Purcell-induced suppression of superradiance for molecular overlayers on noble atom surfaces

TL;DR

This paper develops a quantum-mechanical theory to analyze how a dielectric environment influences molecular excitation lifetimes and superradiance, revealing that surface-bound molecules exhibit suppressed superradiance at reduced length scales.

Contribution

It introduces a novel theoretical framework for predicting molecular excitation lifetimes and superradiance effects near dielectric surfaces, emphasizing the role of geometry and environment.

Findings

Superradiance depends on molecular arrangement and environment.

Dielectric surfaces can suppress superradiance effects.

Collective effects occur at much smaller length scales than in free space.

Abstract

We study the impact of an environment on the electromagnetic responses of a molecule in the presence of a dielectric medium. By applying the dipole-dipole coupling between the molecule's and the environment's degrees of freedom, we can reduce the complex system into its components and predict excitation lifetimes of single and few molecules attached to a dielectric surface by knowing the entire quantum-mechanical properties of the molecules, such as transition energies and dipole moments. The derived theory allows for the description of superradiance between two molecules depending on the geometric arrangement between both concerning their separation and orientation with respect to each other. We analyse the possibility of superradiance between two molecules bound to a dielectric sphere and determine a change of the relevant length scale where the usually considered wavelength in free space is replaced with the binding distance, drastically reducing the length scales at which collective effects can take place.