Sharma Devansh, Bose Amartya
Department of Chemical Sciences, Tata Institute of Fundamental Research, Mumbai 400005, India.
J Chem Theory Comput. 2025 Jun 24;21(12):5858-5866. doi: 10.1021/acs.jctc.5c00497. Epub 2025 Jun 12.
Efficiency of quantum transport through aggregates with multiple endpoints or traps proves to be an emergent and a highly nonequilibrium phenomenon. We present an exact approach for computing the emergent time-scale and amount of extraction specific to particular traps, leveraging a non-Hermitian generalization of the recently introduced state-to-state transport analysis [Bose and Walters, J. Chem. Theory Comput. 2023, , 15, 4828-4836]. This method is able to simultaneously account for the coupling between various sites, the many-body effects brought in by the vibrations and environment held at a nonzero temperature, and the local extraction processes described by non-Hermitian terms in the Hamiltonian. In fact, our non-Hermitian state-to-state analysis goes beyond merely providing an emergent loss time-scale. It can parse the entire dynamics into the constituent internal transport pathways and loss to the environment. We demonstrate this method using examples of exciton transport in a lossy polaritonic cavity. The loss at the cavity and the extraction of the exciton from a terminal molecule provide competing mechanisms that our method helps to unravel, revealing nonintuitive physics. This non-Hermitian state-to-state analysis technique contributes an important link to understanding and elucidating the routes of transport in open quantum systems.
通过具有多个端点或陷阱的聚集体进行量子传输的效率被证明是一种涌现的且高度非平衡的现象。我们提出了一种精确方法，用于计算特定陷阱所特有的涌现时间尺度和提取量，该方法利用了最近引入的态到态传输分析[Bose和Walters，《化学理论与计算杂志》，2023年，第15卷，4828 - 4836页]的非厄米推广。这种方法能够同时考虑不同位点之间的耦合、由处于非零温度的振动和环境所带来的多体效应，以及哈密顿量中非厄米项所描述的局部提取过程。实际上，我们的非厄米态到态分析不仅仅提供一个涌现的损失时间尺度。它可以将整个动力学解析为组成内部传输路径以及向环境的损失。我们使用有损极化子腔中激子传输的例子来演示这种方法。腔中的损失以及激子从终端分子的提取提供了相互竞争的机制，我们的方法有助于揭示这些机制，从而揭示出非直观的物理现象。这种非厄米态到态分析技术为理解和阐明开放量子系统中的传输路径提供了重要的一环。
