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.
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.
We demonstrate a strong influence of the phonon environment on the coherent dynamics of the quantum dot (QD)-cavity system in the quantum strong coupling regime. This regime is implemented in the nonlinear QD-cavity QED and can be reliably measured by heterodyne spectral interferometry. We present a semianalytic asymptotically exact path integral-based approach to the nonlinear optical response of this system, which includes two key ingredients: Trotter's decomposition and linked-cluster expansion. Applied to the four-wave-mixing optical polarization, this approach provides access to different excitation and measurement channels, as well as to higher-order optical nonlinearities and quantum correlators. Furthermore, it allows us to extract useful analytic approximations and analyze the nonlinear optical response in terms of quantum transitions between phonon-dressed states of the anharmonic Jaynes-Cummings (JC) ladder. Being well described by these approximations at low temperatures and small exciton-cavity coupling, the exact solution deviates from them for stronger couplings and higher temperatures, demonstrating remarkable non-Markovian effects, spectral asymmetry, and strong phonon renormalization of the JC ladder.
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 (50K) and strong exciton-cavity coupling (g≳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=1.5 meV).
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.
We develop an exact analytical approach to four-wave mixing and higher-order optical nonlinearities of a quantum dot-microcavity system. This approach allows us \nto analyse the non-linear response in terms of coherent transitions between rungs \nof the Jaynes-Cummings ladder, finding their complex amplitudes and frequencies. \nIncreasing the pulse area of the excitation field, a transition from quantum strong \ncoupling to coherent classical regime is observed, which manifests itself in a formation of the famous Mollow triplet, with the observation in the three-level model \nof a quantum dot, including a biexciton, to predict two new effects: One is the \nexistence of a Mollow-like quintuplet, the other is a complete elimination of the \nfour-wave-mixing optical non-linearity under certain parameter constraints. We further develop a simple and accurate approximation in the low-damping limit of the \nJaynes-Cummings model of the quantum dot-microcavity system, for nonlinear response of any order in a closed analytic form, predicting the positions and widths \nof the spectral lines. For higher damping, we demonstrate a strong relaxation down \nthe ladder, shown by both numerical and analytic calculation.
In the first part of this dissertation, a dissipative quantum dot (QD) -cavity system coupled to a longitudinal acoustic (LA) phonon reservoir is studied using a numerically exact real-time path-integral approach. Three distinct dynamical regimes of weak (WC), strong (SC), and coherent coupling (CC) are discussed and more accurate conditions identifying them are presented. Our results show that to have the CC regime, which is characterized by clear vacuum Rabi oscillation (VRO), vacuum Rabi splitting (VRS) should be larger than the sum of the widths of the corresponding peaks. In order to distinguish between contributions of population decay and impure dephasing, induced by LA phonons and the dissipations, on the quantum dynamics of the QD-cavity system, we propose a two-part phenomenological expression which fits the QD-cavity decay curves perfectly and is used to calculate the corresponding spectra. The emission rate increases from the carrier recombination rate to a maximum value, which is the mean of the QD and cavity dissipation rates, with QD-cavity coupling strength. We introduce a quantity that can be applied in determining the distinct coupling regimes; This quantity enables us to identify the onset of the SC regime as the point where the impure dephasing term begins to contribute to the central band of the spectrum significantly, as a result of the existence of VRO with a very small frequency (unclear VRO) at the corresponding decay curve. Its contribution to the width of the central band increases with the coupling strength up to the onset of the CC regime, then reduces as a result of the appearance of sidebands in the spectra. The effective population decay and impure dephasing rate contribute solely to the width—of the central and sideband peaks of the triplet spectra respectively—only beyond a very large coupling strength which is the same across the considered temperature range. In the second part, we demonstrate that all the available experimental data of temperature (T)-dependent shift of photoluminescence (PL) peak of In(Ga)As QD samiii ples can be modeled successfully by using a two-oscillator model if and only if the whole temperature interval (0–300 K) is divided into a few parts (at most four parts), depending on dispersion degree of the PL peak from a monotonic behavior. Analysis of the numerical results show that excitons mostly interact (inelastically) with acoustic (AC) or optical (OP) phonons separately. Increasing QDs uniformity, by using some improved growth techniques, results in decreasing or removing the sigmoidal behavior, enhancing total AC phonon contribution to the redshift of the PL peak. Elevation of the zero bandgap (ZBG) energy up to a critical value about 1.4 eV, for In(Ga)As QDs grown using molecularbeam epitaxy, results in enhancement of QD symmetry and total OP phonon contribution and reduction of QDs uniformity and total AC phonon contribution, while a rollover happens for further increase of the ZBG. Therefore we find that the highest QD symmetry and the lowest exciton fine structure splitting correspond to this critical value of ZBG, in accordance with previous experimental results.
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.