Center for Quantum Technology Research, School of Physics, Beijing Institute of Technology, Beijing 100081, China.
J Chem Phys. 2019 Mar 14;150(10):105102. doi: 10.1063/1.5045706.
We investigate exciton transport through one-dimensional molecular aggregates interacting strongly with a cavity mode. Unlike several prior theoretical studies treating the monomers as simple two-level systems, exciton-vibration coupling is explicitly included in the description of open quantum dynamics of the system. In the framework of the Holstein-Tavis-Cummings model with truncated vibrational space, we investigate the steady-state exciton transfer through both a molecular dimer and longer molecular chains. For a molecular dimer, we find that vibration-assisted exciton transfer occurs at strong exciton-cavity coupling regime where the vacuum Rabi splitting matches the frequency of a single vibrational quantum, whereas for longer molecular chains, vibration-assisted transfer is found to occur at the ultrastrong exciton-cavity coupling limit. In addition, finite relaxation of vibrational modes induced by the continuous phonon bath is found to further facilitate the exciton transport in vibrational enhancement regimes.
我们研究了一维分子聚集体与腔模的强相互作用下的激子输运。与之前将单体视为简单的双能级系统的几个理论研究不同,我们在系统的开放量子动力学描述中明确包含了激子-振动耦合。在截断振动空间的 Holstein-Tavis-Cummings 模型框架内,我们研究了通过分子二聚体和更长分子链的稳态激子转移。对于分子二聚体,我们发现振动辅助激子转移发生在强激子-腔耦合 regime 下,其中真空拉比分裂与单个振动量子的频率匹配,而对于更长的分子链,发现振动辅助转移发生在超强度激子-腔耦合极限下。此外,连续声子浴引起的振动模式的有限弛豫被发现进一步促进了振动增强 regime 中的激子输运。