发表机构
Department of Chemistry, Texas A&M University; Department of Chemistry, Columbia University（德克萨斯农工大学化学系; 哥伦比亚大学化学系）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本文提出非马尔可夫主方程方法，实现激子-极化激元全量子动力学模拟，捕捉声子诱导退相干与兰姆位移，并成功再现TIPS-并五苯中实验观察到的群速度重整化。
AI 中文摘要
激子-极化激元是一种混合光-物质准粒子，当材料与受限电场相互作用时形成，实验已证明其表现出在室温下依然稳健的介观尺度相干量子传播。然而，对这一现象进行不借助半经典近似的准确且直接的量子动力学模拟，在计算上代价过高，限制了在集体光-物质耦合下对声子、光子和电子之间丰富动力学相互作用的微观理解。为应对这一根本性挑战，我们发展了一种非马尔可夫主方程方法，能够实现非平衡激子-极化激元动力学的全量子力学模拟，并捕捉超出传统马尔可夫极限的声子诱导退相干和耗散。为完成此任务，我们开发了一种程序，其中波矢空间被粗粒化，密度矩阵的每个对角元素并行演化。为展示该方法的实用性，我们模拟了TIPS-并五苯中的激子-极化激元输运。我们发现，我们的方法合理捕捉了实验观察到的极化激元群速度重整化，该重整化源于声子诱导的非马尔可夫兰姆位移。我们进一步表明，这种重整化无法在传统马尔可夫理论中再现。
英文摘要
Exciton-polaritons, hybrid light-matter quasiparticles formed when a material interacts with a confined electric field, have experimentally been shown to exhibit mesoscale coherent quantum propagation that remains robust at room temperature. However, an accurate and direct quantum dynamical simulation of this phenomenon that does not resort to semi-classical approximations is prohibitively expensive computationally, limiting the microscopic understanding of the rich dynamical interplay among phonons, photons, and electrons under collective light-matter coupling. To address this fundamental challenge, we develop a non-Markovian master equation approach which enables the fully quantum mechanical simulation of non-equilibrium exciton-polariton dynamics and captures phonon-induced decoherence and dissipation beyond the conventional Markovian limit. To carry out this task, a procedure is developed in which the wave vector space is coarse-grained and each diagonal element of the density matrix is evolved in parallel. To demonstrate the utility of this approach, we simulate exciton-polariton transport in TIPS-pentacene. We find that our approach reasonably captures the experimentally observed renormalization of the polariton group velocity, which originates from the phonon-induced non-Markovian Lamb shift. We further show that this renormalization cannot be reproduced within conventional Markovian theories.
