Resonant Excitation Induced Vibronic Mollow Triplets

TL;DR

This paper predicts and models the emergence of vibronic Mollow triplets in systems where quantum emitters are coupled to phonons, revealing new coherence signatures in complex molecular systems under strong resonant driving.

Contribution

It introduces a scalable analytical formalism to predict vibronic Mollow triplets in multi-mode molecular systems, expanding understanding of coherence in vibronically coupled emitters.

Findings

Vibronic Mollow triplets appear on phonon sidebands under strong resonant drive.

The formalism applies to complex systems like dibenzoterrylene.

Provides conditions for experimental observation of these spectral features.

Abstract

The Mollow triplet is the definitive spectral signature of an optically dressed quantum emitter. We predict that for emitters coupled to localized phonons, this signature is not confined to the zero-phonon line. Under a strong resonant drive, we show that Mollow triplets are strikingly replicated on the associated phonon sidebands -a surprising result, given that phonon sidebands are typically viewed as incoherent, inelastic scattering pathways. These vibronic Mollow triplets are a direct fingerprint of dynamically generated dressed states that hybridize the emitter's electronic, photonic, and vibrational degrees of freedom. We develop a scalable analytical formalism to model this effect in complex, multi-mode molecular systems, such as dibenzoterrylene. Our work provides the precise driving conditions for observing these novel spectral features, establishing a new signature of coherence in vibronically coupled systems.