Made available in DSpace on 2014-12-17T14:13:28Z (GMT). No. of bitstreams: 1 AmandaKAS_partes_autorizadas_pelo_autorpdf.pdf: 421894 bytes, checksum: 15a14d2d358700ee07c4f1523c7254c8 (MD5) Previous issue date: 2008-12-16 / This work aimed to develop a suitable magnetic system for administration by the oral route. In addition to that, it was intended to review the current uses of magnetic systems and the safety related to magnetic field exposure. Methods: Coprecipitation and emulsification/crosslinking were carried out in order to synthesize magnetite particles and to coat them, respectively. Results: According to literature review, it was found that magnetic particles present several properties such as magnetophoresis in magnetic field gradient, production of a surrounding magnetic field, and heat generation in alternated magnetic field. When the human organism is exposed to magnetic fields, several interaction mechanisms come into play. However, biological tissues present low magnetic susceptibility. As a result, the effects are not so remarkable. Concerning the development of a magnetic system for oral route, uncoated magnetite particles did undergo significant dissolution at gastric pH. On the other hand, such process was inhibited in the xylan-coated particles. Conclusions: Due to their different properties, magnetic systems have been widely used in biosciences. However, the consequent increased human exposure to magnetic fields has been considered relatively safe. Concerning the experimental work, it was developed a polymer-coated magnetic system. It may be very promising for administration by the oral route for therapy and diagnostic applications as dissolution at gastric pH hardly took place / Realizar um trabalho multidisciplinar a fim de revisar os usos biom?dicos de sistemas magn?ticos, analisar os aspectos sobre a seguran?a relativa ? exposi??o de organismos vivos a campos magn?ticos e desenvolver um sistema magn?tico apropriado para administra??o por via oral. Metodologia: Inicialmente, part?culas magn?ticas foram produzidas pela coprecipita??o de sais de ferro no meio alcalino. A etapa seguinte consistiu no processo de emulsifica??o/reticula??o interfacial realizado a fim de produzir part?culas magn?ticas revestidas por xilana. Resultados: Constata-se que as part?culas magn?ticas apresentam diversas propriedades tais como mobilidade magnetofor?tica em gradiente de campo magn?tico, produ??o de um campo magn?tico capaz de influenciar a regi?o em sua volta e gera??o de calor em campo magn?tico alternado. A exposi??o a campos magn?ticos implica em diversos mecanismos de intera??o, mas os efeitos tendem a ser m?nimos em virtude da baixa susceptibilidade magn?tica dos tecidos. Quanto ao uso de part?culas de magnetita por via oral, os dados sobre a caracteriza??o das amostras e os resultados do teste de dissolu??o in vitro em pH g?strico demonstraram a viabilidade do m?todo de revestimento apresentado para proteger as part?culas de magnetita da dissolu??o g?strica. Conclus?es: Devido ?s suas diferentes propriedades, os sistemas magn?ticos t?m encontrado ampla aplicabilidade em ci?ncias biom?dicas, sendo o conseq?ente aumento da exposi??o humana a campo considerado relativamente seguro. Experimentalmente, foi desenvolvido um sistema magn?tico promissor para administra??o por via oral, que poder? encontrar aplicabilidade como marcador de motilidade intestinal, contraste para resson?ncia nuclear magn?tica ou para a vetoriza??o de f?rmacos

Cette thèse porte sur l'utilisation de plusieurs techniques de diffusion de neutrons polarisés pour la conduite d'expériences de diffraction et de spectroscopie inélastique à haute résolution. Nous décrivons de façon exhaustive l'option à écho de spin neutronique résonant ZETA, installée sur le spectromètre triple axe thermique CRG IN22 à l'Institut Laue Langevin. Grâce à elle, nous étudions la structure nucléaire et la dynamique de spin de plusieurs systèmes modèles. Dans un premier temps, nous nous intéressons à la série BaM2(XO4)2 (M = Co, Ni; X = As, P) dont les membres sont de bons exemples de systèmes magnétiques quasi-bidimensionnels. L'effet de la mise en ordre magnétique sur leurs paramètres de maille est révélé par diffraction de Larmor. De plus, nous montrons que l'évolution thermique de la durée de vie du mode de magnon optique dans BaNi2(PO4)2 est fortement affecté par la présence de défauts dans sa structure. Ensuite, nous abordons le composé à chaînes et échelles de spin 1/2 Sr14Cu24O41. Nous nous focalisons d'abord sur l'étude du pic inélastique associé au gap de spin des échelles et présentons une méthode capable de montrer de façon directe la dégénérescence de la transition concernée. Ensuite, nous évaluons sa largeur énergétique intrinsèque et observons l'effet des différentes mises en ordre de charge sur la structure cristallographique du matériau. Finalement, nous adaptons l'instrumentation disponible pour mener des expériences de réflectométrie résolues en temps, par le biais de la méthode MIEZE, sur une multicouche magnétique pouvant posséder des propriétés intéressante pour des applications en spintronique / This thesis is mainly concerned with the use of several polarized neutron scattering techniques for carrying high resolution diffraction and inelastic spectroscopy experiments. We describe exhaustively our neutron resonant spin-echo option ZETA, installed on the thermal triple-axis spectrometer CRG IN22 at Institut Laue Langevin. Through it, we study the nuclear structure and spin dynamics of several model systems. First, we are interested in the BaM2(XO4)2 (M = Co, Ni; X = As, P)-family which members are good prototypes of quasi-2D magnetic systems. The effect of magnetic ordering on lattice constants is revealed thanks to Larmor diffraction. Moreover, we show that the thermal evolution of optic magnon lifetime in BaNi2(PO4)2 is strongly affected by the presence of defects in its structure. Then, we address the spin-chain and -ladder compound Sr14Cu24O41. We first focus on the study of the inelastic peak associated with the spin gap in the ladders spectrum and introduce a method capable of showing directly the degeneracy of the associated spin transition. We also evaluate its intrinsic linewidth and observe the effect of different charge ordering process on the material crystallographic structure. Ultimately, we adapt our instrumentation to perform time-resolved reflectometry experiments on a magnetic multilayer which can possess interesting properties for spintronics applications, through the so-called MIEZE technique.

L'objectif de cette thèse est d'étudier l'effet du champ magnétique Oersted sur le mouvement induit par courant de parois de domaines magnetiques dans des nanobandes de bicouches IrPy. Nous avons optimisé la croissance épitaxiale des couches minces IrPy avec faible rugosité de surface et d'interface, peu de défauts structurels et un faible champ coercitif. Cela peut réduire le piégeage de parois et donc augmenter sa mobilité. Nanobandes polycristallins PtPy préparées par pulvérisation ont également été étudiées pour comparer les résultats avec des échantillons épitaxiés. Une première preuve directe de l'effet du champ Oersted sur la configuration magnétique de nanobandes magnétiques a été donnée par V. Uhlir et al. utilisant des mesures XMCD-PEEM résolues en temps. Ils ont observé une grande inclinaison transversale de l'aimantation du Py et CoFeB dans les nanobandes en tricouchesCoCuPy et CoCuCoFeB. Nous avons observé le changement de chiralité des parois transverses sous champ Oersted avec des impulsions de courant en utilisant la microscopie à force magnétique. Un mouvement de parois stochastique a été observé en raison du piégeage, ce qui donne lieu à une large distribution de vitesses de paroi de domaine. Déplacement de paroi opposé au flux d'électrons et transformations de paroi ont également été observés en raison de Joule chauffage. Les grains de grande taille (comparable à la largeur de bande) dans nos couches minces épitaxiales bi-cristallins par rapport aux échantillons polycristallins (~10nm) peut être la source possible du fort piégeage. Néanmoins, des vitesses de parois maximales très élevées (jusqu'à 700 et 250m/s) pour des densités de courant relativement faible (1.7x1012 et 1x1012 A/m2) ont été observées dans échantillons épitaxiales et pulvérisées respectivement. Ces vitesses sont 2 à 5 fois plus élevées avec des densités de courant similaires ou plus faible que celles observées dans des nanobandes de Py seul, rapportés dans la littérature. Le champ Oersted est peut-être à l'origine de la plus grande efficacité du couple de transfert de spin dans ces bandes en bicouche. Des simulations micromagnétiques réalisées dans notre groupe confirment qu'un champ magnétique transverse appliqué en plus d'un champ longitudinal pour déplacemer la paroi peut stabiliser le cœur d'une paroi vortex au centre de la nanobande, supprimant ainsi l'expulsion de cœur au bord de la nanobande et donc empêchant la transformation de parois vortex. De même, il peut stabiliser les parois transverses, empêchant des transformations. Cela peut conduire à une décalage du seuil de Walker vers des courants plus élevés, résultant en une augmentation de la vitesse de paroi. Des mesures XMCD-PEEM résolue en temps seront réalisées dans un avenir proche pour confirmer l'effet du champ Oersted sur le mouvement de la paroi. / The aim of this thesis is to study the effect of the magnetic Oersted field on current-induced domain wall (DW) motion in IrPy bilayer nanostripes. We optimized the epitaxial growth of IrPy films on sapphire (0001) substrates with less structural defects, small surface and interface roughness and small coercive fields. This was expected to reduce the DW pinning and hence increase the DW mobility. Polycrystalline PtPy nanostripes prepared by sputtering were also studied to compare the results with epitaxial samples. A first direct evidence of the effect of the Oersted field on the magnetic configuration of magnetic nanostripes was given by V. Uhlir et al. using time-resolved XMCD-PEEM measurements. They observed a large tilt of the Py and CoFeB magnetization in the direction transverse to the stripes in CoCuPy and CoCuCoFeB trilayer nanostripes. We observed chirality switching of transverse walls induced by the Oersted field due to current pulses using magnetic force microscopy. DW motion was found to be stochastic due to DW pinning, which results in a distribution of velocities. DW motion opposite to the electron flow and DW transformations were also observed due to Joule heating. The large grain size (comparable to the stripe width) in our epitaxial bi-crystalline films with respect to the polycrystalline samples (~10nm) may be a possible source of pinning. Nevertheless, very high maximum DW velocities (up to 700 and 250m/s) for relatively low current densities (1.7 x1012 and 1 x1012 A/m2) were observed in epitaxial and sputtered samples respectively. These velocities are 2 to 5 times higher with similar or even smaller current densities than observed in single layer Py nanostripes, reported in the literature. The Oersted field may be at the origin of the high efficiency of the spin transfer torque in these bilayer stripes. Micromagnetic simulations performed in our group confirm that when a transverse magnetic field is applied in addition to a longitudinal field along the nanostripe for VW motion, the vortex core can be stabilized in the center of nanostripe, suppressing the core expulsion at the nanostripe edge and hence preventing the VW transformation. Similarly, it can stabilize transverse walls, preventing DW transformations. This can result in a shift of the Walker breakdown to higher fields/currents, resulting in an increase in DW velocity. Time-resolved XMCD-PEEM measurements will be performed in the near future to confirm the effect of the Oersted field on the DW motion.

Consideramos os efeitos de desordem ou aperiodicidade sobre três sistemas magnéticos distintos. Inicialmente, apresentamos um modelo fenomenológico para descrever a dependência térmica da magnetização remanente induzida por diluição numa classe de antiferromagnetos quase-unidimensionais. O modelo trata exatamente as correlações ao longo da direção dominante, levando em conta as demais interações por meio de um campo efetivo. Em seguida, utilizamos uma aproximação autoconsistente de Bethe-Peierls para avaliar os efeitos de um campo cristalino aleatório sobre os diagramas de fases de um modelo de Ising de spins mistos. Mostramos que a desordem é capaz de modificar a natureza dos pontos multicríticos existentes no limite uniforme do modelo. Finalmente, estudamos os efeitos de interações aleatórias ou aperiódicas sobre o comportamento da cadeia XX quântica em baixas temperaturas, através de câlculos numéricos baseados no mapeamento do sistema em um modelo de férmions livres. Apontamos evidências de que, em temperatura zero, existe um único ponto fixo universal, característico de uma fase de singleto aleatório, que governa o comportamento do modelo na presença de interações desordenadas. No caso de interações aperiódicas,obtemos resultados consistentes com previsões de grupo de renormalização, indicando, para uma certa classe de seqüências de substituição, um comportamento semelhante àquele associado à desordem. / We consider effects of disorder or aperiodicity on three different magnetic systems. First, we present a phenomenological model to describe the thermal dependence of the dilution-induced remanent magnetization in a class of quasi-one-dimensional antiferromagnets. The model treats correlations along the dominant direction in an exact way, while including the remaining inte-. i ractions via an effective field. Then, we use a self-consistent Bethe-Peierls ~ j .. approximation to gauge the effects of a random crystal field on the phase diagram of a mixed-spin Ising mode!. We show that disorder may have profound effects on the multicritical behavior associated with the uniform limit of the mo de!. Finally, we study effects of random or aperiodic interactions on the behavior of the quantum XX chain at low temperatures, by performing numerical calculations based on a mapping of the system onto a free-fermion mo de!. . We present evidence that, at zero temperature, there exists a single, universal fixed-point, associated with a random-singlet phase, which governs the behavior of the model in the presence of disordered interactions. In the case of aperiodic interactions, our results are consistent with renormalizationgroup predictions, indicating, for a certain class of substitution sequences, a behavior similar to the one induced by disorder.

Consideramos os efeitos de desordem ou aperiodicidade sobre três sistemas magnéticos distintos. Inicialmente, apresentamos um modelo fenomenológico para descrever a dependência térmica da magnetização remanente induzida por diluição numa classe de antiferromagnetos quase-unidimensionais. O modelo trata exatamente as correlações ao longo da direção dominante, levando em conta as demais interações por meio de um campo efetivo. Em seguida, utilizamos uma aproximação autoconsistente de Bethe-Peierls para avaliar os efeitos de um campo cristalino aleatório sobre os diagramas de fases de um modelo de Ising de spins mistos. Mostramos que a desordem é capaz de modificar a natureza dos pontos multicríticos existentes no limite uniforme do modelo. Finalmente, estudamos os efeitos de interações aleatórias ou aperiódicas sobre o comportamento da cadeia XX quântica em baixas temperaturas, através de câlculos numéricos baseados no mapeamento do sistema em um modelo de férmions livres. Apontamos evidências de que, em temperatura zero, existe um único ponto fixo universal, característico de uma fase de singleto aleatório, que governa o comportamento do modelo na presença de interações desordenadas. No caso de interações aperiódicas,obtemos resultados consistentes com previsões de grupo de renormalização, indicando, para uma certa classe de seqüências de substituição, um comportamento semelhante àquele associado à desordem. / We consider effects of disorder or aperiodicity on three different magnetic systems. First, we present a phenomenological model to describe the thermal dependence of the dilution-induced remanent magnetization in a class of quasi-one-dimensional antiferromagnets. The model treats correlations along the dominant direction in an exact way, while including the remaining inte-. i ractions via an effective field. Then, we use a self-consistent Bethe-Peierls ~ j .. approximation to gauge the effects of a random crystal field on the phase diagram of a mixed-spin Ising mode!. We show that disorder may have profound effects on the multicritical behavior associated with the uniform limit of the mo de!. Finally, we study effects of random or aperiodic interactions on the behavior of the quantum XX chain at low temperatures, by performing numerical calculations based on a mapping of the system onto a free-fermion mo de!. . We present evidence that, at zero temperature, there exists a single, universal fixed-point, associated with a random-singlet phase, which governs the behavior of the model in the presence of disordered interactions. In the case of aperiodic interactions, our results are consistent with renormalizationgroup predictions, indicating, for a certain class of substitution sequences, a behavior similar to the one induced by disorder.

This thesis consists of six chapters. The first chapter gives an introduction to the field of low-dimensional magnetic and electronic systems and relevant numerical techniques. The recent developments in molecular magnets are highlighted. The numerical techniques are reviewed along with their advantages and disadvantages from the present perspective. Study of entanglement of a system can give a great insight into the system. At the last part of this chapter a general overview is given regarding entanglement, its measures and its significance in studying many-body systems. Chapter 2 deals with the technique that has been developed by us for the full symmetry adaptation of non-relativistic Hamiltonians. It is advantageous both computationally and physically/chemically to exploit both spin and spatial symmetries of a system. It has been a long-standing problem to target a state which has definite total spin and also belongs to a definite irreducible representation of a point group, particularly for non-Abelian point groups. A very general technique is discussed in this chapter which is a hybrid method based on valence-bond basis and the basis of the z-component of the total spin. This technique is not only applicable to a system with arbitrary site spins and belonging to any point group symmetry, it is also quite easy to implement computationally. To demonstrate the power of the method, it is applied to the molecular magnetic system, Cu6Fe8, with cubic symmetry. In chapter 3, the extension of the previous hybrid technique to electronic systems is discussed. The power of the method is illustrated by applying it to a model icosahedral half-filled electronic system. This model spans a huge Hilbert space (dimension 1,778,966) and is in the largest non-Abelian point group. All the eigenstates of the model are obtained using our technique. Chapter 4 deals with the thermodynamic properties of an important class of single-chain magnets (SCMs). This class of SCMs has alternate isotropic spin-1/2 units and anisotropic high spin units with the anisotropy axes being non-collinear. Here anisotropy is assumed to be large and negative, as a result, anisotropic units behave like canted spins at low temperatures; but even then simple Ising-type model does not capture the essential physics of the system due to quantum mechanical nature of the isotropic units. A transfer matrix (TM) method is developed to study statistical behavior of this class of SCMs. For the first time, it is also discussed in detail that how weak inter-chain interactions can be treated by a TM method. The finite size effect is also discussed which becomes important for low temperature dynamics. This technique is applied to a real helical chain magnet, which has been studied experimentally. In the fifth chapter a bipartite entanglement entropy of finite systems is studied using exact diagonalization techniques to examine how the entanglement changes in the presence of long-range interactions. The PariserParrPople model with long-range interactions is used for this purpose and corresponding results are com-pared with those for the Hubbard and Heisenberg models with short-range interactions. This study helps understand why the density matrix renormalization group (DMRG) technique is so successful even in the presence of long-range interactions in the PPP model. It is also investigated if the symmetry properties of a state vector have any significance in relation to its entanglement. Finally, an interesting observation is made on the entanglement profiles of different states, across the full energy spectrum, in comparison with the corresponding profile of the density of states. The entanglement can be localized between two noncomplementary parts of a many-body system by performing local measurements on the rest of the system. This localized entanglement (LE) depends on the chosen basis set of measurement (BSM). In this chapter six, an optimality condition for the LE is derived, which would be helpful in finding optimal values of the LE, besides, can also be of use in studying mixed states of a general bipartite system. A canonical way of localizing entanglement is further discussed, where the BSM is not chosen arbitrarily, rather, is fully determined by the properties of a system. The LE obtained in this way, called the localized entanglement by canonical measurement (LECM), is not only easy to calculate practically, it provides a nice way to define the entanglement length. For spin-1/2 systems, the LECM is shown to be optimal in some important cases. At the end of this chapter, some numerical results are presented for j1 −j2 spin model to demonstrate how the LECM behaves.