Cavity-mediated hybridization of several molecules in the strong coupling regime

TL;DR

This paper introduces the concept of a molecular optical bond created by cavity-mediated electromagnetic coupling of molecules, demonstrating collective effects and two-photon transitions, advancing hybrid light-matter material research.

Contribution

It presents the experimental realization of cavity-mediated molecular hybridization and explores collective optical phenomena predicted by the Tavis-Cummings model.

Findings

Observation of collective vacuum Rabi splitting enhancement

Identification of super- and sub-radiant states

Demonstration of two-photon transitions in the hybrid system

Abstract

Molecular complexes are held together via a variety of bonds, but they all share the common feature that their individual entities are in contact. In this work, we introduce and demonstrate the concept of a \textit{molecular optical bond}, resulting from the far-field electromagnetic coupling of several molecules via a shared mode of an optical microcavity. We discuss a collective enhancement of the vacuum Rabi splitting and study super- and sub-radiant states that arise from the cavity-mediated coupling both in the resonant and dispersive regimes. Moreover, we demonstrate a two-photon transition that emerges between the ground and excited states of the new optical compound. Our experimental data are in excellent agreement with the predictions of the Tavis-Cummings Hamiltonian and open the door to the realization of hybrid light-matter materials.