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

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 Møller–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.