Different aspects of the photoluminescence from semiconductor quantum-confined structures are studied in this dissertation, for a better understanding of fundamental physics of semiconductors.The precursor of any photoluminescence study is the characterization of the linear optical properties of the semiconductor structure. High resolution absorption measurements were performed in order to study the interplay of disorder and acoustic phonon scattering in a quantum well. Also, reflectivity measurements, together with a fitting procedure based on the transfer matrix formalism, are used to determine the thickness of samples.Excitons are atom-like quasi-particles, formed from a bound electron-hole pair. They follow a Bose-Einstein statistic, so in principle it is possible to achieve an excitonic Bose-Einstein condensate. Time resolved photoluminescence measurements were performed over an extensive range of lattice temperatures and carrier concentrations, in order to determine the fraction of excitons formed from the electron-hole plasma in a quantum well, after non-resonant excitation. The experimental spectra were compared to a pure plasma calculation first, then excitons were taken into account. The highest fraction of formed excitons is found for low temperatures and intermediate carrier densities. This fraction is found to be very small, and this has clear implications on the excitonic Bose-Einstein condensation studies.The photoluminescence emitted left and right from a quantum well is interfered in a modified Mach-Zender interferometer. It is shown that the light emitted on the two paths will interfere for a V-shape geometry and will not for any other paths.A structure formed by placing a quantum well in a field antinode of a resonant planar microcavity exhibits normal mode coupling: splitting of the resonance spectral line. The coherence properties of the photoluminescence from a normal-mode-coupling microcavity are studied using another version of the Mach-Zender interferometer. The degree of coherence measured in this way depends greatly on the pump wavelength and intensity, ranging from zero to 0.8. However, direct observation of the emission speckle shows significant coherence in all cases. The difference is explained by the different methods used to evaluate the coherence.The strong coupling between a quantum dot and a photonic crystal nanocavity is investigated by observation of photoluminescence. A new method of tunning the cavity wavelength by deposition of a thin film of solid Xenon on all the surfaces of the sample is presented. The method allows the scanning of the cavity wavelength with about 5 nm without a decrease in the quality factor and without changing the temperature.Finally, an extensive study of the quality factors of quantum dot photonic crystal nanocavities is presented. The role of the quantum dot ensemble absorption is investigated. At higher excitation levels, lasing is observed and discussed.
Different aspects of the photoluminescence from semiconductor quantum-confined structures are studied in this dissertation, for a better understanding of fundamental physics of semiconductors.The precursor of any photoluminescence study is the characterization of the linear optical properties of the semiconductor structure. High resolution absorption measurements were performed in order to study the interplay of disorder and acoustic phonon scattering in a quantum well. Also, reflectivity measurements, together with a fitting procedure based on the transfer matrix formalism, are used to determine the thickness of samples.Excitons are atom-like quasi-particles, formed from a bound electron-hole pair. They follow a Bose-Einstein statistic, so in principle it is possible to achieve an excitonic Bose-Einstein condensate. Time resolved photoluminescence measurements were performed over an extensive range of lattice temperatures and carrier concentrations, in order to determine the fraction of excitons formed from the electron-hole plasma in a quantum well, after non-resonant excitation. The experimental spectra were compared to a pure plasma calculation first, then excitons were taken into account. The highest fraction of formed excitons is found for low temperatures and intermediate carrier densities. This fraction is found to be very small, and this has clear implications on the excitonic Bose-Einstein condensation studies.The photoluminescence emitted left and right from a quantum well is interfered in a modified Mach-Zender interferometer. It is shown that the light emitted on the two paths will interfere for a V-shape geometry and will not for any other paths.A structure formed by placing a quantum well in a field antinode of a resonant planar microcavity exhibits normal mode coupling: splitting of the resonance spectral line. The coherence properties of the photoluminescence from a normal-mode-coupling microcavity are studied using another version of the Mach-Zender interferometer. The degree of coherence measured in this way depends greatly on the pump wavelength and intensity, ranging from zero to 0.8. However, direct observation of the emission speckle shows significant coherence in all cases. The difference is explained by the different methods used to evaluate the coherence.The strong coupling between a quantum dot and a photonic crystal nanocavity is investigated by observation of photoluminescence. A new method of tunning the cavity wavelength by deposition of a thin film of solid Xenon on all the surfaces of the sample is presented. The method allows the scanning of the cavity wavelength with about 5 nm without a decrease in the quality factor and without changing the temperature.Finally, an extensive study of the quality factors of quantum dot photonic crystal nanocavities is presented. The role of the quantum dot ensemble absorption is investigated. At higher excitation levels, lasing is observed and discussed.
Nonlinear optical phenomena in both semiconductor microcavities and sodium vapor are investigated. Systems displaying atomic and excitonic coupling are studied in detail in order to unravel underlying physical principles. Possible applications for these systems are evaluated where appropriate. Normal-mode coupling (NMC) in a semiconductor microcavity is achieved when a narrow-linewidth quantum well exciton resonance is coincident with the cavity mode of a high-finesse microcavity. This interaction leads to a double-peaked spectrum in either transmission, reflection, or photoluminescence (PL). The high-quality microcavities studied here at liquid-Helium temperatures reveal intensity dependent behavior that has not previously been observed. Nonlinear saturation of the exciton leads to a spectral broadening of the excitonic absorption without a significant loss in oscillator strength. This results in a reduction of the two transmission peaks with almost no change in the splitting between the peaks. Such behavior is easily explained using phenomenological nonlinear dispersion theory. In this nonlinear regime, the luminescence from the microcavity shows a gradual transition from the nonperturbative regime of NMC to lasing with increasing excitation. The observed behavior is explained by density-dependent changes in both the transmission of the microcavity and the bare-exciton emission, rather than a boson-condensation of excitons which has been previously proposed. An intermediate-finesse microcavity also modifies the emission distribution from a bulk-semiconductor at room temperature. Angularly resolved emission spectra and quantum efficiency measurements show the PL is strongly dependent on the reflectivity of the microcavity. Unfortunately, the enhancement in the decay rate of excitons due to high-reflectivity mirrors seen previously by our group does not result in an increased quantum efficiency. High-gain optical-wavefront amplification in atomic sodium vapor is demonstrated via both the three-photon effect and stimulated Raman scattering (SRS). In both cases, single-pass weak-field gain of nearly 400 is achieved with only 800 mW of pump power near 589 nm. In the case of SRS, phase preservation of the amplified wavefront, which is necessary in adaptive imaging applications, is also demonstrated.
This dissertation presents investigations of fundamental optical nonlinearities in semi-conductor microstructures. Two distinct effects are studied. In the first part the excitonic optical Stark effect in InGaAs and GaAs multiple quantum-well structures is investigated by means of pump-probe spectroscopy. For nonresonant excitation below the excitonic transition the direction of the shift of the resonance depends on the polarization of the pump and probe pulses. In particular, for anti-circular polarization a surprising red-shift is observed. For resonant excitation, induced absorption energetically above and below the exciton transition and bleaching of the resonance is found. Experiments using both resonant and nonresonant excitation reveal the importance of bound and unbound two-exciton states in absorption changes of the 1s heavy-hole exciton resonance. It is found that higher-order Coulomb contributions determine the intensity as well as the time dependence of the differential excitonic absorption. In addition, the influence of light-hole excitons is analyzed. It is shown that the direction of the optical Stark shift for nonresonant excitation depends also sensitively on the heavy-hole to light-hole splitting and the detuning of the pump pulse. For very high pump intensities and nonresonant excitation the absorption is split when a circularly polarized pump and a linearly polarized probe beam are used. For co-circular excitation traces of hyper-Raman gain are observed. In the second part of this dissertation, the nonlinear optical response of semiconductor microcavities in the nonperturbative regime is studied in resonant single-beam transmission and pump-probe experiments. In both types of experiment, a pronounced third transmission peak lying spectrally between the two normal modes is observed. Its dependence on the probe intensity, pump intensity, pump-probe delay, exciton-cavity detuning and pump detuning is investigated. For single-beam transmission, the energy of the third peak parallels the position of the cavity resonance. It is more pronounced for circularly polarized excitation and lasts longer than the two normal modes. For pump-probe experiments, the third peak increases with decreasing probe intensity and increasing pump intensity. Its energy is close to the low-energy side of the pump spectrum and virtually unaffected by the cavity-exciton detuning. The appearance of the third peak requires temporal overlap of pump and probe pulses. The origin of this complex nonlinearity is the quantum nature of light, which induces intraband polarizations in the presence of a coherent driving field and a finite carrier density. It is found that the coupling of the intraband polarizations via guided modes to the polarization of the fundamental longitudinal mode is responsible for the third transmission peak. A fully quantized theory reproduces the experimental observations.
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.
The three-dimensional confinement created by the ultrasmall semiconductor structures known as quantum dots greatly modifies the optical properties of the spatially localized carriers. These systems are presently of great interest to the research community, both for the improved understanding of the physics of confined structures, and for the potential applications of these systems to areas such as optoelectronics and quantum computing. Here, the techniques of transient coherent nonlinear optical spectroscopy are applied to the investigation of excitons confined within InAs/GaAs self-assembled quantum dots. These methods provide a powerful tool for the study of dynamic processes in these novel materials. The nonlinear measurements are based on the differential transmission experimental geometry, and utilize ultrafast pulsed lasers in order to temporally resolve the carrier dynamics after excitation. The experiments performed here are resonant with the ground state absorption of the quantum dots, as evidenced by comparison with the photoluminescence measurements which are used to characterize the sample. The incoherent relaxation dynamics of the population of photoexcited excitons are examined, allowing for a determination of both the lifetime of the excitons and the time scale for relaxation between the two polarization eigenstates of the system. The three-dimensional quantum confinement results in the suppression of these relaxation processes, as predicted. The use of coherent spectroscopic techniques allows for the first unambiguous demonstration of an optically-induced nonradiative Raman coherence in these quantum dots. Simultaneous excitation of both polarization states of the exciton results in a coherent superposition state, whose temporal evolution is observed through the homodyne-detection scheme. In these transient experiments, this is manifested as a beating in the nonlinear response, which allows us to directly measure the fine-structure splitting between the polarization states. Utilizing optical pulse shaping techniques, transient spectral hole burning is performed, which allows for the nonlinear response to be spectrally resolved. As expected for the strongly confined quantum dot excitons, the results show that diffusion among the localized states is not a significant effect. Temperature dependent measurements show that at elevated temperatures, extra dephasing processes, potentially related to acoustic phonon scattering, become important. Finally, this technique allows for the first direct observation of the induced absorption from the exciton to biexciton transition in these InAs quantum dots, and a measurement of the associated binding energy. These results lay the foundation for future studies in this material system, and for the possible development of quantum logic devices utilizing quantum dots.
Semiconductor quantum microcavities are interesting physical systems in which fundamental interactions between light and excitons can be explored. For example, in the weak - coupling limit, modified excitonic spontaneous emission can be observed. In the strong-coupling limit, the cavity field modes and the quantum well exciton modes become coupled; the normal modes of the system are "cavity-polaritons" [1,2]. For in-plane wavevectors k// near zero, the normal modes are split by the dipole coupling between the excitons and the cavity vacuum field. This splitting is often referred to as a vacuum-Rabi splitting (VRS), as it has the same physical origin as the VRS observed in the interactions of atoms with single-mode cavities. The physical system in this work consists of a λ planar microcavity formed by two distributed-Bragg reflectors, with five GaAs quantum wells situated in the center of the cavity. In all the experiments described here, the exciton and cavity modes are on resonance (the low-field VRS is 6 meV for this sample).
This thesis is devoted to theoretically study the systems of single quantum dots (QDs) embedded in various photonic nanostructures, in close relation with experimental data. The word single is essential: due to their nanometer size, QDs have mainly been studied as ensembles. It is only recently that the experimental progress, in particular in the domain of QDs growth, has allowed to address single QDs. This helped to observe that the confined states in a QD resemble those of an atom, leading in turn to the macro-atom picture for QDs. It opened the path to the study of cavity quantum electrodynamics (CQED) in the solid state, as the analogous of a system of an atom in an electromagnetic cavity. However, already at the level of the QD (i.e. without a solid state cavity), the macro-atom picture has been proven to be oversimplified. Various effects related to the solid state environment of the QD have been experimentally and theoretically evidenced, like the influence of acoustic and optical phonons. These are channels of decoherence for the otherwise well isolated and confined QD levels. When adding the cavity, these effects are possibly enhanced, which can lead to very large deviations from the CQED ideal picture. Therefore the clear understanding of these effects is of essential importance, especially in view of the application of solid state systems to quantum information science. In Chapter 2, we address the radiation-matter coupling between two QDs in a nanocavity. This field of research combines the high quality of light resonators to the nonlinearities of the semiconductor material. It is promising in view of manipulating and transferring single long-lived excitations, an essential goal for quantum information science. Then, we study the deviations of a QD from the idealized macroatom picture. First, in Chapter 3, we include the influence of acoustic phonons on the light emitted by a QD-cavity system. We show that the QD modified susceptibility leads to the qualitative explanation of the cavity feeding effects, which is one of the most striking deviations of the QD-cavity system from the ideal CQED picture. In addition to phonons are extended two-dimensional states populated by the non resonant pumping laser in the QD's wetting layer (WL). In Chapters 4 and 5 we build a Monte-Carlo model of the excitation-decay mechanism in a QD-cavity system. We use it to describe the influence of WL states on the dynamics of the QD, leading in turn to a non-CQED behavior. This approach is particularly successful in the case of large QD-cavity detuning, where it predicts both time-dependent and spectral characteristics of the emitted light. Finally, in Chapter 6, we discuss our conclusions, emphasizing in particular that the knowledge of the actual solid state environment of the QD leads to a better control over the parameters allowing to reach the CQED regime. We also discuss the possible extensions of this work, in particular in relation to the analysis of the stimulated emission regime.