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This thesis studies different Eu optical centers in MgS:Eu and CaS:Eu thin films produced by Chemically Controlled Pulse Laser Deposition (CCPLD) and evaluates their suitability for the development of spectral storage devices of the future. The produced thin films consist of one or more optically active layer(s), MgS:Eu, CaS:Eu or a similar material, and a corresponding ZnS capping layer that functions as a protecting barrier for the other layers and preserves their composition and integrity. Given that the synthesis of the materials used to produce the multilayer structures in this work proved a great challenge, careful attention was given to the optimization of all fabrication parameters. Mass Spectrometry was used during the deposition of the thin films and the data obtained resulted on improvements and optimization of the deposition process. Scanning electron microscopy studies of these thin films were conducted to study degradation upon long-term storage. Microscopy results show that the morphology of the produced thin films is correlated to the growth environment during deposition and deterioration of the deposited materials could be initiated by nano-gaps and cracks in the capping layer of the thin films. In addition to optical centers in MgS:Eu and CaS:Eu, new centers were created by changing the thin film growth environment inside a hi-vacuum chamber, modifying the composition of the ablation target material, or both. For example, introducing O2, or alternatively HCl, inside the CCPLD chamber while producing MgS:Eu thin films results in the formation of impurity associated centers across lattice sites throughout the deposited structures. In another method of impurity doping studied, Cl- and Na+ were introduced into the MgS:Eu and CaS:Eu lattices by mixing trace amounts of the impurity ions into these materials in polycrystalline form and making this mixture a deposition target by hi-pressure cold compression technique. The introduction of these impurity ions will alter the crystal field environment around the Eu ions thus creating new optical centers with a shift in energy of their characteristic Zero Phonon Line. After extensive characterization of the optical properties of the thin films produced, laser-induced fluorescence spectroscopy and absorption spectroscopy measurements confirm that they are suitable candidates to be used in conjunction with power-gated spectral holeburning technique and could potentially provide ultrahigh, terabits per square inch, storage densities. / Physics

Experiments with polarized "ultracold neutrons" (UCN) offer a new way to measure the decay correlations of neutron beta decay; these correlations can be used to test the completeness of the Standard Model and predict physics beyond it. Ultracold neutrons are very low energy neutrons that can be trapped inside of material and magnetic bottles. The decay correlations in combination with the neutron and muon lifetimes experimentally find the first element (Vud) of the Cabibbo-Kobayashi-Maskawa (CKM) quark mixing matrix. The CKM matrix is a unitary transform between the mass and weak eigenstates of the d, s and b quarks; if the matrix is not unitary this would imply that the Standard Model is not complete. Currently the first row of the CKM matrix is over 2 sigma from unitarity and Vud is the largest component of the row. The UCNA experiment looks at the correlation between the polarization of the neutron and the momentum of the electron resulting from the beta decay of the neutron (the A-correlation). The keys to making a high precision measurement of A-correlation are a near 100% polarization of the neutrons that decay, low"backscatter electron detectors, and small, well characterized backgrounds. UCN can be 100% polarized by passing them through a seven Telsa magnetic field. The key to the UCNA experiment is keeping them polarized until they decay or are lost. This dissertation covers the development of guides that are minimally depolarizing and efficient transporters of UCN and their use in the UCNA experiment. The entire guide development process is covered from conception to manufacturing and testing. This process includes development of a pulsed laser deposition, diamond-like carbon coating system and materials studies of the resulting coatings. After the initial studies of the guide coating, meter"long sections of guide are tested with UCN to determine their depolarization and transport properties. The guide technology developed in this dissertation has been used in the entire UCNA experiment. Also, this technology is currently the state of the art for polarized and non-polarized UCN guide systems and it is being implemented in several new UCN experiments. / Ph. D.

Barium Titanate (BaTiO3 or BTO) has attracted an ever increasing research interest because of its wide range of potential applications. Nano-sized or nanostructured BTO has found applications in new, useful smart devices, such as sensors and piezoelectric devices. Not only limited to one material, multi-layers or multi-phases can lead to multifunctional applications; for example, nanocomposites can be fabricated with ferrite or metal phase with BTO. In this study, I synthesized various BTO-ferrites, ranging from nanoparticles, nanowires to thin films. BTO-ferrite coaxial nanotubes, BTO-ferrite self-assemble thin films, and BTO single phase films were prepared by pulsed laser deposition (PLD) and sol-gel process. BTO-ferrite nanocomposites were grown by solid state reaction. Furthermore, BTO-metal nanostructures were also synthesized by solid state reaction under hydrogen gas which gave us a great inspiration to fabricate metal-ceramic composites. To understand the relationship between metal and BTO ceramic phase, I also deposited BTO film on Au buffered substrates. A metal layer can affect the grain size and orientation in BTO film which can further help us to control the distribution of dielectric properties of BTO films. After obtaining different nanomaterials, I am interested in the applications of these materials. Recently, many interesting electric devices are developed based on nanotechnology, e.g.: memristor. Memristor is a resistor with memory, which is very important in the computer memory. I believe these newly-synthesized BTO based nanostructures are useful for development of memristor, sensors and other devices to fit increasing needs. / Ph. D.

Nanodiamonds are a promising platform for quantum technologies due to the combinations of their inherent properties and the properties of the fluorescent color centers hosted in diamond. They can be employed as quantum sensing devices with spatial resolution in the range of the nanometer and capable of withstanding harsh conditions while also being biocompatible, allowing applications with sensitive biological systems; but they also find application in quantum computing and photonics fields. For all these applications the central features are the properties of the photoluminescent color centers employed, the color centers on which this thesis is focused are the Nitrogen-Vacancy (NV) and Silicon-Vacancy (SiV) centers of diamond. Both centers are of high interest due to spin dependent properties of their fluorescent emission which can be accessed at room temperature. The development of quantum technologies based on such fluorescent nanodiamonds is stifled by the the lack of production techniques that can be easily scaled to industrial levels. In fact most of the more prominent techniques found in literature exhibit drawbacks both in terms of control of particle properties and of scalability. This thesis focuses on the synthesis of nanodiamonds by Pulsed Laser Ablation in Liquid, with particular interest in the possibility of producing continuously nanodiamonds containing NV and SiV centers. For the NV center the technique of choice have been Pulsed Laser Ablation in liquid nitrogen focusing on the yield of the process as the technique has already been experimentally validated. For the SiV centers the ablation process was performed in water and the graphite precursor have been substituted for a composite graphite and silicon carbide precursor.

The thesis deals with the preparation, characterization and, in particular, with the switching properties of phase-change material (PCM) thin films. The films were deposited using the Pulsed Laser Deposition (PLD) technique. Phase transformations in these films were triggered by means of thermal annealing, laser pulses, and electrical pulses. The five major physical aspects structure transformation, crystallization kinetics, topography, optical properties, and electrical properties have been investigated using XRD, TEM, SEM, AFM, DSC, UV-Vis spectroscopy, a custom-made nanosecond UV laser pump-probe system, in situ resistance measurements, and conductive-AFM. The systematic investigation of the ex situ thermally induced crystallization process of pure stoichiometric GeTe films and O-incorporating GeTe films provides detailed information on structure transformation, topography, crystallization kinetics, optical reflectivity and electrical resistivity. The results reveal a significant improvement of the thermal stability in PCM application for data storage. With the aim of reducing the switching energy consumption and to enhance the optical reflectivity contrast by improving the quality of the produced films, the growth of the GeTe films with simultaneous in situ thermal treatment was investigated with respect to optimizing the film growth conditions, e.g. growth temperature, substrate type. For the investigation of the fast phase transformation process, GeTe films were irradiated by ns UV laser pulses, tailoring various parameters such as pulse number, laser fluence, pulse repetition rate, and film thickness. Additionally, the investigation focused on the comparison of crystallization of GST thin films induced by either nano- or femtosecond single laser pulse irradiation, used to attain a high data transfer rate and to improve the understanding of the mechanisms of fast phase transformation. Non-volatile optical multilevel switching in GeTe phase-change films was identified to be feasible and accurately controllable at a timescale of nanoseconds, which is promising for high speed and high storage density of optical memory devices. Moreover, correlating the dynamics of the optical switching process and the structural information demonstrated not only exactly how fast phase change processes take place, but also, importantly, allowed the determination of the rapid kinetics of phase transformation on the microscopic scale. In the next step, a new general concept for the combination of PCRAM and ReRAM was developed. Bipolar electrical switching of PCM memory cells at the nanoscale can be achieved and improvements of the performance in terms of RESET/SET operation voltage, On/Off resistance ratio and cycling endurance are demonstrated. The original underlying mechanism was verified by the Poole-Frenkel conduction model. The polarity-dependent resistance switching processes can be visualized simultaneously by topography and current images. The local microstructure on the nanoscale of such memory cells and the corresponding local chemical composition were correlated. The gained results contribute to meeting the key challenges of the current understanding and of the development of PCMs for data storage applications, covering thin film preparation, thermal stability, signal-to-noise ratio, switching energy, data transfer rate, storage density, and scalability.

Die vorliegende Arbeit befasst sich mit magnetischen Tunnelkontakten (magnetic tunnel junctions, MTJs) auf Basis des Oxids Zinkferrit (ZnxFe3-xO4). Dabei soll das Potential dieses Materials durch die Demonstration des Tunnelmagnetowiderstandes (tunnel magnetoresistance, TMR) in zinkferritbasierten Tunnelkontakten gezeigt werden. Dazu wurde ein Probendesign für MTJs auf Basis der „pseudo spin valve“-Geometrie entwickelt. Die Basis für dieseStrukturen ist ein Dünnfilmstapel aus MgO (Substrat) / TiN / ZnxFe3-xO4 / MgO / Co. Dieser ist mittels gepulster Laserabscheidung (pulsed laser deposition, PLD) hergestellt. Im Rahmen dieser Arbeit wurden die strukturellen, elektrischen und magnetischen Eigenschaften der Dünnfilme untersucht. Des weiteren wurden die fertig prozessierten MTJ-Bauelemente an einem im Rahmen dieser Arbeit entwickeltem und aufgebautem TMR-Messplatz vermessen. Dabei ist es gelungen einen TMR-Effekt von 0.5% in ZnxFe3-xO4-basierten MTJs nachzuweisen. Das erste Kapitel der Arbeit gibt eine Einführung in die spintronischen Effekte Riesenmagnetowiderstand (giant magnetoresistance, GMR) und Tunnelmagnetowiderstand (TMR). Deren technologische Anwendungen sowie die grundlegenden physikalischen Effekte und Modelle werden diskutiert. Das zweite Kapitel gibt eine Übersicht über die Materialklasse der spinellartigen Ferrite. Der Fokus liegt auf den Materialien Magnetit (Fe3O4) sowie Zinkferrit (ZnxFe3-xO4). Die physikalischen Modelle zur Beschreibung der strukturellen, magnetischen und elektrischen Eigenschaften dieser Materialien werden dargelegt sowie ein Literaturüberblick über experimentelle und theoretische Arbeiten gegeben. Im dritten Kapitel werden die im Rahmen dieser Arbeit verwendeten Probenpräparations- und Charakterisierungsmethoden vorgestellt und technische Details sowie physikalische Grundlagen erläutert. Die Entwicklung eines neuen Probendesigns zum Nachweis des TMR-Effekts in ZnxFe3-xO4-basierten MTJs ist Gegenstand des vierten Kapitels. Die Entwicklung des Probenaufbaus sowie die daraus resultierende Probenprozessierung werden beschrieben. Die beiden letzten Kapitel befassen sich mit der strukturellen, elektrischen und magnetischen Charakterisierung der mittels PLD abgeschiedenen Dünnfilme sowie der Tunnelkontaktstrukturen.

Neste trabalho, foi desenvolvido um laser pulsado utilizando um chaveador-Q passivo em uma cavidade com a tecnologia de controle de modo por duplo-passo. Utilizando um cristal de Nd:LiYF4 com 0,8 mol% de dopagem, foi possível gerar um pulso com duração de 5,5 ns (FWHM), com 1,2 mJ de energia e potência pico de 220 kW para utilização na técnica Cavity Ring-Down Spectroscopy (CRDS). A técnica (CRDS), que pode ser traduzida por espectroscopia de cavidade ressonante, é utilizada para medida de espectros de absorção de gases, líquidos e sólidos. Com a técnica CRDS é possível medir perdas com altíssimo grau de precisão, ressaltando sua sensibilidade que é confirmada pela utilização de espelhos com alta refletividade. Foram avaliadas, com essa técnica, as perdas por reflexão e espalhamento de materiais transparentes. Após a calibração da cavidade ressonante, foi possível medir as perdas nas amostras com resolução de até 0,045%, sendo o valor máximo alcançado de 1,73%. Essa calibração foi possível, pois obteve se um tempo de decaimento de aproximadamente 20 μs com a cavidade desobstruída. Também foi conseguido um método de determinação do índice de refração dos materiais transparentes com precisão de cinco casas decimais. / In this work, a pulsed and Q-switched laser resonator was developed using the double-beam mode-controlling technique. A Nd:LiYF4 crystal with 0,8mol% of doping concentration was used to generate a giant pulse with duration of 5,5 ns (FWHM), 1,2 mJ of energy and 220 kW peak power for the Cavity Ring-Down Spectroscopy (CRDS) technique. The CRDS technique is used to measure absorption spectra for gases, liquids and solids. With the CRDS technique it is possible to measure losses with high degree of accuracy, underscoring the sensitivity that is confirmed by the use of mirrors with high reflectivity. With this technique, the losses by reflection and scattering of transparent materials were evaluated. By calibrating the resonant cavity, it was possible to measure the losses in the samples with resolution of 0,045%, the maximum being reached by 1,73%. The calibration was possible because there was obtained to measure a decay time of approximately 20 μs with the empty cavity. Besides was obtained a method for determining the refractive index of transparent materials with accuracy of five decimals.