Unveiling chiral electron-photon correlation effects in circularly polarized optical devices

TL;DR

This paper develops a mean-field theoretical framework to understand electron-photon interactions in chiral optical devices, highlighting its ability to model cavity effects but limitations in describing chiral discrimination.

Contribution

Introduces a systematic mean-field theory for electron-photon interactions in chiral cavities, incorporating strong coupling perturbation methods.

Findings

Captures cavity frequency dispersion effects.

Fails to describe chiral discrimination from coupled excitations.

Provides a foundation for improved theoretical models.

Abstract

Strong coupling with circularly polarized vacuum fluctuations offers a viable route to manipulate molecular chirality. While experiments are advancing toward the realization of chiral cavities, a mean-field theoretical framework for describing electron-photon interaction in this platform has been missing. Here, we present a mean-field theory that can be systematically improved to capture the chiral correlation effects responsible for the enantioselective power of chiral light. We use strong coupling M{\o}ller-Plesset perturbation theory for accessing the excitation manifold of electrons and chiral virtual photons. We apply the developed methods to selected chiral systems and show that the mean-field theory captures cavity frequency dispersion, but fails to describe the chiral discrimination arising from coupled electron-photon excitations.