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Semiconductor nanostructures exhibit many remarkable electronic and optical properties. The key to designing and utilising semiconductor quantum structures is a physical understanding of the detailed excitation, transport and energy relaxation processes. Thus the nonequilibrium dynamics of semiconductor quantum structures have attracted extensive attention in recent years. Ultrafast spectroscopy has proven to be a versatile and powerful tool for investigating transient phenomena related to the relaxation and transport dynamics in semiconductors. In this thesis, we report investigations into the electronic and optical properties of various semiconductor quantum systems using a variety of ultrafast techniques, including up-conversion photoluminescence, pump-probe, photon echoes and four-wave mixing. The semiconductor quantum systems studied include ZnO/ZnMgO multiple quantum wells with oxygen ion implantation, InGaAs/GaAs self-assembled quantum dots with different doping, InGaAs/InP quantum wells with proton implantation, and silicon quantum dots. The spectra of these semiconductor nanostructures range from the ultraviolet region, through the visible, to the infrared. In the UV region we investigate excitons, biexcitons and oxygen implantation effects in ZnO/ZnMgO multi-quantum wells using four-wave mixing, pump-probe and photoluminescence techniques. Using time-resolved up-conversion photoluminescence, we investigate the relaxation dynamics and state filling effect in InGaAs self-assembled quantum dots with different doping, and the implantation effect in InGaAs/InP quantum wells. Finally, we study the optical properties of silicon quantum dots using time-resolved photoluminescence and photon echo spectroscopy on various time scales, ranging from microseconds to femtoseconds.

Le développement de couches minces dopées terres rares a suscité un regain d'intérêt au cours des dernières années. Dans ce rapport, nous présentons l'élaboration de couches minces de titanate de terres rares de type Y2-xLnxTi2O7 (Ln=Er, Tm, Yb, Nd) par procédé Aérosol-gel et leur caractérisation. Le procédé Aérosol-gel est une technique de dépôt originale fondée sur la transformation sol-gel d'un film liquide déposé par pulvérisation ultrasonore. Diverses procédures de traitement thermique ont été mises en œuvre de façon à étudier l'influence de la microstructure de la couche mince sur ses propriétés spectroscopiques. Les couches cristallisent dans une phase cubique de type pyrochlore autour de 750-785°C, suivant la durée du traitement. Les couches Y2-xErxTi2O7 (YETO) amorphes et cristallisées présentent une forte émission à 1530 nm lorsqu'elles sont excitées à 977 nm en configuration guidée. Une relation a été établie entre la microstructure de la couche et ses propriétés spectroscopiques. L'élaboration d'une solution solide YETO permet de diluer de façon homogène les ions erbium tout en protégeant efficacement la terre rare des impuretés. Ce travail montre que la concentration d'auto-extinction des couches cristallisées est plus grande (9. 1020 ions/cm3) que celle des couches amorphes (2. 1020 ions/cm3). L'introduction d'ions ytterbium dans la maille YETO permet d'améliorer d'un facteur 10 l'intensité de l'émission à 1530 nm des ions erbium et exacerbe également leur émission par up-conversion dans le vert. Des couches amorphes Y2-x-yTmxYbyTi2O7 ont également été élaborées et présentent une forte émission par up-conversion dans le bleu sous excitation à 977 nm. Des couches YETO ont également été introduites dans des dispositifs optiques élémentaires. Des guides d'ondes confinés (inversés et chargés) ont été fabriqués et caractérisées. Ils présentent une bonne émission à 1530 nm et un bon confinement optique. Une microcavité verticale a également été élaborée en intégrant une couche YETO demi-onde entre deux miroirs de Bragg formés par une alternance de couches SiO2/TiO2. La cavité présente un mode de résonance unique à 525 nm, et l'émission de l'erbium à cette longueur d'onde est augmentée d'un facteur 30.

Le projet s'inscrit dans le développement de sources lasers RGB miniaturisées pour l'affichage et la vidéoprojection, la conversion de fréquence dans les cellules solaires.Les verres fluorés ZLAG (ZrF4-LaF3-AlF3-GaF3) codopés terres rares ont été considérés. Ce verre possède une faible énergie de phonon, une forte solubilité des terres rares et peut être fabriqué en couche mince par la technique PVD. Il est de plus le précurseur de vitrocéramiques transparentes. On a observé dans les verres massifs et les guides d'onde des émissions bleue, orange et rouge avec un codopage Pr3+-Yb3+, bleue et rouge avec un co-dopage Tm3+-Yb3+. L'émission RGB dans les verres tri-dopés Tm3+-Er3+-Yb3+ semble prometteuse. Par ailleurs, la vitro-céramisation a permis d'augmenter de plus de 30% les sections efficaces d'absorption des ions Pr3+ et Yb3+.Une efficacité de transfert de 92% a été obtenue dans les verres co-dopés 0,5Pr3+-10Yb3+ pour le processus de conversion d'un photon bleu en deux photons IR.

This thesis describes the specification, design and implementation of a software-defined radio system on a two-channel 14-bit digitizer/generator. The multi-stage interpolations and decimations which are required to operate two analog-to-digital converters at 800 megasamples per second (MSps) and two digital-to-analog converters at 1600 MSps from a 25 MSps software-side interface, were designed and implemented. Quadrature processing was used throughout the system, and a combination of fine-tunable low-rate mixers and coarse high-rate mixers were implemented to allow frequency translation across the entire first Nyquist band of the converters. Various reconstruction filter designs for the transmitter side were investigated and a cheap implementation was done through the use of programmable base-band filters and polynomial approximation.

Video frame rate up-conversion is an important issue for multimedia systems in achieving better video quality and motion portrayal. Motion-compensated methods offer better quality interpolated frames since the interpolation is performed along the motion trajectory. In addition, computational complexity, regularity, and memory bandwidth are important for a real-time implementation. Motion-compensated frame rate up-conversion (MC-FRC) is composed of two main parts: motion estimation (ME) and motion-compensated frame interpolation (MCFI). Since ME is an essential part of MC-FRC, a new fast motion estimation (FME) algorithm capable of producing sub-sample motion vectors at low computational-complexity has been developed. Unlike existing FME algorithms, the developed algorithm considers the low complexity sub-sample accuracy in designing the search pattern for FME. The developed FME algorithm is designed in such a way that the block distortion measure (BDM) is modeled as a parametric surface in the vicinity of the integer-sample motion vector; this modeling enables low computational-complexity sub-sample motion estimation without pixel interpolation. MC-FRC needs more accurate motion trajectories for better video quality; hence, a novel true-motion estimation (TME) algorithm targeting to track the projected object motion has been developed for video processing applications, such as motion-compensated frame interpolation (MCFI), deinterlacing, and denoising. Developed TME algorithm considers not only the computational complexity and regularity but also memory bandwidth. TME is obtained by imposing implicit and explicit smoothness constraints on block matching algorithm (BMA). In addition, it employs a novel adaptive clustering algorithm to keep the low-complexity at reasonable levels yet enable exploiting more spatiotemporal neighbors. To produce better quality interpolated frames, dense motion field at the interpolation instants are obtained for both forward and backward motion vectors (MVs); then, bidirectional motion compensation using forward and backward MVs is applied by mixing both elegantly.

Ce travail de thèse a été consacré au développement d'un système multicouche constitué de nanoparticules dopées par des ions terres rares (le cœur), entourées d'une première couche cristalline non dopée, permettant de préserver les propriétés optiques du cœur. Une coquille de silice mésoporeuse est ensuite déposée, permettant l'incorporation d'un photosensibilisateur (ZnPc) via les pores de la couche de silice pour une application thérapeutique : la photothérapie dynamique. Différentes matrices ont été étudiées à savoir Y2O3, KY3F10 et NaYF4. Ces matrices ont été codopées Yb3+/Er3+ afin d'obtenir des émissions dans le visible sous l'effet d'une excitation infrarouge (upconversion), le but ultime étant d'exciter le ZnPc in situ. Chacune des matrices a été caractérisée d'un point de vue structural et morphologique dans une première partie, et d'un point de vue spectroscopique dans une deuxième partie. La structure cœur-coquille cristalline renforce l'émission rouge issue du niveau 4F9/2 de l'Er, effet déduit de l'analyse des spectres et de la dynamique de luminescence.La détection de l'oxygène singulet a été réalisée par le protocole de " bleaching " en présence ou pas du ZnPc en évaluant l'intensité de fluorescence de l'ABDA.

Un-doped, Er3+ doped (TiO2:Er3+) as well as Er3+/Yb3+ co-doped (TiO2:Er3+/Yb3+) nanocrystals with different concentrations of RE3+ (Er3+, Yb3+) were successfully synthesized using the sol-gel method. The powder X-ray diffraction (XRD) spectra revealed that all undoped and doped samples remained in anatase after annealing at 400°C. The presence of RE3+ ions in the TiO2 host lattice was confirmed by conducting elemental mapping on the samples using Scanning electron microscope (SEM) equipped with energy dispersive X-ray spectrometer (EDX), which was in agreement with X-ray photoelectron spectroscopy (XPS) results. Transmission electron microscope (TEM) images approximated particle sizes of the samples to be between 1.5 – 3.5 nm in diameter and this compares well with XRD analyses. Phonon quantification in TiO2 was achieved using Fourier transform infrared (FT-IR) spectroscopy. Optical bandgap from Ultraviolet/Visible/Near-Infrared was extrapolated from Kubelka-Munk relation and the narrowing of the bandgap for the doped samples as compared to the undoped sample was observed. The photoluminescence PL study of the samples revealed two emission peaks attributed to direct band-gap and defect-related emissions. A laser beam with 980 nm wavelength was used to irradiate the samples, and the displayed emission lines of the TiO2: Er3+ in the visible region of the electromagnetic spectrum confirmed up-conversion luminescence. Enhancement of up-conversion luminescence intensity due to Yb3+ co-doping was observed, indicating an efficient energy transfer process from the sensitizer Yb3+ to the activator Er3+. / Physics / M. Sc. (Physics)

The hydration and dynamics of the biomolecules appear to be vital for their proper biological functioning. In the presented thesis, various fluorescence techniques were developed and applied to access these properties and their changes upon the mutual interactions of the biomolecules. Initially, the solvent relaxation method based on recording time-dependent fluorescence shift (TDFS) was used to map DNA interactions with proteins and lipids by the newly synthesised fluorene dye covalently bound to the DNA. Secondly, copper-transporting ATPase was probed by Badan attached to the copper-binding cysteine-proline-cysteine motif. The variations in hydration were found to be crucial for the proper ATPase function. Third, a detailed study on quenching of Badan/Prodan fluorescence by tryptophan revealed the limitations of the TDFS method for protein studies, which is essential finding for further applications of TDFS. Fourth application involves investigations of heavy atom effects on the excited state relaxation processes by up-conversion approach in iodinated metallocorroles, which are promising dyes for biological imaging. The obtained findings shall help in further tuning of the optical properties of the corroles desired for the variety of applications. Finally, fluorescence correlation spectroscopy...

We are living in an age where the demand for energy is growing rapidly. This means that supplies to easily accessible oil and natural gas is unlikely to keep up with the demand as times goes on. The world will have to use energy more efficiently and increase its use of other sources of energy. This study is aiming at developing materials that will improve the power conversion efficiency of photovoltaic cells by using up and down-converting phosphor materials. ZnTiO3-Zn2TiO4 composite and ZnTiO3 phosphors doped with Er3+,Yb3+, Eu3+ and Al3+, which display up and down-converted luminescence were synthesized by a simple high temperature conventional solid state reaction method. The structure, particle morphology, absorption, photoluminescent properties and elemental distribution were analyzed using X-ray diffraction (XRD), scanning electron microscopy (SEM), UV-Vis-NIR absorption spectrometer, photoluminescence (PL) spectroscopy and time of flight secondary ion mass spectroscopy (TOF-SIMS), respectively. ZnTiO3-Zn2TiO4 composite doped with different concentration of Er3+ ions was synthesized via solid state chemical reaction method at 1100 ℃. The X-ray diffraction (XRD) confirmed the crystallization of both the hexagonal ZnTiO3 and cubic spinel Zn2TiO4 phases of the composite. The SEM images of ZnTiO3-Zn2TiO4:Er3+ composite showed that the particle morphology was made up of faceted hexagons. Furthermore, the ZnTiO3-Zn2TiO4:Er3+ phosphors were excited in the near-infrared (NIR) region using a laser diode with a wavelength of 980 nm and displayed both green and red up-conversion emission bands in the visible range at 543, 553, 650 – 670 nm. These emission bands correspond to 2H11/2, 4S1/2→ 4 I15/2 and 4F9/2→ 4 I15/2 transitions of Er3+ ions. However, the interaction mechanisms involved in the upconversion process of ZnTiO3-Zn2TiO4:Er3+ phosphor is discussed with the help of an energylevel schematic diagram and the number of the photons involved in the up-conversion luminescence process were of a double photon mechanism. The decay lifetimes were studied by fitting the luminescence decay curve with a single-component exponential decay. Er3+ and Yb3+ incorporated zinc titanate (ZnTiO3) phosphor powders were synthesized using conventional solid-state reaction method at 800 ℃. A ZnTiO3:Er3+,Yb3+ phosphor that resembled an ecandrewsite single phase with space group R-3 (148) was obtained, as proven by X-ray diffraction (XRD). The SEM image showed a surface morphology composed of agglomerated irregular shaped particles. The energy band gap of ZnTiO3 was engineered by incorporating different concentration of the dopant ions. After irradiating ZnTiO3:Er3+with a 980 nm laser beam, the phosphor up-converted the photon energy to display green and red emissions in the visible range that were positioned at 527, 545 and 665 nm. Enhancement of the luminescence intensity of ZnTiO3:Er3+ phosphor was achieved by variation of Er3+ concentration. Co-doping with Yb3+ ions proved to be effective in enhancing the luminescence intensity of the optimized Er3+ ion emission and new emission bands at 410 and 480 nm, through an energy transfer mechanism were observed. The enhancement of the lifetime of the up-conversion luminescence was also achieved by co-doping ZnTiO3:Er3+ phosphor with Yb3+ ion. The energy transfer mechanisms involved in Er3+ - Yb3+ co-doped ZnTiO3 phosphor was illustrated and discussed in detail. The ZnTiO3:Er3+, Yb3+ thin films were successfully deposited by pulsed laser deposition (PLD) by varying the silicon (100) substrate temperature. The distribution of the ions in the films was investigated and the TOF-SIMS showed that the ions were homogeneously distributed throughout the ZnTiO3 host lattice which indicated a successful incorporation of the Er3+ and Yb3+ ions. The optical response of the phosphors revealed that the reflectance percentages of the ZnTiO3:Er3+, Yb3+ vary with the silicon substrate temperature due to the differences in the thickness and morphological roughness of the thin films. The ZnTiO3:Er3+, Yb3+ thin films also exhibited up-conversion emission from Er3+ electronic transitions, with violet, blue, green and red emission lines at 410, 480, 525, 545 and 660 nm from 2H9/2 → 4 I15/2, 4F7/2 → 4 I15/2, 2H11/2 → 4 I15/2, 4S3/2 → 4 I15/2 and 4F9/2 → 4 I15/2 transitions, respectively. These up-conversion emissions were enhanced by increasing the silicon substrate temperature during the deposition. ZnTiO3 host co-doped with Eu3+ and Al3+ was synthesized by solid state reaction to convert the UV photons to visible photons. Charge compensation effects of Al3+ incorporated ZnTiO3:Eu3+ as a co-dopant ion was reported in detail. The structural and morphological characterization show that the addition of Eu3+ and Al3+ does not affect the phase formation and the surface morphology of the host. The visible emission intensity of Eu3+ ions for an optimal concentration of 2 mol% under 395 nm excitation, was enhanced by incorporating Al3+. The energy level diagram showing the charge compensation mechanism was proposed for the co-doped system. / College of Engineering, Science and Technology