Ce travail a pour objectif de contribuer à l'étude du magnétisme dans les oxydes isolants de type AB_2O_6 (A= Fe, Co, Ni; B= Ta, Sb). Ces composés cristallisent dans une structure trirutile et présentent une variété très riche de phases magnétiques. Tous les ordres observés peuvent être classés comme antiferromagnétiques mais diffèrent d'un ordre simple de type Néel. En outre, les substitutions comme Fe_xCo_{1-x}Ta_2O_6, Fe_xNi_{1-x}Ta_2O_6 et Co_xNi_{1-x}Ta_2O_6 conduisent à des domaines de coexistence de phases magnétiques et à des points bicritiques dans les diagrammes de phases T(x). Une caractéristique particulièrement intéressante de ces composés est le caractère quasi-bidimensionnel de leur magnétisme, puisque les ions de métaux de transitions A apparaissent dans des réseaux plans séparés par deux plans d'ions non magnétiques B. Une forte anisotropie de champ cristallin est observée sur les sites magnétiques, résultant de la distorsion axiale des octaèdres d'oxygènes qui entourent ces ions A. Nous avons abordé deux aspects complémentaires: théorique et expérimental. Du point de vue théorique, une reformulation du modèle bidimensionnel jusqu'à present utilisée pour décrire la susceptibilité paramagnétique nous a permi d'obtenir des constants d'échange compatibles avec les types d'ordre magnétique planaire observés. Considérant que le caractère tridimensionnel des structures magnétiques révélées par diffraction neutronique indique l'importance du couplage entre plans, quoique faible, à basse température, nous proposons un modèle tridimensionnel coherent avec les ordonnements observés aussi dans le plan ab qu'au long de l'axe c. Du point de vue expérimental, nous faisons des substitutions sur le site non magnétique pour modifier de façon systematique l'espacement entre les plans magnétiques et, en consequence, le couplage entre eux. En particulier, nous avons synthétisé des composés du type ANb_xTa_{2-x}O_6 avec A = Fe, Ni et Co, restant dans le domaine de stabilité de la phase quadratique, puisque la présence de Nb favorise une phase orthorhombique. Une caractérisation structurale et magnétique de ces systèmes est faite par diffraction de rayons X et de neutrons, complétées par des mesures de susceptibilité magnétique, chaleur spécifique et aimantation en fonction du champ appliqué. Nous étudions également des séries avec Sb à la place de Nb où nous avons également effectué des remplacements sur le site magnétique. / This work aims to contribute to the study of magnetism in insulating oxides of the type AB_2O _6 (A = Fe, Co, Ni, Ta = B, Sb). These compounds crystallize in a trirutile structure and present a rich variety of magnetic phases. All the observed orderings can be classified as antiferromagnetic, but they differ from a simple Néel type order. Moreover, substitutions such as Fe_xCo_{1-x}Ta_2O_6, Fe_xNi_{1-x}Ta_2O_6 and Co_xNi_{1-x}Ta_2O_6 produce several regions of phase coexistence and bicritical points in the phase diagram T vs. x. A particularly interesting characteristic of these compounds is the quasi-two-dimensional nature of their magnetism, since the transition-metal ions A appear in layers separated by two planes of the non-magnetic ions B. They also show strong crystal-field anisotropy on the magnetic sites due to axial distortion of the oxygen octahedra surrounding the A ions. Our approach involves two complementary aspects: theoretical and experimental. From the theoretical point of view, a reformulation of the two-dimensional model used until now to describe the paramagnetic susceptibility allows us to obtain exchange parameters compatible with the observed planar magnetic orderings. Considering that the three-dimensional character the magnetic structures revealed by neutron diffraction indicates that the coupling between planes, although weak, plays an important role to low temperatures, we propose a three-dimensional model consistent with the observed orderings both in the ab plane and along the c axis. From the experimental point of view, we make substitutions on the non-magnetic sites, in order to systematically modify the spacing between planes and, consequently, the coupling between them. In particular, we have synthesized compounds of type ANb_xTa_{2-x}O_6 with A = Fe, Ni and Co, remaining in the stability region of tetragonal phase, since the presence of Nb favors an orthorhombic phase. The structural and magnetic characterization of the systems is done via the X-ray and neutron diffraction as well as measurements of magnetic susceptibility, specific heat, and magnetization as a function of the applied field. We also study series with Sb in place of Nb where we additionally include substitutions in the magnetic site.

In this study, the ageing effects on powder used for cemented carbide insert production are examined. Ageing is throughout this study, defined as the time dependent change of the magnetic properties: coercive field strength and saturation magnetization. Testing is done using eight different powder compositions stored in both air and in an argon cabinet for 10 weeks, where sampling is done at specific intervals. Samples are stored in vacuum sealed bags for a combined sintering at the last phase of the test. Magnetic properties are assumed to be dependent on the amount of oxides needed to be reduced by taking carbon from the material itself during the vacuum stage of the sintering. To achieve interpretive results, this study also tested available sintering furnaces (DMK and DEK) by sintering trays with patterns of test pieces. This shows that DEK furnaces are much better for the ageing tests performed in this study, since less variation of the magnetic properties are measured because of the symmetrical heat gradient over each tray. Ageing tests strongly suggest that the cause of ageing comes from water absorbed by the PEG in the powder composition. Changing the molecular weight of the PEG seems to have an effect on the powder's ageing sensitivity. Measurements performed in this study show less ageing for Cr-rich DA-powders than for cubic carbide rich DQ-powders.

Submitted by Maike Costa (maiksebas@gmail.com) on 2016-03-18T13:56:29Z No. of bitstreams: 1 arquivo total.pdf: 1539512 bytes, checksum: 4aa510877c1a4800c42aaf9dfdae33d3 (MD5) / Made available in DSpace on 2016-03-18T13:56:29Z (GMT). No. of bitstreams: 1 arquivo total.pdf: 1539512 bytes, checksum: 4aa510877c1a4800c42aaf9dfdae33d3 (MD5) Previous issue date: 2015-03-26 / In this thesis, we investigate by the first time the impact of non-inertial effects associated with the rotation of the reference system on charged and neutral particles confined by a quantum ring, which is described by the potential of Tan-Inkson. The contribution of the rotation is introduced by its coupling with angular momentum of the system. We show that the rotation is introduced via a non-minimum coupling to the kinetic part of the Hamiltonian describing the quantum dynamics of systems studied here. Thus, we show that non-inertial effects of the rotation induce on the quantum properties of the particles similar effects generated by a magnetic field. We also investigated the contribution of a screw dislocation on the physical properties of the particles. The topological defect contributes as a torsion source, presenting a contribution similar to the Aharonov-Bohm flux. Besides charged particles (electrons and holes), we also study the effects of rotation on neutral particles in three different scenarios: a neutral particle with a permanent magnetic dipole moment coupled by the Aharanov-Casher interaction; a neutral particle with a permanent electric dipole moment coupled by the interaction proposed by He-McKellar-Wilkens and a neutral particle with an electric dipole moment induced by the field configuration proposed by Wei-Han-Wei. In all three cases it is shown the similarity between the neutral and charged particles. We analyze the non-relativistic quantum dynamics of these particles by solving the Schrödinger equation. In addition to the energy spectrum and wave functions, we calculate the persistent current and the magnetization for the four systems studied here, and we also analyzed, from the expression for the persistent current for quantum rings, the limit case for quantum dots. / Neste trabalho, investigamos pela primeira vez na literatura o impacto de efeitos nãoinerciais associados com a rotação do sistema de referência de partículas carregadas e neutras confinadas por um anel quântico, descrito pelo potencial de Tan-Inkson. A contribuição da rotação é introduzida através de seu acoplamento com o momento angular do sistema. Mostramos que a rotação entra como uma espécie de acoplamento mínimo na parte cinética do Hamiltoniano que descreve a dinâmica quântica dos sitemas em questão. Com isso, mostramos que a rotação induz efeitos típicos de campos magnéticos sobre as propriedades quânticas das partículas. Também investigamos os efeitos da contribuição de uma deslocação tipo-hélice sobre as propriedades físicas das partículas. O defeito topológico contribui como uma fonte de fluxo de torção, tendo um comportamento similar ao do fluxo Aharonov-Bohm. Além de partículas carregadas (elétrons e buracos), estudamos os efeitos da rotação sobre partículas neutras em três cenários diferentes: uma partícula neutra com momento de dipolo magnético permanente acoplado pela interação proposta por Aharanov- Casher; uma partícula neutra com momento de dipolo elétrico permanente acoplada pela interação proposta por He-McKellar-Wilkens e uma partícula neutra como momento de dipolo elétrico induzido pela interação proposta por Wei-Han-Wei. Em todos os três casos mostramos que existe uma estreita analogia entre partículas neutras e carregadas. A metodologia utilizada consiste em analizar a dinâmica quântica não-relativistica dessas partículas via resolução da equação de Schrödinger. Além do espectro de energia e das funções de onda, calculamos as correntes persistentes e a magnetização para os quatro sistemas aqui estudados, e também analizamos, a partir da expressão para a corrente persistes para anéis quânticos, o caso limte para pontos quânticos.

Submitted by MARCO ANTONIO BAPTISTELLA null (marco_baptistella@terra.com.br) on 2016-08-23T19:37:34Z No. of bitstreams: 1 REV 17. MARCO A. BAPTISTELLA.pdf: 11920777 bytes, checksum: ba33aea22870d52b190f07f07f6e333c (MD5) / Approved for entry into archive by Ana Paula Grisoto (grisotoana@reitoria.unesp.br) on 2016-08-25T20:22:58Z (GMT) No. of bitstreams: 1 baptistella_ma_me_guara.pdf: 11920777 bytes, checksum: ba33aea22870d52b190f07f07f6e333c (MD5) / Made available in DSpace on 2016-08-25T20:22:58Z (GMT). No. of bitstreams: 1 baptistella_ma_me_guara.pdf: 11920777 bytes, checksum: ba33aea22870d52b190f07f07f6e333c (MD5) Previous issue date: 2016-08-04 / Atualmente, as cargas aplicadas nos eixos de vagões ferroviários têm sofrido aumento de esforços devido ao choque e tração no engate ferroviário. Neste trabalho o estudo foi realizado no engate tipo “F”, que tem maior utilização e interesse por parte da ferrovia, por se tratar de um engate rotativo e utilizado para descarregamento de vagões com os mais diversos tipos de carga. Este trabalho tem como objetivo, verificar se existem transformações da microestrutura no material do engate, e possíveis gerações de trincas, através do estudo do aço AAR M-201 Grau E, após o ensaio de partículas magnéticas, com corrente alternada através da aplicação de Prods. A faixa de amperagem variou-se de 100 a 1000 ampères e como meio de resfriamento, utilizou-se a água a temperatura ambiente e o ar forçado. A preparação foi feita partindo de um engate Tipo “F” completo, fornecido por um operador logístico, a cauda foi magnetizada por inteiro e depois separados os corpos de prova por corte de serra, refrigerado para não haver aquecimento. Para a caracterização microestrutural, utilizou-se uma preparação metalográfica de laboratório de bancada e ataque com Nital 2%, e fez-se uso de microscopia ótica convencional e microscopia eletrônica de varredura (MEV). Através da utilização da microscopia ótica e da microscopia eletrônica de varredura (MEV), pode-se verificar a microestrutura nas áreas que sofreram alterações microestruturais. Concluiu-se que o aço do engate, AAR M-201 grau E, após a magnetização por Prods de 300 a 1000 ampères, apresentou alteração microestrutural, onde observou-se uma estrutura de martensita acicular não revenida e geração de trincas, a mesma alteração microstrutural foi observada em amostras com resfriamento ao ar, porém sem a geração de trincas, em ampliações de 50 vezes foi nítido o efeito de queima provocado pelo Prods no material, bem como sua extensão, evidenciando áreas centrais de atuação do Prods, zonas de transição e áreas não afetadas. As trincas tiveram comportamento de propagação intergranular, para ampliações de 9300 vezes em MEV, pode-se observar que as mesmas se propagaram somente nas áreas com martensita e contornaram as áreas com maior presença da fase ferrítica. / Currently, the applied loads on the axles of railway cars has been increasing efforts due to shock and traction in railway coupling. In this work, the study was performed on the coupling type "F", which has increased use and interest on the part of the railway, because it is a rotary coupling and used for unloading of wagons with the most diverse types of cargo. This work aims, check for microstructural changes on the coupling material, and possible generation of cracks through the study of steel AAR M-201 grade and after the test of magnetic particles with alternating current by applying Prods. As amperage range, was varied from 100 to 1000 amps and as cooling medium water was used at room temperature and forced air. The preparation was made starting from a coupling type "F" full, provided by a logistics operator, the tail was magnetized in full and then separate the specimens by cutting saw, cooled to no heating. For microstructural characterization, we used a metallographic preparation of benchtop laboratory and attack Nital 2%, and was made use of conventional optical microscopy and scanning electron microscopy (SEM). By using light microscopy and scanning electron microscopy (SEM), you can check the microstructure in areas that suffered microstructural changes. It was concluded that the coupling of steel, AAR M-201 grade And after magnetization by Prods 300-1000 amps, presented change microstructural where there was a martensite acicular structure not tempered and generation of cracks, the same change microstructural was observed in air to cooling with samples, but without generating cracks at magnifications of 50 times was clear the burning effect caused by Prods in the material as well as its extension, showing the central areas of the Prods activities, transition zones and unaffected areas. The intergranular crack propagation behavior had to 9300 times magnification under SEM, it can be seen that they have spread only in areas with martensite and rounded areas with the greatest presence of the ferritic phase.

Made available in DSpace on 2014-12-17T15:14:57Z (GMT). No. of bitstreams: 1 TiberioMLA_DISSERT.pdf: 5996955 bytes, checksum: 689080ca5f207d43776c16e5aab237d7 (MD5) Previous issue date: 2012-07-27 / Conselho Nacional de Desenvolvimento Cient?fico e Tecnol?gico / Today, one of the topics that attracts interest of the scientific community is the understanding of magnetic properties of magnetic systems with reduced dimensions, in particular, ferromagnetic thin films. In this case, the comprehension and control of these properties, as well as the development of routes to obtain them, are crucial issues in many aspects of current and future technologies for storage and transmission of information in the electro-electronic industry. There are several materials that exhibit soft magnetic properties, and we highlight the amorphous alloys and that ones obtained by partial crystallization, so-called nanocrystalline materials. The production of these alloys as magnetic ribbons is very common in scientific and technological area, but there are just a few works related to the production of these alloys as thin films. In this work, we studied the quasi-static magnetic properties of ferromagnetic thin films based on FeCuNbSiB in a wide range of thicknesses, from 20 to 500 nm, produced by sputtering. In particular, after the structural characterization performed via X-ray diffraction, the magnetic properties of the sets of samples were investigated using experimental magnetization curve, obtained using a vibrating sample magnetometer, as well as through theoretical curves obtained by theoretical modeling and numerical computation. The modeling process is based on the Stoner Wohlfarth model applied to three dimensions, and adds some energy terms, using as reference experimental results of magnetization. In this case, from the comparison between theoretical and experimental results and the analysis of the constant anisotropy behavior as a function of film thickness, we aim to obtain further information on the magnetization process of the samples, to identify routes for the production of thin films and develop a theoretical to films to use it, in the future, in the obtainment of the theoretical curves of some magnetic measurements, such as magnetoimpedance and magnetoresistance / Dentre os temas que despertam interesse da comunidade cient?fica atualmente est? o entendimento das propriedades magn?ticas de sistemas magn?ticos com dimens?es reduzidas, em particular, filmes finos ferromagn?ticos. Neste caso, a compreens?o e o controle destas propriedades, bem como o desenvolvimento de rotas para sua obten??o, s?o temas cruciais em muitos aspectos das tecnologias atuais e futuras de armazenagem e transmiss?o da informa??o na ind?stria eletro-eletr?nica. Dos materiais que exibem propriedades magn?ticas macias, destacam-se as ligas amorfas e as ligas obtidas por cristaliza??o parcial das mesmas, os chamados materiais nanocristalinos. A produ??o destas ligas na forma de fitas magn?ticas tem sido muito comum no meio tecnol?gico e cient?fico, por?m s?o escassas as produ??es de filmes finos desta liga. Neste trabalho, realizamos um estudo das propriedades magn?ticas quase-est?ticas de filmes ferromagn?ticos ? base de FeCuNbSiB, em uma vasta faixa de espessuras, de 20 a 500 nm, produzidos pela t?cnica de sputtering. Em particular, ap?s caracteriza??o estrutural, realizada via difratometria de raios-X, as propriedades magn?ticas dos conjuntos de amostras foram investigadas atrav?s de curvas de magnetiza??o experimentais, obtidas utilizando-se um magnet?metro de amostra vibrante, bem como atrav?s de curvas te?ricas obtidas atrav?s de modelagem e computa??o num?rica. O processo de modelagem toma como base o modelo Stoner-Wohlfarth aplicado para tr?s dimens?es, e acrescenta os alguns outros termos de energia, tomando como refer?ncia os resultados experimentais para magnetiza??o. Neste caso, a partir da compara??o dos resultados te?ricos e experimentais e da an?lise do comportamento das constantes de anisotropia em fun??o da espessura dos filmes, busca-se obter informa??es sobre o processo de magnetiza??o das amostras, identificar rotas para a produ??o de filmes finos e desenvolver uma abordagem te?rica para filmes com o intuito de, no futuro, utiliz?-la para a obten??o de curvas te?ricas de outras medidas magn?ticas, tais como magnetoimped?ncia e magnetoresist?ncia

Neste trabalho, calculam-se o calor específico e a entropia do Modelo de Anderson simétrico de uma impureza usando o Grupo de Renormalização Numérico (GRN). O método é baseado na discretização logarítmica da banda de condução do metal hospedeiro a qual a impureza está acoplada. Porém, esta discretização introduz oscilações nas propriedades termodinâmicas. Esta inconveniência, inerente ao método, é contornável para a suscetibilidade magnética, mas é crítica para o calor específico, restringindo o alcance do GRN. Para sobrepor essa dificuldade, é usado o novo procedimento denominado intercalado que foi desenvolvido para o cálculo da suscetibilidade magnética de modelos de duas impurezas. Para reduzir as matrizes e o tempo computacional, é usado, também, o operador carga axial, recentemente definido no contexto do Modelo de Kondo de duas impurezas, e que é conservado pelo Hamiltoniano de Anderson simétrico. As curvas obtidas são comparadas com resultados exatos obtidos por ansatz de Bethe e pelo Modelo de Nível Ressonante. / The specific heat and the entropy of the one-impurity symmetric Anderson Model are calculated using the Numerical Renormalization Group (NRG). The heart of the method is the logarithmic discretization of the metal conduction band where the impurity is coupled. However, this discretization, inherent in the method, introduces oscillations in the thermodynamical properties. For the susceptibility it is not so critical but for the specific heat the usual calculation is prohibitive. To overcome this difficulty, we use the new procedure called interleaved that was developed to calculate the susceptibility of two-impurity models. In order to reduce the matrices and computation time, use is made of the axial charge operator recently defined in the two-impurity Kondo Model context and that is conserved by the symmetric Anderson Hamiltonian. The curves obtained are compared with exacts results of Bethe ansatz and Resonant Level Model.

As diversas aplicações tecnológicas de nanopartículas magnéticas (NPM) vêm intensificando o interesse por materiais com propriedades magnéticas diferenciadas, como magnetização de saturação (MS) intensificada e comportamento superparamagnético. Embora MNP metálicas de Fe, Co e bimetálicas de FeCo e FePt possuam altos valores de MS, sua baixa estabilidade química dificulta aplicações em escala nanométrica. Neste trabalho foram sintetizadas NPM de Fe, Co, FeCo e FePt com alta estabilidade química e rigoroso controle morfológico. NPM de óxido metálicos (Fe e Co) também foram obtidas. Dois métodos de síntese foram empregados. Usando método baseado em sistemas nanoheterogêneos (sistemas micelares ou de microemulsão inversa), foram sintetizadas NPM de Fe3O4 e Co metálico. Foram empregados surfactantes cátion-substituídos: dodecil sulfato de ferro(III) (FeDS) e dodecil sulfato de cobalto(II) (CoDS). Para a síntese das NPM, foram estudados e determinados a concentração micelar crítica do FeDS em 1-octanol (cmc = 0,90 mmol L-1) e o diagrama de fases pseudoternário para o sistema n-heptano/CoDS/n-butanol/H2O. NPM esferoidais de magnetita com3,4 nm de diâmetro e comportamento quase-paramagnético foram obtidas usando sistemas micelares de FeDS em 1-octanol. Já as NPM de Co obtidas via microemulsão inversa, apesar da larga distribuição de tamanho e baixa MS, são quimicamente estáveis e superparamagnéticas. O segundo método é baseado na decomposição térmica de complexos metálicos, pelo qual foram preparadas NPM esféricas de FePt e de óxidos metálicos (Fe3O4, FeXO1-X, (Co,Fe)XO1-X e CoFe2O4) com morfologia controlada e estabilidade química. O método não mostrou a mesma efetividade na síntese de NPM de FeAg e FeCo: a liga FeAg não foi obtida enquanto que NPM de FeCo com estabilidade química foram obtidas sem controle morfológico. NPM de Fe e FeCo foram preparadas a partir da redução térmica de NPM de Fe3O4 e CoFe2O4, as quais foram previamente recobertas com sílica. A sílica previne a sinterização inter-partículas, além de proporcionar caráter hidrofílico e biocompatibilidade ao material. As amostras reduzidas apresentaram aumento dos valores de MS (entre 21,3 e 163,9%), o qual é diretamente proporcional às dimensões das NPM. O recobrimento com sílica foi realizado via hidrólise de tetraetilortosilicato (TEOS) em sistema de microemulsão inversa. A espessura da camada de sílica foi controlada variando-se o tempo de reação e as concentrações de TEOS e de NPM, sendo então proposto um mecanismo do processo de recobrimento. Algumas amostras receberam um recobrimento adicional de TiO2 na fase anatase, para o qual foi empregado etilenoglicol como solvente e ligante para formação de glicolato de Ti como precursor. A espessura da camada de TiO2 (2-12 nm) é controlada variando as quantidades relativas entre NPM e o precursor de Ti. Ensaios de hipertermia magnética foram realizados para as amostras recobertas com sílica. Ensaios de hipertermia magnéticas mostram grande aumento da taxa de aquecimento das amostras após a redução térmica, mesmo para dispersões diluídas de NPM (0,6 a 4,5 mg mL-1). Taxas de aquecimento entre 0,3 e 3,0oC min-1 e SAR entre 37,2 e 96,3 W g-1. foram obtidos. A atividade fotocatalítica das amostras recobertas foram próximas à da fase anatase pura, com a vantagem de possuir um núcleo magnético que permite a recuperação do catalisador pela simples aplicação de campos magnéticos externos. Os resultados preliminares dos ensaios de hipertermia magnética e fotocatálise indicam um forte potencial dos materiais aqui relatados para aplicações em biomedicina e em fotocatálise. / The most diverse technological applications of magnetic nanoparticles (MNP) have intensifiedthe interest for materials with different magnetic properties such as enhanced saturationmagnetization (MS) and superparamagnetic behavior. Despite the high MS values of metalparticles of Fe, Co, FeCo and FePt, their low chemical stability hinders most applications at thenanoscale. This thesis reports the synthesis of metallic Fe and Co and bimetallic FeCo and FePtMNP with high chemical stability and strict morphological control. MNP of iron oxide and mixediron-cobalt oxide were also synthesized. Two methods were employed. The first method, basedon nanoheterogeneous systems (micellar or reverse microemulsion systems), was used toprepare magnetite and metallic Co NPM. The method applies cation-substituted surfactants:iron(III) dodecyl sulfate iron (FeDS) and cobalt(II) dodecyl sulfate (CoDS). Before the MNPsyntheses, it were studied e determined the critical micelle concentration of FeDS in 1-octanol(cmc = 0.90 mmol L-1) and the pseudo-ternary phase diagram of n-heptane/CoDS/nbutanol/H2O. Spheroidal MNP of magnetite with 3.4 nm in diameter and quasi-paramagneticbehavior were prepared in octanolic FeDS micellar systems. Despite their broad sizedistribution and low MS, metallic Co MNP were produced in reverse microemulsions withchemical stability and superparamagnetic behavior. The second synthesis method, based onthermal decomposition of metal complexes, was employed to prepare spherical FePt and metaloxides (Fe3O4, FeXO1-X, (Co, Fe)XO1-X and CoFe2O4) MNP. Strict morphological control and highchemical stability were reached. Such method does not show the same effectiveness tosynthesize FeAg and FeCo MNP: the FeAg bimetallic alloy was not obtained while FeCo MNPwith chemical stability and compositional control were prepared with no morphological control.Fe and FeCo MNP were produced by thermal reduction of silica-coated Fe3O4 and CoFe2O4 MPN. The coating, beyond to prevent inter-particle sintering, provides biocompatibility andhydrophilic character. The reduced samples showed a significant increase in MS values(between 21.3 and 163.9%), which is directly proportional to MNP size. The silica coating wasaccomplished by tetraethylorthosilicate (TEOS) hydrolysis in reverse microemulsions. Thethickness of the silica layer is controlled by varying the reaction time and concentration of TEOSand NPM. The observations during coating process allowed to propose its probable mechanism.An additional coating of TiO2 (anatase phase) was performed onto silica layer for somesamples. Anatase coating was achieved by using ethylene glycol as both solvent and ligand toproduce an intermediate complex Ti precursor. The variation of the relative amounts of NPMand the Ti precursor allows to control the thickness of the anatase layer between 2 and 12 nm. Assays of magnetic hyperthermia were performed for silica-coated samples. The heating rate of the reduced samples increases after thermal reduction, even for dilute MNP dispersions (0.6 to4.5 mg mL-1). Heating rates between 0.3 and 3.0o C min-1 and SAR in the range of 37.2 96.3 Wg-1 were obtained. The photocatalytic activities of pure anatase particles and TiO2 -coated MNPwere close, but the magnetic samples has the advantage of being recovered from reactionmedia by applying the external magnetic fields. The preliminary results of magnetichyperthermia and photocatalysis assays indicate such materials have strong potential forapplications in biomedicine and photocatalysis.

Orientador: Flávio César Guimarães Gandra / Dissertação (mestrado) - Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin / Made available in DSpace on 2018-08-19T11:06:30Z (GMT). No. of bitstreams: 1 Monteiro_JoseCarlosBotelho_M.pdf: 5466679 bytes, checksum: 3148a9c0487d05fa44922d063e525114 (MD5) Previous issue date: 2011 / Resumo: Neste trabalho apresentamos os resultados das medidas de magnetização e calorimetria em policristais da série RZn (R= Tb, Gd, Er e Ho). Através da análise das curvas de magnetização em função da temperatura, obtidas em campos de até 5 T, avaliamos e obtemos o efeito magnetocalórico (EMC) para os compostos da série, expresso através da variação isotérmica da entropia. O composto GdZn é o mais simples da série sendo o único que não apresenta efeitos inerentes à anisotropia magnética. Pelas medidas de magnetização observamos uma transição de ordenamento magnético em 260 K. Para este composto utilizamos um hamiltoniano simples, considerando apenas as contribuições devido à interação de troca e ao efeito Zeeman para simular curvas de calor específico e magnetização. Com os dados obtidos observamos uma variação de entropia máxima de 3,49 mJ/gK para um campo de 5 T em torno de Tc. O ErZn apresenta transição ferromagnética em 18 K e uma queda na magnetização em temperaturas abaixo de Tc, que é resultado de uma transição de reorientação de spin (TRS) induzida por campo. Essa transição é um efeito da anisotropia do sistema e é observada apenas em curvas obtidas em baixos campos magnéticos. Para simular as curvas de magnetização do ErZn e dos demais compostos da série adicionamos ao hamiltoniano utilizado a contribuição devido ao campo cristalino. Ao avaliarmos o EMC do ErZn vemos que existe uma pequena anomalia, resultado da TRS, em torno de 11K para variações em até 2 T de campo. Em campos maiores a anomalia desaparece e obtemos um ?S de até 14,83 mJ/gK em campos de 5 T. Os compostos TbZn e HoZn apresentam transições ferromagnéticas em 195 e 66 K, respectivamente, e ambos apresentam transições de reorientação de spin em temperaturas abaixo de Tc. Diferentemente do ErZn, porém, nesses compostos as TRS não são induzidas por campo, sendo resultado apenas da anisotropia do sistema, mostrando efeitos muito mais pronunciados nas curvas de magnetização e calor específico. Ao calcularmos o EMC desses compostos, observamos dois picos pronunciados relativos à mudança da entropia no material, um devido ao ordenamento magnético em Tc e outro devido à reorientação de spin no material. Essa característica faz com que o EMC nesses compostos tenha uma área de atuação muito maior do que em materiais que só apresentam um ?Smax em Tc, tornando materiais desse tipo fortes candidatos à refrigeração magnética / Abstract: This work presents the results of calorimetric and magnetization measurements on polycrystalline RZn series (R = Tb, Gd, Er and Ho). By analyzing the curves of magnetization as a function of temperature, obtained under fields up to 5 T (6 T for TbZn), we obtain and evaluate the magnetocaloric effect (MCE) for compounds of the series, expressed by the isothermal entropy change. The GdZn compound is the simplest of the series being the only one that has no inherent magnetic anisotropy effects. Through magnetization measurements we observe a magnetic ordering transition at 260 K. For this compound we use a simple Hamiltonian, considering only the contributions due to exchange interaction and the Zeeman Effect to simulate curves of specific heat and magnetization. With the data obtained, GdZn presented a maximum entropy change of 3.49 mJ/gK for a magnetic field of 5 T around Tc. The ErZn presents a ferromagnetic transition at 18 K and a drop in magnetization at temperatures below Tc, which is the result of a spin reorientation transition (SRT) induced by magnetic field. This transition is an effect of the system¿s anisotropy and is observed only in curves at low magnetic fields. To simulate the magnetization curves of ErZn and the other compounds of the series we added to the Hamiltonian the contribution due to the crystalline field. In evaluating the MCE of ErZn we find that there is a small anomaly, the result of SRT, around 11K for field variations up to 2 T. In larger fields the anomaly disappears and we get ?S up to 14.83 mJ / gK at fields of 5 T. The compounds HoZn and TbZn have ferromagnetic transitions at 195 and 66 K, respectively, and both have spin reorientation transitions at temperatures below Tc. Unlike the ErZn compound, however, those SRT are not field-induced, being the sole result of anisotropy of the system and showing effects much more pronounced in the curves of magnetization and specific heat. In calculating the EMC of these compounds, we observe two pronounced peaks on the entropy change in the material, one due to a magnetic ordering at Tc and the other due to spin reorientation in the material. This feature shows that the MCE in these compounds act in a much wider range than the usual materials that shows a peak only in Tc, making them strong candidates for magnetic refrigeration / Mestrado / Física da Matéria Condensada / Mestre em Física

The present work addresses in-depth magnetic films with magnonic surface patterning of variable size. Two different kinds of such structures referred to as surface-modulated magnonic crystals were investigated: Ion-irradiated magnonic crystals and structurally etched magnonic crystals. To achieve that, two different experimental approaches were pursued. On the one hand, the magnetic moment at the surface of lithographically patterned permalloy (Ni80Fe20) films was periodically reduced by means of ion irradiation. On the other hand, structural trenches were introduced at the surface of a pre-patterned thin film by sequential ion milling. The goal is the acquisition of a fundamental understanding of the behavior of spin-wave modes in the transition from a continuous magnetic thin film to a full magnonic crystal, i.e. separated periodic magnetic structures. In the framework of this thesis, the spin-wave eigen-modes of such magnonic crystals were mainly investigated spectroscopically by means of ferromagnetic resonance. Thereby, the “Two-magnon scattering perturbation theory” and the “plane-wave method” were employed as the theoretical methodologies to understand the complex dynamics of such systems. The first is a reliable method to calculate the dynamic response of surface-modulated magnonic crystals where the modulation is of a perturbation character, i.e. small compared to the film thickness. The latter is a quasi-analytical approach to calculate the dynamic eigen-modes of magnonic crystals consisting of different components with significantly varying properties. Moreover, numerical methods were employed to get further insight into the spin dynamics of these structures. In such systems, the spin-wave behavior follows the well-known dispersion relation of flat magnetic thin films as long as the surface-modulation is small compared to the film thickness. In this work, it was shown that this circumstance can be exploited for a parameter-free determination of the exchange constant A, which is not experimentally accessible for magnetic thin films in a straightforward manner. However, once the modulation height is of significant magnitude, the dynamics of surface-modulated magnonic crystals become substantially more complex. A straightforward understanding of such kind of system is hampered by the complex interplay of different effects. On the one hand, the internal demagnetizing field reveals an alternating character and depends itself on the modulation height and the field angle. On the other hand, the dynamic eigen-modes are hybridized, i.e., they reveal different characteristics in different regions of the magnonic crystal and, in addition, they couple to each other. Here, the approach is particularly favorable to investigate the spin dynamics of surface-modulated magnonic crystals by systematically altering the modulation height of the same sample. This is mainly due to two reasons. First, the two edge cases, namely the thin film and the full magnonic crystal, are already well understood and, second, other magnetic and structural parameters remain constant. With the help of the measurement results and the simulations, the quasi-analytical theory was validated. Subsequently, the mode profiles were calculated by theory and simulation in order to analyze the mode character in the transition from a thin film to a full magnonic crystal. Two kinds of dynamic eigen-modes were identified, namely hybridized modes and localized modes. For both types, simple formulae were derived describing their characteristic dynamic behavior. Besides, transition rules were found connecting the mode number n of film modes with the mode number m of modes in the full magnonic crystal. In order to correlate the symmetry and magnitude of the demagnetizing field with the spin-wave eigen-modes, the internal fields of a strongly surface-modulated magnonic crystal were reconstructed by electron holography measurements. By reemploying the measurement results for micromagnetic simulations, the dynamics of the whole system could be reproduced. This strategy allowed for a better understanding of the link between the demagnetizing field and the spin-wave mode characteristics. Based on these results, a simplified model for the analytical description of the inplane angular dependence was found. The acquired understanding of such systems led to the elaboration of specific applications, such as the spin-wave channelization. It should be noted that the coupling of uniform to non-uniform spin-wave phenomena, which is an intrinsic property of these structures, holds out the prospect of several applications in the future.

This work presents a detailed investigation of magnetization dynamics in synthetic antiferromagnets (SAFs), which has been studied both experimentally, using electrically-detected ferromagnetic resonance (ED-FMR) and vector-network analyzer-based ferromagnetic resonance (VNA-FMR), and theoretically. Two modes, one with in-phase and one with 180° out-of-phase precessing magnetizations of the layers, are identified in all applied field regimes, namely, a low-field antiferromagnetically coupled regime (when magnetizations of the layers have opposite directions), a spin-flop regime at intermediate field values (when magnetizations are non-collinear) and a high-field saturation regime (when both magnetazations are collinear to each other and the external magnetic field direction). The qualitative theoretical description, found to be in good agreement with the experimental data, is given using a system of coupled Landau-Lifshitz equations. In this work, for the first time to our knowledge, it is shown that for SAFs with different magnetic moments of the individual layers, dynamic, and not static, Zeeman and interlayer exchange coupling energies are solely resposible for the frequency-field dependence in the antiferromagnetically coupled regime. The changes in the dynamical energy terms lead to the changes in the dynamical components of the precessing magnetizations. As the external magnetic field is varied, the amplitude of the components vary continiously in different ways for different modes, dropping to zero in the spin-flop regime, which is reflected in the amplitudes of ED-FMR and VNA-FMR. This effect appears only in SAFs with different magnetic moments of the layers and is related to the different increase in the Zeeman energy of the layers as the externally applied field increases. The variation of the dynamical components leads to the modulation of an exchange of spin-angular momentum between the layers (so called spin-pumping effect).This is directly reflected in the measured linewidths for the modes in both ED-FMR and VNA-FMR. As was shown before in the literature and is also confirmed here, spin-pumping leads to a constant difference in linewidths between two modes for SAFs in the saturated case. Here, we extend the previous findings to non-saturated regimes. We show that in non-saturated states, the linewidth difference does not remain constant and varries with the external magnetic field. This linewidth difference changes can be qualitatively explained using the modulation of the dynamical magnetization components. In order to directly model the spin-pumping effects, additional terms are introduced in the coupled Landau-Lifshitz equations, related to the intrinsic damping in the magnetic layers and spin-pumping induced effects. The calculations of linewidth dependences using the extended model are not in full agreement with the experiments, suggesting that additional effects must be added to the model (for example, potential domain formations). Additionly, due to the dependence of the effect on the Zeeman energy asymmetry between the layers of the SAF, SAFs with different ratio of thicknesses are studied. Although the trends described above are common to all the samples, no significant enhancement of spin-pumping effects are observed. Modeling shows that, although the evolution of the dynamical magnetization components does depend on the magnetic moment ratio between the layers, the difference between maximum and minimum values remains almost constant and does not alter the observed linewidth-field dependence.:1 Fundamentals 1 1.1 Magnetic moment 1 1.2 Magnetic energy contributions 6 1.2.1 Zeeman energy 6 1.2.2 Demagnetization energy 7 1.2.3 Magnetic anisotropy 9 1.2.4 Direct Exchange Energy 13 1.2.5 Indirect Exchange. Interlayer Exchange Coupling Energy 15 1.3 Magnetoresistance 17 1.3.1 Ordinary Magnetoresistance 17 1.3.2 Anisotropic Magnetoresistance 20 1.3.3 Giant Magnetoresistance 22 1.4 Magnetization dynamics 25 1.4.1 Classical motivation 25 1.4.2 Quantum mechanical justification 27 1.5 Spin-currents and Spin-pumping 29 2 Experimental methods 33 2.1 Vibrating Sample Magnetometry 33 2.2 Ferromagnetic resonance 34 2.2.1 Cavity-FMR 35 2.2.2 VNA-FMR 36 2.3 Electrically detected ferromagnetic resonance 39 3 Synthetic antiferromagnets. Theoretical model 47 3.1 Static model 47 3.2 Dynamical model 54 4 Sample fabrication and characterization 58 4.1 Fabrication 58 4.2 Static characterization 62 5 Magnetization dynamics in asymmetric SAFs 68 5.1 Dynamical measurements on Py(3nm)/ Ru(0.85 nm)/Py(9 nm) 68 5.2 Theoretical explanation 71 5.3 Dynamics in SAFs with varying asymmetry of the layers 80 6 High-frequency spin-pumping in SAFs 86 6.1 Spin-pumping in magnetic trilayers 86 6.2 Spin-pumping in SAFs 88 6.3 Dependence on the asymmetry between the layers 94 7 Conclusions and outlook 99 A General description of the trilayer system without damping and spin-pumping contributions 102 A.1 Effective fields 103 A.2 Final equations 107 B Mathematica program used for the theoretical modeling 108 B.1 Matrix Elements 108 B.2 Frequency-Modes 109 B.3 Dynamical components and corresponding dynamical energies 112 B.4 Equilibrium condition 114 B.5 Dynamical Energies 118 B.6 Dynamical Trajectories 121 Bibliography 125