Une sous-classe intéressante de matériaux multiferroïques est celle des composés multiferroïques magnétoélectriques, dans lesquels il existe un couplage entre les paramètres d’ordres ferroïques (magnétique et électrique). De ce point de vue, la classe des matériaux Ga₂₋ₓFeₓO₃ a attiré l’attention des chercheurs. Ces composés sont actuellement connus pour leur température de transition élevée ainsi que pour l’interaction possible entre leurs propriétés ferrimagnétiques et piézoélectriques. Leur structure cristallographique et magnétique est assez complexe, du fait du désordre de substitution interne Fe/Ga. Les oxydes M₂Ga₂Fe₂O₉ (M=In, Sc) appartiennent à cette même famille de matériaux et ont été synthétisés pour la première fois afin d’obtenir une structure cristallographique ordonnée de GaFeO₃. Afin d’étudier les propriétés physiques de ces différents composés, nous avons synthétisé par la méthode de la zone flottante (au four à image), en utilisant différentes conditions de croissance, des monocristaux de composition Ga₂₋ₓFeₓO₃ (x=0.90, 1.00 et 1.10). Nous avons également élaboré des échantillons polycristallins de composés GaFeO₃ faiblement dopés en indium ainsi que le composé M₂Ga₂Fe₂O₉ (M=In, Sc). Nous avons enfin préparé de monocristaux de composition In₂Ga₂Fe₂O₉ par la méthode de croissance en flux. L’affinement Rietveld des diffractogrammes des rayons X et des neutrons nous a permis de montrer que les céramiques de GaFeO₃ faiblement dopées en indium et les monocristaux de Ga₂₋ₓFeₓO₃ cristallisent dans le groupe d’espace Pc2₁n. Les paramètres cristallins et la température de Néel caractéristiques pour les monocristaux de Ga₂₋ₓFeₓO₃ varient de manière linéaire avec la teneur en fer. Les affinements nous ont permis de conclure que la structure de ces composés est caractérisée par un désordre élevée (25% de la quantité du fer se trouve sur les sites natifs du gallium). L’incorporation graduelle de l’indium s’accompagne d’une augmentation du volume de la maille ainsi qu’à une diminution de la température de transition magnétique. Le spectre d’excitations magnétiques mesuré pour les cristaux de Ga₂₋ₓFeₓO₃ nous a permis de mettre en évidence une coexistence de l’ordre ferrimagnétique à longue portée et d’un signal de diffusion diffuse en-dessous de la température de Néel. Ce signal diffus suggère l’existence d’une composante de type verre de spin du fait du désordre interne des sites. L'étude de la variation thermique de la constante diélectrique sur un cristal de GaFeO₃ révèle l’absence d’un couplage magnétoélectrique au sein de ces matériaux. L’affinement Rietveld des diagrammes de diffraction des rayons X et des neutrons mesurés sur les poudres de M₂Ga₂Fe₂O₉ (M=In, Sc) révèle une structure orthorhombique de type Pba2 fortement désordonnée, avec quatre sites cationiques d’occupation mixte. Les données de susceptibilité DC et AC couplées avec les mesures de chaleur spécifique et les spectres Mössbauer indiquent, en-dessous d’une température de Tg ≈ 19 K, l’existence d’un état fondamental de type verre de spin dans ce système. Les mesures du spectre d’excitations magnétiques ont mis en évidence l’absence d’ordre magnétique à longue portée et confirment l’existence d’une transition d’un état paramagnétique vers un état verre de spins. L’existence d’un comportement de type verre de spin dans les systèmes Ga₂₋ₓFeₓO₃ et M₂Ga₂Fe₂O₉ (M=In, Sc) souligne l’importance du désordre interne pour la caractérisation de l'état fondamental magnétique. / An interesting sub-class of the multiferroic materials are the multiferroic magnetoelectrics, in which exists a coupling between the two ferroic order parameters (magnetic and electric). From this viewpoint, the case of the (Ga₂₋ₓFeₓO₃)-class of materials has retained special attention. These compounds are now well-known for their high transition temperature as well as for the potential interaction between their ferrimagnetic and piezoelectric properties. Their crystallographic and magnetic structure are quite complicated, due to the existence of an internal site disorder. M₂Ga₂Fe₂O₉ (M=In, Sc) belongs to the (Ga₂₋ₓFeₓO₃)-class of materials and it was first synthesized in an attempt to obtain an ordered GaFeO₃ crystallographic structure. In order to study the physical properties of these compounds, Ga₂₋ₓFeₓO₃ (x=0.90, 1.00 and 1.10) single crystals have been synthesized by the floating zone method in an infrared image furnace, using different growth conditions. Indium doped GaFeO₃ (up to 10% indium content amount) and M₂Ga₂Fe₂O₉ (M=In, Sc) polycrystalline materials have been prepared by solid state reaction. Also, In₂Ga₂Fe₂O₉ single crystals were prepared by the flux method. The indium doped GaFeO₃ and Ga₂₋ₓFeₓO₃ samples crystallize in the Pc2₁n space group as determined from Rietveld refinement of the X-ray and neutron single crystals and powder patterns. The cell parameters and the Néel temperature (TN) of the Ga₂₋ₓFeₓO₃ single crystals varies linearly with the iron content amount. The occupation factors were calculated by refinement and the results showed a disordered structure (25% of the iron amount is found on the native gallium sites). The gradual incorporation of indium is accompanied by an increase of the cell volume and a decrease of the magnetic transition temperature. The magnetic excitations spectra measured for the Ga₂₋ₓFeₓO₃ single crystals revealed a coexistence of a ferrimagnetic ordering and a diffuse scattering signal below the Néel temperature. The diffuse signal suggests the existence of a spin glass like component due to the internal site disorder. Dielectric investigations showed no temperature dependent anomaly of the dielectric constant for the GaFeO₃ single crystal, suggesting a lack of a magnetoelectric coupling signal in this system. The Rietveld refinement of the X-ray and neutron powder patterns for the M₂Ga₂Fe₂O₉ (M=In, Sc) revealed a highly disordered orthorhombic Pba2 structure, offering four mixed cationic crystallographic sites. DC and AC susceptibility data in conjunction with the heat capacity data and Mössbauer measurements indicated a spin-glass-like behavior in this system, with a freezing temperature near Tf ≈ 19 K. The absence of an long range magnetic ordering and the existence of a transition from a paramagnetic state to a «frozen» state were showcased by the spin dynamics spectra measurements. The evidence for glassy behavior in the Ga₂₋ₓFeₓO₃ and M₂Ga₂Fe₂O₉ (M=In, Sc) systems highlights the importance of site disorder in determining the ground state magnetic properties.

Na primeira parte deste trabalho propomos uma aproximacão de campo médio dinâmico para analisar modelos de Ising com elementos e aleatoriedade definidos por distribuicões de probabilidades discretas. Analisamos o modelo com campo aleatório (S = 1/2), com interações aleatórias (S = 1/2), com diluição de sítios (S = 1/2) e com anisotropia aleatória (S = 1), obtendo  os respectivos diagramas de fases.   Na segunda parte analisamos modelos de vidros de spin (S= 3/2) com anisotropia de campo cristalino. Estudamos o modelo de van Hemmen, e o modelo clássico à la Sherrington e Kirkpatrick dentro do esquema de réplicas simétricas, obtendo os  diagramas de fases correspondentes. / In the first part of this work we propose a dynamical mean field approximation to analyse Ising models with elements of randomnss, defined by discret probability functions. We have analysed the random field model (S = 1/2); the random bond model (S = 1/2); the site diluted model (S = 3/2) and the random crystal field model (S = 1), obtaining the respective phase diagrams.   In the second part we have analysed spinglass models (S = 3/2) in the presence of a crystal field. We have studied the van Hemmen and the classic spin glass model à la Sherrington and Kirkpatrick, using replica symmetric scheme, to obtain the corresponding phase diagrams.

Le sujet principal de cette thèse est la physique des verres de spin. Les verres de spin ont été introduits au début des années 70 pour décrire alliages magnétiques diluées. Ils ont désormais été considerés pour comprendre le comportement de liquides sousrefroidis. Parmis les systèmes qui peuvent être décrits par le langage des systèmes desordonnés, on trouve les problèmes d'optimisation combinatoire. Dans la première partie de cette thèse, nous considérons les modèles de verre de spin avec intéraction de Kac pour investiguer la phase de basse température des liquides sous-refroidis. Dans les chapitres qui suivent, nous montrons comment certaines caractéristiques des modèles de verre de spin peuvent être obtenues à partir de résultats de la théorie des matrices aléatoires en connection avec la statistique des valeurs extrêmes. Dans la dernière partie de la thèse, nous considérons la connexion entre la théorie desverres de spin et la science computationnelle, et présentons un nouvel algorithme qui peut être appliqué à certains problèmes dans le domaine des finances.

The central concern of this thesis is the study of non-equilibrium behaviour in magnetic materials and its interpretation within the framework of the Preisach model of hysteresis. Comprehensive experimental characterizations of the field and temperature and time dependence of a suite of standard magnetic response functions have been performed on a variety of magnetic materials, including a naturally occurring mineral of nanodimensional titanomagnetite particles embedded in volcanic glass, a compressed powder of nanodimensional magnetite particles immobilized in an organic binder, a thin film of nanodimensional Fe particles embedded in alumina, and a series of sintered, bond-disordered CaxSr1-xRuO3 ferromagnets. The measurements were compared with numerical simulations based on a model Preisach ensemble of thermally activated two-level subsystems, characterized individually by a double well free energy profile in a two-dimensional configuration space, an elementary moment reversal, a dissipation field and a bias field, and characterized collectively by a distribution of these characteristic fields. Our efforts were concentrated on two principal spheres of investigation. (1) By performing detailed numerical simulations of the relaxation response of model Preisach collections of two-level subsystems under the same field and temperature protocols used to probe experimentally the relaxation dynamics of spin glasses, we have been able to show that aging, memory and rejuvenation effects are ubiquitous features of all materials which possess a broad distribution of free energy barriers which block the approach to thermal equilibrium. (2) We propose a general strategy for isolating and quantifying the two principal mechanisms, thermal fluctuations and barrier growth, which are jointly responsible for shaping the measured temperature dependence of the magnetic properties of all magnetic materials which exhibit a history dependent response to an external field excitation, and is based on the analysis of viscosity isotherms and, in particular, on a plot of T ln(tr/0) versus Ha , where tr is the time at which a viscosity isotherm measured in a field Ha at temperature T reverses sign. When thermal activation dominates barrier growth, this plot will yield a universal curve while, in the opposite limit the plot fractures into a family of isothermal curves. The strategy is applied to the analysis of each magnetic material listed above. / February 2009

The central concern of this thesis is the study of non-equilibrium behaviour in magnetic materials and its interpretation within the framework of the Preisach model of hysteresis. Comprehensive experimental characterizations of the field and temperature and time dependence of a suite of standard magnetic response functions have been performed on a variety of magnetic materials, including a naturally occurring mineral of nanodimensional titanomagnetite particles embedded in volcanic glass, a compressed powder of nanodimensional magnetite particles immobilized in an organic binder, a thin film of nanodimensional Fe particles embedded in alumina, and a series of sintered, bond-disordered CaxSr1-xRuO3 ferromagnets. The measurements were compared with numerical simulations based on a model Preisach ensemble of thermally activated two-level subsystems, characterized individually by a double well free energy profile in a two-dimensional configuration space, an elementary moment reversal, a dissipation field and a bias field, and characterized collectively by a distribution of these characteristic fields. Our efforts were concentrated on two principal spheres of investigation. (1) By performing detailed numerical simulations of the relaxation response of model Preisach collections of two-level subsystems under the same field and temperature protocols used to probe experimentally the relaxation dynamics of spin glasses, we have been able to show that aging, memory and rejuvenation effects are ubiquitous features of all materials which possess a broad distribution of free energy barriers which block the approach to thermal equilibrium. (2) We propose a general strategy for isolating and quantifying the two principal mechanisms, thermal fluctuations and barrier growth, which are jointly responsible for shaping the measured temperature dependence of the magnetic properties of all magnetic materials which exhibit a history dependent response to an external field excitation, and is based on the analysis of viscosity isotherms and, in particular, on a plot of T ln(tr/0) versus Ha , where tr is the time at which a viscosity isotherm measured in a field Ha at temperature T reverses sign. When thermal activation dominates barrier growth, this plot will yield a universal curve while, in the opposite limit the plot fractures into a family of isothermal curves. The strategy is applied to the analysis of each magnetic material listed above.

The central concern of this thesis is the study of non-equilibrium behaviour in magnetic materials and its interpretation within the framework of the Preisach model of hysteresis. Comprehensive experimental characterizations of the field and temperature and time dependence of a suite of standard magnetic response functions have been performed on a variety of magnetic materials, including a naturally occurring mineral of nanodimensional titanomagnetite particles embedded in volcanic glass, a compressed powder of nanodimensional magnetite particles immobilized in an organic binder, a thin film of nanodimensional Fe particles embedded in alumina, and a series of sintered, bond-disordered CaxSr1-xRuO3 ferromagnets. The measurements were compared with numerical simulations based on a model Preisach ensemble of thermally activated two-level subsystems, characterized individually by a double well free energy profile in a two-dimensional configuration space, an elementary moment reversal, a dissipation field and a bias field, and characterized collectively by a distribution of these characteristic fields. Our efforts were concentrated on two principal spheres of investigation. (1) By performing detailed numerical simulations of the relaxation response of model Preisach collections of two-level subsystems under the same field and temperature protocols used to probe experimentally the relaxation dynamics of spin glasses, we have been able to show that aging, memory and rejuvenation effects are ubiquitous features of all materials which possess a broad distribution of free energy barriers which block the approach to thermal equilibrium. (2) We propose a general strategy for isolating and quantifying the two principal mechanisms, thermal fluctuations and barrier growth, which are jointly responsible for shaping the measured temperature dependence of the magnetic properties of all magnetic materials which exhibit a history dependent response to an external field excitation, and is based on the analysis of viscosity isotherms and, in particular, on a plot of T ln(tr/0) versus Ha , where tr is the time at which a viscosity isotherm measured in a field Ha at temperature T reverses sign. When thermal activation dominates barrier growth, this plot will yield a universal curve while, in the opposite limit the plot fractures into a family of isothermal curves. The strategy is applied to the analysis of each magnetic material listed above.

A very important step in the art of cooking up models for the study of natural phenomena is the identification of the relevant ingredients. Taking into account too many details will lead to an overly complicated model, not at all useful to work with, but neglecting some crucial elements will lead to an equally useless model. So it is often the case that the actual experimental situation presents unavoidable sources of local randomness, whilst the analysed phenomenon does not really rely on presence/absence of such imperfections. For some other set of phenomena, however, disorder can play a crucial role, and must be carefully taken into account. Such is for example the case in certain phases of matter, the spin-glass phase, or the many-body localised phase. In this thesis we explore disorder in both of these situations and also as a theoretical means of testing the regime of liquidity in certain two-dimensional highly frustrated magnetic models. The focus here is placed on classical Heisenberg models defined on lattices consisting of clusters all sites of which interact mutually pairwise. This natural way to introduce frustration has been known in the literature to lead to so-called Coulomb spin-liquids, the single class of classical spin-liquids acknowledged to exist so far in Heisenberg models. Here we show that in fact two different classes of classical spin-liquids can be obtained from similarly defined frustrated models. In one of these, algebraic correlations exist at $T=0$, similar to the Coulomb phase, but the system exhibits a rather different low$-T$ effective action from the Coulomb phase. In the other class, the spin-liquid has spin correlations that decay exponentially with distance, with a correlation length smaller than a lattice spacing even at $T=0$. One special effect of disorder in these models, considered in the form of dilution by non-magnetic impurities, is to nucleate local degrees of freedom, so-called orphans, which express the concomitant spin-liquid phase through their non-trivial fractionalisation. When the associated spin-liquid exhibit algebraic correlations, it is also possible to find new effective spin-glass models as an effective $T=0$ description for interactions between the orphans, leading to so-called `random Coulomb magnets'. One part of this thesis is devoted to the first study of these new models. This investigation consists mainly of Monte Carlo simulations and numerical solution of the relevant large$-n$ equations ($n$ being the number of spin components). A clear spin-glass transition for infinitely large coupling strength is determined for the case of spins with an infinite number of components. The results presented on the situation for a finite number of spin components are more of an exploratory character, and large-scale simulations with further optimization schemes to ensure equilibration are still required to locate the transition. The final investigation treated in this thesis deals with the dynamics in a quantum model with disorder displaying the many-body localized phase, where in addition a periodic drive is applied. For a certain range of driving frequencies and amplitudes, it was found recently that the many-body localized phase is robust. These pioneering studies restricted themselves to an analysis of the stability of such a phase in the long time limit, while very little was known about the dynamics towards the asymptotic fate. Our study focuses on this aspect, and analyses the different dynamical behaviors as one varies the driving parameters, so that the many-body localized phase survives or is destroyed by the driving. We discover that on the border between these two asymptotic fates, a new dynamical behavior emerges, where the system heats up at a very slow, logarithmic in time, rate. / Die Bestimmung der wichtigsten Bestandteile stellt einen sehr wichtigen Schritt in der Kunst des Erstellens von Modellen dar. Die Annahme von zu vielen Details ergibt ein sehr kompliziertes, zu nichts zu gebrauchendes Modell, doch die Vernachlässigung von bedeutenden Zusammenhängen führt ebenfalls zu einem unbrauchbaren Ergebnis. Es ist so z.B. häufig der Fall, dass ein Experiment unter dem Einfluss von unvermeindlichen lokalen Zufälligkeiten steht, die allerdings kaum einen Einfluss auf ein beobachtetes Phänomen haben. Für gewisse Phänomene spielt Unordnung jedoch eine wesentliche Rolle und sie muss sehr genau in Betracht gezogen werden. Das ist für bestimmte Phasen, wie beispielsweise Spinglas oder die Vielteilchen-Lokalisation, der Fall. In dieser Dissertation untersuchen wir ungeordnete Systeme, die solche Phasen aufweisen. Außerdem verwenden wir Unordnung als ein theoretisches Werkzeug für die Analyse von bestimmten `Spinflüssigkeiten' in zweidimensionalen Spinmodellen. Der Fokus liegt hierbei auf klassischen Heisenberg Modellen definiert auf Gittern, die aus einer Anordnung von Clustern bestehen, sodass jede einzelne paarweise Heisenberg-Wechselwirkung innerhalb eines Clusters stattfindet. Dadurch weist das System geometrische Frustration auf und in mehreren Fällen tritt eine sogennante Coulomb Spinflüssigkeit ---die bislang einzig bekannte Klasse von klassischen Spinflüssigkeit in Heisenberg Modellen--- auf. Wir zeigen, dass mindestens zwei weitere Arten von klassischen Spinflüssigkeiten in solchen Modellen zu finden sind. Für die eine Klasse sind Spinkorrelationen zu erwarten, die algebraisch mit der Entfernung bei $T=0$ abnehmen, ähnlich wie für eine Coulomb Phase. Diese neu entdeckte Spinflüssigkeit lässt sich jedoch von der Coulomb Phase durch eine neue effektive Tieftemperatur-Theorie unterscheiden. Für die andere Klasse von Spinflüssigkeiten sind die Spinkorrelationen kurzreichweitig, und selbst bei $T=0$ nehmen sie exponentiell ab, mit einer Korrelationslänge, die kleiner als ein Gitterabstand ist. Unordnung, in der Form von nicht-magnetischen Störstellen, kann lokale Freiheitsgrade entstehen lassen (diese werden in der Literatur auch als `Orphans', Waisen, bezeichnet). Die Orphans verweisen durch ihre `Fraktionierung' eindeutig auf die nicht trivialen Korrelationen der spinflüssigen Phase. Falls die Spinflüssigkeit algebraische Korrelationen aufweist, findet man auch langreichweitige Wechselwirkungen zwischen den Orphans bei $T=0$. Dies führt zu neuen Spinglasmodellen, sogenannten `Random Coulomb Magnets'. Ein Teil dieser Dissertation ist der Untersuchung solcher Modelle gewidmet. Diese Untersuchung besteht hauptsächlich aus Monte Carlo Simulationen und numerischer Lösung der relevanten Large-$n$ Gleichungen (wobei $n$ hier auf die Anzahl an Spinkomponenten hinweist). In dem Fall von Spins mit unendlich vielen Spinkomponenten können wir einen eindeutigen Spinglas Phasenübergang für eine unendlich große Kopplungsstärke bestimmen. Die entsprechenden Ergebnisse für den Fall von Spins mit einer endlichen Anzahl an Spinkomponenten sind von einem exploratorischen Charakter. Zusätzliche Simulationen, die möglicherweise weitere Optimierungsschema verwenden um Äquilibrium zu gewährleisten, sind noch von nöten um eine eindeutige Aussage über den Übergang in solchen Fällen zu treffen. Der letzte Teil dieser Dissertation widmet sich der Untersuchung der Dynamik eines ungeordneten Quantenmodells. Das ausgewählte Modell weist die sogennante Vielteilchen-lokalisierte Phase auf, und wir untersuchen insbesondere den Effekt eines periodischen Antriebs auf die Dynamik des Systems. Für eine bestimmte Auswahl der Antriebs-frequenz und -amplitude, wurde es bereits vor kurzem bewiesen, dass die Vielteilchen-lokalisierte Phase diese Störung übersteht. Unsere Studie ist darauf ausgelegt, wie sich die Dynamik des Systems durch Variation der Antriebsparameter ändert, so dass die Vielteilchen-lokalisierte Phase für lange Zeit entweder den Antrieb übersteht oder von ihm zerstört wird. Wir konnten dadurch entdecken, dass an der Grenze zwischen diesen beiden Fällen ein neues dynamisches Verhalten entsteht, bei der das System eine sehr langsame, logarithmisch mit der Zeit, Erwärmung aufweist.

Heusler compounds form a large class of intermetallic materials, which attracted a lot of interest in recent years. The reason is their enormous flexibility, which makes it possible to observe almost every physical effect in one of the 1000 members known nowadays. Especially many magnetic Heusler compounds display promising properties, which offer potential application in fields like rare-earth free permanent magnets, magnetocalorics, spin transfer torque devices and tunnel junctions. Apart from that, magnetic Heusler systems are also interesting for fundamental research since some members host skyrmion lattices and other magnetically complex orders. The search for new Heusler compounds is therefore fruitful in many ways. Accordingly, the present thesis followed the approach of synthesizing and characterizing such Heusler compounds that were either entirely new or had unexplored magnetic properties. Exactly this second approach was demonstrated in Chapter 3, namely for IrMnGa. With help of combined neutron and x-ray diffraction experiments it was possible to correct the structural model from literature and show that the compound crystallizes indeed within the half-Heusler space group but with a substantial degree of Y -disorder. In contrast to older suggestions, the subsequent magnetic characterization revealed a robust canonical spin glass state instead of antiferromagnetic order. The magnetic phase diagram was found to be similar to Au1−xFex and thus hinted on a Heisenberg-like spin glass with considerable anisotropy. Contrary to synthesis route and heat treatment, changing the composition allowed to tune the spin glass state extensively. Increasing the Mn content caused a transition from spin to cluster glass behavior and for Mn contents above 40 at%, it was even possible to introduce ferrimagnetic order. Notably, the composition dependence of spin glasses was only studied for binary systems before. It turned out that many trends are quite similar for the Ir-Mn-Ga ternary scenario with the exception of magnetic behavior near the percolation limit being more complex. Generally, spin glass order is rather rare in Heusler compounds and especially for half-Heusler systems a report remained elusive up to IrMnGa. Chapter 4 then summarized investigations on the Heusler series Fe3−xMnxSi, which features a spin reorientation transition at low temperatures. Despite being one of the most studied Heusler systems, the magnetotransport properties were not yet covered systematically in literature. The presented investigations unveiled that the mechanisms of longitudinal as well as Hall resistivity change upon cooling through the spin reorientation transition. For the Hall effect, skew scattering dominates above TR whereas it is the intrinsic mechanism below. The finding emphasizes the dependency of the intrinsic Hall contribution on the magnetic structure and it should be possible to generalize this change of the Hall mechanism to all magnetic transitions, where the intrinsic contribution is affected. The subsequent Chapter 5 provided a reevaluation of the Fe-Mn-Si phase diagram. The approach seemed well justified since the obtained phase boundaries agreed better with theory than the old experimental studies. Furthermore, it was found that those compounds, which were previously identified as β-Mn, actually crystallize in a superstructure. The ordered version has a Mn3IrSi as prototype and derives from β-Mn by splitting of the 8c site into two 4a sites. Due to the close relation of both structures, this phase was named β’-Mn. Moreover, it turned out that the ’mysterious’ secondary phase, which was mentioned for Mn-rich Fe3−xMnxSi Heusler compounds but never specified, is given exactly by β’-Mn. The investigations of its magnetic properties indicated a transition to a canonical spin glass state at low temperatures. β’-Mn thus adds a further type of magnetic ordering to the Fe-Mn-Si system. Indeed, the latter comprised all kinds of solid state magnetism but no spin glass order was reported before. Finally, the spin glass state was demonstrated to exhibit a similar composition dependence as in Ir-Mn-Ga, which illustrated nicely the universal character of the spin glass concept. The last chapter dealt with the difficult search for entirely new Heusler compounds. It was explained that high-throughput studies struggle to predict phase stabilities, which is why they have to be treated with care. To overcome these issues, some design rules were suggested to evaluate whether a Heusler compound is likely to be experimentally stable or not. Usually, there are no reports for systems, which do not form as single phase. Since this is a highly inefficient habit, 26 multi-phase ’Heusler compounds’ were listed. In the end of the chapter, the successful synthesis of three new compounds was presented, namely Ru2CrAl, Ru2CrGa and Ru2CrSb. Ru2CrGa was identified as Pauli paramagnet whereas Ru2CrSb exhibited an antiferromagnetic transition around 100 K. A second transition at 40 K was accompanied by a small increase of magnetization, which hinted on some more complex magnetic structure at low temperatures.

Les oxydes de métaux de transition sont largement utilisés en raison de leurs propriétés fondamentales intéressantes et de leurs applications importantes. En particulier, CuCrO2 est d’un intérêt particulier parce qu’il possède un état multiferroïque en absence de champ magnétique. Dans cette thèse, nous modélisons les propriétés magnéto-électriques de CuCrO2 par simulations Monte Carlo basées sur des paramètres magnétiques déterminés par calculs ab initio. Nous étudions également l’effet du dopage du Ga sur les propriétés magnéto-électriques du composé CuCr1-xGaxO2 (0 ≤ x ≤ 0:3). Nos résultats sontqualitativement en accord avec les observations expérimentales. / Transition metal oxides are widely used due to their interesting fundamental properties and important applications. In particular, CuCrO2 is of special interest because it enters the multiferroic state in zero magnetic fields. In this thesis we model the magnetoelectric properties of CuCrO2 using Monte Carlo simulations with the help of ab initio calculations.We also investigate the effect of Ga doping on the magnetoelectric properties of CuCr1-xGaxO2 (0 ≤ x ≤ 0:3). Our results are well comparable to the experimental observations.

Neste trabalho consideramos o modelo de Potts na árvore de Cayley submetida a um campo magnético. Esse campo pode ser representado pela interação dos spins da árvore com um spin adicional, denominado spin fantasma. Essa nova rede passa a ser chamada de árvore de Cayley fechada e assimétrica. Sendo uma rede hierárquica, ela representa soluções exatas que são obtidas quando as técnicas do grupo de renormalização no espaço real são aplicadas. Subtraindo os efeitos de superfície e considerando somente o interior da árvore (rede de Bethe), esses resultados reproduzem os resultados da aproximação de campo médio de Bethe-Peierls. Com a finalidade de estudar a função de correlação do modelo de Potts na rede de Bethe, consideramos primeiramente uma cadeia de Potts interagindo com um spin fantasma. Através das regras de composição em série e paralelo e do método da quebra e colapso para as trasmissividades térmicas (função de correlação) obtemos uma fórmula de recorrência para a função de correlação entre quaisquer dois spins na cadeia. Mostramos então que pela invariança translacional da rede de Bethe qualquer par de spins pode ser mapeado no sistema anterior. A seguir consideramos o modelo de Potts de um estado na árvore de Cayley fechada e assimétrica. Decimando os spins interiores da unidade geradora da rede, obtemos um mapa polinomial quadrático para a transformação do grupo de renormalização (mapa de Bethe-Peierls). O diagrama de fase desse sistema é então obtido do conjunto de Mandelbrot através de uma transformação de Mobius. O mapa de Bethe-Peierls apresenta dois pontos fixos, que são relacionados com as fases ferro e paramagnética e o regime caótico é identificado com a fase vidro de spin. Esse sistema revela ser o exemplo mais simples de vidro de spin de McKay-Berker-Kirkpatrick. Na rede de Bethe e a campo nulo esse sistema apresenta transições de fase de segunda ordem. Analisando o comportamento crítico da função de correlação e de suas derivadas, vemos que se identificarmos a função de correlação entre o spin fantasma e qualquer spin da rede com a magnetização (por spin) e a função de correlação entre dois spins primeiros vizinhos com a energia interna do sistema, cinco expoentes críticos ((&#948, &#946, &#947 &#8217, &#945, &#945 &#8217) são calculados e satisfazem as relações de escala. Para ilustrar o procedimento recursivo apresentado para calcular a função de correlação entre dois spins separados por ligações m na rede de Bethe, consideramos os spins de Potts de um estado. Obtemos então de forma explícita as correlações para m=1, 2 e 3.0 / In this work we consider the Potts model on the Cayley tree subjected to a magnetic Field. This field can be represented by the interaction of the tree spins with an additional one, denominated ghost spin. This new lattice is then called closed-asymmetric Cayley tree. Being a hierarchical lattice it comes to have exact solutions which are obtained when the real-space renormalization group techniques are applied. Subtracting the surface effects and considering only the tree interior (Bethe lattice), these results reproduce the results of Bethe-Peierls mean-field approximation. With the objective of studying the pair-correlation function of the Potts model on the Bethe lattice, we at first consider a Potts chain interacting with a ghost spin. Throughout the series-parallel composition rules and the break-collapse method for the thermal transmissivities (pair-correlation function) we obtain a recursive relation for the correlation function between any two spins on the chain. We then show, due to the translational invariance of the Bethe lattice, that any pair of spins can be mapped into the latter system. Next we consider the one-state Potts model on the closed asymmetric tree. Decimating the inner spins of the generating unit for the lattice, we obtain a quadratic polynomial map for the renormalization group transformation (Bethe-Peierls map). The phase diagram of this system is obtained from the Mandelbrot set throughout a Mobius transformation. The Bethe-Peierls map has two stable fixed points which are related to the ferro and paramagnetic phases and the chaotic regime is identified with the spin-glass phase. This system turns out to be the simplest example of a McKay-Berker-Kirkpatrick spin glass. On the Bethe lattice with vanishing field this system presents second-order phase transitions. Analyzing the critical behavior of the pair-correlation function and of this derivatives, we see that if we identify the correlation function between the ghost spin and any spin on the lattice with the magnetization (per spin), and the correlation function between two nearest-neighbor spins with the internal energy of the system, five critical exponents (&#948, &#946, &#947 &#8217, &#945, &#945 &#8217) are calculated and they satisfy the scaling relations. In order to illustrate the recursive procedure presented to calculate the pair-correlation function between spins m bonds apart on the Bethe lattice, we consider the one-state Potts spins. We obtain explicitly the correlation for m=1, 2 and 3.