Collective Vibronic Cascade in Cavity-Coupled Jahn-Teller Active Molecules

TL;DR

This paper explores how collective coupling of multiple Jahn-Teller active molecules to a cavity modifies their vibronic states and dynamics, revealing new pathways for angular momentum transfer and spectrum broadening.

Contribution

It demonstrates that collective coupling enables access to high-angular-momentum vibronic states and alters polaritonic spectra, a phenomenon absent in single-molecule systems.

Findings

Collective coupling broadens the polaritonic spectrum.

Access to high-angular-momentum vibronic states is enabled.

Photon polarization dynamics are suppressed under broadband excitation.

Abstract

We study the polaritonic states and dynamics of multiple Jahn-Teller (JT) active molecules coupled to the modes of a Fabry-Perot cavity. We find that collective effects dramatically alter the interplay of electronic, vibrational and cavity angular momenta, giving rise to markedly different polaritonic spectra and dynamics even when going from one to two JT molecules. Starting from the ground vibronic state, we find that JT molecules collectively coupled to a common cavity can access a cascade of high-angular-momentum vibronic states in the presence of a single cavity photon, in sharp contrast to the single molecule case where the range of accessible vibronic angular momentum values are bounded. The observable consequences are a broadening of the cavity-molecular polariton spectrum and a suppression of photon polarization dynamics under broadband excitation of the system. Our results uncover new pathways for vibronic angular momentum transfer unique to collective molecular polaritonics with potential implications for cavity-assisted photo-physics and photo-chemistry.