Department of Chemistry and Cherry Emerson Center for Scientific Computation, Emory University, Atlanta, Georgia 30322, United States.
J Phys Chem Lett. 2023 Jun 22;14(24):5681-5691. doi: 10.1021/acs.jpclett.3c01082. Epub 2023 Jun 14.
We present a comprehensive study of the exciton wave packet evolution in disordered lossless polaritonic wires. Our simulations reveal signatures of ballistic, diffusive, and subdiffusive exciton dynamics under strong light-matter coupling and identify the typical time scales associated with the transitions between these qualitatively distinct transport phenomena. We determine optimal truncations of the matter and radiation subsystems required for generating reliable time-dependent data from computational simulations at an affordable cost. The time evolution of the photonic part of the wave function reveals that many cavity modes contribute to the dynamics in a nontrivial fashion. Hence, a sizable number of photon modes is needed to describe exciton propagation with a reasonable accuracy. We find and discuss an intriguingly common lack of dominance of the photon mode on resonance with matter in both the presence and absence of disorder. We discuss the implications of our investigations for the development of theoretical models and analysis of experiments where coherent intermolecular energy transport and static disorder play an important role.
我们对无序无损耗极化子线中激子波包演化进行了全面研究。我们的模拟揭示了在强光物质耦合下弹道、扩散和亚扩散激子动力学的特征，并确定了与这些定性不同的输运现象之间转换相关的典型时间尺度。我们确定了在可承受的成本下从计算模拟中生成可靠时变数据所需的物质和辐射子系统的最优截断。波函数的光子部分的时间演化表明，许多腔模以非平凡的方式对动力学做出贡献。因此，需要大量的光子模式来以合理的精度描述激子传播。我们发现并讨论了在存在和不存在无序的情况下，与物质共振的光子模式通常缺乏主导地位的情况。我们讨论了我们的研究对发展理论模型和分析实验的影响，其中相干的分子间能量输运和静态无序起着重要作用。
