Trajectory Ensemble Methods Provide Single-Molecule Statistics for Quantum Dynamical Systems
Trajectory Ensemble Methods Provide Single-Molecule Statistics for Quantum Dynamical Systems
复制标题
轨迹系综方法为量子动力系统提供单分子统计
DOI：
10.1021/acs.jctc.1c00477
复制
发表时间：
2022
影响因子：
5.5
通讯作者：
Willard, Adam P.
中科院分区：
文献类型：
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作者：
Dodin, Amro;Provazza, Justin;Coker, David F.;Willard, Adam P.
能够在单分子水平上探测量子动力学的实验的出现需要开发能够模拟和分析这些动力学的新理论工具，而不仅仅是整体平均描述。在这篇文章中，我们提出了一个有效的方法来采样和模拟的单个量子系统的动力学，构成一个系综，并将其应用于研究无处不在的自旋玻色子模型的非平衡动力学。我们生成一个合奏的单系统的轨迹，我们分析这个轨迹合奏使用经典统计力学的工具。我们的研究结果表明，量子相干的动力学是高度异质性的单系统水平上，由于初始浴配置的变化，这显着影响系统和它的浴之间的相干性的瞬态交换。我们观察到，单系统往往保持一致性超过时间尺度长于合奏。我们还计算了一个新的热力学纠缠熵，量化有利于系统浴纠缠的热力学驱动力。
The emergence of experiments capable of probing quantum dynamics at the single-molecule level requires the development of new theoretical tools capable of simulating and analyzing these dynamics beyond an ensemble-averaged description. In this article, we present an efficient method for sampling and simulating the dynamics of the individual quantum systems that make up an ensemble and apply it to study the nonequilibrium dynamics of the ubiquitous spin-boson model. We generate an ensemble of single-system trajectories, and we analyze this trajectory ensemble using tools from classical statistical mechanics. Our results demonstrate that the dynamics of quantum coherence is highly heterogeneous at the single-system level due to variations in the initial bath configuration, which significantly affects the transient exchange of coherence between the system and its bath. We observe that single systems tend to retain coherence over time scales longer than that of the ensemble. We also compute a novel thermodynamic entanglement entropy that quantifies a thermodynamic driving force favoring system–bath entanglement.