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arXiv 2203.02812quant-phcond-mat.mes-hallphysics.bio-phphysics.chem-phphysics.comp-ph
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部分极化子变换的量子主方程用于激子和电荷传输动力学

Partially polaron-transformed quantum master equation for exciton and charge transport dynamics

Seogjoo J. Jang

AI总结:

本文提出了一种部分极化子变换方法,用于解决极化子变换在描述电荷和激子传输动力学时出现的过度弛豫问题。

摘要:

极化子变换的量子主方程(PQME)提供了一个统一的框架,用于描述量子系统在弱耦合和强耦合环境自由度极限下的动力学。因此,PQME成为了一种有效的方法,用于描述在凝聚或复杂环境中广泛参数范围内的电荷和激子转移/传输动力学。然而,在某些情况下,用于公式中的极化子变换(PT)会引发对慢模式的过度弛豫,并导致重要相干项的提前抑制。本文通过采用权重较低的低频浴模式的部分PT,开发了一个正式的框架来解决这个问题。在此,证明了对于一般形式的部分PT,可以推导出包含所有非均匀项的二阶时间局部PQME的闭合表达式,尽管比完全PT的表达式更复杂。所有需要数值计算的表达式都进行了详细推导。应用于两个能级系统耦合到谐振子浴的模型,测试计算集中在由均匀弛豫项引起的那些上,证明了本方法的可行性和实用性。

英文摘要:

Polaron-transformed quantum master equation (PQME) offers a unified framework to describe the dynamics of quantum systems in both limits of weak and strong couplings to environmental degrees of freedom. Thus, PQME serves as an efficient method to describe charge and exciton transfer/transport dynamics for a broad range of parameters in condensed or complex environments. However, in some cases, the polaron transformation (PT) being employed in the formulation invokes an over-relaxation of slow modes and results in premature suppression of important coherence terms. A formal framework to address this issue is developed in the present work by employing a partial PT that has smaller weights for low frequency bath modes. It is shown here that a closed form expression of a 2nd order time-local PQME including all the inhomogeneous terms can be derived for a general form of partial PT, although more complicated than that for the full PT. All the expressions needed for numerical calculation are derived in detail. Applications to a model of two-level system coupled to a bath of harmonic oscillators, with test calculations focused on those due to homogeneous relaxation terms, demonstrate the feasibility and the utility of the present approach.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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