Resonant Excitation Induced Vibronic Mollow Triplets

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.