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arXiv:1411.6050 · Optics Letters

Theory of phonon-modified quantum dot photoluminescence intensity in structured photonic reservoirs

Kaushik Roy‐Choudhury, Stephen Hughes

Published Apr 9, 2015• 12 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1364/ol.40.001838

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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.
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.
A microscopic theory to study the combined dynamics of a quantum dot exciton coupled to a single cavity mode as well as acoustic phonons is presented. By considering the phonon subsystem in the coherent state representation, the phonon’s impact on the emitted photons is investigated. The single photon emission probability and phonon effects on this quantity are studied. On the other hand, we illustrate that while a quantum dot interacts with a single cavity mode, the collapse and revival phenomenon will occur. It is demonstrated that acoustic phonons have a pronounced impact on the collapse and revival of the quantum dot exciton. Our finding reveals that at elevated temperatures the phonon interaction decreases the Rabi frequency. Moreover, the cavity mode possesses non-classical features such as sub-Poissonian statistics.
In this thesis we study the role of nonradiative degrees of freedom on quantum optical properties of mesoscopic quantum dots placed in the structured electromagnetic reservoir of a photonic crystal. We derive a quantum theory of the role of acoustic and optical phonons in modifying the optical absorption lineshape, polarization dynamics, and population dynamics of a two-level atom (quantum dot) in the ``colored" electromagnetic vacuum of a photonic band gap (PBG) material. This is based on a microscopic Hamiltonian describing both radiative and vibrational processes quantum mechanically. Phonon sidebands in an ordinary electromagnetic reservoir are recaptured in a simple model of optical phonons using a mean-field factorization of the atomic and lattice displacement operators. Our formalism is then used to treat the non-Markovian dynamics of the same system within the structured electromagnetic density of states of a photonic crystal. We elucidate the extent to which phonon-assisted decay limits the lifetime of a single photon-atom bound state and derive the modified spontaneous emission dynamics due to coupling to various phonon baths. We demonstrate that coherent interaction with undamped phonons can lead to enhanced lifetime of a photon-atom bound state in a PBG by (i) dephasing and reducing the transition electric dipole moment of the atom and (ii) reducing the quantum mechanical overlap of the state vectors of the excited and ground state (polaronic shift). This results in reduction of the steady-state atomic polarization but an increase in the fractionalized upper state population in the photon-atom bound state. We demonstrate, on the other hand, that the lifetime of the photon-atom bound state in a PBG is limited by the lifetime of phonons due to lattice anharmonicities (break-up of phonons into lower energy phonons) and purely nonradiative decay. We demonstrate how these additional damping effects limit the extent of the polaronic (Franck-Condon) shift of the atomic excited state. We also derive the modified polarization decay and dephasing rates in the presence of such damping. This leads to a microscopic, quantum theory of the optical absorption lineshapes. Our model and formalism provide a starting point for describing dephasing and relaxation in the presence of external coherent fields and multiple quantum dot interactions in electromagnetic reservoirs with radiative memory effects.
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 present a semiconductor master equation technique to study the input/output characteristics of coherent photon transport in a semiconductor waveguide-cavity system containing a single quantum dot. We use this approach to investigate the effects of photon propagation and anharmonic cavity-QED for various dot-cavity interaction strengths, including weakly-coupled, intermediately-coupled, and strongly-coupled regimes. We demonstrate that for mean photon numbers much less than 0.1, the commonly adopted weak excitation (single quantum) approximation breaks down, even in the weak coupling regime. As a measure of the multiphoton correlations, we compute the Fano factor and the correlation error associated with making a semiclassical approximation. We also explore the role of electron--acoustic-phonon scattering and find that phonon-mediated scattering plays a qualitatively important role on the light propagation characteristics. As an application of the theory, we simulate a conditional phase gate at a phonon bath temperature of 20 K in the strong coupling regime.