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arXiv:2601.14963

Resonant Excitation Induced Vibronic Mollow Triplets

Devashish Pandey, Corne Koks, Martijn Wubs, Nicolas Stenger, Jake Iles-Smith

quant-phcond-mat.mes-hallphysics.opticsSubmitted Jan 21, 2026• Announced Jan 22, 2026• 0 citations
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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.

Comments
Main text 7 pages, 3 Figures: Supplementary Information 7 Pages, 4 Figures

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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.
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Resonant excitation of solid state quantum emitters has the potential to deterministically excite a localized exciton while ensuring a maximally coherent emission. In this work, we demonstrate the coherent coupling of an exciton localized in a lithographically positioned, site-controlled semiconductor quantum dot to an external resonant laser field. For strong continuous-wave driving we observe the characteristic Mollow triplet and analyze the Rabi splitting and sideband widths as a function of driving strength and temperature. The sideband widths increase linearly with temperature and the square of the driving strength, which we explain via coupling of the exciton to longitudinal acoustic phonons. We also find an increase of the Rabi splitting with temperature, which indicates a temperature induced delocalization of the excitonic wave function resulting in an increase of the oscillator strength. Finally, we demonstrate coherent control of the exciton excited state population via pulsed resonant excitation and observe a damping of the Rabi oscillations with increasing pulse area, which is consistent with our exciton-photon coupling model. We believe that our work outlines the possibility to implement fully scalable platforms of solid state quantum emitters. The latter is one of the key prerequisites for more advanced, integrated nanophotonic quantum circuits.
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We present a semiconductor quantum optics formalism to study the dynamics of a coherently-driven semiconductor quantum dot interacting with an acoustic phonon bath and a high Q microcavity. A quantum master equation is derived in the polaron frame, where multiphoton and multiphoton effects are included to all orders. As applications of the theory, we study the Mollow triplet of a driven quantum dot in the regime of semiconductor cavity-QED. Pronounced signatures of electron-phonon-photon scattering are observed through excitation-induced dephasing and off-resonant cavity coupling. We also present an effective phonon master in Lindblad form and show example quantum trajectory simulations that help one to understand the features in the Mollow triplet spectra.
We present both experimental and theoretical investigations of a laser-driven quantum dot (QD) in the dressed-state regime of resonance fluorescence. We explore the role of phonon scattering and pure dephasing on the detuning-dependence of the Mollow triplet and show that the triplet sidebands may spectrally broaden or narrow with increasing detuning. Based on a polaron master equation approach, which includes electron-phonon interaction nonperturbatively, we derive a fully analytical expression for the spectrum. With respect to detuning dependence, we identify a crossover between the regimes of spectral sideband narrowing or broadening. We also predict regimes of phonon-induced squeezing and anti-squeezing of the spectral resonances. A comparison of the theoretical predictions to detailed experimental studies on the laser detuning-dependence of Mollow triplet resonance emission from single In(Ga)As QDs reveals excellent agreement.