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arXiv:2506.14643 · Physical review. B./Physical review. B

Dynamically dressed states of a quantum four-level system

Carolin Calcagno, Friedrich Sbresny, Thomas K. Bracht, Sang Kyu Kim, Eduardo Zubizarreta Casalengua, Katarina Boos, William Rauhaus, Hubert Riedl, Jonathan J. Finley, Doris E. Reiter, Kai Müller

Published Nov 18, 2025• 1 citation
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Abstract

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.

DOI
10.1103/yqjn-w5m8

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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 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.
We theoretically analyze the steady state emission spectrum and transient temporal dynamics in a coupled biexciton quantum dot (QD)—cavity system. For steady state, a phonon-assisted biexciton—exciton cascade model under continuous wave (CW) excitation is presented to explain the asymmetric QD—cavity emission spectrum intensities (intensities of cavity, exciton, and biexciton emission peak) in off-resonance condition. Results demonstrate that the electron—phonon process is crucial to the asymmetry of emission spectrum intensity. Moreover the transient characteristics of the biexciton—exciton cascade system under pulse excitation show abundant nonlinear temporal dynamic behaviors, including complicated oscillations which are caused by the four-level structure of QD model. We also reveal that under off-resonance condition the cavity outputs are slightly reduced due to the electron—phonon interaction.
We analyse the population dynamics and the photon emission statistics of a single semiconductor quantum dot with an exciton–biexciton–triexciton multilevel driven by a pulse field, in which the quantum regression theorem and optical Bloch equations are employed. The populations of the three states are comparable under resonant excitation with the input pulse area around 1.5π. Three second-order cross-correlation functions demonstrate the correlated three-photon emissions at a given order from triexciton, biexciton and exciton states driven by single pulses, while the probability of the bunched three-photon cascaded emissions decreases to the minimum as the input pulse area increases to 2π in every period.
We report nonlinear resonance fluorescence of an individual semiconductor quantum dot. By driving a single semiconductor quantum dot via a two-photon transition, we probe the linewidth of two-photon excitation processes and show that, similar to their single-photon counterparts, they are close to being Fourier limited at low temperatures. The evolution of the population of excitonic states with increasing Rabi energy exhibits a clear S-shaped behavior, indicative of the nonlinear response via the two-photon excitation process. Numerical calculations of the nonlinear response using a four-level atomic system representing the manifold of excitonic and biexcitonic states in the quantum dot are in excellent agreement with our experiments and reveal the effect of interactions with LA phonons in the solid-state environment. Finally, we demonstrate the formation of dressed states emerging from a nonlinear two-photon interaction between the quantum dot and the optical excitation field. The nonlinear optical dressing induces a mixing of all four excitonic states that allows direct optical tuning of the polarization selection rules and energies of the dressed states in the artificial atom. We expect our results to play a pivotal role for the generation of nonclassical photon pairs desired for applications in quantum communication and fundamental experiments on quantum optical properties of photons.
We demonstrate the simultaneous dressing of both vacuum-to-exciton and exciton-to-biexciton transitions of a single semiconductor quantum dot in a high-Q micropillar cavity, using photoluminescence spectroscopy. Resonant two-photon excitation of the biexciton is achieved by spectrally tuning the quantum dot emission with respect to the cavity mode. The cavity couples to both transitions and amplifies the Rabi frequency of the likewise resonant continuous wave laser, driving the transitions. We observe strong-field splitting of the emission lines, which depend on the driving Rabi field amplitude and the cavity-laser detuning. A dressed state theory of a driven 4-level atom correctly predicts the distinct spectral transitions observed in the emission spectrum, and a detailed description of the emission spectra is further provided through a polaron master equation approach which accounts for cavity coupling and acoustic phonon interactions of the semiconductor medium.