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Theory of Propagation and Manipulation of Excitons in GaAs Structures

Baijie Gu

Published Jan 1, 2012• 0 citations
OpenAlex

Abstract

This dissertation presents research on the propagation and manipulation of excitons in GaAs. There are three main aspects to be addressed. In the first part, we provide a comprehensive understanding of the slow- and fast-light propagation based on excitonic resonances. Propagation (or transit) times of optical pulses through a medium near an absorptive resonance with and without spatial dispersion are studied and contrasted. We show that, when the broadening of the resonance (i.e., dephasing rate) is below a critical value, a frequency range exists near resonance where the transit times are determined by interference between co-propagating exciton-polaritons and deviate strongly from expectations based on the group velocities of the individual exciton-polariton branches. Our theory puts the well-known slow- and fast-light effects in systems without spatial dispersion into a broader context by interpreting them as a limiting case of systems with spatial dispersion. An important ingredient of the exciton theory is the light-matter coupling that can be expressed either in terms of the dipole or the momentum matrix elements. We re-examine the validity of a frequently used relation between the interband momentum and dipole matrix elements ('p-r relation') in semiconductors. An additional correction term was obtained when we applied the 'p-r relation' to finite-volume crystals treated with periodic boundary conditions. The correction term does not vanish in the limit of infinite volume. We illustrate this with numerical examples for bulk GaAs and GaAs superlattices. For bulk GaAs, the correction term is found to be always important; while for a GaAs superlattice, the importance of the correction term for the transition depends strongly on the origin of the unit cell.As an example for manipulation of excitons, we consider mechanical deformations of GaAs nanomembranes. The nanomembranes with lateral sizes much larger than their thicknesses exhibit great flexibility in non-planar deformations and thus promise applications in flexible electronic and photonic devices. These non-planar deformations do not fit in the well-established theory for planar deformations induced by lattice mismatch. Our theory relates the general mechanical deformations (planar or non-planar) of nanomembranes to their excitonic spectra, and is numerically evaluated within the average-strain approximation.

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This dissertation presents research on the propagation and manipulation of excitons in GaAs. There are three main aspects to be addressed. In the first part, we provide a comprehensive understanding of the slow- and fast-light propagation based on excitonic resonances. Propagation (or transit) times of optical pulses through a medium near an absorptive resonance with and without spatial dispersion are studied and contrasted. We show that, when the broadening of the resonance (i.e., dephasing rate) is below a critical value, a frequency range exists near resonance where the transit times are determined by interference between co-propagating exciton-polaritons and deviate strongly from expectations based on the group velocities of the individual exciton-polariton branches. Our theory puts the well-known slow- and fast-light effects in systems without spatial dispersion into a broader context by interpreting them as a limiting case of systems with spatial dispersion. An important ingredient of the exciton theory is the light-matter coupling that can be expressed either in terms of the dipole or the momentum matrix elements. We re-examine the validity of a frequently used relation between the interband momentum and dipole matrix elements ('p-r relation') in semiconductors. An additional correction term was obtained when we applied the 'p-r relation' to finite-volume crystals treated with periodic boundary conditions. The correction term does not vanish in the limit of infinite volume. We illustrate this with numerical examples for bulk GaAs and GaAs superlattices. For bulk GaAs, the correction term is found to be always important; while for a GaAs superlattice, the importance of the correction term for the transition depends strongly on the origin of the unit cell.As an example for manipulation of excitons, we consider mechanical deformations of GaAs nanomembranes. The nanomembranes with lateral sizes much larger than their thicknesses exhibit great flexibility in non-planar deformations and thus promise applications in flexible electronic and photonic devices. These non-planar deformations do not fit in the well-established theory for planar deformations induced by lattice mismatch. Our theory relates the general mechanical deformations (planar or non-planar) of nanomembranes to their excitonic spectra, and is numerically evaluated within the average-strain approximation.
This dissertation addresses both fundamental aspects of the coherent exciton kinetics in single semiconductor quantum wells and more application-oriented aspects of the collective excitonic optical properties in quantum well Bragg structures. We use a bosonic theory to investigate the ultrafast coherent exciton dynamics after an optical excitation in a single semiconductor quantum well. It is shown that, on intermediate time scales, nonlinear mean-field interactions between excitons lead to a coherent, wave-like evolution in the momentum distribution of optically inactive excitons, which can survive for some time before dephasing sets in. Driven by two-exciton correlations, this coherent quantum kinetic effect bridges the well-known kinetics associated with optical excitation on the one hand and incoherent relaxation on the other. We also study more general dynamical properties of bosonic mean field systems with N-species of excitons (in a single semiconductor quantum well). We find that the momentum-conserving exciton mean field equations, including the coupling to external fields and fermionic corrections, have the dynamical structure su(N,N). We show that one can define a non-real generalized "Bloch vector" and a non-hermitian "density matrix" description, which allow us to explicitly obtain all the constants of motion associated with the su(N,N) symmetry. The many-body effects and correlations of excitons in a single quantum well are mainly induced by the Coulomb interactions. In the case of a semiconductor quantum well Bragg structure, the light induced coupling between different quantum wells also dramatically affects the excitons' behavior, especially through the collective excitations of excitons in the whole structure. We investigate the linear excitonic optical properties of the quantum well Bragg structure induced by the collective excitations using the transfer matrix approach. We show that the so called "intermediate band" (IB) created by the exciton resonance, which does not exist in conventional photonic crystals, can be used for the stopping, storing and releasing of light, which is important in information processing devices. We also discuss the compensation of the dispersive distortion in the light delay process through reversing the IB band structure. Other conceptual and practical issues such as the decay rate of the IB modes and the generalized anti-reflection coating are also investigated.
Propagation of light pulses in wide-gap semiconductors, GaN and ZnO, has been studied by time-of-flight spectroscopy. It has been demonstrated that significant light delay exists near an exciton resonance and that this delay is accompanied by pulse distortion and attenuation. Simulation of the pulse shape in the time-energy plane has permitted us to refine excitonic parameters inherent for bulk materials. The time-of-flight studies done over a wide temperature range demonstrate the strong influence of resonant scattering by phonons on the light delay in polar semiconductors. Optical dispersion at exciton resonances in semiconductors results in a delay of light transfer, which is induced by the variation of the group velocity — a phenomenon studied long ago(1-3). Thisdelayhasbeenobservedbytime-of-flightspec- troscopy in different semiconductors (4-6). The current inter- estinsuchretardationisenhancedbecauseitisoneoftheways toobtaintheso-calledslowlight,whichisneededforoptical communication and data processing. Wide-gap semiconduc- tors, like ZnO and GaN, possess strong excitonic resonances thatmakesthemsuitableforsuchapplication. Lightvelocities as low as 6000 km/s in ZnO (4) and 2100 km/s in GaN (5) have been recently measured. In view of these findings, the distortion of a pulse shape has attracted special attention (7). It is worth mentioning that early experiments showed no sig- nificant changes in the shape of a light pulse at the excitonic resonances in GaAs (8) and GaP (9), while the optical dis- persion near the resonances implies a different group velocity and attenuation for the higher- and lower-energy edges of the pulses (10), that inevitably means their distortion in the time- energy plane. The optical pulse modification is also important for a set of optoelectronic devices — high-frequency ones or those, where the light should propagate a long distance. The
Excitons, the bound states of an electron and a hole, in semiconductors are interesting objects and they continue to attract attention of researchers from all over the world. Despite intense research on exciton physics over last three-four decades, many interesting phenomena related to the dynamics and the nonlinear optical properties of excitons in semiconductors and their nanostructures in the coherent and incoherent regimes are still to be explored. This thesis presents our effort to study the nonlinear optical properties as well as the exciton dynamics in coherent and incoherent regime in semiconductor nanostructures including GaAs quantum wells (QWs) and InAs quantum dots (QDs). We have set up several time-resolved and steady-state optical spectroscopic measurement techniques in our laboratory to carry out our study on excitons dynamics in semiconductor QWs and QDs. We work out a clear and detailed theory of the pump-probe signal taking account of all aspect of the measurement, namely, the lock-in detection, spectral selection by the monochromator and time-integration at the slow photodetector. We have used the formalism of optical Bloch equations conventionally used to analyse wave mixing experiments. Our analysis puts the pump-probe technique on the same footing as the wave mixing experiments. We show that pumpprobe experiments can be used to study both coherent and incoherent dynamics. We also present a clear physical picture of the measured signal using the Lorentz harmonic oscillator model. We report the investigation of the coherent exciton dephasing dynamics using pumpprobe reflectivity measurement in GaAs QWs for resonant excitation. Two GaAs/AlGaAs QWs with well thicknesses 8 nm and 17.5 nm are used. We found a strong dependence of the dephasing rate of the excitons with increasing exciton density due to exciton-exciton scattering. We found that the exciton dephasing rate of 8 nm QWs at low excitation density and at low lattice temperature is larger than the corresponding dephasing rate of the 17.5 nm QWs, possibly due to larger effect of inhomogeneous broadening. We also report that the dephasing rates for both QWs are linear with the sample temperature below the 30 K. We report the study of ionization equilibrium between the exciton and the electronhole plasma population in the temperature and pressure (excitation density) phase space. Non-resonant excitation of semiconductor creates a nonequilibrium state of electron-hole plasma. We investigate this ionization equilibrium using steady state photoluminescence and time-resolved excitation correlation PL measurements. We present a clear phase diagram (in temperature and carrier density phase space) of this ionization process.A clear density-dependent increase in the ionization ratio is observed and its connection with the Mott transition is discussed. Semiconductor nanocrystals and QDs are another important area of research, mainly due to their huge potential for device application. We present a simple model which combines carrier loss kinetics, detailed balance principle in thermodynamic equilibrium and Pauli exclusion principle to quantitatively explain the observed behaviour of the experimental data.
After light became a part of the telecommunication system, the manipulation of light, especially the control of the speed of light, became a focus of research. By using the different approaches of the interaction between light and matter, there have been many successful attempts to slow down the speed of light, even to several meters per second. In the first part of my thesis, I studied pulse propagation in absorptive media (GaAs/AlGaAs multiple quantum well structures-MQWs) to gain insight into the linear interaction between matter and light. Systematic and fundamental measurements of pulse propagation in GaAs/AlGaAs multiple quantum well structures will be presented. These measurements are simulated by treating MQWs as a slab. These measurements and simulations will be compared while using a newly introduced general formalism.\nIn the second part of my thesis, I will present another aspect of manipulating light: all-optical switching. Eric Gansen demonstrated all-optical switching in GaAs/AlGaAs MQWs at cryogenic temperatures. I will demonstrate that the same design of all-optical switch, which is based on polarized virtual carriers, can work without any serious loss of performance at near-room temperatures.\nAnother material used in all-optical switches is Bragg-spaced-quantum-well structures (BSQWs) which are grown by molecular beam epitaxy. The growth of BSQW is challenging because of the associated unusually long growth times. In the last part of this dissertation, I will discuss the challenges involved in MBE growth of 210 period long GaAs/InGaAs BSQWs. By presenting basic characterization measurements of the successful and unsuccessful attempts of BSQW growths, I will demonstrate the challenges of BSQW growth and how they can be addressed.