We review the nonlinear-optical effects observed at room temperature in semiconductor quantum-well structures photoexcited near the band gap. A comprehensive discussion of optical transitions in these microstructures is given, including excitonic effects and the specific features of room-temperature exciton resonances. Experimental investigations using continuous-wave, picosecond-, and femtosecond-laser sources are presented. They show extremely efficient nonlinear processes. In the case of excitations that are long compared with the exciton-ionization time, the induced changes in absorption and refraction do not depend on the wavelength or on the duration of excitation. These changes depend only on the density of absorbed photons and are interpreted in terms of electron–hole plasma screening and band filling. In contrast, for ultrashort excitation, nonlinear processes depend critically on the excitation wavelength. The selective generation of excitons is found to produce effects larger than a plasma of the same density. This unexpected result is shown to arise from the low temperature of the exciton gas before it interacts with the lattice and from the decrease of screening that is the reduced dimensionality of quantum-well structures.
We review the nonlinear-optical effects observed at room temperature in semiconductor quantum-well structures photoexcited near the band gap. A comprehensive discussion of optical transitions in these microstructures is given, including excitonic effects and the specific features of room-temperature exciton resonances. Experimental investigations using continuous-wave, picosecond-, and femtosecond-laser sources are presented. They show extremely efficient nonlinear processes. In the case of excitations that are long compared with the exciton-ionization time, the induced changes in absorption and refraction do not depend on the wavelength or on the duration of excitation. These changes depend only on the density of absorbed photons and are interpreted in terms of electron–hole plasma screening and band filling. In contrast, for ultrashort excitation, nonlinear processes depend critically on the excitation wavelength. The selective generation of excitons is found to produce effects larger than a plasma of the same density. This unexpected result is shown to arise from the low temperature of the exciton gas before it interacts with the lattice and from the decrease of screening that is the reduced dimensionality of quantum-well structures.
The purpose of this research is to study the relaxation of optically generated excitons and carriers in semiconductor microstructures using four wave mixing (FWM) spectroscopy. The systems studied include CdSSe microcrystallite doped glasses and GaAs/AlGaAs multiple quantum well structures (MQWS). Exposing a semiconductor to optical radiation near the fundamental band gap results in the creation of populations of elementary excitations including electrons, holes, and excitons, and also results in the creation of a superposition state between the ground and excited state of the solid. The work in this dissertation examines the relaxation of the populations of elementary excitations and the relaxation of the coherence between the ground and excited state using four wave mixing spectroscopy. First, the nonlinear optical response of simple two level systems is examined in order to provide insight into the types of line shapes expected from semiconductors. It is shown that the line shape is strongly dependent on how the system is coupled to the reservoir and the consequences of coupling to a reservoir are examined in a FWM measurement made in atomic sodium. The first semiconductor system studied is CdSSe microcrystallite doped glass. This system is shown to have a very slow component to the nonlinear response which has a optical intensity dependence and temperature dependence which suggests that the FWM response in these materials is trap mediated. Room temperature FWM measurements in GaAs MQWS enables the measurement of the carrier recombination time and the ambipolar diffusion coefficient. Using the technique of correlated optical fields, a slow component to the nonlinear response was measured showing an interference profile which suggests a possible shift of the exciton resonance due to the optically generated carriers. At low temperatures (2-20 K), measurements of the exciton line shape and relaxation time were made and evidence for exciton spectral diffusion was found. The low temperature line shapes can be qualitatively reproduced using Modified Optical Bloch equations which include the effects of spectral diffusion.
Optical bistability and bright and dark resonator solitons exist in semiconductor resonator at room temperature [C.O. Weis and Ye. Larionova, Rep. Prog. Phys. 70 (2007) 255-335], with the usual semiconductor nonlinearity. At low temperature in the strong coupling regime between quantum well excitons and the optical field in a semiconductor microcavity the nonlinearities are strong and based on “polariton nonlinearity”. The strong coupling results in a quasi-particle “exciton-polariton” which gives access to positive and negative reactive and dissipative optical nonlinearities, as opposed to the usual room temperature semiconductor nonlinearities possessing essentially only one sign. The type of nonlinearity and the properties of solitons can be varied widely by the detuning between the photon- and exciton resonances. We show for the first time experimentally the existence of patterns, bright and dark solitons based on polariton nonlinearity. 1. INTRODUCTION Bright and dark spatial solitons were shown to exist in such microresonators with and without population inversion [1-3]. At room temperature the nonlinearity which is at the origin of the soliton existence is the usual mixed absorptive/refractive semiconductor nonlinearity which can have transverse effects (e.g. self-focusing) and longitudinal effects such as nonlinear resonance, both ingredients for soliton stability. At low temperature (or at large exciton binding energies) the exciton, which merges with the absorption band at room temperature, is well separated spectrally from the absorption band so that the nonlinearity becomes that of a 2-level system. If the exciton resonance is strongly coupled with the field inside a resonator the exciton- and the photon resonances mix. At coincidence of the two resonance frequencies, the photon- and the exciton resonances hybridize in an avoided crossing and the two hybrid resonances are ascribed to a quasi-particle, the excitonpolariton. This quasi-particle has unusual optical properties. E.g. is the photon nonlinearity determined by exciton collisions. That the exciton-polariton system has interesting nonlinearities (e.g. induced absorption as opposed to the usual saturable absorption) has been shown previously [4]. It was realized that semiconductor microresonators in the strong field-exciton coupling regime might show optical bistability and first experimental proofs for bistability were given recently [5]. As optical bistability of a resonator is a precondition for the existence of spatial resonator solitons, the question arises whether semiconductor microresonators with polariton nonlinearity can support spatial resonator solitons, which, as a consequence of the large nonlinearity of the polaritons, could be expected to exist at rather small light intensities, as it is of importance for all applications. 2. EXPERIMENTAL ARRANGEMENT AND RESULTS The cooled resonator sample (4 K) is illuminated by light at the polariton resonance wavelengths, and the light reflected from the resonator is observed. The light source is a Ar
We report on an experimental study of the origin of the nonlinearities and the size of the nonlinear index at various wavelengths close to the exciton resonance and the material band gap. It is concluded that for intensities required for optical bistability, the nonlinearity is mainly excitonic for MQWs with well sizes W of 50 and 152 Å which are either smaller or slightly larger than the exciton radius a. For 299-Å MQW, (W ≃ 2a), where the MQW behaves more like bulk but still has distinct excitonic features, the nonlinearity is due to the combination of exciton screening, band filling, and screening of the continuum states. For bulk GaAs, the effect of exciton is comparatively small and the latter two effects are responsible almost equally for the change in the refractive index. The measured nonlinear indices are rather similar for all these samples with the bulk GaAs and 299-Å MWQ exhibiting slightly larger Δn (change in index) for similar carrier densities (or for similar light intensities). The 50-Å MQW has a slightly smaller value of nonlinear index because the nonlinearity which in this sample is due to the saturation of the exciton resonance occurs at higher excitation intensities due to larger exciton binding energy.
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.
We have identified several physical processes by which below-gap photons can modify excitonic absorption in GaAs quantum wells.1-3 These different phenomena can be distinguished by their temporal response times, which range from tens of nanoseconds to less than one picosecond. Our experiments also show that the relative contributions of these mechanisms to below-gap optical modulation of exciton absorption depend strongly on temperature as well as on the wavelength of the below-gap modulating beam. The size of the modulation indicates that a new class of absorptive and dispersive devices for optical signal processing is possible in which signals propagate in the transparent region of the crystal and experience negligible attenuation. In order to successfully interpret and calculate the magnitude of these exciting new effects, we show that it is necessary to take into account the special properties of two-dimensional excitons in semiconductor quantum wells.
Ultrafast nonlinear optical spectroscopy is used to study the coherent dynamics of optically excited electron-hole pairs in semiconductors. Coulomb interaction implies that the optical inter-band transitions are dominated, at least at low temperatures, by excitonic effects. They are further enhanced in quantum confined lower-dimensional systems, where exciton and biexciton effects dominate the spectra even at room temperature. The coherent dynamics of excitons are at modest densities well described by the optical Bloch equations and a number of the dynamical effects known from atomic and molecular systems are found and studied in the exciton-biexciton system of semiconductors. At densities where strong exciton interactions, or many-body effects, become dominant, the semiconductor Bloch equations present a more rigorous treatment of the phenomena. Ultrafast degenerate four-wave mixing is used as a tool to study the coherent exciton dynamics, and the importance of performing transform limited spectroscopy is demonstrated throughout.