No description available.

The research described in this thesis relates to the design, fabrication and testing of novel semiconductor-based light sources that have been designed for the generation of infra-red light. The thesis is formatted to account for two distinct components of my work, where the first part concerns sources producing coherent light by direct laser emission, notably, ultrashort-pulse quantum-dot lasers. These types of lasers continue to show considerable promise as efficient, compact sources of ultrashort pulses with durations of hundreds of femtoseconds, while giving rise to unique and interesting electronic properties such as low lasing thresholds through the quantum nature of their density of states. At the outset a study of the most relevant aspects of the lasing dynamics of an optically pumped quantum-dot laser is outlined. Pumping of the device with intense discrete optical pulses leads to output from multiple electronic states, each having a characteristic wavelength and temporal properties. I show that pulses produced by excited-state emission have shorter durations (24 ps) and arrive earlier in time than those due to transitions from the ground state, which themselves have durations of around 180 ps. Investigations are then made on two different mode-locked quantum-dot laser systems. One is an all-quantum-dot external-cavity laser that is mode locked using a quantum-dot SESAM device at a repetition frequency of 860 MHz with output power approaching 20 mW. This is followed by a study of a monolithic two-section quantum-dot laser that is mode locked stably in a wide temperature range of 20°C to 70°C. The excellent performance characteristics presented serve to demonstrate both the versatility of quantum-dot material as components in mode-locked laser systems and the temperature stability of such laser devices. The second part of the thesis relates to structures that are designed to take advantage of nonlinear frequency conversion in GaAs-based semiconductors. This material system possesses a nonlinear coefficient of ~170 pm/V and is transparent from around 0.9 μm through to 17 μm, making it attractive for the realisation of a new class of efficient, integrable, quasi-phase-matched, optical parametric oscillator devices. Initially, ion implantation is utilised as a vector to create a periodically-switched nonlinear ridge waveguided device. The observation is made that in the course of implantation the transmissive properties of the device are severely degraded. Unfortunately, the high losses incurred, which reached 250 dB/cm, could not be removed without also destroying the modulation in nonlinearity. During the course of this investigation, significant technological advances were made in the production of orientation-patterned GaAs structures. By recognising the elegance and potential of this new orientation-patterned (OP) methodology, a study of its implications and applicability in the context of my project is initiated.

"Molecular engineering of some 2,4,6-(substituted biarylamino)-1,3,5-triazines and crystal data belonging to the products 2,4,6-(m,m’-ditolylamino)-1,3,5-triazine, 2,4,6-(p,p’-ditolylamino)-1,3,5-triazine and 2,4,6-(phenyl-p-tolylamino)-1,3,5-triazine were reported. Retrosynthetic analysis of trigonal octupolar networks led to the identification of tris-substituted diarylamino-triazines as molecular analogs of Piedfort units formed by cofacial dimers of 2,4,6-triaryloxy-1,3,5-triazine molecules. Synthesis of mono and diarylamiono triazines is achieved by coupling of the corresponding anilines with cyanuric chloride. Synthesis of diarylamines exhibiting different functional groups on two phenyl rings is attempted; the successful attempt in the case of phenyl-p-tolylamine is described. All the crystals obtained so far belong to centrosymmetric space group P21/c. Though none of the molecules retain trigonal symmetry in the crystal structures, pseudo-trigonal assembly of molecules is identified in some cases. The assembly of molecules within the crystals results in columnar structures formed by C-H..N and C-H..pi interactions."

Developing a greater understanding of multiferroic materials, particularly those in which a strong coupling is exhibited between magnetic and electrical orderings, is of great importance if potential applications are to be realised. This thesis reports new experimental findings on several multiferroics using the techniques of X-ray and neutron diffraction together with nonlinear optical experiments. Spherical neutron polarimetry measurements on RbFe(MoO<sub<4</sub>)₂ show how this system's chiral magnetic structure can be controlled by an external electric field. Consideration is given to the axial distortion that the crystal structure makes, and the effect that this has on the stabilised magnetic structures. A ferroaxial coupling is invoked to explain, from a symmetry point of view, the spin driven multiferroicity in this proper screw system. The charge ordering in YbFe₂O₄ is examined by a detailed imaging of reciprocal space measured by elastic X-ray diffraction. Continuous helices of scattering are observed above the three-dimensional ordering transition temperature, whereas the intensity is concentrated onto separated maxima below this. The low temperature data are modelled using a simple oxygen displacement pattern, generalised to an incommensurate structure. The observed incommensurability implies that YbFe₂O₄ cannot be truly ferroelectric. The low field magnetic structures of a Y-type hexaferrite Ba_0.5Sr_1.5Zn₂Fe₁₂O₂₂ are observed in a resonant soft X-ray diffraction study. In zero field the system is helimagnetic, and with small applied fields peaks corresponding to a new phase appear. Energy calculations are used to suggest a suitable magnetic structure for the new phase and to show how this relates to the known commensurate phases that are present in low fields. Finally, an experimental setup designed to measure second harmonic generation from non-centrosymmetric crystals is presented, along with static measurements on the multiferroic system MnWO₄. An optical pump / second harmonic probe study is then undertaken, with the result that a pump induced enhancement in the efficiency of the second harmonic generation is observed.

The topic of this thesis is about experimental study of phenomena which are associated with light propagation in nonlinear dielectric media. In the first part of this work, we study experimentally the snake instability of the bright soliton stripe of the (2+1)-dimensional hyperbolic nonlinear Schrödinger equation. The instability is observed, through spectral measurements, on spatially extended femtosecond pulses propagating in a normally dispersive self-defocusing semiconductor planar waveguide. The second part of this thesis is about light propagation in nonlinear periodic media. We experimentally observe a stationary spatial gap (or Bragg) soliton in a periodic semiconductor planar waveguide. Based on the interference pattern of the soliton beam, we measure the power parameter of the soliton which is related to the position of the spatial spectrum in the linear band gap. Cette thèse de doctorat a pour sujet l’étude expérimentale de phénomènes associés à la propagation de la lumière dans les milieux diélectriques non linéaires. La première partie porte sur la démonstration expérimentale de l’instabilité serpentine d’une bande solitonique dans un système décrit par une équation de Schrödinger non linéaire à (2+1)-dimensions. L’instabilité est observée sur base de mesures du spectre spatial ainsi que du profil spatio-fréquentiel d’une impulsion femtoseconde après propagation dans un guide plan semi-conducteur qui présente une dispersion normale et une non-linéarité défocalisante. Le second thème abordé concerne la propagation de la lumière dans les milieux non linéaires périodiques. Les expériences réalisées ont montré l’existence du soliton de Bragg spatial stationnaire sous forme de faisceaux se propageant dans des guides plans semi-conducteurs périodiquement gravés. Sur base du profil de la distribution modale en intensité du faisceau soliton, il a été possible de mesurer le paramètre de puissance du soliton de Bragg qui détermine la position du spectre spatial dans la bande interdite linéaire.

No description available.

The nonlinear optical properties of a semiconductor-doped glass (SDG) channel waveguide were measured on a picosecond time-scale; namely, fluence-dependent changes in the absorption and the refractive index as well as the relaxation time of the nonlinearity. Slower, thermally-induced changes in the refractive index were also observed. The saturation of the changes in the absorption and the refractive index with increasing optical fluence is explained using a plasma model with bandfilling as the dominant mechanism. The fast relaxation time of the excited electron-hole plasma (20 ps) is explained using a surface-state recombination model. A figure of merit for a nonlinear directional coupler fabricated in a material with a saturable nonlinear refractive index is presented. The measured nonlinear change in the refractive index of the SDG saturates below the value required to effect fluence-dependent switching in a nonlinear directional coupler. Experiments with a channel-waveguide directional coupler support this prediction. However, absorption switching due to differential saturation of the absorption in the two arms of the directional coupler was observed.

Since the discovery of optical bistability a considerable amount of research activity has been aimed toward the realization of general-purpose all-optical computers. The basic premise for most of this work is the widely held notion that a reliable optical switch can be fabricated from a piece of optically bistable material. To date only a very small number of published articles have addressed the subject of the engineering issues (that is, the optimization and tolerancing) of these optical switches. This dissertation is a systematic treatment of these issues. From the starting point of Maxwell's equations a simple model of optically bistable Fabry-Perot etalons is outlined, in which the material is assumed to be a pure Kerr medium having linear absorption. This model allows for a relatively straightforward optical switch optimization procedure. The procedure is applicable for optimizing any number of switch parameters. The emphasis in this dissertation is on the optimization of the contrast of the switch's output signals, with the other parameters (switching energy, tolerance sensitivity) assuming a secondary yet critical role. Following the optimization of the optical switch is a tolerance analysis which addresses the manufacturability and noise immunity of the optimized switch. In the first part of this analysis equations describing the propagation of errors through a large scale system of like devices are derived from the truth tables of the switches themselves. From these equations worst case tolerances are established on the optical switch's transfer function parameters. In the second part of the tolerance analysis the bistability model is used to arrive at tolerances on the physical parameters of the switch. These tolerances are what determine the manufacturability of the optical switches. The major conclusion of the dissertation is that, within the range of validity of the model and the other simplifying assumptions, optically bistable Fabry-Perot etalons cannot be used reliably as logic gates in large-scale computing systems.

This dissertation describes the study of excitonic optical nonlinearities in semiconductors and semiconductor microstructures. The main emphasis is placed on the evolution of optical nonlinearities as one goes from bulk to quantum-confined structures. Included are experimental studies of molecular-beam-epitaxially-grown bulk GaAs and ZnSe, GaAs/AlGaAs multiple-Quantum-Wells (MQW's), and finally, quantum-confined CdSe-doped glasses. The microscopic origins and magnitudes of the optical nonlinearities of bulk GaAs and ZnSe were investigated and the exciton recovery time in ZnSe was measured. A comparison with a plasma theory indicates that in GaAs, band filling and screening of the continuum-state Coulomb enhancement are the most efficient mechanisms, while in ZnSe, exciton screening and broadening are the dominating mechanism for the nonlinearity. The maximum nonlinear index per excited electron-hole pair of ZnSe at room temperature is comparable to that of bulk GaAs and the exciton recovery times are of the order of 100 ps or less. A systematic study of the dependence of the optical nonlinearities on quantum well thickness for GaAs/AlGaAs MQWs and the results of nonlinear optical switching and gain in a 58 A GaAs/AlGaAs MQW are reported and discussed. The maximum change in the refractive index is greatest for the MQWs with the smallest well size and decreases with increasing well size, reaching a minimum for bulk GaAs. The maximum index change per photoexcited carrier increases by a factor of 3 as the well size decreases from bulk to 76 A MQW. A differential energy gain of 0.2 and the contrast of 4 are measured for a 58 MQW using 3 ns laser pulses. The linear and nonlinear optical properties of CdSe semiconductor microcrystallites grown under different heat treatments in borosilicate glasses are investigated. Pump-probe spectroscopic techniques and interferometric techniques were employed to study size quantization effects in these microcrystallites (quantum dots). Nonlinear optical properties due to the transitions between quantum confined electron and hole states are reported for low temperature and room temperature. A relatively large homogeneous linewidth is observed. Single beam saturation experiments for quantum confined samples were performed to study the optical nonlinearities as a function of microcrystallite size. Results indicate that the saturation intensity is larger for smaller size quantum dots.

This dissertation describes the study of various nonlinear optical effects in both bulk and quantum-confined semiconductors. Transverse effects in increasing absorption optical bistability are considered in bulk CdS for both single beam and wave mixing geometries. Measurement of the temporal response of BiI₃ quantum dots is described using degenerate four-wave mixing and explained theoretically. Finally, the experimental techniques developed to measure the one- and two-photon absorption coefficients of CdS quantum dots in glass are described along with the latest theoretical description and interpretation of the experimental spectra. The basic theory of increasing absorption optical bistability is presented along with experimental observation of this effect in CdS at low temperature. Transverse effects in increasing absorption optical bistability were observed in single beam experiments with CdS at low temperatures. The ring structures observed experimentally are explained theoretically. Degenerate four-wave mixing performed with this nonlinearity is theoretically shown to produce new scattering orders compared with a standard Kerr analysis. Experimental observation of these new scattering orders is presented. The temporal response of the nonlinearity in a solution of BiI₃ quantum dots in acetonitrile is determined using degenerate four-wave mixing. The independent contributions to the phase-conjugate signal are determined for both of the spatial gratings induced in the solution. The observed temporal responses indicated that a thermal mechanism was responsible for the nonlinearity. A theoretical analysis based on a thermal nonlinearity is presented which provides good agreement with the observed responses. The experimental techniques necessary to measure the one- and two-photon absorption coefficients of CdS quantum dots are described. The resultant measurements of quantum dot samples with microcrystallites ranging from 3.6 to 10.8 nm in diameter indicate no splitting of the energy levels associated with the hole. Theoretical spectra indicate this can be partially explained by the inclusion of Coulombic effects of the charged electron-hole pair.