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arXiv:2509.25847 · Physical Review Letters

Hybrid Acousto-Optical Double Dressing of a Two-Level System

Anonymous, Zixuan Wang, Richard P. Mirin, Kevin L. Silverman, Shuo Sun

Published Jun 15, 2026• 0 citations
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Abstract

We experimentally investigate resonance fluorescence from a two-level system in a novel configuration where a strong laser drives an optical Rabi oscillation while an acoustic field parametrically modulates the frequency of the two-level system. We observe emission spectra that deviate markedly from the standard Mollow triplet, including dynamical cancellation of the central peak. A doubly dressed state model incorporating hybridization among the emitter, optical field, and acoustic field captures these features. Guided by this model, we experimentally validate the condition for optimal cooling of acoustic phonons in an emitter-optomechanical system. These results reveal new regimes of strongly driven quantum nonlinear interactions.

DOI
10.1103/xjpt-q14w

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We experimentally investigate resonance fluorescence from a two-level system in a novel configuration where a strong laser drives an optical Rabi oscillation while an acoustic field parametrically modulates the frequency of the two-level system. We observe emission spectra that deviate markedly from the standard Mollow triplet, including dynamical cancellation of the central peak. A doubly dressed state model incorporating hybridization among the emitter, optical field, and acoustic field captures these features. Guided by this model, we experimentally validate the condition for optimal cooling of acoustic phonons in an emitter-optomechanical system. These results reveal new regimes of strongly driven quantum nonlinear interactions.
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The coherent interaction between a two-level system and electromagnetic fields serves as a foundation for fundamental quantum physics and modern photonic quantum technology. A profound example is resonance fluorescence, where the non-classical photon emission appears in the form of a Mollow-triplet when a two-level system is continuously driven by a resonant laser. Pushing resonance fluorescence from a static to dynamic regime by using short optical pulses generates on-demand emissions of highly coherent single photons. Further increasing the driving strength in the dynamical regime enables the pursuit of exotic non-classical light emission in photon number superposition, photon number entanglement, and photon bundle states. However, the long-sought-after spectrum beyond the Mollow-triplet, a characteristic of dynamic resonance fluorescence under strong driving strength, has not been observed yet. Here we report the direct observation and systematic investigations of dynamic resonance fluorescence spectra beyond the Mollow-triplet in a solid-state cavity quantum electrodynamic system. The dynamic resonance fluorescence spectra with up to five pairs of side peaks, excitation detuning induced spectral asymmetry, and cavity filtering effect are observed and quantitatively modeled by a full quantum model with phonon scattering included. Time-resolved measurements further reveal that the multiple side peaks originate from interference of the emission associated with different temporal positions of the excitation pulses. Our work facilitates the generation of a variety of exotic quantum states of light with dynamic driving of two-level systems.
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.
Abstract The coherent interaction between a two-level system and electromagnetic fields serves as a foundation for fundamental quantum physics and modern photonic quantum technology. A profound example is resonance fluorescence, where the non-classical photon emission appears in the form of a Mollow-triplet when a two-level system is continuously driven by a resonant laser. Pushing resonance fluorescence from a static to dynamic regime by using short optical pulses generates on-demand emissions of highly coherent single photons. Further increasing the driving strength in the dynamical regime enables the pursuit of exotic non-classical light emission in photon number superposition, photon number entanglement, and photon bundle states. However, the long-sought-after spectrum beyond the Mollow-triplet, a characteristic of dynamic resonance fluorescence under strong driving strength, has not been observed yet. Here we report the direct observation and systematic investigations of dynamic resonance fluorescence spectra beyond the Mollow-triplet in a solid-state cavity quantum electrodynamic system. The dynamic resonance fluorescence spectra with up to five pairs of side peaks, excitation detuning induced spectral asymmetry, and cavity filtering effect are observed and quantitatively modeled by a full quantum model with phonon scattering included. Time-resolved measurements further reveal that the multiple side peaks originate from interference of the emission associated with different temporal positions of the excitation pulses. Our work facilitates the generation of a variety of exotic quantum states of light with dynamic driving of two-level systems.