Short-Lived Electron Transfer in Donor-Bridge-Acceptor Systems

TL;DR

This paper explores time-dependent electron transfer in donor-bridge-acceptor systems, revealing non-perturbative effects, different interference patterns, and distinct transmission regimes not captured by traditional scattering theories.

Contribution

It provides new insights into electron transfer dynamics, especially for small bridges, challenging conventional perturbation-based approaches and identifying novel transmission behaviors.

Findings

Lack of destructive interference in certain arrangements

Featureless spectrum in wavepacket transmission

Identification of sequential and direct transmission regimes

Abstract

We investigate time-dependent electron transfer (ET) in benchmark donor-bridge-acceptor systems. For the small bridge sizes studied, we obtain results far different from the perturbation theory which underlies scattering-based approaches, notably a lack of destructive interference in the ET for certain arrangements of bridge molecules. We also calculate wavepacket transmission in the non-steady-state regime, finding a featureless spectrum, while for the current we find two types of transmission: sequential and direct, where in the latter, the current transmission increases as a function of the energy of the transferred electron, a regime inaccessible by conventional scattering theory.