流动是超分子机器功能的中心，核酸中的电荷传输与分子信号和DNA修复有关。我们研究电子通过核酸的输运，以了解共振和非共振载流子输运机制的相互作用。这项研究报道了具有Gblock结构的多肽核酸(PNA)的STM断裂连接测量，并将这些结果与以前的DNA双链结果进行了对比。G-块PNA双链的电导远高于相同序列的相应DNA双链的电导，但它们不像G-块DNA那样表现出强烈的奇偶依赖电导振荡。理论分析发现，与DNA双链相比，PNA的电导振荡幅度被抑制，这是因为PNA中G-块之间的电子耦合作用增加，以及PNA与电极的相互作用更强。G-嵌段PNA双链中的强相互作用对5 nm双链产生高达3%G(0)的分子电导，其中G(0)是电导量。
The flow of charge through molecules is central to the function of supramolecular machines, and charge transport in nucleic acids is implicated in molecular signaling and DNA repair. We examine the transport of electrons through nucleic acids to understand the interplay of resonant and nonresonant charge carrier transport mechanisms. This study reports STM break junction measurements of peptide nucleic acids (PNAs) with a Gblock structure and contrasts the findings with previous results for DNA duplexes. The conductance of G-block PNA duplexes is much higher than that of the corresponding DNA duplexes of the same sequence; however, they do not display the strong even-odd dependence conductance oscillations found in G-block DNA. Theoretical analysis finds that the conductance oscillation magnitude in PNA is suppressed because of the increased level of electronic coupling interaction between G-blocks in PNA and the stronger PNA-electrode interaction compared to that in DNA duplexes. The strong interactions in the G-block PNA duplexes produce molecular conductances as high as 3% G(0), where G(0) is the quantum of conductance, for 5 nm duplexes.