Photon pumping, photodissociation and dissipation at interplay for the fluorescence of a molecule in a cavity

TL;DR

This paper presents a comprehensive model of a diatomic molecule in an optical cavity, capturing complex interactions between photon pumping, dissociation, and fluorescence, with exact treatment of electron and nuclear motions.

Contribution

It introduces a novel, exact model that simultaneously considers electron and nuclear dynamics in a cavity, enabling detailed analysis of optical responses and molecular behavior.

Findings

Analysis of Mollow spectrum hindered by electron correlations

Competition between harmonic generation and molecular dissociation

Fluorescence dependence on photon pumping rate and dissipation

Abstract

We introduce a model description of a diatomic molecule in an optical cavity, with pump and fluorescent fields, and electron and nuclear motion are treated on equal footing and exactly. The model accounts for several optical response temporal scenarios: a Mollow spectrum hindered by electron correlations, a competition of harmonic generation and molecular dissociation, a dependence of fluorescence on photon pumping rate and dissipation. It is thus a general and flexible template for insight into experiments where quantum photon confinement, leakage, nuclear motion and electronic correlations are at interplay.