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Mixed metal oxynitrides have attracted attention due to their interesting chemical and physical properties in the past twenty years. In this thesis, four series of mixed metal oxynitrides have been investigated. The samples have been synthesized by both thermal ammonolysis and high pressure high temperature methods. The structural exploration covers perovskite, scheelite and pyrochlore types. The structural studies were carried out using powder X-ray and neutron diffraction, and magnetic and conducting properties have been explored. A series of new RZrO2N (R = Pr, Nd and Sm) perovskites were synthesized using high pressure high temperature methods (HPHT) via a direct solid state reaction of R2O3 with Zr2ON2. All three new phases crystallize in the orthorhombic Pnma perovskite superstructure, and the structural distortion increases with decreasing R3+ ionic radius. RZrO2N contains both R3+ and d0 Zr4+ and thus shows a potential for multiferroic properties. EuWO1-xN2+x perovskites with a wide range of nitrogen contents (-0.16 ≤ x ≤ 0.46) were synthesized by thermal ammonolysis of an oxide precursor Eu2W2O9. Ferromagnetic ordering below a Curie temperature TC =12 ± 1 K and negative colossal magnetoresistances (CMR) have been discovered in these samples. In particular, for the lowest doped sample, EuWO0.96N2.04, CMR ≥ 99.7% was observed at 7 K. The possibility of tuning the physical properties by altering the chemical composition has been demonstrated. A linear relationship between the lattice parameter and nitrogen content of EuWO1+xN2-x was observed. An investigation has been made of the Eu-Mo-O-N system. A new pyrochlore oxynitride series Eu2Mo2O6-xN2+2x/3 (0.20 ≤ x ≤ 2.25) was synthesized by ammonolysis of Eu2Mo2O7. A ferrimagnetic ordering and semiconducting behavior has been observed in these samples. A detailed structural study of SrMO2N (M = Nb, Ta) has been performed using variable temperature neutron and electron diffraction. Partial anion order has been observed in both samples up to 750 oC. It is consistent with cis-ordering of the two nitrides in each MO4N2 octahedron. At low temperatures, this order directs the tilting of the octahedron to form a pseudo-tetragonal superstructure. It creates zig-zag MN chains in two or three dimensions within the lattice. This principle can be used to predict the local structures of perovskite-related oxynitrides AMO3-xNx.

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Made available in DSpace on 2014-12-17T15:42:11Z (GMT). No. of bitstreams: 1 UlisandraRL_TESE_capa ate cap 4.pdf: 8084157 bytes, checksum: 1a4040f8da9be5f2ef606430865398fe (MD5) Previous issue date: 2011-08-01 / Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior / Different compositions of Ni0,5-xCuxZn0,5Fe2O4 and Ni0,5-xCoxZn0,5Fe2O4 0 ? x ? 0.3 were synthesized ferrite y the citrate precursor method. The stoichiometric compositions were calcined in air at 350?C and then pressed into pellets and toroids. The pressed samples were sintered at temperatures of 1000, 1050 and 1100?C/3h in air control at the speed of heating and cooling. The calcined powders were characterized by XRD, TGA / DTG, FTIR, SEM and vibrating sample magnetometry (VSM) and the sintered samples by XRD, SEM, MAV, density and measurements of permeability and magnetic losses. There was pure phase formation ferrimagnetism applied at all temperatures except for A-I composition at all sintering temperatures and A-II only at a temperature of 1100?C. Crystallite sizes were obtained by Rietveld analysis, nanometer size from 11 to 20 nm for the calcined powders. For SEM, the sintered samples showed grain size between 1 and 10 micrometers. Bulk density (?) of sintered material presented to the Families almost linear behavior with increasing temperature and a tendency to decrease with increasing concentration of copper, different behavior of the B Family, where the increase in temperature decreased the density. The magnetic measurements revealed the powder characteristics of a soft ferrimagnetic material. Two processes of magnetization were considered, the superparamagnetism at low temperatures (350?C) and the formation of magnetic domains at higher temperatures. Obtaining the best parameters for P and B-II magnetic ferrites at high temperatures. The sintered material at 1000?C showed a relative permeability (?) from 50 to 800 for the A Family and from 10 to 600 for the B Family. The samples sintered at 1100?C, B Family showed a variation from 10 to 1000 and the magnetic loss (tan ?) of A and B Families, around of 1. The frequency response of the toroidal core is in the range of 0.3 kHz. Several factors contribute to the behavior of microstructure considering the quantities ? and tan ?, such as the grain size, inter-and intragranular porosity, amount of grain boundary and the aspects of the dynamics of domain walls at high frequencies. / Foram sintetizadas diferentes composi??es da ferrita Ni0-5-xCuxZn0,5Fe2O4 e Ni0,5- xCoxZn0,5Fe2O4 com 0 ? x ? 0,3 pelo m?todo dos citratos precursores. As composi??es estequiom?tricas foram calcinadas em atmosfera ambiente na temperatura de 350?C e depois prensadas em pastilhas e tor?ides. As amostras prensadas foram sinterizadas nas temperaturas de 1000, 1050 e 1100?C/3h em atmosfera ambiente com controle na velocidade de aquecimento e resfriamento. Os p?s calcinados foram caracterizados por DRX, TGA/DTG, FTIR, MEV e magnetometria de amostra vibrante (MAV) e as amostras sinterizadas por DRX, MEV, MAV, massa espec?fica e medidas de permeabilidade e perdas magn?ticas. Observou-se a forma??o da fase pura ferrimagn?tica em todas as temperaturas aplicadas com exce??o para a composi??o A-I em todas as temperaturas de sinteriza??o e A-II apenas na temperatura de 1100?C. Foram obtidos tamanhos de cristalitos, pela an?lise de Rietveld, nanom?tricos, de 11 a 20 nm para os p?s calcinados. Por MEV, as amostras sinterizadas apresentaram tamanho de gr?os entre 1 e 10 ?m. A densidade aparente (?) do material sinterizado apresentou para a Fam?lia A comportamento quase linear com o aumento da temperatura e uma tend?ncia a diminuir com o aumento da concentra??o de cobre, comportamento diferente da Fam?lia B, onde o aumento da temperatura diminuiu a densidade. As medidas magn?ticas do p? revelaram caracter?sticas de um material ferrimagn?tico macio. Dois processos de magnetiza??o foram considerados, o superparamagnetismo em temperaturas baixas (350?C) e a forma??o de dom?nios magn?ticos em altas temperaturas. Obtendo-se melhores par?metros magn?ticos para as ferritas P e B-II em altas temperaturas. Os materiais sinterizados a 1000?C apresentaram permeabilidade (?) de 50 a 800 para a Fam?lia A e de 10 a 600 para a Fam?lia B. As amostras sinterizadas a 1100?C, Fam?lia B mostraram uma varia??o de 10 a 1000 e as perdas magn?ticas (tan?) das Fam?lias A e B, por volta de 1. A resposta de frequ?ncia dos n?cleos toroidais est? na faixa de 0,3 kHz. V?rios fatores da microestrutura contribuem para o comportamento das grandezas ? e tan?, tais como: o tamanho dos gr?os, porosidade inter e intragranular, quantidade de contorno de gr?os e os aspectos da din?mica das paredes dos dom?nios em altas frequ?ncias.

L'objectif de cette thèse est de développer des méthodes théoriques et numériques pour calculer la diffusion d'ondes de spin et leur transport balistique à travers deux types de nanomatériaux magnétiques désordonnés de terres rares - métaux de transition, à savoir le cobalt-gadolinium et le fer-gadolinium, comme éléments constitutifs des systèmes de nanojunctions. La modélisation développée dans ce travail décrit proprement les conséquences du désordre caractéristique de ces systèmes, à savoir de type alliage et celui de type structurel. Les méthodes théoriques et numériques développées servent en particulier à explorer les attributs de ces nanojonctions comme des filtres et des éléments de transmission assistée par résonance dans des dispositifs magnoniques. La thèse développe une version dynamique et non-locale pour l'approximation du potentiel (DNLCPA) afin d'étudier la dynamique de spin des systèmes ultraminces magnétiques désordonnés Fe-Gd et Co-Gd. Les potentiels aléatoires dynamiques de diffusion sont dérivés d'une manière inédite, exploitant les propriétés de phase des excitations de spin élémentaires dans le cadre du formalisme de Dyson. La méthode théorique est ensuite développée en deux manières fondamentales différentes, pour l'appliquer convenablement aux nano systèmes désordonnés qui présentent les types de désordre alliage et structurel. L'approche DNLCPA est ensuite conjuguée avec la théorie de raccordement de phase des champs (PFMT) pour étudier le transport balistique d'ondes de spin à travers les nanojonctions Co-Gd et Fe-Gd entre des gUides d'ondes de Co et Fe respectivement. L'approche PFMT-DNLCPA donne pour la première fois une modélisation des propriétés de diffusion et de transport d'ondes de spin incidents sur les nanojonctions, elle réussit à démontrer, modéliser et à quantifier la perte d'énergie en diffusion balistique due à chaque type de désordre. / The aim of this thesis is to develop theoretical and numerical methods to analyze the ballistic spin waves scattering and transport across two types of rare earth - transition metals disordered magnetic nanomaterials, namely the cobalt-gadolinium and the iron-gadolinium types, as building blocks for nanojunction systems. The theoretical computations developed in this work account properly for the consequences of the characteristic disorder present in these systems, whether alloy disorder for the former or structural amorphous-like disorder for the latter. The developed methods serve, in particular, to explore the attributes of these nanojunctions as filters and elements for resonance assisted transmission in a magnonic device. The thesis develops a novel and dynamic non-local version of the coherent potential approximation (DNLCPA), to study the spin dynamics on disordered ultrathin Co-Gd and Fe-Gd magnetic systems. The dynamic random scattering potentials are derived in a completely novel approach, exploiting the phase properties of the elementary spin excitations within the Dyson formalism. This approach is then developed in two different fundamental manners, and applied appropriately for the disordered nanosystems presenting alloy and structural disorder. The DNLCPA approach is incorporated with the phase field matching theory (PFMT) to study the spin waves ballistic transport across the Co-Gd and the Fe-Gd nanojunctions, sandwiched between Co and Fe leads respectively. This PFMT-DNLCPA method yields for the first time the description of the scattering and transport properties for the spin waves incident on the nanojunctions. Furthermore, our computations successfully demonstrate, model and quantify the diffusive energy loss in ballistic scattering due to each type of disorder.

Title: Optical and magneto-optical studies of ferrimagnetic garnets for photonic and spintronic applications Author: RNDr. Lukáš Beran Department: Intitute of Physics of Charles University Supervisor: RNDr. Martin Veis, PhD., Institute of Physics of Charles University Abstract: This doctoral thesis is devoted to fabrication and systematic char- acterization of physical properties of thin films of iron garnets with potential applications in photonic and spintronic devices. Investigated samples were pre- pared by metallo-organic decomposition and pulsed laser deposition. The study was focused on structural and magnetic characterizaiton along with optical and magneto-optical properties. Obtained experimental results were further con- fronted with theoretical calculations. The application potencial of garnets for photonic devices was discussed based on determined Figure of Merit (Faraday rotation to optical loss ratio). High values were achieved for single crystal thin film of Ce doped yttrium iron garnet on galium gadolinium garnet substrate as well as for pollycrystalline Bi doped yttrium iron garned on silicon substrate. Furthermore, new rare-earth garnets were prepared with attempt to achieve per- pendicular magnetic anisotropy of these film. This was achieved for three di erent materials, which were not...

The aim of this master thesis is to prepare and systematically characterize two groups of ultra-thin films of iron garnets with different compositions and deposition conditions. The first set consists of approximately 10 nm thick samples of gallium-doped yttrium-iron garnet on gadolinium gallium garnet (Gd3Ga5O12) (GGG) substrates with different crys- tallographic orientations and different annealing temperatures. The second group con- tains gallium-bismuth-doped neodymium-iron garnet on GGG substrates. These samples have different thicknesses, the concentration of individual elements and different annealing temperatures. All samples were prepared by the metal-organic decomposition method. The analysis of their physical properties was done by magneto-optical Kerr effect (MOKE) and optical experiments. Specifically, MOKE spectroscopy, Faraday hystere- sis loops measurements and spectroscopic ellipsometry. Obtained experimental results were further used to deduce the spectral dependence of complete permittivity tensor. Its spectral dependence was than discussed with relation to the electronic structure of in- vestigated materials which helped to select the best deposition conditions and substrate orientation. 1