论文标题

激子和电荷传输动力学的部分偏极转化的量子主方程

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

论文作者

Jang, Seogjoo J.

论文摘要

Polaron转换的量子主方程(PQME)提供了一个统一的框架,以在环境自由度上以弱和强耦合的范围描述量子系统的动力学。因此,PQME是一种有效的方法,用于描述凝结或复杂环境中广泛参数的电荷和激子传输/传输动力学。但是,在某些情况下,在制剂中采用了极化子转化(PT)会引起缓慢模式的过度释放,并导致对重要相干项的过早抑制。在本工作中,通过采用部分PT来解决该问题的正式框架来解决此问题,该PT具有较小的低频浴模模式的重量。这里显示的是,包括所有不均匀术语的第二阶时时间内pqme的封闭形式表达式可以针对部分PT的一般形式得出,尽管比整个PT更为复杂。数值计算所需的所有表达式详细得出。在两级系统模型上的应用与谐波振荡器的浴缸相连,并且由于均匀放松项而着重于测试计算,证明了当前方法的可行性和实用性。

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.

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