Understanding the fundamental connection between electronic correlation and decoherence

TL;DR

This paper establishes a fundamental link between electronic correlation and quantum coherence in matter, revealing how electron interactions influence decoherence rates through exact simulations.

Contribution

It introduces a new theory connecting electron correlation with decoherence, highlighting conditions where effects decouple, and demonstrates this with precise simulations.

Findings

Electronic correlation affects decoherence rates.

Decoupling occurs when dynamics are pure-dephasing, i.e., [H^S, H^{SB}]=0.

Increasing electron interactions can either enhance or suppress coherence loss.

Abstract

We introduce a theory that exposes the fundamental and previously overlooked connection between the correlation among electrons and the degree of quantum coherence of electronic states in matter. For arbitrary states, the effects only decouple when the electronic dynamics induced by the nuclear bath is pure-dephasing in nature such that $[H^{S},H^{SB}]=0$, where $H^{S}$ is the electronic Hamiltonian and $H^{SB}$ is the electron-nuclear coupling. We quantitatively illustrate this connection via exact simulations of a Hubbard-Holstein molecule using the Hierarchical Equations of Motion that show that increasing the degree of electronic interactions can enhance or suppress the rate of electronic coherence loss.