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<p>This thesis comprises studies on two ferromagnetic superconductors, URhGe (Tcurie=9.SK and Tsc=2S0mK) and UCoGe (Tcurie=2.SK and Tsc=800mK). These properties are interesting because the current theory to explain superconductivity predicts that ferromagnetism should destroy superconductivity. Not only is that not true in these materials, but ferromagnetism and superconductivity are thought to arise from a common mechanism. The studies conducted on these materials arise from that possibility, in an attempt to understand the unconventional nature of these materials.<br />Original work is contained in chapters 4, Sand 6. All of this work is currently not published in sources other than this thesis. <br /> Chapter 1 will give an introduction to these materials, and the work that has been done on them by other groups, and work done on related materials. <br /> Chapter 2 will give details of the various experimental methods used in measuring the structure and properties of the materials studied. This work was conducted by the author at McMaster University, with the assistance of individuals from the Brockhouse Institute for Materials Research, and the Center for Electron Microscopy at McMaster University.<br /> Chapter 3 will provide an introduction to the technique of muon Spin Resonance/Relaxation (μSR). This work was done at the TRIUMF facility in Vancouver, British Columbia, with the assistance of several TRIUMF staff. The data was collected by the author, and other members of Dr. Luke's research group as well as collaborators from TRlUMF and from Columbia University. <br /> Chapter 4 will present the measurements made on UCoGe, while Chapter 5 presents the measurements of URhGe. Details of the crystal growth and structure characterization measurements are included in these chapters, along with resistivity, bulk magnetization and μSR measurements. <br /> Both zero- field (ZF) and transverse field (TF) μSR has been performed. This work focuses on studying the magnetic moment size, and the magnetic volume fraction around the ferromagnetic transition, and to temperatures as low as 20mK. Consideration is also given to the magnetic and superconducting properties in the low-temperature region. <br /> In the Introduction, URhGe is presented first, followed by UCoGe, since this was the order in which they were discovered. The results obtained from UCoGe are presented first, since work on that compound was started before the work on URhGe. <br /> Chapter 6 focuses on the conclusions drawn from this work, comparing the measurements of both materials.</p> / Master of Science (MS)

1979 wurde mit CeCu2Si2 erstmalig ein Schwere-Fermionen-Supraleiter entdeckt. Diese Verbindung, entdeckt von Steglich und Mitarbeitern, befindet sich nahe an einem quantenkritischen Punkt, an dem die magnetische Ordnung gerade unterdrückt wird. Der Abstand zu diesem Punkt kann sowohl durch Druck als auch durch Germaniumsubstitution auf dem Siliziumplatz variiert werden. Dabei treten neben der Supraleitung in CeCu2Si2 auch verschiedene magnetische Phasen bei höherem Germaniumgehalt auf. CeCu2Si2 ordnet magnetisch unterhalb von TN = 0.8 K in einer Spindichtewelle, während das Schwere-Fermionen-System CeCu2Ge2 unterhalb von TN = 4.1 K antiferromagnetisch ordnet. In dieser Arbeit wurde die Substitutionsreihe CeCu2(Si1-xGex)2 mittels Neutronendiffraktion untersucht. Ausgehend von Proben mit hohem Germaniumgehalt von x = 0.45, deren magnetische Struktur detailliert untersucht wurde, wurden schrittweise die Eigenschaften von Proben mit kleinerem x erschlossen, um schließlich die (bis dato unbekannte) magnetische Struktur in CeCu2Si2 aufzuklären. Weiterhin wurden Untersuchungen zumWechselspiel zwischenMagnetismus und Supraleitung durchgeführt. Hierzu wurde mit einem selbstentwickelten Aufbau dieWechselfeldsuszeptibilität simultan zu den Diffraktionsexperimenten aufgezeichnet. Durch die direkte Korrelation konnte nachgewiesen werden, dass in CeCu2Si2 keine mikroskopische Koexistenz von Supraleitung und magnetischer Ordnung vorliegt, sondern mikroskopische Phasenseparation. - Die Arbeit ist auch über den Cuvillier-Verlag; Nonnenstieg 8; 37075 Göttingen mit der ISBN 978-3-86727-587-3 erhältlich. / In 1979 the first heavy-fermion superconductor CeCu2Si2 was discovered by Steglich et al. The system is near a quantum critical point (QCP), where the magnetic order is just suppressed. The distance to the QCP can be variied with hydrostatic pressure as well as by germanium substitution on the silicon site. Next to the superconductivity in CeCu2Si2 one finds distinct magnetic phases while increasing the germanium content. CeCu2Si2 shows a magnetic order of a spin-density-type below TN = 0.8 K, whereas the heavy fermion system CeCu2Ge2 orders below TN = 4.1 K as an antiferromagnet. The focus of this thesis is on neutron-diffraction in the system CeCu2(Si1-xGex)2. Starting with a sample with a high germanium content of x = 0.45, the magnetic structures are investigated in detail. Following a step-by-step approach, samples with reduced x are investigated subsequently to figure out the properties of pure CeCu2Si2, which were not accessible before. Furthermore, the complex interaction between magnetism and superconductivity is investigated in detail. Using a specially designed setup, the ac-susceptibility could be recorded simultaneously during the neutron diffraction experiments. Due to the direct correlation between antiferromagnetic signals and diamagnetic features, the microscopic coexistence of superconductivity and magnetic order can be ruled out. Instead, a phase separation on the microscopic scale is found. - The thesis is also available from the publisher Cuvillier-Verlag; Nonnenstieg 8; 37075 Göttingen under the ISBN 978-3-86727-587-3.

Dans cette thèse, j'ai étudié l'évolution de la surface de Fermi sous l'influence d'un champ magnétique dans des systèmes massifs facilement polarisables à basse température. La première partie est dévouée aux cas du supraconducteur ferromagnétique UCoGe et du supraconducteur paramagnétique CeIrIn5, où la surface de Fermi peut être modifiée sans transition magnétique. Dans UCoGe, plusieurs anomalies successives ont été détectées dans l'effet Seebeck, la résistivité et l'effet Hall, sans transition nette dans l'aimantation. L'observation d'oscillations quantiques montre que ces anomalies sont reliées à des changements de topologie de la surface de Fermi, aussi appelés transitions de Lifshitz. Dans CeIrIn5, une anomalie est détectée dans l'effet Seebeck à HM = 28 T et les oscillations quantiques observées en magnétométrie torque montrent qu'une transition de Lifshitz à lieu à ce champ.Dans la deuxième partie, j'ai étudié comment varie la surface de Fermi à travers une transition magnétique du premier ordre induite par le champ magnétique dans le supraconducteur ferromagnétique URhGe avec le champ selon l'axe de difficile aimantation b et le supraconducteur antiferromagnétique UPd2Al3 avec le champ dans le plan basal. Dans URhGe, l'effet Seebeck permet d'observer un changement de la surface de Fermi à la transition de réorientation des spins à HR = 11.75 T et avec la résistivité confirme le caractère premier ordre de la transition en plus de fournir la localisation dans le diagramme de phase du point tricritique. Dans UPd2Al3, une nouvelle branche de la surface de Fermi est observée dans les oscillations quantiques de de Haas-van Alphen dans l'état antiferromagnétique et l'effet Seebeck montre que la surface de Fermi change à la transition métamagnétique à HM = 18 T. En outre, quatre nouvelles branches sont observées dans la phase polarisée au delà de HM et qui ne peuvent être associées à celles calculées dans les états paramagnétique et antiferromagnétique. / In this thesis, we have studied the evolution of the Fermi surface under the influence of a magnetic field in bulk materials that can be easily polarized at low temperature. The first part was devoted to the cases of the ferromagnetic superconductor UCoGe with a magnetic field applied along the easy magnetization c-axis and the paramagnetic superconductor CeIrIn5 with the field along the c-axis. In UCoGe, several successive anomalies were detected in resistivity, Hall effect and thermoelectric power, without any thermodynamic transition being detected in magnetization. The direct observation of quantum oscillations showed that these anomalies are related to topological changes of the Fermi surface, also known as Lifshitz transitions. In CeIrIn5, the thermoelectric power detected an anomaly at HM = 28 T and the quantum oscillations observed in torque magnetometry showed that a Lifshitz transition occurs at this field.In the second part of this thesis, we studied the evolution of the Fermi surface through first order magnetic transitions induced by magnetic field. In the ferromagnetic superconductor URhGe with the field applied along the hard magnetization b-axis and the antiferromagnetic superconductor UPd2Al3 with the field in the basal plane. In URhGe, the thermoelectric power allowed to observe a change in the Fermi surface at the spin reorientation transition at HR = 11.75 T defining the ferromagnetic state and along with resistivity confirmed the first order character of the transition as well as give a location of the tricritical point. In UPd2Al3, a new branch was observed in de Haas-van Alphen experiment in the antiferromagnetic phase and the thermoelectric power showed that the Fermi surface is reconstructed at the metamagnetic transition at HM = 18 T where the antiferromagnetic state is suppressed and could suggest that the Fermi surface changes before this transition. Additionally, four new branches were observed in the polarized paramagnetic phase, above HM, that cannot be associated with calculated branches in the paramagnetic of antiferromagnetic states.

Cette thèse montre de nouveaux résultats sur les supraconducteurs ferromagnétiques UCoGe et URhGe et sur l’ordre caché dans URu2Si2. Le diagramme de phase pression température d’UCoGe a été étudié jusqu’à 10.5 GPa. L’ordre ferromagnétique subsiste jusqu’à la pression critique pc≈1 GPa et la supraconductivité non conventionnelle jusqu’à p = 4 GPa. Les fluctuations magnétiques responsables de la supraconductivité peuvent être réduites par l’application d’un champ magnétique. Les surfaces de Fermi d’UCoGe et d’URhGe ont été mesurées grace aux oscillations quantiques. Quatre poches ont été détectées dans UCoGe, elles subissent une succession de transition de Lifshitz de la surface de Fermi sous champ magnétique. Les poches détectés évoluent continument avec la pression jusqu’à 2.5 GPa, sans montrer de reconstruction de la surface de Fermi à la pression critique pc. Dans URhGe, trois poches lourdes de la surface de Fermi ont aussi été découvertes. Enfin dans la phase d’ordre caché d’URu2Si2, les oscillations quantiques ont révélé une forte anisotropie du facteur gyromagnétique g pour deux poches de la surface de Fermi, qui est comparable à l’anisotropie macroscopique. Cette dernière a été étudiée à partir du champcritique supérieur de la supraconductivité. / This thesis is concentrated on the ferromagnetic superconductors UCoGe and URhGe andon the hidden order state in URu2Si2. In the first part the pressure temperature phase diagram of UCoGe was studied up to 10.5 GPa. Ferromagnetism vanishes at the critical pressure pc≈1 GPa. Unconventional superconductivity and non Fermi liquid behavior can be observed in a broad pressure range around pc. The superconducting upper critical field properties were explained by the suppression of the magnetic fluctuations under field. In the second part the Fermi surfaces of UCoGe and URhGe were investigated by quantum oscillations. In UCoGe four Fermi surface pockets were observed. Under magnetic field successive Lifshitz transitions of the Fermi surface have been detected. The observed Fermi surface pockets in UCoGe evolve smoothly with pressure up to 2.5 GPa and do not show any Fermi surface reconstruction at the critical pressure pc. In URhGe, three heavy Fermi surface pockets were detected by quantum oscillations. In the last part the quantum oscillation study in the hidden order state of URu2Si2 shows a strong g factor anisotropy for two Fermi surface pockets, which is compared to the macroscopic g factor anisotropy extractedfrom the upper critical field study.

Orientador: Pascoal Jose Giglio Pagliuso / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Fisica Gleb Wataghin / Made available in DSpace on 2018-08-15T21:09:50Z (GMT). No. of bitstreams: 1 Bittar_EduardoMatzenbacher_D.pdf: 12237565 bytes, checksum: 74dcda9fcb1da9b6fc8d992b53297127 (MD5) Previous issue date: 2010 / Resumo: Séries de compostos que apresentam a ocorrência de fenômenos físicos interessantes em materiais estruturalmente simples constituem uma excelente oportunidade para se estudar sistematicamente a inter-relação entre tais fenômenos e suas origens microscópicas, sem se ater a efeitos associados com estruturas cristalinas complexas, de mais baixa simetria. Nesse sentido, esta Tese se propôs a estudar três temas de investigação: o sistema CeIn3-xSnx e o seu análogo não magnético LaIn3-xSnx, o sistema CeIn3-xCdx e o composto YbAl3 e o seu composto de referência LuAl3. O sistema CeIn3-xSnx apresenta um ponto crítico quântico (QCP) em x ? 0.7, onde a ordem antiferromagnética (TN = 10 K no CeIn3) é totalmente suprimida. Para 0.7 < x < 2 os compostos são líquidos de Fermi e a partir de x = 2 apresentam valência intermediária. Nesse sistema, dopado com Gd3+, medidas de ressonância de spin eletrônico (ESR) indicaram que o elétron 4f do Ce passa de um comportamento com momento localizado para itinerante com a dopagem de Sn. Os resultados de ESR do Gd3+ no sistema LaIn3-xSnx foram analisados com um modelo de uma única banda (tipo s) e sem dependência com a transferência de momento. Também investigamos o sistema CeIn3-xCdx através de medidas de susceptibilidade magnética, calor específico e resistividade elétrica. A substituição do In por Cd diminui a TN do CeIn3 e igualmente faz o coeficiente do calor específico eletrônico decrescer, indicando que o sistema não está na direção de um QCP. Os compostos YbAl3 e LuAl3, dopados com Gd3+, também foram estudados por ESR, porém, na análise, utilizou-se um modelo de múltiplas bandas para explicar os resultados. Medidas de calor específico e susceptibilidade magnética, nessas amostras, mostraram que interações de troca elétron-elétron estão presentes em ambos os compostos. Esses resultados microscópicos podem ser importantes em modelos teóricos mais realistas para materiais férmions pesados de valência intermedi'aria a base de Yb / Abstract: Series of compounds which have interesting physical phenomena, occurring in structurally simple materials, provide an excellent opportunity to systematically study the interrelationship between these phenomena and their microscopic origins, without worrying about effects associated with other complex crystal structures of lower symmetry. Thus, this thesis set out to study three research themes: the CeIn3-xSnx system and its nonmagnetic analogue LaIn3-xSnx, the CeIn3-xCdx system and the YbAl3 compound and its reference compound LuAl3. The CeIn3-xSnx system has a quantum critical point (QCP) at x ? 0.7, where the antiferromagnetic order (TN = 10 K in CeIn3) is totally suppressed. For 0.7 < x < 2 the compounds are Fermi liquids and from x = 2 the materials show intermediate valence behavior. In this system, doped with Gd3+, measurements of electron spin resonance (ESR) indicated that the Ce 4f electron presents a crossover between a localized to itinerant behavior with Sn doping. The ESR results of Gd3+ in the LaIn3-xSnx system were analyzed with a single band model (s type) and no q dependence. We also investigated the CeIn3-xCdx system by measuring magnetic susceptibility, specific heat and electrical resistivity proprieties. The substitution of In by Cd decreases the TN of CeIn3 and also decreases the electronic specific heat coefficient, indicating that the system is not being tuned to a QCP. The YbAl3 and LuAl3 compounds, doped with Gd3+, were also studied by ESR, but in the analysis, we used multiband model to explain the results. Specific heat and magnetic susceptibility measurements in these samples showed that electron-electron exchange interactions are present in both compounds. These ESR results may be relevant to construct more realistic models of the microscopic behavior of other heavy fermion-based intermediate valence Yb compounds / Doutorado / Física da Matéria Condensada / Doutor em Ciências

Second-order phase transitions involve critical fluctuations just below and above the transition temperature. Macroscopically, they manifest in the power-law behaviour of many physical properties such as the susceptibility and the specific heat. The power-laws are predicted to be universal, i.e. the same exponents are expected for a certain class of transitions irrespective of the microscopic details of the system. The underlying commonality of such transitions is the divergence of the correlation length ξ and the correlation time ξ_τ of the critical fluctuations at the transition temperature. Both ξ and ξ_τ can be directly observed by neutron scattering experiments, making them an ideal tool for the study of critical phenomena. At classical phase transitions, the critical fluctuations will be thermal in nature. However, if a second-order transition occurs at T = 0, thermal fluctuations are frozen, and the transition is driven by quantum fluctuations instead. This is called a quantum critical point. The quantum nature of the fluctuations influences observable properties, also at finite temperatures, and causes unusual behaviour in the vicinity of the quantum critical point or the existence of exotic phases, e.g. unconventional superconductivity. Heavy-fermion compounds are a class of materials that is well suited for the study of quantum criticality. They frequently show second-order transitions into a magnetically ordered state at very low temperatures, which can easily be tuned to T = 0 by the application of pressure, magnetic fields or element substitution. In this thesis, fluctuations near a quantum critical point are investigated for three heavy-fermion systems. CeCu2Si2 shows unconventional superconductivity close to an antiferromagnetic quantum critical point. Results from single-crystal neutron spectroscopy and thermodynamic measurements are discussed and some details are also given about the synthesis of large single crystals. The focus of the study is the comparison of the inelastic response of magnetic and superconducting samples, which are found to be very similar for ΔE > 0.2 meV. CePdAl has an antiferromagnetic state with partial magnetic frustration. The ordering temperature can be suppressed by Ni substitution towards a quantum critical point. Single-crystal neutron diffraction experiments of three members of the substitution series were analysed. They revealed several unusual effects of the frustrated state in the pure sample, and show that magnetic order and frustration persist in the substituted samples. YbNi4P2 is a rare example of a compound with ferromagnetic quantum criticality, which has only been studied in the last few years. The aim of the powder neutron spectroscopy experiments presented here was to obtain an overview of the relevant energy scales, i.e. the crystal electric field, local magnetic fluctuations and ferromagnetic fluctuations. Simulations using the program McPhase were performed for a thorough understanding of the crystal electric field.

Une première partie de ce mémoire portera sur l’analyse des états fondamentaux ma- gnétiques de deux composés isolants et magnétiquement frustrés SrDy2O4 et SrHo2O4. Une étude de la chaleur spécifique à basse température sous l’effet de champs magné- tiques de ces échantillons a été menée afin de détecter la présence de transitions de phases. L’utilisation d’un composé isotructurel non magnétique, le SrLu2O4, a permis l’isolement de la composante magnétique à la chaleur spécifique. Les comportements observés sont non conformes avec les transitions magnétiques conventionnelles. De plus, le calcul de l’entropie magnétique ne montre qu’un recouvrement partiel de l’entropie associée à un système d’ions magnétiques. En second lieu, une analyse des oscillations quantiques de Haas-van Alphen a été effectuée dans le LuCoIn5, composé apparenté au supraconducteur à fermions lourds CeCoIn5. Les résultats obtenus montrent une topologie de la surface de Fermi très différente comparativement aux CeCoIn5 et LaCoIn5, ayant un comportement beaucoup plus tridimensionnel sans les cylindres caractéristiques présents chez les autres membres de cette famille. Finalement, le montage d’un système de détection PIXE a permis l’analyse nucléaire d’échantillons afin de déterminer la concentration de chacun des éléments les constituant. L’analyse a été effectuée sur une série d’échantillons YbxCe1−xCoIn5 dont le changement de concentration a des effets importants sur les propriétés du système. / The first part of this thesis consist of the analysis the magnetic ground states of two magnetically frustrated insulator compounds SrDy2O4 and SrHo2O4. A study of the low temperature specific heat in magnetic fields has been carried on in order to detect phase transitions. The magnetic contribution to the specific heat has been determined using the isostructural but non magnetic compound SrLu2O4. The observed behaviour does not conform with conventional magnetic phase transitions. Also, the calculated magnetic entropy shows only a partial recovery of the entropy normally associated with magnetic ions in the systems. In the second study, I measured and analyzed de Haas-van Alphen quantum oscil- lations in LuCoIn5, a compound related to the heavy fermion superconductor CeCoIn5. The obtained results show a Fermi surface topology greatly differing from the CeCoIn5 and LaCoIn5, having a much more tridimensional behaviour, compared to the characteristics cylinder exhibited by the other members of this family. In the last part of my thesis, I’m am describing the set up of a PIXE detection system used for the nuclear analysis of thick samples in order to calculate the concentra- tion of each element present. The analysis has been carried on a series of samples of YbxCe1−xCoIn5, where the variation of concentration has major repercussions on the electronic and magnetic properties of the system.

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