论文标题
单分子连接中的非绝热振动效应：使用运动方法层次方程的理论研究
Nonadiabatic vibronic effects in single-molecule junctions: A theoretical study using the hierarchical equations of motion approach
论文作者
论文摘要
储层计算是预测湍流的有力工具，其简单的架构具有处理大型系统的计算效率。然而，其实现通常需要完整的状态向量测量和系统非线性知识。我们使用非线性投影函数将系统测量扩展到高维空间，然后将其输入到储层中以获得预测。我们展示了这种储层计算网络在时空混沌系统上的应用，该系统模拟了湍流的若干特征。我们表明，使用径向基函数作为非线性投影器，即使只有部分观测并且不知道控制方程，也能稳健地捕捉复杂的系统非线性。最后，我们表明，当测量稀疏、不完整且带有噪声，甚至控制方程变得不准确时，我们的网络仍然可以产生相当准确的预测，从而为实际湍流系统的无模型预测铺平了道路。
The interaction between electronic and vibrational degrees of freedom is an important mechanism in nonequilibrium charge transport through molecular nanojunctions. While adiabatic polaron-type coupling has been studied in great detail, new transport phenomena arise for nonadiabatic coupling scenarios corresponding to a breakdown of the Born-Oppenheimer approximation. Employing the numerically exact hierarchical equations of motion approach, we analyze the effect of nonadiabatic electronic-vibrational coupling on electron transport in molecular junctions considering a series of models with increasing complexity. The results reveal a significant influence of nonadiabatic coupling on the transport characteristics and a variety of interesting effects, including negative differential conductance. The underlying mechanisms are analyzed in detail.
