有机极化子物理学建模的均场和累积方法

Piper Fowler-Wright
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摘要

在本论文中,我们开发了多体开放量子系统的方法,并将其应用于有机极化子系统。这些方法采用均值场方法来降低大规模问题的维度。这种方法最初假定多体态中不存在相关性,并在此基础上从两个方面进行了改进。首先,我们展示了如何将均值场近似与矩阵积算子方法相结合,以高效模拟与多种环境强耦合的多体系统的非马尔可夫动力学。我们应用这种方法计算了一个现实有机激光器模型的阈值和光致发光。其次,我们通过对海森堡运动方程的累积展开,系统地纳入了高阶相关性,从而扩展了均场描述。对于具有多对一网络结构的多体系统,我们研究了这些展开在展开阶数和系统规模方面的有效性和收敛性。然后,我们展示了如何利用累积展开来计算有机极化子的空间分辨动力学。这使得我们能够研究有机极化子的传输,在其中我们观察到向暗激发子态的可逆转换和子群-velocitypropagation。这项工作中建立的方法为分析大型多体开放量子系统和研究有限尺寸效应提供了多功能工具。它们的应用揭示了强光-物质耦合和振动效应相互作用下有机极化子错综复杂的动力学。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Mean-field and cumulant approaches to modelling organic polariton physics
In this thesis we develop methods for many-body open quantum systems and apply them to systems of organic polaritons. The methods employ a mean-field approach to reduce the dimensionality of large-scale problems. Initially assuming the absence of correlations in the many-body state, this approach is built upon in two ways. First, we show how the mean-field approximation can be combined with matrix product operator methods to efficiently simulate the non-Markovian dynamics of a many-body system with strong coupling to multiple environments. We apply this method to calculate the threshold and photoluminescence for a realistic model of an organic laser. Second, we extend the mean-field description by systematically including higher-order correlations via cumulant expansions of the Heisenberg equations of motion. We investigate the validity and convergence properties of these expansions, both with respect to expansion order and system size, for many-body systems with many-to-one network structures. We then show how the cumulant expansions may be used to calculate spatially resolved dynamics of organic polaritons. This enables a study of organic polariton transport in which we observe reversible conversion to dark exciton states and sub-group-velocity propagation. The methods established in this work offer versatile tools for analysing large, many-body open quantum systems and investigating finite-size effects. Their application reveals the intricate dynamics of organic polaritons resulting from the interplay of strong light-matter coupling and vibrational effects.
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