利用非相干玻恩-马尔可夫速率模型的三位点系统的电子激励传递动力学。

IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL
Amit Kumar Upadhyay, Karthik Sasihithlu
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引用次数: 0

摘要

相干性在多点系统电子激发转移动力学中的作用通常是通过比较精确量子动力学方法的结果与非相干方法(如费米黄金法则(FGR)模型)的结果来研究的。最近关于三位点系统的研究[1,2]强调了EET动力学对特定构型的位点间耦合的显著依赖。为了探索相干性对这种行为的影响,我们采用了世俗的Redfield理论,通过系统地排除在站点基础上耦合种群和相干性的术语,建立了一个非相干模型。然后将该模型预测的动力学与相干林德布拉迪亚主方程和非相干FGR模型预测的动力学进行了比较。该框架提供了一种通用的方法来评估在弱系统池耦合状态下运行的大范围开放量子系统中相干性的作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Electronic Excitation Transfer Dynamics in a 3-Site System Using an Incoherent Born-Markov Rate Model.

The role of coherence in electronic excitation transfer (EET) dynamics in multi-site systems is typically investigated by comparing results from exact quantum dynamical methods with those derived from incoherent approaches such as the Fermi's Golden Rule (FGR) model. Recent studies on three-site systems have highlighted a remarkable dependence of EET dynamics on intersite coupling for specific configurations. To explore the influence of coherence in such behavior, we adapt the secular Redfield theory to develop an incoherent model by systematically excluding terms that couple populations and coherences in the site basis. The dynamics predicted by this model are then compared with those obtained from the coherent Lindbladian master equation and the incoherent FGR models. This framework provides a general approach for evaluating the role of coherence in a wide range of open quantum systems operating within the weak system-bath coupling regime.

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来源期刊
Chemphyschem
Chemphyschem 化学-物理:原子、分子和化学物理
CiteScore
4.60
自引率
3.40%
发文量
425
审稿时长
1.1 months
期刊介绍: ChemPhysChem is one of the leading chemistry/physics interdisciplinary journals (ISI Impact Factor 2018: 3.077) for physical chemistry and chemical physics. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies. ChemPhysChem is an international source for important primary and critical secondary information across the whole field of physical chemistry and chemical physics. It integrates this wide and flourishing field ranging from Solid State and Soft-Matter Research, Electro- and Photochemistry, Femtochemistry and Nanotechnology, Complex Systems, Single-Molecule Research, Clusters and Colloids, Catalysis and Surface Science, Biophysics and Physical Biochemistry, Atmospheric and Environmental Chemistry, and many more topics. ChemPhysChem is peer-reviewed.
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