Cavity-mediated localization and collective electron correlation phases

TL;DR

This paper introduces a theoretical framework for understanding cavity-mediated electron correlations in molecular ensembles, revealing two novel collective phases and an entropy-driven localization mechanism.

Contribution

It maps complex intermolecular electronic correlations to an exactly solvable model, predicting new collective phases beyond traditional regimes.

Findings

Prediction of paracorrelated and spin-glass phases

Identification of an entropy-driven localization-delocalization mechanism

Establishment of cavity-mediated correlations as a microscopic phase mechanism

Abstract

Collective strong coupling of molecular ensembles to optical cavities opens a route to modifying matter through genuinely collective electronic correlations. Yet even in the absence of a cavity, Coulomb correlations are notoriously difficult to describe, and cavity coupling adds transverse correlation channels extending over the entire molecular ensemble. Here we show that this seemingly intractable problem admits a controlled description by mapping the collective intermolecular electronic correlations to the analytically solvable spherical Sherrington-Kirkpatrick model. The resulting theory predicts two collective correlation phases, a paracorrelated phase and a spin-glass correlation phase, beyond the conventional uncorrelated molecular regime. These phases reveal an entropy-driven localization-delocalization mechanism that transfers molecular electronic states into collectively correlated cavity-dressed states. Our work establishes cavity-mediated electron correlations as a microscopic mechanism for emergent phases in strongly coupled molecular ensembles.