Evidence for cavity-induced metallic phase from entropic electron correlation effects

Abstract

Experiments have revealed that collective strong coupling in optical cavities can drastically alter the conductivity and dielectric properties of molecular ensembles, or even trigger abrupt phase transitions (in Rayleigh scattering or dispersion force driven conformational equilibrium). Until now, the underlying physical mechanism has remained unknown. A recently proposed theory attributes these collective effects to cavity-induced electron correlations that share properties of the known spherical Sherrington-Kirkpatrick model of a spin glass. As a consequence, entropic effects can trigger a phase transition in the inter-molecular electron correlations that could potentially explain the above experiments. In the following work, we derive analytic expressions for the correlation (free-)energy-induced polarizability changes, which reveal that under certain conditions collective strong coupling can even render our molecular ensemble metallic by entropically ionizing collectively degenerate molecular orbitals. Our results are a first major step towards a holistic theory of cavity-mediated electron correlation effects.