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arXiv:1504.03356 · Physical Review B

Quantum theory of the emission spectrum from quantum dots coupled to structured photonic reservoirs and acoustic phonons

Kaushik Roy‐Choudhury, Stephen Hughes

Published Nov 4, 2015• 58 citations
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Abstract

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-$Q$ 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.

DOI
10.1103/physrevb.92.205406

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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 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.
The spontaneous emission rate of a quantum dot coupled to a structured photonic reservoir is determined by the frequency dependence of its local density of photon states. Through phonon-dressing, a breakdown of Fermi's golden rule can occur for certain photonic structures whose photon decay time becomes comparable to the longitudinal acoustic phonon decay times. We present a polaron master equation model to calculate the photoluminescence intensity from a coherently excited quantum dot coupled to a structured photonic reservoir. We consider examples of a semiconductor microcavity and a coupled cavity waveguide, and show clear photoluminescence intensity spectral features that contain unique signatures of the interplay between phonon and photon bath coupling.
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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.
We investigate the effect of electron-phonon interactions on the coherence properties of single photons emitted from a semiconductor cavity QED (quantum electrodynamics) system, i.e., a quantum dot embedded in an optical cavity. The degree of indistinguishability, governing the quantum mechanical interference between two single photons, is calculated as a function of important parameters describing the cavity QED system and the phonon reservoir, e.g., cavity quality factor, light-matter coupling strength, temperature, and phonon lifetime. We show that non-Markovian effects play an important role in determining the coherence properties for typical parameter values and establish the conditions under which a Markovian approximation may be applied. The calculations are performed using a recently developed second-order perturbation theory, and the limits of validity are established by comparing to an exact diagonalization approach. We find that for large cavity decay rates the perturbation theory may break down.
The effect of phonons on a nonlinear optical response of a quantum dot-cavity system in quantum strong coupling regime can be accounted for by a fully analytical treatment, provided that the exciton-phonon dynamics is much faster than the exciton-cavity dynamics. Modern experiments involving semiconductor quantum dots embedded in optical microcavities typically meet this criterion. We find that, for a relatively small exciton-cavity coupling, the effect of phonons is concentrated mainly in the polaron shift of the exciton frequency and reduction of exciton-cavity coupling by the Huang-Rhys factor. We have generalized this result to an arbitrary optical nonlinearity and demonstrated a good agreement with the exact solution in a wide range of temperatures. This generalization provides access to higher rungs of the Jaynes-Cummings ladder, where exact numerical approaches are impractical or even impossible. At larger coupling strengths and low temperatures, our approximation is also in good agreement with the exact solution, which makes it a very useful tool for addressing the phonon contribution to the coherent dynamics of a nonlinear optical system. We demonstrate our results for third-order optical polarization with varying observation time and delay time between excitation pulses in the form of two-dimensional spectra. These spectra provide useful information about the coherent coupling between the exciton and the cavity modes. The presented analytical approach is also compared with another useful approximation, having the form of a matrix product, which is a special case of the asymptotically exact solution in the limit of a short phonon memory time.