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Nature Photonics

Dynamic resonance fluorescence in solid-state cavity quantum electrodynamics

Shunfa Liu, Chris Gustin, Hanqing Liu, Xueshi Li, Ying Yu, Haiqiao Ni, Zhichuan Niu, Stephen Hughes, Xuehua Wang, Jin Liu

Published Jan 10, 2024• 26 citations
Publisher

Abstract

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.

DOI
10.1038/s41566-023-01359-x

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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.
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.
We discuss the long sought after regime of “dynamical resonance florescence,” which adds significant modification and control to the usual CW resonance florescence schemes such as the Mollow triplet, when using excitation pulses whose time duration is shorter than the inverse decay time of the quantum emitter. We present several examples, including (i) semiconductor quantum dot cavity systems, where we will show recent experiments and simulations side by side, and (ii) waveguide QED systems excited with few photon Fock state pulses. Using state of the art quantum simulation algorithms, including tensor networks, we describe how the usual emission spectrum and intensity outputs are dynamically modified with short pulse excitation, and demonstrate how even single photon population effects are uniquely accessed in this regime. These short-pulsed emission regimes allow for the generation of a variety of exotic quantum states of light.
Quantum optics provides a fundamental framework for understanding the interaction between light and matter at the quantum level. Recently, it has been shown that under incoherent pumping, the resonance fluorescence spectrum dramatically changes. Engineering the resonance fluorescence spectrum paves the way towards solid-state-based single-photon sources. In this paper, we start by reviewing and reproducing some of the results concerning the resonance fluorescence spectrum, single-photon sources, dressed-state lasers, and luminescence spectrum of a quantum dot in a microcavity. Photon correlations in quantum optical systems and spectral properties of radiation emitted by atomic and semiconductor systems interacting with external fields are investigated. The well known Mollow triplet structure of the emission spectrum is discussed, together with the role of dressed states in explaining the origin of the three spectral peaks. Furthermore, the luminescence spectra of quantum emitters coupled to microcavities are reviewed. The numerical results presented here contribute to the theoretical understanding of resonance fluorescence, photon correlations, and engineered emission in quantum optical systems. These studies highlight the rich physical properties arising from light matter interaction at the quantum level and demonstrate their relevance for emerging quantum technologies.
We study the resonance fluorescence spectra of a driven quantum dot placed inside a high-Q semiconductor cavity and interacting with an acoustic phonon bath. The dynamics is calculated using a time-convolutionless master equation in the polaron frame. We predict pronounced spectral broadening of the Mollow sidebands through off-resonant cavity emission which, for small cavity-coupling rates, increases quadratically with the Rabi frequency in direct agreement with recent experiments using semiconductor micropillars [S. M. Ulrich et al., preceding Letter, Phys. Rev. Lett. 106, 247402 (2011)]. We also demonstrate that, surprisingly, phonon coupling actually helps resolve signatures of the elusive second rungs of the Jaynes-Cummings ladder states via off-resonant cavity feeding. Both multiphonon and multiphoton effects are shown to play a qualitatively important role on the fluorescence spectra.
We show that the resonance fluorescence spectrum of a quantum dot excited by a strong optical pulse contains multiple peaks beyond those of the Mollow triplet. We show that as the area of the optical pulse is increased, new side peaks split off the central peak and shift in frequency. A simple analytical theory has been derived, which quantitatively accounts for the appearance and position of the peaks. This theory explains the physics responsible for the multiple peaks. By considering the time-dependent spectrum we demonstrate a time ordering of the side peaks, which is further evidence for the suggested physical explanation.
The interaction of a resonant light field with a quantum two-level system is of key interest both for fundamental quantum optics and quantum technological applications employing resonant excitation. While emission under resonant continuous-wave excitation has been well-studied, the more complex emission spectrum of dynamically dressed states, a quantum two-level system driven by resonant pulsed excitation, has so far been investigated in detail only theoretically. Here, we present the first experimental observation of the complete resonance fluorescence emission spectrum of a single quantum two-level system, in form of an excitonic transition in a semiconductor quantum dot, driven by finite Gaussian pulses. We observe multiple emerging sidebands as predicted by theory with an increase of their number and spectral detuning with excitation pulse intensity and a dependence of their spectral shape and intensity on the pulse length. Detuning-dependent measurements provide additional insights into the emission features. The experimental results are in excellent agreement with theoretical calculations of the emission spectra, corroborating our findings.