论文标题

具有随机结构过渡的分子电子连接

Molecular electronic junctions with stochastic structural transitions

论文作者

Kosov, Daniel S.

论文摘要

我们提出了一种理论方法,包括分子结构波动的动态方面,例如形成和破坏氢键,异构化和动力学超分子结构,在非平衡的绿色功能电子传输计算中。结构过渡被视为一个随机电报过程,而利益的主要量是在实现随机过程中平均绿色的功能。使用Novikov-Furutsu功能随机演算法,我们得出了随机平均延迟的绿色功能的运动方程。因此,我们获得了通过过渡的电流的表达式,这不仅取决于观察特定分子结构的概率,还取决于动力学。但是,所提出的方法具有显着的限制 - 我们必须假设由左右电极产生的智障自我能力的虚构部分相互成比例。这显着限制了该理论的可能应用。几个例子说明了提出的方法。

We present a theoretical approach to include dynamical aspects of molecular structural fluctuations, such as, for example, forming and breaking hydrogen bonds, isomerizations, and dynamical supramolecular structures, in nonequilibrium Green's functions electron transport calculations. Structural transitions are treated as a stochastic telegraph process, and the primary quantity of interest is a retarded Green's function averaged over realizations of a stochastic process. Using the Novikov-Furutsu functional stochastic calculus method, we derive equations of motion for stochastically averaged retarded Green's function in closed form. Consequently, we obtain the expression for electric current averaged over transitions, which depends not only on probabilities of observing particular molecular structures but also on the dynamics. However, the proposed method has a significant limitation - we have to assume that the imaginary parts of retarded self-energies produced by left and right electrodes are proportional to each other; this significantly restricts possible applications of the theory. Several examples illustrate the proposed approach.

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