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arXiv:1111.4415 · Physical Review B

Polaron master equation theory of the quantum-dot Mollow triplet in a semiconductor cavity-QED system

C. Roy, Stephen Hughes

Published Mar 16, 2012• 77 citations
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Abstract

We present a comprehensive theoretical study of the resonance fluorescence spectra of an coherently-driven quantum dot (QD) placed inside a high-$Q$ 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.

DOI
10.1103/physrevb.85.115309

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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.
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 present a semiconductor quantum optics formalism to study the dynamics of a coherently-driven semiconductor quantum dot interacting with an acoustic phonon bath and a high Q microcavity. A quantum master equation is derived in the polaron frame, where multiphoton and multiphoton effects are included to all orders. As applications of the theory, we study the Mollow triplet of a driven quantum dot in the regime of semiconductor cavity-QED. Pronounced signatures of electron-phonon-photon scattering are observed through excitation-induced dephasing and off-resonant cavity coupling. We also present an effective phonon master in Lindblad form and show example quantum trajectory simulations that help one to understand the features in the Mollow triplet spectra.
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.
A semiconductor quantum dot (QD) embedded within an optical microcavity is a system of fundamental importance within quantum information processing. The optimization of quantum coherence is crucial in such applications, requiring an in-depth understanding of the relevant decoherence mechanisms. We provide herein a critical review of prevalent theoretical treatments of the QD-cavity system coupled to longitudinal acoustic phonons, comparing predictions against a recently obtained exact solution. Within this review we consider a range of temperatures and exciton-cavity coupling strengths. Predictions of the polaron Nakajima-Zwanzig (NZ) and time-convolutionless (TCL) master equations, as well as a variation of the former adapted for adiabatic continuous wave excitation (CWE), are compared against an asymptotically exact solution based upon Trotter's decomposition (TD) theorem. The NZ and TCL implementations, which apply a polaron transformation to the Hamiltonian and subsequently treat the exciton-cavity coupling to second order, do not offer a significant improvement accuracy relative to the polaron transformation alone. The CWE adaptation provides a marked improvement, capturing the broadband features of the absorption spectrum (not present in NZ and TCL implementations). We attribute this difference to the effect of the Markov approximation, and particularly its unsuitability in pulsed excitation regime. Even the CWE adaptation, however, breaks down in the regime of high temperature (50K50K50K) and strong exciton-cavity coupling (g≳0.2g \gtrsim 0.2g≳0.2 meV). The TD solution is of comparable computational complexity to the above-mentioned master equation approaches, yet remains accurate at higher temperatures and across a broad range of exciton-cavity coupling strengths (at least up to g=1.5g=1.5g=1.5 meV).
We present both experimental and theoretical investigations of a laser-driven quantum dot (QD) in the dressed-state regime of resonance fluorescence. We explore the role of phonon scattering and pure dephasing on the detuning-dependence of the Mollow triplet and show that the triplet sidebands may spectrally broaden or narrow with increasing detuning. Based on a polaron master equation approach, which includes electron-phonon interaction nonperturbatively, we derive a fully analytical expression for the spectrum. With respect to detuning dependence, we identify a crossover between the regimes of spectral sideband narrowing or broadening. We also predict regimes of phonon-induced squeezing and anti-squeezing of the spectral resonances. A comparison of the theoretical predictions to detailed experimental studies on the laser detuning-dependence of Mollow triplet resonance emission from single In(Ga)As QDs reveals excellent agreement.
We introduce an intuitive and semianalytical polaron master equation approach to model pulse-driven population inversion and emitted single photons from a quantum dot exciton. The master equation theory allows one to identify important phonon-induced scattering rates analytically and fully includes the role of the time-dependent pump field. As an application of the theory, we first study a quantum dot driven by a time-varying laser pulse on and off resonance, showing the population inversion caused by acoustic phonon emission in direct agreement with recent experiments of Quilter et al. [Phys. Rev. Lett. 114, 137401 (2015)]. We then model quantum dots in weakly coupled cavities and show the difference in population response between exciton-driven and cavity-driven systems. Finally, we assess the nonresonant phonon-assisted loading scheme with a quantum dot resonantly coupled to a cavity as a deterministic single-photon source. We also compare and contrast the important single photon figures of merit with direct Rabi oscillation of the population using a resonant $\ensuremath{\pi}$ pulse, and show that the resonant scheme is much more efficient.