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DNA 电荷输运的中间隧穿-跳跃态

Intermediate tunnelling-hopping regime in DNA charge transport.

机构信息

1] Center for Biosensors and Bioelectronics, Biodesign Institute, Arizona State University, Tempe, Arizona 85287, USA [2] Department of Chemistry and Biochemistry, Arizona State University, Tempe, Arizona 85287, USA.

Center for Biosensors and Bioelectronics, Biodesign Institute, Arizona State University, Tempe, Arizona 85287, USA.

出版信息

Nat Chem. 2015 Mar;7(3):221-6. doi: 10.1038/nchem.2183.

Abstract

Charge transport in molecular systems, including DNA, is involved in many basic chemical and biological processes, and its understanding is critical if they are to be used in electronic devices. This important phenomenon is often described as either coherent tunnelling over a short distance or incoherent hopping over a long distance. Here, we show evidence of an intermediate regime where coherent and incoherent processes coexist in double-stranded DNA. We measure charge transport in single DNA molecules bridged to two electrodes as a function of DNA sequence and length. In general, the resistance of DNA increases linearly with length, as expected for incoherent hopping. However, for DNA sequences with stacked guanine-cytosine (GC) base pairs, a periodic oscillation is superimposed on the linear length dependence, indicating partial coherent transport. This result is supported by the finding of strong delocalization of the highest occupied molecular orbitals of GC by theoretical simulation and by modelling based on the Büttiker theory of partial coherent charge transport.

摘要

分子系统(包括 DNA)中的电荷输运涉及许多基本的化学和生物学过程,如果要将其用于电子设备,就必须对其加以理解。这一重要现象通常被描述为短距离下相干隧穿或长距离下非相干跳跃。在这里,我们证明双链 DNA 中存在两种过程共存的中间状态。我们通过测量连接到两个电极的单 DNA 分子中的电荷输运,来研究 DNA 序列和长度的函数关系。通常,DNA 的电阻随长度呈线性增加,这与非相干跳跃的预期一致。然而,对于具有堆叠鸟嘌呤-胞嘧啶(GC)碱基对的 DNA 序列,在线性长度依赖性上叠加了周期性振荡,表明存在部分相干输运。这一结果得到了理论模拟中 GC 最高占据分子轨道强烈离域的支持,也得到了基于部分相干电荷输运的 Büttiker 理论的建模支持。

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