论文标题

分子连接中的电子传输:具有初始接触和相关性的广义Kadanoff-baym ansatz

Electronic transport in molecular junctions: The generalized Kadanoff-Baym ansatz with initial contact and correlations

论文作者

Tuovinen, Riku, van Leeuwen, Robert, Perfetto, Enrico, Stefanucci, Gianluca

论文摘要

广义的Kadanoff-Baym Ansatz(GKBA)提供了一种计算廉价的方法,可以在非平衡绿色功能的框架内模拟平衡量子系统。对于有限系统,最近已经克服了常规GKBA方法中忽略初始相关性的局限性[Phys。 Rev. B 98,115148(2018)]。但是,在量子运输的背景下,最初状态的联系性质,即连接到散装铅的连接,需要进一步扩展GKBA方法。在这项工作中,我们制定了一个GKBA方案,该方案包括无分区设置中的初始相关性。实际上,这意味着最初相关和接触的分子连接的平衡可以与实时演变分开。有关接触初始状态的信息通过对嵌入自我能源的内存积分进行明确评估,包括在不平衡计算中,可以执行该积分,而无需使用模拟时间和系统大小影响计算缩放。我们证明了开发的基于碳的分子连接中的方法,在该方法中,我们研究了电子相关性在瞬态电流特征中的作用。

The generalized Kadanoff-Baym ansatz (GKBA) offers a computationally inexpensive approach to simulate out-of-equilibrium quantum systems within the framework of nonequilibrium Green's functions. For finite systems the limitation of neglecting initial correlations in the conventional GKBA approach has recently been overcome [Phys. Rev. B 98, 115148 (2018)]. However, in the context of quantum transport the contacted nature of the initial state, i.e., a junction connected to bulk leads, requires a further extension of the GKBA approach. In this work, we lay down a GKBA scheme which includes initial correlations in a partition-free setting. In practice, this means that the equilibration of the initially correlated and contacted molecular junction can be separated from the real-time evolution. The information about the contacted initial state is included in the out-of-equilibrium calculation via explicit evaluation of the memory integral for the embedding self-energy, which can be performed without affecting the computational scaling with the simulation time and system size. We demonstrate the developed method in carbon-based molecular junctions, where we study the role of electron correlations in transient current signatures.

扫码加入交流群

加入微信交流群

微信交流群二维码

扫码加入学术交流群,获取更多资源