Cavity Jahn-Teller Polaritons in Molecules

TL;DR

This paper explores the formation and properties of Jahn-Teller polaritons in molecules within a cavity, revealing how their mixed polarization states and angular momentum exchange lead to unique dynamical optical responses.

Contribution

It introduces the concept of cavity Jahn-Teller polaritons, highlighting their mixed polarization and angular momentum exchange due to vibronic coupling, a novel insight in molecular cavity QED.

Findings

Cavity Jahn-Teller polaritons exhibit mixed circular polarization.

The polarization response is frequency-dependent and can differ from external excitation.

Photonic-vibronic coupling enables efficient angular momentum exchange.

Abstract

We investigate Jahn-Teller (JT) polaritons, which emerge from the interaction of the two normal-incidence electromagnetic modes with perpendicular polarizations in a Fabry-Perot cavity resonator with JT active systems. These JT polaritons are characterized by a mixed $(+/-)$--circular electromagnetic polarization that originates from the molecular JT vibronic coupling of the material subsystem. Consequently, the exchange of photonic and vibronic angular momenta can be very efficient; exciting the cavity-JT system with short, polarized light pulses results in a dynamical and oscillatory response of the polarization in the cavity medium. Due to the photonic-vibronic coupling, we show how the cavity polarization direction becomes frequency dependent and does not necessarily coincide with the polarization direction of the external fields used to drive the system.