Non-Equilibrium Dynamics of Correlated Electron Transfer in Molecular Chains

TL;DR

This paper investigates the non-equilibrium relaxation dynamics of correlated electron transport in molecular chains using an advanced path integral Monte Carlo method, revealing how correlations and dissipation influence thermalization and control in quantum systems.

Contribution

It introduces a numerically exact PIMC approach to study correlated electron dynamics in a Hubbard chain coupled to a bosonic bath, highlighting the impact of particle statistics on thermalization.

Findings

Correlations and dissipation lead to non-Boltzmann equilibrium distributions.

Dynamics can be mapped onto a single particle motion, showing sensitivity to particle statistics.

Robust control schemes are possible in quantum aggregates based on these effects.

Abstract

The relaxation dynamics of correlated electron transport (ET) along molecular chains is studied based on a substantially improved numerically exact path integral Monte Carlo (PIMC) approach. As archetypical model we consider a Hubbard chain containing two interacting electrons coupled to a bosonic bath. For this generalization of the ubiquitous spin-boson model, the intricate interdependence of correlations and dissipation leads to non-Boltzmann thermal equilibrium distributions for many-body states. By mapping the multi-particle dynamics onto an isomorphic single particle motion this phenomenon is shown to be sensitive to the particle statistics and due to its robustness allows for new control schemes in designed quantum aggregates.