No description available.

The magnetocaloric effect (MCE) is the temperature change in a magnetic material due to a change in an applied magnetic field. How the MCE behaves in different magnetic materials and at different phase transitions is fundamental to understand. The driver of the MCE is a change in entropy which has multiple contributions: magnetic, lattice, and electron. In this thesis the MCE is studied in a simple antiferromagnetic (AFM) model andin a realistic noncollinear spin glass Neodymium model using Monte Carlo and Atomistic Spin Dynamics simulations. For the simple AFM system, no clear results were achieved, indicating that MCE in AFM materials is not due to a change solely in the magnetic entropy. For the complex magnetic material Nd, a more clear result is seen, indicating that frustration in the system might be important to the MCE in noncollinear materials. Nd results also signify more phase transitions than previously reported.

This paper discusses the search of an FeNi25-based alloy with a face-centered cubic crystal structure exhibiting a Curie point around room temperature, for magnetocaloric applications. Fe was substituted in various amounts with FCC-stabilising elements Mn and Co as these elements respectively decrease and increase the Curie Temperature, thus enabling to tune the Curie point. Three characterization methods were carried out on the samples: Magneto- thermo-gravimetry (MTG), X-ray diffraction (XRD) and finally, vibrating sample magnetometer (VSM) measurements were performed. All samples displayed several Curie points, each corresponding to various FCC phases. Also, the last sample, FeNi25Mn6Co2, had an FCC phase fraction of almost 99% and presented two Curie points in the continuity of one another one at -35°C and another at 91°C. Hence, at room temperature, the sample underwent a magnetic phase transition passing from its ferromagnetic state to a paramagnetic one. / Detta arbete består i att utröna möjligheterna att med utgångspunkt från den binära sammansättningen FeNi25 erhålla en ytcentrerad kubisk fas (fcc) med en Curie punkt vid rumstemperatur. Syftet är att använda dessa legeringar i magnetokaloriska tillämpningar. Strategin är att både Mn och Co är fcc stabliliserande grundämnen, och att Mn sänker och Co ökar Curie temperaturen. Tre olika karakteriseringsmetoder användes; röntgendiffraktometri (struktur), Magneto-Termo-Gravimetri (magnetisering vs temperatur) och konventionell magnetometri vid rumstemperatur (magnetisering vs magnetiskt fält, Vibrating Sample Magnetometry VSM). Resultaten visar att även om kristallstrukturen i det närmaste är fullständigt fcc, så ger de magnetiska mätningarna vid handen att flera olika faser är vid handen med avesvärt olika Curie temperaturer. Som en illustration av detta förhållande kan nämnas att sammansättningen FeNi25Mn6Co2 uppvisar en fcc-fraktion på i det närmaste 99%, men har vid en M(T) mätning ett förlopp som enklast förklaras med en Curie punkt vid ca -35C och en ytterligare vid ca 90°C. Denna observation signalerar att de magnetiska egenskaperna torde vara mer beroende av exakt distribution av de ingående atomslagen i fcc strukturen än vad de röntgendiffraktometriska undersökningarna kan detektera.

No description available.

The search for novel quantum states is a fundamental theme in condensed matter physics. The almost boundless number of possible materials and complexity of the theory of electrons in solids make this both an experimentally and theoretically exciting and challenging research field. Particularly, the concept of quantum criticality resulted in a range of discoveries of novel quantum phases, which can become thermodynamically stable in the vicinity of a second order phase transition at zero temperature due to the existence of quantum critical fluctuations. One of the materials in which a novel quantum phase is believed to form close to a proposed quantum critical point is Sr₃Ru₂O₇. In this quasi-two-dimensional metal, the critical end point of a line of metamagnetic first order phase transitions can be suppressed towards zero temperature, theoretically leading to a quantum critical end point. Before reaching absolute zero, one experimentally observes the formation of an anomalous phase region, which has unusual ‘nematic-like’ transport properties. In this thesis magnetocaloric effect and specific heat measurements are used to systematically study the entropy of Sr₃Ru₂O₇ as a function of both magnetic field and temperature. It is shown that the boundaries of the anomalous phase region are consistent with true thermodynamic equilibrium phase transitions, separating the novel quantum phase from the surrounding ‘normal’ states. The anomalous phase is found to have a higher entropy than the low and high field states as well as a temperature dependence of the specific heat which deviates from standard Fermi liquid predictions. Furthermore, it is shown that the entropy in the surrounding ‘normal’ states increases significantly towards the metamagnetic region. In combination with data from other experiments it is concluded that these changes in entropy are most likely caused by many body effects related to the underlying quantum phase transition.

La première partie des travaux réalisés a été dédiée à l' élaboration de composés LaFe13-xSix (1,3 ¡U x ¡U 2,2) par broyage à haute énergie. Il a fallu déterminer les conditions de synthèse et de recuit optimales pour l'obtention d'échantillons monophasés. Leur homogénéité a été analysée par diffraction des rayons X et microsonde électronique. Les résultats ont montré qu'une microstructure plus fine favorise la formation de la phase désirée : un recuit de 30 min (au lieu de 30 jours pour les massifs) à 1373K suffit à l'obtention d'un composé quasi-monophasé. D'après les mesures magnétiques effectuées, les composés synthétisés par broyage mécanique ont des proprié¦tés magnétiques et magnétocaloriques similaires aux massifs. Ils présentent une transition métamagnétique des électrons itinérants induite par le champ ou la température. Leur température de Curie augmente avec le Si, variant de 200K à 235K pour x = 1,4 à 2,0 alors que leur variation d'entropie magnétique diminue de 20 J/kg K à 4 J/kg K sous une variation de champ de 0-2 T. La deuxième partie de l'étude a consisté à améliorer les propriétés magnétocaloriques des intermétalliques par l'insertion d'atomes interstitiels (H, C). Les mesures magnétiques ont montré une nette augmentation de la température de transition (jusqu'à Tamb.) par effet magnétovolumique tout en conservant un effet magnétocalorique important. Les analyses par diffraction des neutrons en température effectuées sur les composés deutérés ont permis de suivre l'évolution des données cristallographiques et des moments magnétiques par Fe. Il ressort de cette étude que ces composés présentent un grand intérêt dans la recherche de futurs matériaux magnétocaloriques pour la réfrigération magnétique à température ambiante. Dans le cadre de l'exploration de nouveaux systèmes, les propriétés magnétocaloriques des composés Y1-xRxFe2D4,2 (R = Er, Tb) ont également été étudiés en couplant les études magnétiques avec des mesures de diffraction des neutrons / The first part of this work was devoted to the elaboration of the LaFe13-xSix (1.3 ¡Ü x ¡Ü 2.2) alloys by high energy ball-milling. The synthesis and annealing conditions were defined in order to obtain single phase samples. Their homogeneity was checked by X ray diffraction and electron microprobe analysis. The results show that a finer microstructure is convenient for the formation of the NaZn13 phase and that only a 30 minutes heat treatment at 1373K is sufficient to obtain almost single phase LaFe13-xSix compounds. This means that this way of synthesis is cost-effective, and interesting for industrial production. According to the magnetic measurements, the annealed ball-milled compounds show similar magnetic and magnetocaloric properties than the bulk ones. They exhibit an itinerant electron metamagnetic transition induced by a magnetic field or a temperature change. Their Curie temperatures increase with the Si content from 200K to 235K wh en x = 1.4 and 2.0 respectively, while their magnetic entropy variation decreases from 20 J/kg K to 4 J/kg K under a magnetic field change of 0-2 T. The second part of this study consisted to improve the magnetocaloric properties of the intermetallic compounds by the insertion of light elements (H and C). According to the literature, the magnetic measurements show a clear increase of the transition temperature until room temperature in both cases. Moreover, the giant magnetocaloric effect is maintained. The evolutions of the crystallographic data and the magnetic moment by Fe atom were analyzed by neutron powder diffraction in temperature. This work brings out how interesting are those compounds for their application in room temperature magnetic refrigeration devices. In the framework of new magnetocaloric systems investigation, the magnetic and magnetocaloric properties of the Y1-xRxFe2D4,2 (R = Er, Tb) compounds were studied. Neutron powder diffraction measurements were pe rformed in complement to magnetic measurements

Submitted by Biblioteca do Instituto de Física (bif@ndc.uff.br) on 2017-07-06T19:18:30Z No. of bitstreams: 1 mestrado.pdf: 10513746 bytes, checksum: a7e2f977b739ba0ba5022409d941a8f0 (MD5) / Made available in DSpace on 2017-07-06T19:18:30Z (GMT). No. of bitstreams: 1 mestrado.pdf: 10513746 bytes, checksum: a7e2f977b739ba0ba5022409d941a8f0 (MD5) / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Conselho Nacional de Desenvolvimento Científico e Tecnológico / Fundação de Amparo à Pesquisa do Estado do Rio de Janeiro / Em 1881 E. Warburg observou o efeito causado ao aplicar um campo magnético externo em uma amostra de ferro (Fe), observando que a temperatura do material se altera devido à aplicação do campo. Este fenômeno foi chamado, de efeito magnetocalórico (EMC) e pode ser visto desde um processo adiabático como as mudanças na temperatura do material e desde um processo isotérmico com troca de calor e variação na entropia magnética. A principal aplicação do EMC é a refrigeração magnética e tem sido estudado por vários pesquisadores em todo o mundo. Eles estão orientados ao desenvolvimento de materiais magnetocalóricos, como por exemplo, as ligas intermetálicas e as manganitas abordadas neste trabalho. O processo de fabricação das ligas intermetálicas apresenta complicações devido à forma de preparação: fusão em forno a arco voltaico. Portanto, a motivação deste trabalho de dissertação é o desenvolvimento e otimização de técnicas de sintetização de uma amostra monofásica intermetálica para futuros estudos do EMC. As amostras da família tipo RM4B (onde R = Y, La e Lu, M = Mn, Fe, Co e Ni) foram preparadas em um forno a arco, em atmosfera inerte de Argônio (Ar). Na primeira etapa de fabricação as amostras foram confeccionadas com quantidades exatas dos elementos constituintes. Uma segunda etapa de fabricação foi feita utilizando uma quantidade adicional de 3,4% de Y para sintetizar a subfamília YM4B (onde M = Fe, Co e Ni). As amostras foram tratadas termicamente durante 10 dias a 1223 e 1323 K e, mediante medidas de difração de raios X (DRX) foram caracterizadas e, estudadas levando em conta sua forma de preparação. Na segunda etapa de fabricação foi obtida uma amostra monofásica de YCo4B, na qual foram feitas as medições magnéticas de magnetização e susceptibilidade magnética. As manganitas são compostos cerâmicos com estrutura do tipo Perovskita, e sua forma de preparação já é conhecida. Neste trabalho preparamos as manganitas La0,6Sr0,4MnO3 por meio da técnica de Pechine, ou como também é chamada Sol-gel. As amostras foram calcinadas a distintas temperaturas para estudarmos a obtenção de amostras monofásicas com tamanhos de partículas (grão) com dimensões nanométricas. Para esse estudo se utilizou os resultados das medidas de difração de raios X e medidas de microscopia eletrônica de varredura (MEV), onde foi possível observar que ao aumentar a temperatura de tratamento obtínhamos maiores tamanho de partículas (grãos). / In 1881 E. Warburg measured the effect caused by applying an external magnetic field in a sample of iron (Fe), noting that the material temperature changes due to application of the field. This phenomenon has been called then magnetocaloric effect (MCE) and can be seen from an adiabatic process as changes in material temperature and an isothermal process since as a heat exchange and variation in the magnetic entropy. The main application of MCE is the magnetic refrigeration and has been studied by several investigators worldwide. They are oriented in synthesizing the development of magnetocaloric materials, such as intermetallic alloys and manganites, discussed in this work. So one of the motivations of this dissertation work is the development and optimization of techniques for synthesizing of single phase intermetallic sample for future studies of MCE. The family RM4B type samples (where R = Y, La and Lu, M = Mn, Fe, Co and Ni) were prepared in an arc melting furnace in an inert atmosphere of Argon (Ar). In the first stage of manufacturing samples were fabricated with exact amounts of the constituent elements. A second manufacturing stage was carried out using an additional amount of 3.4 % of Y to synthesize the YM4 B subfamily (where M = Fe, Co and Ni). The samples were annealed for 10 days at 1223 and 1323 K and by measurements of X-ray diffraction (XRD) were characterized and studied in form of preparation. In the second stage of manufacture was obtained one sample phase YCo4B, in which the measurements were made magnetic magnetization and magnetic susceptibility. The manganites are ceramic type perovskite compounds, their preparation is simpler than the preparation of intermetallic alloys. In this work, we synthesize the manganites La0.6Sr0.4MnO3 by Pechine technique, or as it is also called Sol-gel. The samples were calcined at different temperatures to analyze the effects of heat treatment on the crystallization and formation of particle sizes. For this study was used the results from mean X-ray diffraction measurements and scanning electron microscopy (SEM), obtaining that increasing the temperature of the treatment effect of sintering is higher, and therefore the sizes of the particles (grains) are larger.

Made available in DSpace on 2016-12-23T14:20:01Z (GMT). No. of bitstreams: 1 EMC_Heusler- parte 1.pdf: 1976712 bytes, checksum: 54cbe3c62f71ef7121b79c6f4e1efaa0 (MD5) Previous issue date: 2008-03-28 / Conselho Nacional de Desenvolvimento Científico e Tecnológico / In this work, magnetic entropy change of nonstoichiometric Ni54[Mn(1-x)Fex]19Ga27 Heusler alloys was experimentally verified by partial substitution (up to 50%) of the Mn atoms by magnetic Fe atoms. Such study was mainly concentrated in the magneto-structural transformation region, at low temperatures. The analysis of X-ray diffraction patterns indicate that the partial substitution of Mn atoms by Fe atoms causes predominance of the L21 -phase, however accompanied by spurious phases. The magnetization measurements as a function of the temperature in the low magnetic field reveals that, in all concentration range (0 x 0.5), the system presents a magnetic transition (Ferromagnetic Paramagnetic) at a temperature, TC, near the room temperature, when the material lay in the austenitic phase. Moreover, as many others Heusler alloys, the material undergoes a martensitic structural transition at low temperatures, TM. As the Fe concentration increases, the Curie temperature, TC, undergoes a little variation, increasing around 5%, while TM decreases slowly and monotonically. The magnetic entropy change, for a field of 5T, presents a maximum SM = - 9,3 J/kg.K, for x = 0.1, at a temperature of 250K, and than decreases for x 0.3, changing linearly with the maximum applied field. / Neste trabalho, verificou-se experimentalmente a variação da entropia magnética nas ligas Heusler não-estequiométricas Ni54[Mn(1-x)Fex]19Ga27, substituindo-se parcialmente (até 50%) os átomos de Mn por átomos de Fe. Tal estudo focalizou-se principalmente na região de transformação magneto-estrutural a baixas temperaturas. A análise dos difratogramas de raios-X indica que a substituição parcial de Mn por Fe nessa faixa de concentração, ocasiona uma predominância da fase- L21, porém acompanhada de outras fases espúrias. As medidas de magnetização em função da temperatura realizadas a campos baixos revelam que, em toda a faixa de concentração estudada (0 x 0,5), o sistema apresenta uma transição magnética (Ferromagnético Paramagnético) ao atingir a temperatura de Curie, TC, um pouco acima da temperatura ambiente, quando o material se encontra na fase austenítica. E, assim como muitas outras ligas Heusler, o material sofre uma transição estrutural ao ser resfriado a temperaturas inferiores à temperatura de transição martensítica, TM. À medida que se aumenta a concentração de Fe, a temperatura de Curie, TC, sofre uma pequena variação, aumentando em torno de 5%, enquanto que TM diminui lenta e monotonicamente. A variação da entropia, para um campo de 5T, apresenta um máximo SM = - 9,3 J/kg.K para x = 0,1, a uma temperatura T = 250K e, então, diminui para x 0,3, variando linearmente com o campo aplicado.

La réfrigération magnétique est une technologie émergente grâce à des avantages considérables par rapport aux technologies de réfrigération classiques. Cette technologie basée sur l’effet magnétocalorique offre d’importants avantages environnementaux car d’une part l’efficacité théorique des cycles utilisés est supérieure à celle des technologies classiques et d’autre part son fonctionnement ne nécessite pas une utilisation de gaz/vapeur `a fort effet de serre. En revanche des verrous scientifiques restent à lever, Le modèle multi-physique proposé dans cette thèse à pour but d’améliorer la précision de calcul. Il consiste à coupler un modèle 3D magnétostatique résolu par la méthode des éléments finis, un modèle magnétocalorique analytique et un modèle thermo-fluidique résolu par méthode des différences finies. Parallèlement, un banc d’essais a été conçu, optimisé et réalisé, ce banc permettra de faire des mesures fines des différents phénomènes qui interagissent dans la réfrigération magnétique. / The magnetic refrigeration technology is a promising alternative technology to the production of cold. The work of this thesis deals with studying and designing a magnetic refrigeration prototype. A multiphysic model is developed, this model taking into account several magnetic and magnetocaloric aspect that never dealt in the literature. It is used to investigate the influence of a range of parameters on the performance of the AMR. A new test bench of magnetic refrigeration is also designed, it is based on a particular electromagnet that was optimally realized. The magnetic performances are showed and concord with design prevision. Finally, suggestions for future works are provided based on the knowledge presented here.

Die magnetische Kühlung ist eine etablierte Technologie im Bereich der Tieftemperaturphysik. Allerdings bieten die Skalierbarkeit des magnetokalorischen Effektes und die Möglichkeit zur kompakten Bauweise auch ein breites Anwendungsspektrum für den Einsatz bei Raumtemperatur. Besonders hervorzuheben ist die Möglichkeit zur Anpassung der magnetostrukturellen Umwandlungstemperatur in La(Fe, Si)13-basierten Materialien an die Arbeitstemperatur einer Kühleinheit. Die Herstellung von Ausgangsmaterial über das Schmelzspinnen, ist von hoher technologischer Relevanz, da im Vergleich zu konventionell gegossenem Massivmaterial die anschließende Glühdauer drastisch reduziert werden kann [1]. In der vorliegenden Arbeit wird zunächst auf die optimalen Glühbedingungen in rasch-erstarrtem Bandmaterial für die Bildung der relevanten magnetokalorischen Phase eingegangen. Durch Variation der Glühtemperatur wird der Einfluss von Sekundärphasen auf den magnetokalorischen Effekt bewertet. Darüber hinaus können bei optimaler Wahl der Legierungszusammensetzung ein großer magnetokalorischer Effekt und der gewünschte Arbeitstemperaturbereich eingestellt werden. Besonderes Augenmerk wird auf die Verknüpfung des Substitutionseffektes (hier: Si für Fe) und der Aufweitung des Gitters durch Hydrierung mit dem resultierenden magnetokalorischen Effekt gelegt. Ein weiterer Punkt, sind die Untersuchungen zur Langzeitstabilität der Eigenschaften von hydriertem Band- und Massivmaterial. Grundlegende und umfassende Untersuchungen zur Substitution von Eisen durch Mangan und zum daraus folgenden Einfluss auf Phasenbildung, Umwandlungstemperatur sowie auf den magnetokalorischen Effekt, insbesondere nach der Hydrierung, werden ebenfalls dargestellt. Die Ergebnisse der vorliegenden Arbeit erlauben damit die Bewertung verschiedener Strategien zur Optimierung der magnetokalorischen Eigenschaften von La(Fe, Si)13.