Cooperative subwavelength molecular quantum emitter arrays

TL;DR

This paper investigates how vibrational interactions influence cooperative light emission in subwavelength molecular quantum emitter arrays, revealing conditions for long-lived dark states and coherent light generation.

Contribution

It provides analytical and numerical insights into vibrational effects on super- and subradiance in molecular rings, extending quantum emitter models to molecular systems.

Findings

Vibrational relaxation can aid in creating long-lived dark states.

Vibronic coupling affects the intensity and coherence of emitted light.

Molecular rings can generate coherent light similar to ideal quantum emitters.

Abstract

Dipole-coupled subwavelength quantum emitter arrays respond cooperatively to external light fields as they may host collective delocalized excitations (a form of excitons) with super- or subradiant character. Deeply subwavelength separations typically occur in molecular ensembles, where in addition to photon-electron interactions, electron-vibron couplings and vibrational relaxation processes play an important role. We provide analytical and numerical results on the modification of super- and subradiance in molecular rings of dipoles including excitations of the vibrational degrees of freedom. While vibrations are typically considered detrimental to coherent dynamics, we show that molecular dimers or rings can be operated as platforms for the preparation of long-lived dark superposition states aided by vibrational relaxation. In closed ring configurations, we extend previous predictions for the generation of coherent light from ideal quantum emitters to molecular emitters, quantifying the role of vibronic coupling onto the output intensity and coherence.