paper

A Non-Hermitian State-to-State Analysis of Transport in Aggregates with Multiple Endpoints

arXiv:2503.16115 · doi:10.1021/acs.jctc.5c00497

Abstract

Efficiency of quantum transport through aggregates with multiple end-points or traps proves to be an emergent and a highly non-equilibrium phenomenon. We present a numerically 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, 19, 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 non-zero 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 environment. We demonstrate this method using examples of an 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 extremely interesting non-intuitive physics. This non-Hermitian state-to-state analysis technique contributes an important link in understanding and elucidating the routes of transport in open quantum systems.

7 pages, 7 figures

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