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Physical Review Letters

Signatures of Dynamically Dressed States

Katarina Boos, Sang Kyu Kim, Thomas K. Bracht, Friedrich Sbresny, Jan M. Kaspari, Moritz Cygorek, Hubert Riedl, Frederik W. Bopp, William Rauhaus, Carolin Calcagno, Jonathan James Finley, Doris E. Reiter, Kai Müller

Published Jan 30, 2024• 21 citations
Publisher

Abstract

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 the 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.

DOI
10.1103/physrevlett.132.053602

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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 the 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.
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.
In this work, we experimentally and theoretically study the dressed-state emission of the biexciton-exciton cascade in a semiconductor quantum dot under pulsed, resonant, two-photon excitation. Building on the well-characterized steady-state dressed emission of the four-level system, we examine its dynamic counterpart under pulsed, resonant excitation, addressing both experimental observations and theoretical modeling. Here we report several sidebands emerging from the biexciton-to-exciton transition, whose number and spectral width depend on the excitation pulse duration and the effective pulse area, while no sidebands emerge from the exciton-to-ground-state transition. Since the biexciton state population follows a nonlinear pulse area function, sidebands with a small spectral nonlinearity result. Detuning- and time-dependent measurements provide deeper insight into the emission properties of the dressed states. They show that side peak emission only occurs in the presence of the excitation pulse. Moreover, when the system is excited by a Gaussian-shaped laser pulse, side peak emission takes place sequentially.
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.
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.
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.