The doped perovskite manganite La1-xCaxMnO3 (0<x<1) has been extensively studied due to the interactions between the electronic, magnetic and crystal lattices, and the wide range of phases that can coexist. The region of greatest interest in the bulk material is around x~0.5, where there is often mesoscopic phase coexistence between a ferromagnetic metal (FM) and an antiferromagnetic insulator (AF). The first part of the dissertation describes a systematic study on a series of La1-xCaxMnO3 films deposited onto SrTiO3 (001) by pulsed laser deposition with compositions in the range 0.40<x<0.45. From electrical transport and magnetisation measurements, the limit of metallic behaviour was found to be x=0.41 whereas ferromagnetism was seen up to x=0.45. Although the transition temperatures of 150-200 K were comparable with the bulk material, the saturation moment at 20 K was about 40% of the fully spin-aligned value, which suggests the possibility of a phase separated mixture of FM and AF regions. The deviation from the bulk behaviour is thought to be due to substrate-induced strain altering the crystal symmetry and making the cubic ferromagnetic state less favourable. In the remainder of this work, the nature of phase separation in 60 nm La0.59Ca0.41MnO3 and La0.60Ca0.40MnO3 films is investigated. The effect of an external magnetic field is studied. A high-field magnetoresistance (Δρ/ρB=0) of 41% in fields of 400 mT was observed for a La0.60Ca0.40MnO3 film, which, while not as large as the values previously reported in the literature, is still significant. The magnetic history of the films was found to be very significant, with the zero-field resistivity depending on the highest field applied. The isothermal time dependence of the resistivity was found to be exponential, with a time constant in the range 100-1000 s. Possible mechanisms for the MR effect and the dependence on magnetic history are discussed.

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Complex magnetic oxides represent a unique intersection of immense technological importance and fascinating physical phenomena originating from interwoven structural, electronic and magnetic degrees of freedom. The resulting energetically close competing orders can be controllably selected through external fields. Competing interactions and disorder represent an additional opportunity to systematically manipulate the properties of pure magnetic systems, leading to frustration, glassiness, and other novel phenomena while finite sample dimension plays a similar role in systems with long-range cooperative effects or large correlation lengths. A rigorous understanding of these effects in strongly correlated oxides is key to manipulating their functionality and device performance, but remains a challenging task. In this dissertation, we examine a number of problems related to intrinsic and extrinsic low dimensionality, disorder, and competing interactions in magnetic oxides by applying a unique combination of standard magnetometry techniques and unconventional magnetocaloric effect and transverse susceptibility measurements. The influence of dimensionality and disorder on the nature and critical properties of phase transitions in manganites is illustrated in La0.7Ca0.3MnO3, in which both size reduction to the nanoscale and chemically-controlled quenched disorder are observed to induce a progressive weakening of the first-order nature of the transition, despite acting through the distinct mechanisms of surface effects and site dilution. In the second-order material La0.8Ca0.2MnO3, a strong magnetic field is found to drive the system toward its tricritical point as competition between exchange interactions in the inhomogeneous ground state is suppressed. In the presence of large phase separation stabilized by chemical disorder and long-range strain, dimensionality has a profound effect. With the systematic reduction of particle size in microscale-phase-separated (La, Pr, Ca)MnO3 we observe a disruption of the long-range glassy strains associated with the charge-ordered phase in the bulk, lowering the field and pressure threshold for charge-order melting and increasing the ferromagnetic volume fraction as particle size is decreased. The long-range charge-ordered phase becomes completely suppressed when the particle size falls below 100 nm. In contrast, low dimensionality in the geometrically frustrated pseudo-1D spin chain compound Ca3Co2O6 is intrinsic, arising from the crystal lattice. We establish a comprehensive phase diagram for this exotic system consistent with recent reports of an incommensurate ground state and identify new sub-features of the ferrimagnetic phase. When defects in the form of grain boundaries are incorporated into the system the low-temperature slow-dynamic state is weakened, and new crossover phenomena emerge in the spin relaxation behavior along with an increased distribution of relaxation times. The presence of both disorder and randomness leads to a spin-glass-like state, as observed in γFe2O3 hollow nanoparticles, where freezing of surface spins at low temperature generates an irreversible magnetization component and an associated exchange-biasing effect. Our results point to distinct dynamic behaviors on the inner and outer surfaces of the hollow structures. Overall, these studies yield new physical insights into the role of dimensionality and disorder in these complex oxide systems and highlight the sensitivity of their manifested magnetic ground states to extrinsic factors, leading in many cases to crossover behaviors where the balance between competing phases is altered, or to the emergence of entirely new magnetic phenomena.

Phase field modeling and simulation is employed to study the underlying mechanism of enhancing electromechanical properties in single crystals and polycrystals of perovskite-type ferroelectrics around the morphotropic phase boundary (MPB). The findings include: (I) Coherent phase decomposition near MPB in PZT is investigated. It reveals characteristic multidomain microstructures, where nanoscale lamellar domains of tetragonal and rhombohedral phases coexist with well-defined crystallographic orientation relationships and produce coherent diffraction effects. (II) A bridging domain mechanism for explaining the phase coexistence observed around MPBs is presented. It shows that minor domains of metastable phase spontaneously coexist with and bridge major domains of stable phase to reduce total system free energy, which explains the enhanced piezoelectric response around MPBs. (III) We demonstrate a grain size- and composition-dependent behavior of phase coexistence around the MPBs in polycrystals of ferroelectric solid solutions. It shows that grain boundaries impose internal mechanical and electric boundary conditions, which give rise to the grain size effect of phase coexistence, that is, the width of phase coexistence composition range increases with decreasing grain sizes. (IV) The domain size effect is explained by the domain wall broadening mechanism. It shows that, under electric field applied along the nonpolar axis, without domain wall motion, the domain wall broadens and serves as embryo of field-induced new phase, producing large reversible strain free from hysteresis. (V) The control mechanisms of domain configurations and sizes in crystallographically engineered ferroelectric single crystals are investigated. It reveals that highest domain wall densities are obtained with intermediate magnitude of electric field applied along non-polar axis of ferroelectric crystals. (VI) The domain-dependent internal electric field associated with the short-range ordering of charged point defects is demonstrated to stabilize engineered domain microstructure. The internal electric field strength is estimated, which is in agreement with the magnitude evaluated from available experimental data. (VII) The poling-induced piezoelectric anisotropy in untextured ferroelectric ceramics is investigated. It is found that the maximum piezoelectric response in the poled ceramics is obtained along a macroscopic nonpolar direction; and extrinsic contributions from preferred domain wall motions play a dominant role in piezoelectric anisotropy and enhancement in macroscopic nonpolar direction. (VIII) Stress effects on domain microstructure are investigated for the MPB-based ferroelectric polycrystals. It shows that stress alone cannot pole the sample, but can be utilized to reduce the strength of poling electric field. (IX) The effects of compressions on hysteresis loops and domain microstructures of MPB-based ferroelectric polycrystals are investigated. It shows that longitudinal piezoelectric coefficient can be enhanced by compressions, with the best value found when compression is about to initiate the depolarization process. / Ph. D.

Orientador: Guillermo Gerardo Cabrera Oyarzun / Dissertação (mestrado) - Universidade Estadual de Campinas, Instituto de Fisica Gleb Wataghin / Made available in DSpace on 2018-09-24T18:55:27Z (GMT). No. of bitstreams: 1 Garcia_FernandoAssis_M.pdf: 623202 bytes, checksum: ec47f534b74f1dafc10e8a0d7c031968 (MD5) Previous issue date: 2007 / Resumo: Esta dissertação tem como objetivo apresentar um estudo da simetria do parâmetro de ordem em supercondutores ferromagnéticos. Nossa abordagem é inspirada na teoria de Landau para Transições de Fase de Segunda Ordem ou, de maneira mais precisa, na idéia que uma transição de fase de segunda ordem está acompanhada por uma redução na simetria do sistema. A nova fase passa a ser descrita por um subgrupo da fase de alta simetria, implicando consequências para o parâmetro de ordem, que em nosso caso determina a estrutura do gap supercondutor. A recente descoberta da coexistência de supercondutividade e ferromagnetismo revelou o problema da classificação das possíveis simetrias do parâmetro de ordem supercondutor quando o estado normal não possui simetria de reversão temporal. Veremos que o problema é resolvido quando a simetria do estado normal é descrita por grupos magnéticos ( ou co-grupos) e que a classificação dos estados supercondutores deve agora ser feita em termos das co-representações destes grupos / Abstract: In this dissertation, we present a study of the order-parameter symmetry in ferromagnetic superconductors. Our approach is inspired on the Landau Theory of Phase Trasition or, more precisely, on the idea that a second order phase transition is a symmetry breaking process where the ordered phase of the system is described by a subgroup of the highly symmetric one, leading to important consequences for the order parameter. In our case, it imposes constraints to the superconducting gap structure. The recent discovery of the coexistence of superconductivity and ferromagnetism brought the problem of the classification of such structures in the situation where time reversal symmetry is broken on the normal state. We argue that this problem is solved when one consider the description of such normal state by magnetic groups (or cogroups) and that the classification of the superconducting states must be done in terms of the corepresentations of such cogroups / Mestrado / Física da Matéria Condensada / Mestre em Física

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Cette étude expérimentale est consacrée à la structure cristalline et aux propriétés magnétiques des phases orthorhombiques ANb2O6 (A = métaux magnétiques) qui ont retenues notre attention en tant que système Ising modèle quasi 1D. Ce comportement magnétique original de basse dimension résulte à la fois de la force des interactions magnétiques le long des chaînes d'atomes magnétiques quasi-unidimensionnelles, et à la faiblesse des interactions entre les chaînes qui sont de nature antiferromagnétique. Lorsque ces composés sont ordonnés l'ensemble de ces interactions inter et intra chaîne conduit à un ordre antiferromagnétique. Notre investigation s'appuie sur une caractérisation systématique de la série de composés AxA'1-xNb2O6 (A et A' = Ni, Fe et Co), par des mesures variées et complémentaires, notamment: diffraction des rayons X à température ambiante, diffraction de neutrons au dessus et en dessous de la température d'ordre magnétique, mesures magnétiques : évolution thermique de courbes d'aimantation isochamp et mesures d'aimantation isotherme. De plus, des mesures de la chaleur spécifique et de spectroscopie Mössbauer ont été réalisées sur certains échantillons sélectionnés. Nous avons mis à jour, selon la concentration, des comportement très différents dans les systèmes pseudo binaires Fe-Co, Ni-Fe ou Co-Ni qui peuvent soit présenter un état ordonné soit conserver un état paramagnétique jusqu'à de très basses températures. Nos mesures démontrent que la température d'ordre magnétique et les vecteurs de propagations diffèrent sensiblement selon la composition car ces systèmes sont caractérisés par une compétition entre les interactions magnétiques mises en jeu dans un réseau triangulaire interchaines. Cette étude montre que le désordre cationique Fe/Co induit une réduction substantielle des interactions tant inter que intra chaînes, ce qui traduit la tendance à défavoriser l'établissement d'un ordre magnétique à longue portée. De manière similaire, le système NixFe1-xNb2O6 ne présente pas d'ordre magnétique pour x=0,2 et ceci jusqu'à 400 mK au moins. / This work is dedicated to the investigation of structural and magnetic properties of these compounds with orthorhombic structure (A = magnetic metals) ANb2O6 that caught our attention as a system of quasi-1D Ising. This unique magnetic behavior is the result of low-dimensional magnetic interaction along the chains of magnetic atoms almost uni-dimensional, and also by weak antiferromagnetic interactions between the chains. When these compounds are ordered all these interactions between and within the chain leads to a global antiferromagnetic order. Our research is based on a systematic characterization of the series of compounds AxA'1-xNb2O6 (A et A' = Ni, Fe and Co) by differents types of complementary measures, such as X-ray diffraction at room temperature, neutron diffraction above and below the magnetic ordering temperature, magnetic measurements: thermal evolution of magnetization curves and isotherm magnetization variation in applied field. In addition, specific heat measurements and Mössbauer spectroscopy were performed on some selected samples. We found interesting results depending on the concentration, different behaviors on these pseudo binary systems Ni-Fe, Fe-Co, or Co-Ni, which can remain in the paramagnetic state up to very low temperatures or to order depending on the series analyzed. Our measurements show that the magnetic ordering temperature and propagation vectors differ substantially depending on the composition, for these systems are characterized by a competition between magnetic interactions that are involved in a triangular lattice intermolecular. This study shows that disorder cationic Fe / Co induced a substantial reduction in both the interactions within and between them; chains, reflecting the tendency to oppose the creation of a long-range magnetic order. Likewise, the system NixFe1-xNb2O6 dont shows magnetic ordering even at measures taken up to 400 mK for x = 0.2.

Ce travail concerne l’altération du comportement de phase de membranes lipidiques lors de leur interaction avec des molécules hydrophiles ou hydrophobes. L’utilisation de sondes moléculaires de fluorescence sensibles à leur micro-environnement constitue un aspect majeur de ce travail. Les techniques de spectroscopie de fluorescence et de microscopie confocale ont été mises à profit pour l’étude du comportement de ces sondes, donnant accès au degré de compacité et d’ordre dans les membranes.Nos résultats montrent que le polystyrène, un plastique rencontré de façon commune dans les régions polluées des océans, présente la capacité de modifier le comportement de phase des membranes lipidiques, entrant notamment en compétition avec le cholestérol.Nous avons montré que la présence élevée de sucres, tel que l’on peut le rencontrer dans certaines situations relevant de la bio-préservation, a pour effet de rompre la qualité de compaction des lipides, et nous avons proposé un nouveau modèle thermodynamique pour interpréter nos résultats.Enfin, les effets sur la membrane de l’incorporation d’un polymère amphiphile comportant un cholestérol greffé ont été étudiés, dans le cadre de l’élaboration de nouvelles stratégies thérapeutiques à base de lipides. / This work focuses on the alterations of lipid membrane phase behavior upon interaction with hydrophobic and hydophilic molecules. One major aspect of this thesis is the employement of environment sensitive probes to obtain information on the lipid bilayer packing by means of confocal spectral imaging and fluorescence spectroscopy. Our results show that polystyrene, a commonly found plastic in ocean wastes, has the ability to disrupt the lipid bilayer phase behavior and has a competitive interaction with cholesterol. The presence of high concentration of sugars, relevant in the field of biopreservation, has been found to alter the lipid bilayer packing and a new thermodynamics model has been proposed to complement the experimental results. Finally, the effects of an amphiphilic cholesterol-grafted polymer on model membrane was investigated, providing insight into potential new lipid therapeutic strategies.

Výměnná anizotropie je zajímavý fyzikální jev vznikající na rozhraní antiferomagnetických (AF) a feromagnetických (FM) materiálů, který již je široce používán v elektronickém průmyslu a magnetickém záznamu. Přestože byl tento jev dlouhou dobu intenzivně studován, jeho přesný mechanizmus zatím nebyl uspokojivě vysvětlen. V této práci je představen přehled studií dokumentujících výměnnou anizotropii v tenkých dvojvrstvách, včetně experimentálních výsledků a teoretických modelů. Experimentální úkoly této diplomové práce zahrnovaly jak výrobu, tak měření různých modelových systémů vykazujících výměnnou anizotropii. Dvojvrstva Fe/FeRh, kde vrstva FeRh prochází fázovou přeměnou z AF fáze na FM fázi při 360 K, poskytuje možnost nastavení parametrů výměnné anizotropie. Dále byly zkoumány účinky výměnné anizotropie a tvarové anizotropie v mikrostrukturách Fe/FeRh. Konečně, přítomnost výměnné anizotropie byla zkoumána mezi FM a AF fází koexistujícími během fázové přeměny v nanodrátech FeRh. Vzorky byly vyrobeny pomocí magnetronového naprašování a elektronové litografie. Všechny prezentované systémy byly analyzovány pomocí magnetooptické Kerrovy mikroskopie. Výměnná anizotropie byla úspěšně nalezena v systému Fe/FeRh, přičemž její velikost byla téměř identická co do rozsahu i orientace s výsledky v literatuře, přestože námi vyrobená dvojvrstva měla horší kvalitu FM-AF rozhraní. Bylo také prokázáno, že v tomto systému existuje tzv. tréninkový efekt (Training effect), což je výrazným důkazem existence výměnné anizotropie. U nanodrátů bylo změřena významná výměnná anizotropie mezi koexistujícími fázemi FM a AF během fázové přeměny.

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