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Quantum Theory of Phonon-Mediated Decoherence and Relaxation of Two-Level Systems in a Structured Electromagnetic Reservoir

C. Roy

Published Jan 1, 2009• 1 citation
OpenAlex

Abstract

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.

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Conference on Lasers and Electro-Optics•Aug 29, 2005•0 citations
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 derive a quantum theory of the role of acoustic and optical phonons in modifying the optical absorption line shape, 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. 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 an enhanced lifetime of a photon-atom bound state in a PBG. 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 (breakup of phonons into lower energy phonons) and purely nonradiative decay. 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 line shapes. 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 study the population and disentanglement dynamics of two identical quantum dots placed inside the structured electromagnetic reservoir of a photonic crystal and coupled to an independent bath of thermal phonons. A formalism based on the method of generalized-Laplace transforms is developed to study the population and disentanglement dynamics. The effect of resonant dipole dipole interaction between the two quantum dots on the population dynamics in the presence of phonons and shows that the two two-level atoms can have a residual population at long times in the structured reservoir of a photonic crystal due to the formation of a photon-atom bound state. The disentanglement dynamics of the two quantum dots (assumed to be initially entangled) is studied using concurrence as a measure and is computed from the reduced two two-level system density matrix using the method of generalized-Laplace transforms. We show that partial disentanglement results from the interaction of the two quantum dots with the electromagnetic and phonon reservoirs. However, substantial entanglement is preserved in the fractionalized steady state formed if the transition frequency of two the quantum dots lies in the vicinity of the photonic band edge. We also discuss in detail the role of acoustic phonons on the population and disentanglement dynamics and the long time residual entanglement.
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 theoretically demonstrate the population switching of quantum dots (QD's), modeled as two-level atoms in idealized one-dimensional (1D) and two-dimensional (2D) photonic crystals (PC's) by self-consistent solution of the Maxwell-Bloch equations. In our semiclassical theory, energy states of the electron are quantized, and electron dynamics is described by the atomic Bloch equation, while electromagnetic waves satisfy the classical Maxwell equations. Near a waveguide cutoff in a photonic band gap, the local electromagnetic density of states (LDOS) and spontaneous emission rates exhibit abrupt changes with frequency, enabling large QD population inversion driven by both continuous and pulsed optical fields. We recapture and generalize this ultrafast population switching using the Maxwell-Bloch equations. Radiative emission from the QD is obtained directly from the surrounding PC geometry using finite-difference time-domain simulation of the electromagnetic field. The atomic Bloch equations provide a source term for the electromagnetic field. The total electromagnetic field, consisting of the external input and radiated field, drives the polarization components of the atomic Bloch vector. We also include a microscopic model for phonon dephasing of the atomic polarization and nonradiative decay caused by damped phonons. Our self-consistent theory captures stimulated emission and coherent feedback effects of the atomic Mollow sidebands, neglected in earlier treatments. This leads to remarkable high-contrast QD-population switching with relatively modest (factor of 10) jump discontinuities in the electromagnetic LDOS. Switching is demonstrated in three separate models of QD's placed (i) in the vicinity of a band edge of a 1D PC, (ii) near a cutoff frequency in a bimodal waveguide channel of a 2D PC, and (iii) in the vicinity of a localized defect mode side coupled to a single-mode waveguide channel in a 2D PC.
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.
Summary form only given. The majority of studies of quantum optical processes occurring in atoms interacting with modified reservoirs, such as microcavities and photonic band gap materials, have concentrated on spontaneous emission dynamics. In this paper we report our recent theoretical results on absorption and dispersion dynamics of a A-type system where one transition spontaneously decays in a two band photonic reservoir. The coupling to this modified reservoir leads to a non-Markovian spontaneous decay of the atomic state, which in return influences the dispersion and absorption properties of a probe laser pulse coupling to the other atomic transition.