论文标题

电流引起的原子运动,结构不稳定性和电子连接分子电极界面上的负温度

Current-induced atomic motion, structural instabilities, and negative temperatures on molecule-electrode interfaces in electronic junctions

论文作者

Preston, Riley J., Kershaw, Vincent F., Kosov, Daniel S.

论文摘要

分子电子连接中的分子电极接口容易容易产生化学反应,结构变化和由电流引起的局部加热效应。这些可以用于设备功能,也可能是限制性能和设备寿命的过程。我们开发了一个非平衡的绿色基于功能的传输理论,其中中央区域原子和更重要的是,允许分子 - 电极接口上的原子移动。慢速核运动和快速电子动力学的时间尺度的分离可以使Wigner空间中的Kadanoff-Baym方程的代数解。结果,产生了对绝热计算的绿色功能的动态校正的分析表达式。这些动态校正不仅取决于瞬时分子几何形状,还取决于核速度。为了使理论方法完全自洽,使用相同的时间分离方法来开发以绝热绿色功能为角度的当前诱导力的绝热,耗散和随机成分的表达式。使用这些当前的诱导力,核自由度的运动方程是以langevin方程的形式施放的。该理论应用于建模分子电子连接。我们观察到,分子电极化学键的弹簧常数与相应电极的电子耦合强度之间的相互作用对于结构不稳定性的出现至关重要,因此,电流中的电报切换。确定模型参数的范围可以观察结构稳定的分子连接以及各种不同类型的电流诱导的电报切换。界面结构不稳定性也根据当前的噪声计算进行量化。

Molecule-electrode interfaces in molecular electronic junctions are prone to chemical reactions, structural changes, and localized heating effects caused by electric current. These can be exploited for device functionality or may be degrading processes that limit performance and device lifetime. We develop a nonequilibrium Green's function based transport theory in which the central region atoms and, more importantly, atoms on molecule-electrode interfaces are allowed to move. The separation of time-scales of slow nuclear motion and fast electronic dynamics enables the algebraic solution of the Kadanoff-Baym equations in the Wigner space. As a result, analytical expressions for dynamical corrections to the adiabatically computed Green's functions are produced. These dynamical corrections depend not only on the instantaneous molecular geometry but also on the nuclear velocities. To make the theoretical approach fully self-consistent, the same time-separation approach is used to develop expressions for the adiabatic, dissipative, and stochastic components of current-induced forces in terms of adiabatic Green's functions. Using these current induced forces, the equation of motion for the nuclear degrees of freedom is cast in the form of a Langevin equation. The theory is applied to model molecular electronic junctions. We observe that the interplay between the value of the spring constant for the molecule-electrode chemical bond and electronic coupling strength to the corresponding electrode is critical for the appearance of structural instabilities and, consequently, telegraphic switching in the electric current. The range of model parameters is identified to observe structurally stable molecular junctions as well as various different kinds of current-induced telegraphic switching. The interfacial structural instabilities are also quantified based on current noise calculations.

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