Zimbovskaya Natalya A
Department of Physics and Electronics, University of Puerto Rico-Humacao, Puerto Rico.
J Chem Phys. 2005 Sep 15;123(11):114708. doi: 10.1063/1.2041387.
Long-distance electron transfer (ET) plays an important part in many biological processes. Also, fundamental understanding of ET processes could give grounds for designing miniaturized electronic devices. So far, experimental data on the ET mostly concern ET rates which characterize ET processes as a whole. Here, we develop a different approach which could provide more information about intrinsic characteristics of the long-range intramolecular ET. A starting point of the studies is an obvious resemblance between ET processes and electric transport through molecular wires placed between metallic contacts. Accordingly, the theory of electronic transport through molecular wires is applied to analyze characteristics of a long-range electron transfer through molecular bridges. Assuming a coherent electron tunneling to be a predominant mechanism of ET at low temperatures, it is shown that low-temperature current-voltage characteristics could exhibit a special structure, and the latter contains information concerning intrinsic features of the intramolecular ET. Using the Buttiker dephasing model within the scattering matrix formalism, we analyze the effect of dephasing on the electron transmission function and current-voltage curves.
长距离电子转移(ET)在许多生物过程中起着重要作用。此外,对电子转移过程的基本理解可为设计小型化电子设备提供依据。到目前为止,关于电子转移的实验数据大多涉及表征整个电子转移过程的转移速率。在此,我们开发了一种不同的方法,该方法可以提供有关远程分子内电子转移内在特性的更多信息。这些研究的出发点是电子转移过程与通过置于金属接触之间的分子线的电传输之间明显的相似性。因此,通过分子线的电子传输理论被应用于分析通过分子桥的长距离电子转移的特性。假设在低温下相干电子隧穿是电子转移的主要机制,结果表明低温电流 - 电压特性可能呈现出一种特殊结构,并且后者包含有关分子内电子转移内在特征的信息。使用散射矩阵形式体系内的布蒂克尔退相模型,我们分析了退相对电子传输函数和电流 - 电压曲线的影响。