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arXiv:2412.20598

Phonon-Induced Effects in Quantum Dot Absorption and Resonance Fluorescence with Hierarchy of Pure States

Sebastian Toivonen, Kimmo Luoma

Published Dec 29, 2024• 0 citations
arXivHTMLPDF

Abstract

We investigate a quantum dot (QD) system coupled to a vibrational environment with a super-Ohmic spectral density and weakly to a leaky cavity mode, a model relevant for semiconductor-based single-photon sources. The phonon coupling induces dephasing and broadens the absorption and emission line shapes, while the weakly coupled cavity mode leads to effective driving of the QD. To capture non-Markovian effects, we use non-Markovian Quantum State Diffusion and its hierarchical extension the Hierarchy of Pure States to compute multitime correlation functions underlying absorption and resonance fluorescence spectra. We present numerical results for the absorption spectra at strong phonon coupling and finite temperature, as well as for resonance fluorescence spectra at varying phonon coupling strengths and temperatures, and analyse the visibility of the resonance fluorescence spectra to provide insights into how phonon coupling and thermal effects influence the spectral features.

DOI
10.48550/arxiv.2412.20598

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We investigate a quantum dot (QD) system coupled to a vibrational environment with a super-Ohmic spectral density and weakly to a leaky cavity mode, a model relevant for semiconductor-based single-photon sources. The phonon coupling induces dephasing and broadens the absorption and emission line shapes, while the weakly coupled cavity mode leads to effective driving of the QD. To capture non-Markovian effects, we use non-Markovian Quantum State Diffusion and its hierarchical extension the Hierarchy of Pure States to compute multitime correlation functions underlying absorption and resonance fluorescence spectra. We present numerical results for the absorption spectra at strong phonon coupling and finite temperature, as well as for resonance fluorescence spectra at varying phonon coupling strengths and temperatures, and analyse the visibility of the resonance fluorescence spectra to provide insights into how phonon coupling and thermal effects influence the spectral features.
We investigate the temperature dependence of photon coherence properties through two-photon interference (TPI) measurements from a single quantum dot (QD) under resonant excitation. We show that the loss of indistinguishability is related only to the electron-phonon coupling and is not affected by spectral diffusion. Through these measurements and a complementary microscopic theory, we identify two independent separate decoherence processes, both of which are associated with phonons. Below 10 K, we find that the relaxation of the vibrational lattice is the dominant contribution to the loss of TPI visibility. This process is non-Markovian in nature and corresponds to real phonon transitions resulting in a broad phonon sideband in the QD emission spectra. Above 10 K, virtual phonon transitions to higher lying excited states in the QD become the dominant dephasing mechanism, this leads to a broadening of the zero phonon line, and a corresponding rapid decay in the visibility. The microscopic theory we develop provides analytic expressions for the dephasing rates for both virtual phonon scattering and non-Markovian lattice relaxation.
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 theoretically investigate the influence of the phonon-mediated coupling on the properties of the laser generated by a single red-detuned quantum dot (QD), where the QD is coherently driven and coupled to a microscopic cavity which can be engineered in a photonic band-gap (PBG) material. In the low-temperature limit, the phonon-mediated coupling is deleterious to the emission of photon into cavity field and the threshold behavior of the laser persists after the inclusion of the phonon-mediated processes. Without being engineered in the PBG material, if the damping rate $\ensuremath{\kappa}$ of the cavity is close to but smaller than the phonon-mediated spontaneous emission rate $\ensuremath{\gamma}$ of the dot, the photon statistics of the cavity field change from super-Poissonian to sub-Poissonian. The nonclassical effect can be achieved due to the phonon-mediated processes induced by the electron-phonon interaction and the off-resonant dot-cavity coupling. The nonclassical effect can be enhanced by the PBG material. When the effect of the thermal phonon is taken into account, the cavity field exhibits the super-Poissonian property. If $\ensuremath{\kappa}$ is much smaller than $\ensuremath{\gamma}$, the phonon-mediated processes can lead to the increase (decrease) of the photons provided that the incoherent pumping rate is lower (higher) than the effective phonon-mediated threshold. But, if $\ensuremath{\kappa}$ is close to or larger than $\ensuremath{\gamma}$, the emission of the photon may dominate the absorption process, strengthening the intensity of the cavity field.
Electron-phonon coupling in semiconductor quantum dots plays a significant role in determining the optical properties of excited excitons, especially the spectral nature of emitted photons. This paper presents a comprehensive theory and analysis of emission spectra from artificial atoms or quantum dots coupled to structured photon reservoirs and acoustic phonons, when excited with incoherent pump fields. As specific examples of structured reservoirs, we chose a Lorentzian cavity and a slow-light coupled-cavity waveguide, which have both been explored experimentally. For the case of optical cavities, we directly compare and contrast the spectra from three well-known and distinct theoretical approaches to treat electron-phonon coupling, including a Markovian polaron master equation, a non-Markovian phonon correlation expansion technique, and a semiclassical linear susceptibility approach, and we point out the limitations of these models. For the cavity-QED polaron master equation, which treats the cavity-mode operator at the level of a system operator, we give closed form analytical solutions to the phonon-assisted scattering rates in the weak excitation approximation, fully accounting for temperature, cavity-exciton detuning, and cavity-dot coupling. We also show explicitly why the semiclassical linear susceptibility approach fails to correctly account for phonon-mediated cavity feeding. For weakly coupled cavities, we calculate the optical spectra using a more general photon reservoir polaron master-equation approach, and explain its differences from the above approaches in the low-QQQ limit of a Lorentzian cavity. We subsequently use this general reservoir approach to calculate the emission spectra from quantum dots coupled to slow-light photonic crystal waveguides, which demonstrate a number of striking photon-phonon coupling effects.
We present a systematic analysis on the role of the quantum dot (QD) shape in the influence of the phonon bath on the dynamics of a QD cavity QED system. The spectral functions of the phonon bath in three representative QD shapes: spherical, ellipsoidal, and disk, are calculated from the carrier wave functions subjected to the confinement potential provided by the corresponding shape. The obtained spectral functions are used to calculate three main effects brought by the phonon bath, i.e., the coupling renormalization, the off-resonance assisted feeding rate and the pure dephasing rate. It is found that the spectral function of a disk QD has the widest distribution, hence the phonon bath in a disk QD can lead to the smallest renormalization factor, the largest dephasing rate in the short time domains(≤ 2 ps), and the off-resonance assisted feeding can support the widest detuning. Except for the pure dephasing rate in the long time domains, all the influences brought by the phonon bath show serious shape dependence.
We present a comprehensive theoretical study of the resonance fluorescence spectra of an coherently-driven quantum dot (QD) placed inside a high-QQQ semiconductor cavity and interacting with an acoustic-phonon bath. We derive a quantum master equation (ME) in the polaron frame, which includes exciton-phonon and exciton-cavity coupling to all orders. This work details and extends the theory used in a recent paper [C. Roy and S. Hughes, Phys. Rev. Lett. 106, 247403 (2011)] to describe the QD Mollow triplet in the regime of semiconductor cavity QED. Here, we introduce two ME forms, Nakajima-Zwanzig and time convolutionless (TC), both to second order in the system--phonon-reservoir perturbation. In the polaron frame, these two ME forms are shown to yield equivalent population dynamics and fluorescence spectra for a continuous wave (cw) driving field. We also demonstrate that a Markov approximation is valid for computing the incoherent scattering processes, and we subsequently exploit the TC ME to explore the resonance fluorescence spectra of an exciton-driven QD. Both cavity-emitted and exciton-emitted spectra are studied, and these are found to have qualitatively different spectral features. Using a coherent driving field, the well-known characteristics of the atomic Mollow triplet are shown to be considerably modified with electron--acoustic-phonon scattering, and we highlight the key effects arising from both cavity coupling and electron-phonon coupling. Regimes of pronounced cavity feeding and anharmonic cavity QED are exemplified, and we find that the cavity coupling depends sensitively on the exciton-cavity detuning and the temperature of the phonon bath. We show how the full width at half maximum (linewidth) of the Mollow-triplet sidebands varies as a function of the square of the Rabi frequency of the cw pump. Phonon-mediated cavity coupling also contributes to the spectral broadening of the Mollow triplet, depending upon the exciton-cavity detuning and the strength of the exciton-cavity coupling rate. Finally, we calculate the fluorescence spectra for off-resonance cw driving and investigate the resulting Mollow-triplet linewidths.