Dissertations / Theses on the topic 'High Order Displacement Field'

The application of static shape control was investigated in this thesis particularly for a composite plate configuration using piezoelectric actuators. A new electro-mechanically coupled mathematical model was developed for the analysis and is based on a third order displacement field coupled with a layerwise electric potential concept. This formulation, TODL, is then implemented into a finite element program. The mathematical model represents an improvement over existing formulations used to model intelligent structures using piezoelectric materials as actuators and sensors. The reason is TODL does not only account for the electro-mechanical coupling within the adaptive material, it also accounts for the full structural coupling in the entire structure due to the piezoelectric material being attached to the host structure. The other significant improvement of TODL is that it is applicable to structures which are relatively thick whereas existing models are based on thin beam / plate theories. Consequently, transverse shearing effects are automatically accounted for in TODL and unlike first order shear deformation theories, shear correction factors are not required. The second major section of this thesis uses the TODL formulation in static shape control. Shape control is defined here as the determination of shape control parameters, including actuation voltage and actuator orientation configuration, such that the structure that is activated using these parameters will conform as close as possible to the desired shape. Several shape control strategies and consequently algorithms were developed here. Initial investigations in shape control has revealed many interesting issues which have been used in later investigations to improve shape controllability and also led to the development of improved algorithms. For instance, the use of discrete actuator patches has led to greater shape controllability and the use of slopes and curvatures as additional control criteria have resulted in significant reduction in internal stresses. The significance of optimizing actuator orientation and its relation to piezoelectric anisotropy in improving shape controllability has also been presented. Thus the major facets of shape control has been brought together and the algorithms developed here represent a comprehensive strategy to perform static shape control.

The application of static shape control was investigated in this thesis particularly for a composite plate configuration using piezoelectric actuators. A new electro-mechanically coupled mathematical model was developed for the analysis and is based on a third order displacement field coupled with a layerwise electric potential concept. This formulation, TODL, is then implemented into a finite element program. The mathematical model represents an improvement over existing formulations used to model intelligent structures using piezoelectric materials as actuators and sensors. The reason is TODL does not only account for the electro-mechanical coupling within the adaptive material, it also accounts for the full structural coupling in the entire structure due to the piezoelectric material being attached to the host structure. The other significant improvement of TODL is that it is applicable to structures which are relatively thick whereas existing models are based on thin beam / plate theories. Consequently, transverse shearing effects are automatically accounted for in TODL and unlike first order shear deformation theories, shear correction factors are not required. The second major section of this thesis uses the TODL formulation in static shape control. Shape control is defined here as the determination of shape control parameters, including actuation voltage and actuator orientation configuration, such that the structure that is activated using these parameters will conform as close as possible to the desired shape. Several shape control strategies and consequently algorithms were developed here. Initial investigations in shape control has revealed many interesting issues which have been used in later investigations to improve shape controllability and also led to the development of improved algorithms. For instance, the use of discrete actuator patches has led to greater shape controllability and the use of slopes and curvatures as additional control criteria have resulted in significant reduction in internal stresses. The significance of optimizing actuator orientation and its relation to piezoelectric anisotropy in improving shape controllability has also been presented. Thus the major facets of shape control has been brought together and the algorithms developed here represent a comprehensive strategy to perform static shape control.

COORDENAÇÃO DE APERFEIÇOAMENTO DO PESSOAL DE ENSINO SUPERIOR
A avaliação da estabilidade do talude da Mina Robert (Canadá) é feita através do campo de deslocamentos de marcos superficiais e subsuperficiais e possíveis mecanismos de ruptura obtidos a partir da análise tensão- deformação usando-se o programa computacional FLAC (V. 3.30). Adotando-se o emprego dos modelos constitutivos elástico perfeitamente plástico e elasto-plástico com amolecimento, são calculados o fator de segurança e a porcentagem da região de plastificação, e são definidas as características de comportamento cinemático do talude sob condições de carregamento gravitacional. Apresenta-se um estudo de sensibilidade considerando-se tensões cisalhantes e deslocamentos acumulados em função da variação dos parâmetros do maciço rochoso e da inclinação do talude, além de se analisar fatores associados à definição dos mecanismos de ruptura em termos de tensão- deformação. Finalmente, são apresentadas as comparações entre os fatores de segurança calculados em função dos resultados da simulação numérica (FLAC) e os fatores de segurança calculados por equilíbrio limite considerando-se as superfícies potenciais de ruptura provenientes da modelagem computacional.
The evaluation of the stability of the Robert Pit Mine (Canada) is made through the field of displacements of superficial and ground marks and possible rupture mechanisms obtained from the results of tension-deformation analysis by using the program computational FLAC (V. 3.30). Two constitutive models, the elastic perfectly plastic model and elastic-plastic with strain softening model, are used for the determination of safety's factor and plastification area. This work also defines the characteristics of cinematic behavior of the rock slope under gravitat ional condit ions. A sensibility study is realized considering shear stress and displacements in function of the variation of the rock parameters and of the inclination of the slope. The analysis of the factors associated to the definition of the rupture mechanisms in tension-deformation terms is also done. Finally, the comparisons are presented among safety's factors calculated in function of the results of the numerical analysis (FLAC) and safety's factors calculated by limit equilibrium methods in function of the potential rupture surfaces of the computational model.
La evaluación de estabilidad del talud de la Mina Robert (Canadá) se realiza a través del campo de deslocamientos de marcos superficiales y subsuperficiales y posibles mecanismos de ruptura obtenidos a partir del análisis tensión-deformación utilizando el programa computacional FLAC (V. 3.30). Se adopta el empleo de los modelos constitutivos elástico perfectamente plástico y elasto-plástico con ablandamiento. Se calculan el factor de seguridad y el portentaje de la región de plastificación, y son definidas las características de comportamiento cinemático del talud bajo condiciones de recarga gravitacional. Se presenta un estudio de sensibilidad considerando las tensiones cisallantes y deslocamientos acumulados en función de la variación de los parámetros del macizo rocoso y de la inclinación del talud, además de nalisa factores asociados a la definición de los mecanismos de ruptura en términos de tensión - deformación. Finalmente, se presentan las comparaciones entre los factores de seguridad calculados en función de los resultados de la simulación numérica (FLAC) y los factores de seguridad calculados por equilibrio límite considerando las superfícies potenciales de ruptura provenientes del modelo computacional.

The generation of high-order harmonics opened an era of attosecond science wherein coherent light bursts are used to probe dynamic processes in matter with a time resolution short enough to resolve the motions of electrons. It enabled the development of extreme ultraviolet (XUV) and X-ray table-top sources with both temporal and spatial coherence, which provides the ability to shape the temporal and spatial structure of the XUV pulses. Scientists developed techniques to control and measure the temporal structure high harmonic emissions. These techniques exploited control of the driving laser pulse in the time domain and facilitated development of more advanced high-harmonic based XUV sources that have greatly impacted ultrafast measurements. In this thesis, I apply techniques to control and measure the spatial structure of high harmonic emissions, and discuss the underlying physics and potential applications of the interaction between spatially structured laser beams and materials. This study exploits the spatial degree of freedom in strong field interaction, which has not been given as much attention as the temporal degree of freedom. I use liquid crystal devices to shape the wave front of a fundamental laser beam to a vortex structure, then imprint this structured wave front onto XUV beams through high harmonic generation. This method provides an alternative to special XUV optics, which can manipulate the wave front of XUV radiation by all optical means. This result also reveals the conservation of orbital angular momentum in this extreme nonlinear wave mixing process. In addition to shaping the wave front, shaping the polarization of the driving beam also allows generation of circularly polarized the XUV radiation using a high harmonic source. This thesis also highlights the interplay between shaping the wave front and polarization in the high harmonic generation process. The topology of the structured beam can be maintained through this extreme nonlinear interaction due to the spin selection rules and spin-orbit conservation. Moreover, this thesis demonstrates an approach to integrate a vector beam into a broadband ultrafast light source and overcome the bandwidth limitation of mode converters. We use this approach to generate a few-cycle structured beam. In the future, this beam will be used to generate a strong ultrafast magnetic impulse in gas and solid targets by driving currents in a loop, which is a valuable tool for the future of magnetic metrology. The novel properties of structured laser beams discussed in this thesis expanded the capabilities of high harmonic based XUV sources and have opened a new field to explore this additional degree of freedom in strong field interactions.

Understanding the electronic structure and dynamics of cyclic organic molecules is becoming increasingly the subject of investigations from different perspectives due to their unique chemical and physical properties. Since they are largely involved in the biochemistry of living organisms, studies on this class of compounds are also valuable to understand biologically relevant complex systems. Compared to other techniques, high-order harmonic generation (HHG) has been increasingly considered as a powerful spectroscopic tool with Angstrom spatial and attosecond temporal resolutions. This thesis demonstrates that high-order harmonic spectroscopy is capable of providing structural and dynamical information on the electronic systems of representative cyclic organic molecules comprising randomly oriented five-membered or six-membered rings. The first part of this thesis shows that the HHG from these molecules is sensitive to their aromatic character, which results from the de-localized pi electrons, and can potentially be a useful qualitative measure of aromaticity. We show that the advantage of utilizing HHG in this direction stems from the result that only pi molecular orbitals, associated with aromatcity, are responsible for the HHG emission in aromatic systems. The capability of HHG to distinguish cyclic isomers is demonstrated in the case of xylene molecules. Supported by numerical calculations, differences in the isomers are attributed to both tunnel ionization and photorecombination, the first and last steps of HHG. These results enable further HHG-based time-resolved studies of the dynamics associated with isomeric effects that these molecules exhibit. The present work also challenges the well-established prediction that strong field ionization from a molecular orbital is suppressed along nodal planes, where the electron density is zero. In fact, our study shows that considerable tunnel ionization in some cyclic molecules can occur near or along nodal planes. This unusual ionization is reported to have its signature on the quantitative and qualitative dependence of harmonic yield on laser ellipticity. The high symmetry displayed by the cyclic molecule, 1,4 cyclohexadiene, is shown to leave its imprints on the HHG in the form of structural interferences even if the target is randomly oriented. Two-color HHG from this molecule also indicates that hole dynamics could be involved in the generation process. A general study on high harmonic spectroscopy of the Cooper minimum in molecules is also reported. The presence of this minimum could affect the interpretation of harmonics spectra in any molecule containing S or Cl atoms. The molecular environment is shown to influence the position of this spectral modulation.

At low temperatures, strongly correlated materials, which typically contain partially filled d- or f-electron shells, often exhibit phases with interesting properties, which may be of both research value and technological significance. The mechanisms of phase formation in them if could be clarified, are believed to be able to provide important insights not only into physics but also into the design of new materials. In this thesis, the experimental study of two strongly correlated materials, Sr₂RuO₄ and CeAuSb₂ is presented. Sr₂RuO₄ is an unconventional superconductor, and a strong candidate for spin-triplet superconductivity. Its potential significance in relation to quantum computing also makes it of great scientific interest. In order to clarify the role of the Van Hove singularity (VHS) in its superconductivity, experimental study has been performed with the recently developed uniaxial strain methods. The experimental results suggest that as the sample is compressed towards the VHS, the transition temperature can be enhanced by a factor of =2.3 whilst the upper critical field can be enhanced by a factor of more than ten. The experimental findings are intriguing and new possibilities are open for future study. CeAuSb₂ is a Kondo lattice system which has been speculated to be close to a quantum critical point. The similarity between some of its low temperature properties and those of a well-known quantum critical system Sr₃Ru₂O₇ makes it especially interesting. In this thesis, new magnetoresistivity and torque magnetometry measurements are used to clarify its low temperature phase diagram, and reveal the strength of its magnetic anisotropy.

This dissertation presents techniques for high-order simulation of electromagnetic fields, particularly for problems involving ships with ferromagnetic hulls and active corrosion-protection systems. A set of numerically constrained hexahedral basis functions for volume integral equation discretization is presented in a method-of-moments context. Test simulations demonstrate the accuracy achievable with these functions as well as the improvement brought about in system conditioning when compared to other basis sets. A general method for converting between a locally-corrected Nyström discretization of an integral equation and a method-of-moments discretization is presented next. Several problems involving conducting and magnetic-conducting materials are solved to verify the accuracy of the method and to illustrate both the reduction in number of unknowns and the effect of the numerically constrained bases on the conditioning of the converted matrix. Finally, a surface integral equation derived from Laplace’s equation is discretized using the locally-corrected Nyström method in order to calculate the electric fields created by impressed-current corrosion protection systems. An iterative technique is presented for handling nonlinear boundary conditions. In addition we examine different approaches for calculating the magnetic field radiated by the corrosion protection system. Numerical tests show the accuracy achievable by higher-order discretizations, validate the iterative technique presented. Various methods for magnetic field calculation are also applied to basic test cases.

The development and improvement of 3-D immersive audio is gaining momentum through the growing interest in virtual reality. Possible applications reach from recreating real world environments to immersive concerts and performances to exploiting big data acoustically. To improve the immersive experience several measures can be taken. The recording of the sound field, the spatialization and the development of the loudspeaker arrays are some of the greatest challenges. In this thesis, these challenges for improving immersive audio will be explored. First, there will be a short introduction about 3D audio and a review about the state of the art technology and research. Next, the thesis will provide an introduction to 3D loudspeaker arrays and describe the systems used during this research. Furthermore, the development of a new 16-element 3rd order sound field microphone will be described. Afterwards, different spatial audio algorithms such as higher order ambisonics, wave field synthesis and vector based amplitude panning will be described, analyzed and compared. For each spatialization algorithm, the quality of soundfield reproduction will be quantified using listener perception tests for clarity and sound source localization.
Master of Science

Scanning transmission electron microscopy (STEM) has been widely used for characterization of materials; to identify micro- and nano-structures within a sample and to analyze crystal and defect structures. High-angle annular dark field (HAADF) STEM imaging using atomic number (Z) contrast has proven capable of resolving atomic structures with better than 2 A lateral resolution. In this work, the HAADF STEM imaging mode is used in combination with multislice simulations. This combination is applied to the investigation of the temperature dependence of the intensity collected by the HAADF detector in silicon, and to convergent beam electron diffraction (CBED) to measure the degree of chemical order in intermetallic nanoparticles. The experimental and simulation results on the high–angle scattering of 300 keV electrons in crystalline silicon provide a new contribution to the understanding of the temperature dependence of the HAADF intensity. In the case of 300 keV, the average high-angle scattered intensity slightly decreases as the temperature increases from 100 K to 300 K, and this is different from the temperature dependence at 100 keV and 200 keV where HAADF intensity increases with temperature, as had been previously reported by other workers. The L10 class of hard magnetic materials has attracted continuous attention as a candidate for high-density magnetic recording media, as this phase is known to have large magnetocrystalline anisotropy, with magnetocrystalline anisotropy constant, Ku, strongly dependent on the long-range chemical order parameter, S. A new method is developed to assess the degree of chemical order in small FePt L10 nanoparticles by implementing a CBED diffraction technique. Unexpectedly, the degree of order of individual particles is highly variable and not a simple function of particle size or sample composition. The particle-to-particle variability observed is an important new aspect to the understanding of phase transformations in nanoparticle systems.
Ph.D.
Department of Physics
Sciences
Physics

High-order Harmonic Generation (HHG) is an extreme nonlinear process that can be intuitively understood as the sequence of 3 steps: i) tunnel ionization of the target atom/molecule, creating an electronic wave packet (EWP) in the continuum, ii) acceleration of the EWP by the strong laser field and iii) recombination to the core with emission of an attosecond burst of XUV coherent light. HHG thus provides a tunable ultrashort tabletop source of XUV/Soft X-ray radiation on attosecond time scale for applications ('direct' scheme). At the same time, it encodes coherently in the XUV radiation the structure and dynamical charge rearrangement of the radiating atoms/molecules ('self-probing' scheme or High Harmonic Spectroscopy). This thesis is dedicated to both application schemes in attophysics based on advanced characterization and control of the attosecond emission. In the so-called 'self-probing' scheme, the last step of HHG, the electron-ion re-collision can be considered as a probe process and the emission may encode fruitful information on the recombining system, including molecular structure and dynamics. In the first part, we performed high harmonic spectroscopy of N₂O and CO₂ molecules that are (laser-)aligned with respect to the polarization of the driving laser. We implemented two methods based on optical and quantum interferometry respectively in order to characterize the amplitude and phase of the attosecond emission as a function of both photon energy and alignment angle. We discovered new effects in the high harmonic generation, which could not be explained by the structure of the highest occupied molecular orbital (HOMO). Instead, we found that during the interaction with the laser field, two electronic states are coherently excited in the molecular ion and form a hole wave packet moving on an attosecond timescale in the molecule after tunnel ionization. We focused on exploring this coherent electronic motion inside the molecule, and compared the measurements in N₂O and CO₂. The striking difference in the harmonic phase behavior led us to the development of a multi-channel model allowing the extraction of the relative weight and phase of the two channels involved in the emission. An unexpected pi/4 phase shift between the two channels is obtained. Moreover, we studied the attosecond profile of the pulses emitted by these two molecules, and we proposed a simple but flexible way for performing attosecond pulse shaping. In the second part, high harmonic spectroscopy was extended to other molecular systems, including some relatively complex molecules, e.g., SF₆ and small hydrocarbons (methane, ethane, ethylene, acetylene). It revealed many interesting results such as phase distortions not previously reported. For the 'direct' scheme, we photoionized rare gas atoms using well characterized attosecond pulses of XUV coherent radiation combined with an infrared (IR) laser "dressing" field with controlled time delay, stabilized down to about ± 60 as. We evidenced marked differences in the measured angular distributions of the photoelectrons, depending on the number of IR photons exchanged. Joined to a theoretical interpretation, these observations bring new insights into the dynamics of this class of multi-color photoionization processes that are a key step towards studying photoionization in the time domain, with attosecond time resolution.

This dissertation attempts to extend the classes of halogen-containing systems which may be studied using solid-state nuclear magnetic resonance (SSNMR). As line shape broadening due to the quadrupolar interaction (QI) scales inversely with the applied field, high-field magnet technology is indispensable for this research. Combining advanced radiofrequency pulse sequences with high-field wideline data acquisition allowed for the collection of very broad SSNMR signals of all quadrupolar halogen nuclei (i.e., 35/37Cl, 79/81Br and 127I) within a reasonable amount of experimental time. The initial systems for study were of the MX2 variety (M = Mg, Ca, Sr, Ba; X = Cl, Br, I). In total, 9 anhydrous compounds were tested. The effects of hydrate formation were tested on 7 additional compounds. Systematic trends in the observed δiso values (and to a lesser extent, Ω and CQ) were found to be diagnostic of the extent of hydration in these materials. Resolving power was successfully tested using SrBr2, which possesses 4 magnetically unique sites. The composition of CaBr2•xH2O was convincingly determined using SSNMR data and the hydration trends noted above. The sensitivity of the QI to the local bonding environment (e.g., bond distance changes of less than 0.05 Å) was used to refine (when coupled with gauge-including projector augmented-wave density functional theory (GIPAW DFT) quantum chemical computations) the structure of MgBr2, and was used to correct prior NMR data for CaCl2 (earlier accounts had been performed upon a CaCl2 hydrate). During NMR data analysis of certain iodine-containing materials, it was found that standard fitting software (which uses perturbation theory) could not reproduce the observations. Proper analysis required the use of exact simulation software and allowed for the observation of high-order quadrupole-induced effects (HOQIE). This motivated further studies using rhenium-185/187 nuclei, where it was expected that HOQIE would be more dramatic. The observed rhenium SSNMR spectra possessed additional fine structure that had never been observed before experimentally, nor would be expected from currently-available perturbation theory analysis software. Lastly, preliminary results are shown where 127I SSNMR is used to study important supramolecular systems, and the composition of the popular synthetic reagent ‘GaI’ is elucidated.

Ce manuscrit de thèse s'articule autour de l'étude de l'interaction entre des impulsions lumineuses ultra brèves et des atomes ainsi que des molécules polyatomiques et chirales en phase gazeuse. En utilisant des techniques développées en physique attoseconde ainsi qu'en femtochimie, notre objectif général est de parvenir à une meilleure compréhension des dynamiques ultrarapides photoinduites dans la matière. Pour ce faire, nous avons développé des sources de lumière à ultra brèves dans le proche infrarouge et l’infrarouge moyen, qui ont été utilisées pour construire une source de rayons X dans la fenêtre de l’eau, basée surla génération d'harmoniques d’ordre élevé (GHOE), ainsi que pour l’étude de nouveaux canaux de GHOE impliquant des états hautement excités (Rydberg). Cette dernière étude a démontré une émission harmonique via l'ionisation depuis des états de Rydberg et la recombinaison radiative sur l'état fondamental, attirant ainsi notre intérêt pour le rôle des états de Rydberg en physique des champs forts. Cela nous a conduit à étudier la décroissance libre de l’induction XUV de paquets d'ondes électroniques comme une nouvelle technique de spectroscopie 2D. De plus, nous avons découvert que l'interaction entre un laser intense et un atome préparé dans une superposition cohérente d'états électroniques peut conduire à la génération de lignes hyper-Raman concomitantes avec la GHOE standard. Ce mécanisme avait été prédit lors des premiers calculs théoriques de GHOE, mais n'avait jamais été démontré expérimentalement. Par la suite, nous nous sommes intéressé à l’étude de systèmes moléculaires, dans lesquelles une excitation électronique induite par la lumière peut déclencher des dynamiques nucléaires. Nous avons étudié la photo isomérisation non-adiabatique de l’acétylène cationique en vinylidène cationique ainsi que le contrôle cohérent de la localisation électronique lors de la photodissociation de H2+. La simplicité de ces systèmes moléculaires a permis la comparaison des résultats expérimentaux avec des calculs théoriques de pointe,révélant l'importance du couplage entre les degrés de liberté nucléaires et électroniques lors de dynamiques moléculaires photoinduites.Un autre pilier majeur de cette thèse est l'étude de l'ionisation de molécules chirales avec des impulsions chirales. On sait depuis les années 70 que l'ionisation d'un ensemble de molécules chirales aléatoirement orientées, en utilisant une impulsion polarisée circulairement, conduit à une forte asymétrie avant-arrière dans le nombre de photoélectrons émis, selon l'axe de propagation de la lumière (DichroismeCirculaire de Photoélectron, DCPE). Avant cette thèse, le DCPE a été largement étudié à l’aide du rayonnement synchrotron (ionisation à un photon) et a récemment été démontré avec des lasers femtoseconde, via des schémas d'ionisation multiphotonique. Dans cette thèse, nous avons montré que le DCPE est un effet universel, c'est-à-dire qu'il émerge dans tous les régimes d'ionisation: l'ionisation àun photon, l'ionisation à multiphonique, l'ionisation au-dessus du seuil ainsi que l’ionisation par effet tunnel. Ensuite, nous avons démontré que la combinaison d’approches standard de femtochimie et du DCPE peuvent être utilisées pour suivre des dynamique de molécules chirales photoexcitées. En utilisant des approches expérimentales similaires, avec des séquences d'impulsions ayant des états de polarisation contre-intuitifs, nous avons démontré un nouvel effet chiroptique, appelé Dichroïsme Circulaire de Photoexcitation (DCPX), qui est décrit par un courant électronique directionnel et chirosensible, lorsque plusieurs niveaux sont peuplés de manière cohérente avec de la lumière chirale. Enfin, nous avons introduit une perspective temporelle à la photoionisation chirale en mesurant l'asymétrie avant arrièredes retards de photoionisation dans les molécules chirales photoionisées par des impulsions lumineuses chirales
This thesis manuscript is articulated around the investigation of the interaction between ultrashort light pulses and gas-phase atoms, polyatomic and chiral molecules. Using the toolboxes developed in attosecond and strong-field physics as well as in femtochemistry, our general goal is to reach a better understanding of subtle effects underlying ultrafast light-induced dynamics in matter.To do so, we developed cutting-edge near-infrared and mid-infrared few-cycle light sources, which were used to build a water-window soft-X-ray source based on high order harmonic generation (HHG), as well as to study new HHG channels involving highly-excited (Rydberg) states. The latter study revealed a delayed HHG emission from the ionization of Rydberg states and radiative recombination onto the electronicground state, triggering our interest in the role of Rydberg states in strong-field physics. This led us to investigate the laser-induced XUV Free Induced Decay from electronic wave packets as a new background-free 2D spectroscopic technique.More over, we have found out that strong-field interaction with a well prepared coherent superposition of electronic states led to the generation of hyper-Ramanlines concomitant with standard high-order harmonics. These spectral features were predicted in the early-days theoretical calculations of HHG but had never been reported experimentally.After these experiments in rare gas atoms, we moved to molecular targets, in whichlight-induced electronic excitation can trigger nuclear dynamics. Using simple benchmark molecules, we have studied dynamics involving the participation of both nuclear and electronic degrees of freedom: first, we studied the ultrafast non adiabatic photoisomerization of the acetylene cation into vinylidene cation, andsecond, we investigated the coherent control of electron localization during molecular photodissociation of H2+. The simplicity of these molecular targets enabled the comparison of the experimental results with state-of-the-art theoretical calculations,revealing the importance of the coupling between nuclear and electronic degrees of freedom in photoinduced molecular dynamics.The other major pillar of this thesis is the study of ionization of chiral molecules usingchiral light pulses. It has been known since the 70s that the ionization from an ensemble of randomly oriented chiral molecules, using circularly polarized light pulse,leads to a strong forward-backward asymmetry in the number of emitted photoelectrons, along the light propagation axis (Photoelectron Circular Dichroism,PECD). Prior to this thesis, PECD was widely studied at synchrotron facilities (single photonionization) and had recently been demonstrated using table-top lasers in resonant-enhanced multiphoton ionization schemes. In this thesis, we have shownthat PECD is a universal effect, i.e. that it emerges in all ionization regimes, from single photon ionization, to few-photon ionization, to above-threshold ionization, up to the tunneling ionization regime. This bridges the gap between chiral photoionizationand strong-field physics. Next, we have shown how the combination of standard femtochemistry approaches and PECD can be used to follow the dynamics of photoexcited chiral molecules using time-resolved PECD. Using similar experimental approaches, but by using pulse sequences with counter-intuitive polarization states,we have demonstrated a novel electric dipolar chiroptical effect, called Photoexcitation Circular Dichroism (PXCD), which emerges as a directional and chirosensitive electron current when multiple excited bound states of chiral molecules are coherently populated with chiral light. Last, we introduced a time-domain perspective on chiral photoionization by measuring the forward-backward asymmetry of photoionization delays in chiral molecules photoionized by chiral light pulses. Our work thus carried chiral-sensitive studies down to the femtosecond and attosecond ranges

As part of this project and in preparation for future experimental studies of gas-phase ion-molecule reactions, extensive modification and characterization of the crossed molecular beam machine in the Department of Chemistry, University of Canterbury has been carried out. This instrument has been configured and some preliminary testing completed to enable the future study of gas-phase ion-molecule collisions of H⁺₃ and Y⁻ (Y = F, Cl, Br) with dipole-oriented CZ₃X (Z = H, F and X = F, Cl, Br). Theoretical calculations (ab initio and density functional theory) are reported on previously experimentally characterized Na + CH₃NO₂, Na + CH₃NC, and K + CH₃NC systems, and several other systems of relevance. All gas-phase experimental and theoretical studies have the common theme of studying collision orientation dependence of reaction under singlecollision conditions. Experimental measurements, theoretical simulations and calculations are also reported on some selected ferrous (Fe²⁺) high-spin (S=2) crystals, in an attempt to resolve microscopic contributions of two fundamental macroscopic tensor properties: the electric-field gradient (efg); and the mean square displacement (msd) in the case when more than one symmetry related site of low local point-group symmetry contributes to the same quadrupole doublet. These determinations have been made using the nuclear spectroscopic technique of Mössbauer spectroscopy, and complemented with X-ray crystallographic measurements.

Dans le cadre du présent travail, une étude approfondie a été menée sur les alliages Co-B en termes d'évolution de la microstructure lors d'une solidification hors équilibre avec ou sans champ magnétique ainsi que sur une transition liquide-liquide induite par la température.Un alliage hypereutectique Co-20at.%B a été sous-refroidi par la technique de l'encapsulation vitreuse. Une transition de l'hypereutectique à l'hypoeutectique a été trouvée à un sous-refroidissement critique de ∆T=119 K. Quand ∆T<119 K, une phase dendritique directionnelle primaire β-Co3B entourée par l'eutectique lamellaire régulière de α-Co+β-Co3B a été observée. Lorsque ∆T>119 K, la microstructure hypereutectique ci-dessus se transforme en structure hypoeutectique avec la phase α-Co comme phase primaire. Selon le modèle de croissance de la dendrite, le passage de l'hypereutectique à l'hypoeutectique peut être attribué à la vitesse de croissance plus élevée de la α-Co que de la β-Co3B, c'est-à-dire un mécanisme contrôlé par la croissance.La surchauffe et le refroidissement cycliques ont été effectués pour les alliages hypereutectiques sous-refroidis Co-20at.%B, eutectiques Co-18.5at.%B et hypoeutectiques Co-17at.%B. Pour chaque alliage, il y a une température critique de surchauffe Tc0 à laquelle il y a une brutale augmentation du sous-refroidissement moyen. Les mesures DSC montrent qu'il y a un pic d'absorption thermique dans le processus de chauffage, dont le pic de température est presque égal à la température critique de surchauffe, ce qui indique qu'une transition structurale liquide-liquide induite par la température se produit et doit être étroitement liée à la nucléation dans le liquide eutectique Co-B sous refroidi. L'effet de la transition structurale liquide-liquide sur la nucléation a été interprété par la récente théorie de la nucléation qui considère les structures des liquides en fusion surchauffées, et la température de surchauffe critique TcO, dépendante de la composition, a été attribuée au changement de structures préférentielles locales.Grace à une mesure in situ de l'aimantation, la transition structurale liquide-liquide induite par la température a été étudiée plus en profondeur. Une anomalie d'aimantation en terme de non dépendance de l'aimantation selon une loi de Curie-Weiss a été observée à l'état surchauffé, ce qui démontre une transition structurale liquide-liquide induite par la température. Ce comportement anormal s'est avéré être une règle universelle pour le système d'alliage binaire Co-B. Une température de transition (T0) et deux températures de Curie paramagnétiques (θ(LI), θ(LII)) correspondant à deux structures différentes des liquides sont déterminées. Les effets de l'intensité du champ magnétique sur la transition liquide-liquide et les températures de Curie paramagnétiques sont étudiés. T0 et θ(LII) ne sont pas sensibles à l'intensité du champ, tandis que θ(LI) passe à des températures plus basses avec une intensité croissante du champ magnétique. Avec une concentration croissante de Cobalt, T0, θ(LI) et θ(LII) passent à des températures plus élevées et les constantes de Curie pour le liquide I et le liquide II diminuent.Sous l'effet d'un champ magnétique imposé, un alignement morphologique a été trouvé pour la phase primaire α-Co avec son tronc primaire de dendrite ou son grand axe parallèle à la direction du champ magnétique. Les phases primaires de α-Co sont de formes cylindriques ou sphériques avec un sous-refroidissement relativement élevé, et l'application d'un champ magnétique est plus propice à l'obtention de ce type de phases α-Co. L'énergie magnétique, le couple magnétique et le temps requis pour la rotation ont été analysés théoriquement pour évaluer l'alignement magnétique et les mécanismes d'alignement. Les forces dipolaires entre les particules ont été calculées sur la base desquelles le phénomène d'auto-organisation des particules primaires de α-Co sous forme d'empilement en chaîne a été décrit
In the present work, a thorough investigation has been conducted on the Co-B alloys in terms of the microstructure evolution during non-equilibrium solidification with/without magnetic field and temperature induced liquid-liquid structure transition.A Co-20at.%B hypereutectic alloys was undercooled by the melt fluxing technique. A transition from hypereutectic to hypoeutectic was found at a critical undercooling of ∆T=119 K. When ∆T<119 K, a primary directional dendritic β-Co3B phase surrounded by the regular of α-Co+β-Co3B lamellar eutectics was found. When ∆T>119 K, the above hypereutectic microstructure changes into hypoeutectic structure with the α-Co phase as the primary phase. According to dendrite growth model, the transition from hypereutectic to hypoeutectic can be ascribed to the higher growth velocity of the α-Co phase than the β-Co3B phase, i.e., the growth-controlled mechanism.Cyclic superheating and cooling were carried out for the undercooled hypereutectic Co-20at.%B, eutectic Co-18.5at.%B and hypoeutectic Co-17at.%B alloys. For each alloy, there is a critical overheating temperature Tc0 at which there is a sharp increase of the mean undercooling. DSC measurements show that there is a thermal absorption peak in the heating process, the peak temperature of which is nearly equal to the critical overheating temperature, indicating that the temperature induced liquid-liquid structure transition does occur and should relate highly to nucleation in the undercooled Co-B eutectic melts. The effect of the liquid-liquid structure transition on nucleation was interpreted by the recent nucleation theory that considers the structures of overheated melts, and the composition-dependent overheating temperature was ascribed to the change of local favored structures.By in situ measuring the magnetization, the temperature induced liquid-liquid structure transition was further investigated. A magnetization anomaly in term of the non-Curie-Weiss temperature dependence of magnetization was observed in the overheated state, demonstrating a temperature induced liquid-liquid structure transition. This anomalous behavior was found to be a universal formula for the Co-B binary alloy system. A transition point (T0), two different Curie constants and two paramagnetic Curie temperatures (θ(LI), θ(LII)) corresponding to two distinct kinds of liquids (i.e., high-magnetization liquid I and low-magnetization liquid II) are determined. The Curie constant of liquid II was found much higher, which is attributed to the survived covalent bond below T0. The effects of magnetic field intensity on the liquid-liquid structure transition and paramagnetic Curie temperatures are studied. T0 and θ(LII) are found not sensitive to the field intensity, whereas, θ(LI) shifts to lower temperatures with the increasing magnetic field intensity. With the increased concentration of Co, T0, θ(LI) and θ(LII) shift to higher temperatures and the Curie constants for the liquid I and liquid II decrease. Based on the location of T0, a guideline was drawn above the liquidus in the Co-B phase diagram, which could provide a significant guidance to the practical melt treatment.Under an imposed magnetic field, a morphological alignment was found for the primary α-Co phase with its primary dendrite trunk or long axis paralleling to the direction of magnetic field. The primary α-Co phases are rod-like or spherical at relatively high undercooling, and the application of magnetic field is more conducive to obtain such kind of α-Co phases. The magnetic energy, magnetic torque and time required for rotation were analyzed theoretically to evaluate the magnetic alignment and alignment mechanisms. The dipolar forces between particles were calculated, based on which the phenomenon that the primary α-Co particles self-organize as chain-like stacking was described

Optical parametric oscillators (OPOs) and optical parametricamplifiers (OPAs) constitute a class of optical frequencyconverting devices that have many possible applications, e.g.in range finding, molecular spectroscopy and medicine. They canconvert the frequency of the incident pump field with highefficiency, and generate two waves at new frequencies that willbe continuously tuneable over a wide spectral range. Virtuallyany wavelengths within the transparency region of the nonlinearmaterial can be generated if the material can bequasi-phasematched (QPM). In addition, QPM gives thepossibility to utilise the largest nonlinear tensor element ofthe material and allows walk-off free interaction between thewaves.

The aims of this thesis have been to investigate thepossibility to use QPM KTiOPO₄crystals as nonlinear material in nanosecond OPOsand OPAs operating at room-temperature, and to explore theadvantages and shortcomings of these devices. The technique ofelectric field poling has been employed to implement the QPMstructure in flux grown KTiOPO₄(KTP).

The main conclusion is that periodically poled KTP (PPKTP)is a suitable material to use in nanosecond OPOs and OPAs. Thematerial properties that foremost make KTP into an attractivenonlinear material are: The large value of the nonlinearcoefficient d₃₃, the high resistance to optically inducedbreakdown, the low susceptibility to grey-track formation, theinsensitivity to the photorefractive effect, the widetransparency and the low coercive field.

The thesis shows that it is possible to pole large volumesof KTP with a high quality of the QPM structure. Highlyefficient nanosecond OPOs have been constructed during thisproject. Maximum conversion efficiencies have reached 45 % inthe case of a singly resonant OPO (SRO) built around a 3 mmthick PPKTP crystal. Total pulse energies for both the signal(1.72 µm) and the idler (2.8 µm) of up to 18 mJ wasreached and an average output power of 2 W was obtained forthis sample. However, up to 24 W was produced in a doublyresonant OPO operating close to degeneracy. The efficiencyreached 48 % for that case. Truly continuous and very widespectral tuning has also been demonstrated, as well as a narrowbandwidth OPO operating on one single longitudinal mode.

Keywords:optical parametric oscillators, opticalparametric amplifiers, quasi-phasematching, KTiOPO₄, nonlinear optics, frequency conversion, periodicelectric field poling, ferroelectrics, high-order secondharmonic generation, electro-optic effect.

Cette etude concerne deux phases, yba#2cu#3o#7#-# et bi#2#+#xsr#2#-#xcuo#6#+#, archetypes des supraconducteurs a haute temperature. Leur anisotropie, respectivement moins de 10 et plus de 200, et leur temperature critique, 92k et moins de 10 k, les situent aux deux extremes de l'eventail des proprietes de ces composes. Cette etude est axee sur leurs proprietes thermodynamiques, chaleur specifique et aimantation. Un travail preliminaire sur des ceramiques d'yba#2cu#3o#7#-# presentant des transitions dedoublees a permis de selectionner les conditions pour obtenir une transition supraconductrice etroite. La chaleur specifique d'un monocristal sur lequel ce traitement a ete applique avec succes a ete mesuree sous champ magnetique entre 0 et 27 t. Une pente anormalement elevee de la composante champ moyen de l'anomalie de chaleur specifique a notamment ete mise en evidence. Une courbure de la ligne de champ critique h#c#2(t) est egalement apparue, coherente avec l'analyse des comportements d'echelle de la chaleur specifique sous champ. A cause d'un diagramme de phase complexe, le compose bi#2#+#xsr#2#-#xcuo#6#+# supraconducteur n'a pu etre elabore que grace a la methode dite de pyrolyse des citrates qui permet des syntheses a basse temperature. Ses proprietes physiques ont ete apprehendees essentiellement au travers de mesures d'aimantation. Grace a l'etendue du domaine reversible, une discussion sur la symetrie du parametre d'ordre a pu etre engagee. Les resultats ne sont pas compatibles avec une symetrie s ou d dans la limite pure. Par contre, des calculs theoriques recents bases sur une hypothese de symetrie d en presence d'impuretes decrivent parfaitement les mesures. Il existe cependant une explication alternative basee sur le terme d'interaction entre vortex, sans reference apparente a une symetrie non-conventionnelle du parametre d'ordre

Les applications en courant fort de la ceramique supraconductrice a haute temperature critique yba#2cu#3o#7## necessitent l'amelioration des qualites supraconductrices et l'augmentation de la taille des materiaux synthetises. Un nouveau procede de synthese, combinant la fusion de zone et l'action du champ magnetique, permet de produire des conducteurs de grande longueur massivement orientes. Cette methode autorise la synthese de barreaux d'yba#2cu#3o#7## de plusieurs centimetres de long, composes d'un petit nombre de grains avec une faible desorientation des plans a,b, la direction de l'axe c etant imposee par le champ magnetique. L'un deux, comportant plusieurs joints de grains, a montre en champ nul un courant critique superieur a 3200 a (> 25. 000 a/cm#2), et egal a 200 a (1500 a/cm#2) dans un champ magnetique applique de 8 teslas. Pour etudier les phenomenes associes au courant critique et au champ critique, nous avons mis au point deux dispositifs de mesure: un appareil de mesure de courants critiques eleves, fonctionnant dans l'azote liquide (77 k), sous champ magnetique applique, et qui permet de faire varier l'angle entre l'axe du champ et les directions cristallographiques du materiau etudie; et un dispositif de mesures de resistance en fonction de la temperature et du champ magnetique, fonctionnant entre t = 8 et 300 k et entre h = 0 et 4,5 teslas. Les mesures de courants critiques, effectuees a l'aide du premier de ces dispositifs, ont permis d'explorer le plan h, a 77 k, entre h = 0 et 20 teslas et de = 0 a 90. Une analyse detaillee et des lois d'echelle etablies a partir de la variable h/h#c#3(), h#c#3() etant le champ critique de surfaces intrinseques a la structure cristallographique, permettent de proposer un diagramme de phase dans ce plan. La precision obtenue sur le dispositif de mesures de resistances a permis de reveler l'existence d'une transition du premier ordre dans l'etat supraconducteur en champ nul, se manifestant entre 30k et tc, pouvant etre attribuee a un changement de symetrie de la supraconductivite

Telemetry system, Optimisation, Sensoric networks, Smart Grid, Internet of Things, Sensors, Information security, Cryptography, Cryptography algorithms, Cryptosystem, Confidentiality, Integrity, Authentication, Data freshness, Non-Repudiation.

In this thesis, we consider the planning problem for first-order mean-field games (MFG). These games degenerate into optimal transport when there is no coupling between players. Our aim is to extend the concept of displacement convexity from optimal transport to MFGs. This extension gives new estimates for solutions of MFGs. First, we introduce the Monge-Kantorovich problem and examine related results on rearrangement maps. Next, we present the concept of displacement convexity. Then, we derive first-order MFGs, which are given by a system of a Hamilton-Jacobi equation coupled with a transport equation. Finally, we identify a large class of functions, that depend on solutions of MFGs, which are convex in time. Among these, we find several norms. This convexity gives bounds for the density of solutions of the planning problem.

This study aims to investigate the behaviour of low-order beam and plate elements especially for their application to laminated structures. The merits and dements of the existing elements are brought out and new low-order elements with better interpolation polynomials are proposed. Two new beam elements are proposed for laminated composite beams that yield better representation of twist due to material coupling. Out of the two elements developed, one is based on the conventional formulation and the other on the coupled-field formulation, both capturing material induced coupling. The beam developed using coupled field formulation shows a novel way of obtaining a fully coupled interpolation function for field variables using the complete set of equilibrium equations for the composite beams. The element has shown a superior coarse mesh performance. These elements can practically capture plate behaviour in beam elements for a wide range of plate thickness. The locking problems in conventional 4-node quadrilateral elements, such as shear locking and geometric locking are studied. Various techniques available in literature to remedy these problems are also studied. A suite of QUAD4 with conventional techniques such as. Reduced Integration, Field Consistency, Mixed Interpolation of Tensorial strain Components, Assumed Natural Strain, Discrete Shear Gap, Incompatible modes Q6 and QM6 is developed. An effort is made to combine these techniques to develop new element that yields improved performance. The element is shown to exhibit improved performance for certain cases. Several four-node rectangular elements are developed based on the coupled-field techniques. First two new-coupled elements are formulated that employ Sabir's [101] plane bending formulation with drilling degree of freedom, and the plate bending rotations are generated using equilibrium equations. However, since Sabir's plane bending interpolation polynomials yielded inaccurate performance for composites, it led to development of elements with fully coupled field formulations. Finally, two new 4-node rectangular elements are developed using coupled-field formulations with six and seven dof freedom per node respectively. Here the interpolation polynomials are derived using the complete equilibrium equations. The elements are extensively tested for static deflection, dynamics and buckling of isotropic and laminated plates/beams. The elements show superior coarse mesh convergence. Several problems pertaining to vibration and buckling of composite plates/beams are solved using the elements developed in this work.

The discretization of time-dependent wave propagation is plagued with dispersion in which the wavefield is perceived to travel with an erroneous velocity. To remediate the problem, simulations are run on dense and computationally expensive grids yielding plausible approximate solutions. This work introduces an error analysis tool which can be used to obtain optimal simulation parameters that account for mesh size, orders of spatial and temporal discretizations, angles of propagation, temporal stability conditions (usually referred to as CFL conditions), and time of propagation. The classical criteria of 10-15 nodes per wavelength for second-order finite differences, and 4-5 nodes per wavelength for fourth-order spectral elements are shown to be unrealistic and overly-optimistic simulation parameters for different propagation times. This work analyzes finite differences, spectral elements, optimally-blended spectral elements, and isogeometric analysis.

The miscible displacement equations provide the mathematical model for simulating the displacement of a mixture of oil and miscible fluid in underground reservoirs during the Enhance Oil Recovery(EOR) process. In this thesis, I propose a stable numerical scheme combining a mixed finite element method and space-time discontinuous Galerkin method for solving miscible displacement equations under low regularity assumption. Convergence of the discrete solution is investigated using a compactness theorem for functions that are discontinuous in space and time. Numerical experiments illustrate that the rate of convergence is improved by using a high order time stepping method. For petroleum engineers, it is essential to compute finely detailed fluid profiles in order to design efficient recovery procedure thereby increase production in the EOR process. The method I propose takes advantage of both high order time approximation and discontinuous Galerkin method in space and is capable of providing accurate numerical solutions to assist in increasing the production rate of the miscible displacement oil recovery process.

This thesis focuses on 3D computer graphics and the continuous maximisation of rendering quality and performance. Its main focus is the critical analysis of numerous real-time rendering algorithms and the construction of an empirically derived system for the high-speed rendering of shader-based special effects, lighting effects, shadows, reflection and refraction, post-processing effects and the processing of physics. This critical analysis allows us to assess the relationship between rendering quality and performance. It also allows for the isolation of key algorithmic weaknesses and possible bottleneck areas. Using this performance data, gathered during the analysis of various rendering algorithms, we are able to define a selection engine to control the real-time cycling of rendering algorithms and special effects groupings based on environmental conditions. Furthermore, as a proof of concept, to balance Central Processing Unit (CPU) and Graphic Processing Unit (GPU) load for and increased speed of execution, our selection system unifies the GPU and CPU as a single computational unit for physics processing and environmental mapping. This parallel computing system enables the CPU to process cube mapping computations while the GPU can be tasked with calculations traditionally handled solely by the CPU. All analysed and benchmarked algorithms were implemented as part of a modular rendering engine. This engine offers conventional first-person perspective input control, mesh loading and support for shader model 4.0 shaders (via Microsoft’s High Level Shader Language) for effects such as high dynamic range rendering (HDR), dynamic ambient lighting, volumetric fog, specular reflections, reflective and refractive water, realistic physics, particle effects, etc. The test engine also supports the dynamic placement, movement and elimination of light sources, meshes and spatial geometry. Critical analysis was performed via scripted camera movement and object and light source additions – done not only to ensure consistent testing, but also to ease future validation and replication of results. This provided us with a scalable interactive testing environment as well as a complete solution for the rendering of computationally intensive 3D environments. As a full-fledged game engine, our rendering engine is amenable to first- and third-person shooter games, role playing games and 3D immersive environments. Evaluation criteria (identified to access the relationship between rendering quality and performance), as mentioned, allows us to effectively cycle algorithms based on empirical results and to distribute specific processing (cube mapping and physics processing) between the CPU and GPU, a unification that ensures the following: nearby effects are always of high-quality (where computational resources are available), distant effects are, under certain conditions, rendered at a lower quality and the frames per second rendering performance is always maximised. The implication of our work is clear: unifying the CPU and GPU and dynamically cycling through the most appropriate algorithms based on ever-changing environmental conditions allow for maximised rendering quality and performance and shows that it is possible to render high-quality visual effects with realism, without overburdening scarce computational resources. Immersive rendering approaches used in conjunction with AI subsystems, game networking and logic, physics processing and other special effects (such as post-processing shader effects) are immensely processor intensive and can only be successfully implemented on high-end hardware. Only by cycling and distributing algorithms based on environmental conditions and through the exploitation of algorithmic strengths can high-quality real-time special effects and highly accurate calculations become as common as texture mapping. Furthermore, in a gaming context, players often spend an inordinate amount of time fine-tuning their graphics settings to achieve the perfect balance between rendering quality and frames-per-second performance. Using this system, however, ensures that performance vs. quality is always optimised, not only for the game as a whole but also for the current scene being rendered – some scenes might, for example, require more computational power than others, resulting in noticeable slowdowns, slowdowns not experienced thanks to our system’s dynamic cycling of rendering algorithms and its proof of concept unification of the CPU and GPU.
Thesis (PhD)--University of Pretoria, 2012.
Computer Science
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