Thesis (MSc (Physics))--University of Stellenbosch, 2010. / ENGLISH ABSTRACT: Through the use of complex Laser Pulse Shaping, numerous fundamental laser induced processes may be controlled as well as studied. This work serves as an introduction into Laser Pulse Shaping, with the focus on a simple Pulse Shaping experiment, as well as to determine whether future, more complex processes may be similarly controlled. A description of Laser Pulse Shaping theory is presented here, along with a full explanation of a simple experiment to maximize second harmonic generation (SHG) through Pulse Shaping. This experiment is simple on a theoretical level yet complicated in both implementation as well as operation. The experimental setup and software integration required hardware compatibility in multiple programming languages. This work was successful in the sense that a fully automated dispersion compensation system, accomplished through the use of a genetic algorithm in a feedback controlled loop, was constructed and tested. The success of this experiment and the understanding gained in this work has laid the foundation for further complex Pulse Shaping systems to be achieved in future. / AFRIKAANSE OPSOMMING: Komplekse Laserpuls-vervorming kan gebruik word om verskeie fundamentele laser-geinduseerde prosesse beide te beheer asook te bestudeer. Hierdie navorsingstuk dien as n inleiding tot Laserpuls-vervorming, spesifiek gefokus op n eenvoudige Pulsvervormings-eksperiment. Meer komplekse Pulsvervormingsopstellings kan toegepas word deur die kennis opgedoen in hierdie tesis. Die teoretiese agtergrond van Laserpuls-vervormings word bespreek, tesame met n eenvoudige eksperiment om die Tweede Harmoniek Skeppingsproses (SHG) te maksimeer deur van Laserpuls-vervorming gebruik te maak. Die eksperiment is teoreties eenvoudig, waar die implimentering asook bedryf meer kompleks is. Die bedryf van die eksperiment word in 2 dele hanteer: die hoofprogram en n Genetiese Algoritme gebruik in optimering. Die werking van Genetiese Algoritmes asook Ultrakort Pulse (USPs) en pulskarakterisering word ook bespreek. Die suksesvolle opstelling van die experiment en ook die eind resultate wat gevind is, maak dit moontlik om meer ingewikkeld komplekse laserpulsvervorming experimente te bestudeer.

Aujourd’hui, les énergies renouvelables comme l’énergie éolienne, l’énergie solaire, l’énergie hydroélectrique et la thermoélectricité jouent un rôle essentiel dans la couverture de nos besoins en énergie. Parmi ces différentes sources d’énergie, la thermoélectricité, qui permet de convertir la chaleur en électricité ou inversement, attire une grande attention grâce à son large champ d’application. Les actuelles avancées dans la recherche thermoélectrique visent l’amélioration du rendement de conversion des modules thermoélectriques, à travers l’optimisation des propriétés thermoélectriques intrinsèques des matériaux utilisés (coefficient de Seebeck, conductivité électrique et conductivité thermique). Pour cela, différentes approches ont été étudiées (dopage, nouveau alliages, nanostucturation …). Parmi ces approches, la nanostructration des matériaux a été largement étudiée pour mener à bien cet objectif. Dans ce travail de thèse, nous nous sommes intéressés à étudier l’effet de la nanostructuration de surface des matériaux (silicium mesoporeux et oxyde de titane déposé en couches minces) par faisceaux laser ultra-court (picoseconde et femtoseconde) sur l’évolution de leurs propriétés thermoélectriques. Dans un premier temps, nous nous sommes focalisés sur l’étude des différents phénomènes physiques impliqués durant l’interaction laser-matière ainsi que sur la formation des différentes nanostructures résultantes (en forme de ripples, spikes, dots et autres) en fonction de la dose laser appliquée (la fluence et le nombre de pulses). La formation de ces nanostructures a été étudiée suivant deux régimes (stationnaire et dynamique). Après l’optimisation des paramètres conduisant à la formation de ces nanostructures, la caractérisation du coefficient de Seebeck et la conductivité électrique avant et après la nanostructuration de ces matériaux a été réalisée grâce à un nouveau dispositif de mesure (ZT-meter) développé au laboratoire GREMI. Les résultats de mesures montrent une importante amélioration du coefficient de Seebeck et la conductivité électrique après la nanostrucutration. Un facteur d’augmentation de la puissance thermoélectrique a été observé pour les deux matériaux étudiés ; notamment dans le cas de couches minces d’oxyde de titane (jusqu’à 500 fois). / Today, renewable energies such as wind, solar, hydropower and thermoelectricity play an essential role to cover our energy needs. Among these different sources of energy, thermoelectricity, which offers the ability to convert a heat into electricity or vice versa, has attracted a great attention due to its wide field of potential applications. The current advances in thermoelectric research are focusing on the improvement of the conversion efficiency of thermoelectric devices through optimizing and improving the thermoelectric properties of the thermoelectric materials (Seebeck coefficient, electrical conductivity and thermal conductivity). For this, different approaches (doping, new materials, nanostucturing...) have been investigated in the literature. Among these approaches, nanostructuring of materials is the most studied in the literature in order to improve the thermoelectric properties of materials. In this thesis work, we aimed to study the effect of surface nanostructuring of materials (mesoporous silicon and titanium oxide deposited in thin film) by ultra-short laser beams (picosecond and femtosecond) on the evolution of their thermoelectric properties. First, we focused on the study of various physical phenomena involved during the laser-matter interaction that yield to the formation of very different nanostructures in form of ripples, spikes, dots and others as function of the applied laser dose (fluence and number of pulses). The formation of these nanostructures has been studied in two regimes (stationary and dynamic). After optimizing the laser parameters leading to the formation of such nanostructures, a characterization of Seebeck coefficient and the electrical conductivity before and after the nanostructuring of these materials was carried out by using a new experimental setup (ZT-meter) designed and validated in GREMI laboratory. The results of measurements showed an important improvement of Seebeck coefficient and electrical conductivity after nanostructuring. This important improvement observed with the both materials leaded to a strong increase in the thermoelectric power factor (reaching roughly 50000%).

In this thesis the InSb(111), InAs(111) and GaSb(001) surfaces have been studied by means of time- and angle-resolved photoemission spectroscopy based upon the femtosecond laser system. The pump-and-probe technique allows to analyse both electron states in the valence band and normally unpopulated electron states above the valence band, which can be occupied by transiently excited carriers at the optically pumped surface. The life time of excited carriers is analysed by controlling over the time delay between pump and probe pulses. Experimental studies of the InSb(111) surface and comparison with a previously studied InSb(110) surface show electron excitations in the bulk region with a minor surface contribution. Time-resolved experiments of carrier dynamics at the polar InAs(111)A and InAs(111)B surfaces show about the same life time of excited carriers, while no populated states above the valence band maximum have been found at the InAs(111)A due to the charge removal. Surface intergap electron states have been found at the GaSb(001) surface located at ~250 meV above the valence band maximum. Angle-resolved experiments showed a strong confinement of this state at the centre of the surface Brillouin zone. A new two dimensional angle-resolved multi-anode analyser for the femtosecond laser photoemission setup has been constructed. The analyser can resolve a cone opening angle of ~1º at a drift distance of ~0.5 m with an energy resolution of ~125 meV. A continuous series of binary system SrTiO3–PbZr0.52Ti0.48O3 has been grown by pulsed laser deposition (PLD) on sapphire substrate with crystalline quality control by x-ray diffraction (XRD). The maximum tunability has been tailored to room temperature, where STO�PZT (71/29) composition shows superior performance. A PbZr0.52Ti0.48O3 thin film pressure sensor has been fabricated by PLD and characterised by XRD and electrical measurements. The piezoelectric constant was found to be ~20 % higher compared to the bulk ceramics. A ferroelectric thin film electro-optical cell Na0.5K0.5NbO3/La0.5Sr0.5CoO3 (NKN/LSCO) on sapphire has been fabricated by PLD. Refractive indices and electro-optical coefficient of the cell were characterised by prism coupling refractometry. The tunability of the PLD fabricated 2 μm slot NKN thin film interdigital capacitor has been found ~23 % at 40 V bias voltage and frequency 1 MHz. / QC 20101015

Cette thèse traite du contrôle et de la caractérisation de l'alignement et de l'orientation du point de vue théorique et expérimental. L'alignement d'une molécule linéaire consiste à obtenir une probabilité élevée de localisation de l'axe internucléaire symétrique autour de l'axe de polarisation du champ tandis que l'orientation privilégie un sens particulier le long du champ. L'orientation à l'aide d'impulsions bi couleur (2+1) non résonnantes est étudiée en détail et les conditions permettant d'obtenir une orientation efficace sont examinées. Un schéma bi couleur où la deuxième harmonique est en quasi-résonance avec un niveau vibrationnel de la molécule est également étudié. Cette technique présente l'avantage d'offrir un paramètre supplémentaire à savoir l'écart à la résonance qui peut être ajusté de manière à optimiser l'orientation moléculaire. Finalement une nouvelle technique expérimentale de détection de l'alignement moléculaire est présentée. Celle-ci permet une détection monocoup de l'alignement moléculaire sur une étendue temporelle jusqu'alors inégalée. / This thesis is about the control and characterisation of the alignment and orientation of molecules by ultra short laser pulses on a theoretical and experimental approach. Alignment corresponds to a symmetric angular distribution of the molecular axis peaked along the laser field axis, whereas orientation provides an asymmetric distribution favouring one spatial direction. Orientation by sudden two-colour (2+1) pulses is studied extensively for the non resonant case and conditions required for achieving significant orientation are explored. A second two-colour scheme, where the second harmonic is in quasi resonance with a vibrational level of the molecule, is also presented and discussed. The last technique has the advantage to offer the detuning of the laser frequency as an additional free parameter, which can be adjusted to enhance molecular orientation. A new experimental polarization imaging 2D technique for the detection alignment is also developed. Experimental results on single shot detection of molecular alignment achieved over an unprecedented temporal span are presented.