Super-Poissonian Squeezed Light in the Ground State of Strongly Coupled Light-matter Systems

TL;DR

This paper demonstrates that strong light-matter coupling in molecular systems can produce nonclassical photonic states, such as squeezing and super-Poissonian statistics, using a first-principles quantum electrodynamical density-functional theory approach.

Contribution

It introduces a novel application of QEDFT combined with pMBD functional to accurately predict quantum-optical properties in strongly coupled systems, capturing multi-photon and many-body correlations.

Findings

Observation of photon squeezing in the ground state.

Detection of super-Poissonian photon statistics.

Importance of many-body correlations for accurate predictions.

Abstract

Strong light-matter coupling enables hybrid states in which photonic and electronic degrees of freedom become correlated even in the ground state. While many-body effects in long-range dispersion interactions are known to reshape electronic properties under such conditions, their impact on quantum-optical observables remains largely unexplored. Here, we address this problem using quantum electrodynamical density-functional theory (QEDFT) combined with the recently developed photon-many-body dispersion (pMBD) functional, which can capture higher-order electron-photon correlations and multi-photon processes. We compute ground-state photonic observables including photon number fluctuations, second-order correlations, and quadrature variances, and find squeezing and super-Poissonian photon statistics emerging from light-matter interactions in the strong coupling regime. Our results demonstrate that capturing the full hierarchy of many-body, electron-photon and multi-photon correlations is essential for a consistent description of quantum-optical properties in strongly coupled molecular systems, establishing QEDFT as a first-principles framework for predicting nonclassical photonic features in the ground state of complex systems.