In this thesis, I study the electronic and structural phase diagrams of the superconducting 122 iron pnictides systems Ba1-xKx(Fe1-yCoy)2As2 and EuFe2(As1-xPx)2 by means of the local probe techniques 57Fe Mössbauer spectroscopy (MS) and muon spin relaxation (muSR). For both isovalent substitution strategies - Co/K for Fe/Ba and P for As, respectively - the antiferromagnetic Fe ordering and orthorhombic distortion of the parent compounds BaFe2As2 and EuFe2As2 are subsequently suppressed with increasing chemical substitution and superconductivity arises, once long-range and coherent Fe magnetic order is sufficiently but not entirely suppressed. For Ba1-xKx(Fe1-yCoy)2As2 in the charge compensated state (x/2=y), a remarkably similar suppression of both, the orthorhombic distortion and Fe magnetic ordering, as a function of increasing substitution is observed and a linear relationship between the structural and the magnetic order parameter is found. Superconductivity is evidenced at intermediate substitution with a maximum Tsc of 15 K coexisting with static magnetic order on a microscopic length scale. The appearance of superconductivity within the antiferromagnetic state can by explained by the introduction of disorder due to nonmagnetic impurities to a system with a constant charge carrier density. Within this model, the experimental findings are compatible with the predicted s± pairing symmetry. For EuFe2(As1-xPx)2, the results from 57Fe MS and ZF-muSR reveal an intriguing interplay of the local Eu 2+ magnetic moments and the itinerant magnetic Fe moments due to the competing structures of the iron and europium magnetic subsystems. For the investigated single crystals with x=0.19 and 0.28, 57Fe MS evidences the interplay of Fe and Eu magnetism by the observation of a transferred hyperfine field below Tafm at which the Eu subsystem orders into a canted A-type AFM magnetic structure. Furthermore, an additional temperature dependent out-of-plane tilting of the static Fe hyperfine field is observed below the onset of static Eu ordering. ZF-muSR shows a strong increase of the local field at the muon site below Tafm=20 K and a crossover from isotropic to anisotropic Eu spin-dynamics between 30 and 10 K. The temperature dependence of the spin dynamics, as derived from the muSR dynamic relaxation rates, are related to a critical slowing down of Eu-spin fluctuations which extends to even much higher temperatures (~100 K). They also effect the experimental linewidth observed in the 57Fe MS experiments. The strong influence of the Eu magnetic order onto the primary observables in both methods prevents conclusive interpretation of the experimental data with respect to a putative interplay of Fe magnetism and superconductivity.

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / This work is dedicated to investigate the spin relaxation in amorphous CoFeSiB glass-covered microwires and multilayered films of Permalloy/Cu. The microwires samples were Joule annealed and axially stressed in order to evaluate the modifications in the damping mechanisms due to the stress induced anisotropy. In the films we were interested in the observation of the modifications in the damping mechanisms imposed by the number of interfaces in the samples. We were able to identify the main damping mechanisms responsible for the spin relaxation in these materials by ferromagnetic resonance experiments. In order to explain the ferromagnetic resonance linewidth, we considered the extrinsic magnetic relaxation mechanisms in addition to the intrinsic Gilbert damping term, the intrinsic one. The extrinsic magnetic relaxation takes in to account the broadening induced by the magnetic inhomogeneities and is consistent with the two-magnon scattering model and anisotropy dispersions. The contribution from the intrinsic magnetization relaxation is constant in both systems of samples and is not sensible neither to Joule annealing and applied stress in microwires, nor to the increasing of the bilayers number in the films. The extrinsic contribution is very sensible to the anisotropy induction and is a signature of magnetic and structural inhomogeneities. / Este trabalho é dedicado ao estudo da relaxação de spin em microfios amorfos recobertos por vidro com composição nominal de CoFeSiB e em filmes multicamadas de Permalloy/Cu. Nos microfios, avaliamos o efeito da indução de anisotropia pela aplicação de tensão mecânica e o efeito do alívio de tensões internas promovido por tratamento térmico aos mecanismos de amortecimento responsáveis pela relaxação de spin. Nos filmes, avaliamos as modificações impostas aos mecanismos de amortecimento quando variamos o número de bicamadas. Identificamos e quantificamos os principais mecanismos responsáveis pela relaxação magnética, através da investigação da largura de linha de ressonância ferromagnética. Para explicar as larguras de linha de ressonância ferromagnética observadas consideramos como mecanismo intrínseco o mecanismo de amortecimento de Gilbert. Como mecanismos extrínsecos consideramos o alargamento da linha de ressonância devido a inomogeneidades magnéticas, consistente com o modelo de espalhamento de mágnons e com a presença de dispersões na anisotropia. O termo intrínseco de relaxação é constante em ambos os conjuntos de amostras estudados, não variando com o tratamento térmico ou tensão aplicada, no caso dos microfios, nem com o aumento do número de bicamadas, no caso dos filmes. A contribuição extrínseca de amortecimento mostrou-se bastante sensível à indução de anisotropias e é uma assinatura das inomogeneidades estruturais e magnéticas presentes nas amostras.

Cette thèse se concentre sur l'étude de composés magnétiques géométriquement frustrés où les ions magnétiques se situent aux sommets d'un réseau de tétraèdres partageant leurs sommets: les composés pyrochlores. Deux familles de formule chimique R2M2O7, où R est un lanthanide et M= Ti, Sn, sont particulièrement intéressantes puisqu'elles présentent une grande variété d'états magnétiques exotiques. Premièrement, nous avons étudié le champ cristallin agissant au site de la terre rare dans l'approximation de Stevens où uniquement le terme fondamental est considéré. Un jeu unique de paramètres a été déterminé pour chaque famille considérée grâce à une analyse globale incluant des spectres de neutrons inélastiques de plusieurs composés. Ensuite, nous avons caractérisé avec un large éventail de techniques les propriétés physiques à basse température de Nd2Sn2O7. En dessous de la température de transition Tc=0.91 K, ce composé possède un ordre magnétique à longue portée dans la configuration de spins dite "all-in-all-out". Une persistance de la dynamique de spins a été révélée dans la phase ordonnée, attribuée à des excitations unidimensionnelles de spins. Une dynamique de spins anormalement lente est également reportée dans la phase paramagnétique. Enfin, nous avons apporté quelques informations sur les deux états fondamentaux proposés pour le composé très étudié Tb2Ti2O7: premièrement, l'apparition d'une transition Jahn-Teller à basse température est suggérée mais l'absence d'élargissement des pics de Bragg réfute la présence d'une transition structurale. Enfin ce composé pourrait être un exemple d'une glace de spin quantique mais l'existence d'un plateau d'aimantation n'est pas évident jusqu'à T=20 mK. / This Phd thesis focuses on the study of magnetically frustrated compounds where magnetic ions lie at the vertices of a corner-sharing tetrahedra network: the pyrochlore compounds. The two series of chemical formula R2M2O7, where R is a lanthanide and M=Ti, Sn, are of peculiar interest since they display a large variety of exotic magnetic ground states. First, we have studied the crystal-electric-field acting at the rare earth within the Stevens approximation where only the ground state multiplet is considered. A single set of parameters for each families of interest has been determined through a global analysis including several inelastic neutron scattering spectra of various compounds. Then, we have characterised with a large panel of techniques the low temperature physical properties of Nd2Sn2O7. This compound enters a long-range magnetic order at transition temperature Tc=0.91 K with an ``all-in-all-out'' spin configuration. A persistence of spin dynamics has been found in the ordered phase, ascribed to one-dimensional spin loops excitations. Anomalously slow paramagnetic spin fluctuations are also reported. Finally, we have brought information on the two proposed ground states of the widely studied compound Tb2Ti2O7: first, a Jahn-Teller transition is claimed to occur at low temperatures but no broadening of the Bragg peaks is seen down to T=4 K precluding premises of a structural transition. Secondly, this compound could be a realisation of a quantum spin-ice but no definitive evidence of a magnetisation plateau is found down to T=20 mK.

Dans cette thèse nous considérons un semi-conducteur de GaAs dopé, où nous étudions la relaxation du spin du côté métallique de la transition metal-isolant. Nous considérons deux types différents d'interaction de spin-orbite. Le premier d'entre eux est associé aux impuretés et l'autre est de type Dresselhaus. La dynamique du spin est traitée à travers une formulation analytique basée sur la diffusion du spin de l'électron, et un calcul numérique de la durée de vie du spin.Ensuite, nous considérons une boîte quantique hébergée dans un nanofil de matériau InAs (avec une structure cristalline de type wurtzite), afin d'étudier l'effet de l'interaction spin-orbite sur les états propres du système. Nous développons ici une solution analytique pour la boîte quantique en incluant l'interaction spin-orbite (de type Dresselhaus propre à la structure wurtzite). Nous avons calculé le facteur g effectif, ainsi que la relaxation du spin dûe aux phonons acoustiques, en utilisant les potentiels d'interaction electron-phonon propres à la structure wurtzite. / In the first part of this thesis we consider a doped GaAs semiconductor and study the spin relaxation on the metallic side of the metal-insulator transition. We take into account two different types of spinorbit coupling, the first of them being associated to the presence of extrinsic impurities, while the other one is the Dresselhaus coupling. To tackle the spin dynamics problem, we develop an analytical formulation based on the spin diffusion of an electron in the metallic regime of conduction of the impurity band. The full derivation provides us with an expression for the spin-relaxation time ,which is free of adjustable parameters. We complement this approach and back our analytical results with the numerical calculation of the spin lifetime.In the second part of the thesis we consider a quantum dot hosted in an InAs nanowire (with awurtzite crystalline structure) and study the effect of spin-orbit coupling on the eigenstates of the zero-dimensional system. We develop here an exact analytical solution for the quantum dot, takinginto account the proper effective spin-orbit coupling for this type of material. We focus on the Dresselhaus coupling, which presents a cubic-in-k term, along with a linear term, characteristic of wurtzite materials. A Zeeman interaction from an external magnetic field is included as well and we compute the effective g-factor as a function of the dot size. Finally, we calculate the spin-relaxation due to acoustic phonons, taking into account the phonon potentials corresponding to the wurtzite structure.

The thesis presents work regarding amphiphilic molecules associated in aqueous solution or at the liquid/solid interface. Two main topics are included: the temperature-dependent behavior of micelles and the adsorption of dispersants on carbon nanotube (CNT) surfaces. Various NMR methods were used to analyze those systems, such as chemical shift detection, spectral intensity measurements, spin relaxation and, in particular, self-diffusion experiments. Besides this, small angle X-ray scattering (SAXS) was also applied for structural characterization.   A particular form of phase transition, core freezing, was detected as a function of temperature in micelles composed by a single sort of Brij-type surfactants. In mixed micelles, that phase transition still occurs accompanied by a reversible segregation of different surfactants into distinct aggregates. Adding a hydrophobic solubilizate shifts the core freezing point to a lower temperature. Upon lowering the temperature to the core freezing point, the solubilizate is released. The temperature course of the release curves with different initial solubilizate loadings is rationalized in terms of a temperature-dependent loading capacity.   The behavior of amphiphilic dispersant molecules in aqueous dispersions of carbon nanotubes (CNTs) has been investigated with a Pluronic-type block copolymer as frequent model dispersant. Detailed dispersion curves were recorded and the distribution of the dispersant among different available environments was analyzed. The amount of dispersed CNT was shown to be defined by a complex interplay of several factors during the dispersion process such as dispersant concentration, sonication time, centrifugation and CNT loading. In the dispersion process, high amphiphilic concentration is required because the pristine CNT surfaces made available by sonication must be rapidly covered by dispersants to avoid their re-attachment. In the prepared dispersions, the competitive adsorption of possible dispersants was investigated that provided information about the relative strength of the interaction of those with the nanotube surfaces. Anionic surfactants were found to have a strong tendency to replace Pluronics, which indicates a strong binding of those surfactants.   CNTs were dispersed in an epoxy resin to prepare nanotube-polymer composites. The molecular mobility of epoxy was investigated and the results demonstrated the presence of loosely associated CNT aggregates within which the molecular transport of epoxy is slow because of strong attractive intermolecular interactions between epoxy and the CNT surface. The rheological behavior is dominated by aggregate-aggregate jamming. / <p>QC 20180103</p>

Tato práce popisuje historicky první multi-frekvenční rapid-scan EPR. Při zavedení mikrovlnného záření z oblasti 200 GHz a následnou sinusovou modulací bylo dosaženo rychlostí změn frekvence až 61 500 THz/s a zkreslení spekter, známé jako ”wiggles”, bylo pozorováno u obou studovaných vzorků organických radikálů – BDPA v polystyrenové matici a LiPc. Tato práce představuje flexibilní metodu provádění rapid-scan EPR experimentů za použití napětím ovládaného oscilátoru (Voltage Controlled Oscillator; VCO) jako zdroje a zero-bias detektoru (ZBD) pro detekci, čímž se otevírá možnost postupu dále do oblastí vyšších polí / vyšších frekvencí. Dále je popsán postup získání ustáleného spektra z rapid-scan výsledků, známý jako Fourierovská dekonvoluce, a dále je zjistěn spinový dekoherenční čas vzorků pomocí srovnání experimentálních spekter s výsledky numericky vyřešených Blochových rovnic. Výsledné hodnoty jsou 50 ns pro BDPA a 12 ns pro LiPc.

Unconventional superconductivity continues to be one of the most striking chapters in condensed matter physics, by posing challenges to our theoretical understanding of its origin. During the last three decades a large number of unconventional superconductors with exotic properties have been found arising great interest, such as the heavy fermion systems, high Tc cuprates as well as the Iron based superconductors etc. Sr2RuO4, the material I have studied, can be considered as an exemplary case in this regard. In spite of more than two decades of comprehensive research, Sr2RuO4 remains one of the most compelling superconductors till date. Various experimental results give evidence that the superconductivity of Sr2RuO4 is chiral: including measurements of the Kerr effect, sound velocities, critical currents across junctions, and muon spin relaxation(μSR), the experimental technique at the heart of this dissertation. Recent NMR Knight shift measurements suggests that the pairing is most likely spin-singlet, and in the tetragonal lattice of Sr2RuO4, the combination of singlet pairing and chirality compels consideration of an seemingly unlikely order parameter: dxz ± idyz. It is unlikely because it comes along with a horizontal line node at kz = 0, whereas Sr2RuO4 has a very low c-axis conductivity. And that makes the question whether or not the superconductivity of Sr2RuO4 is chiral, of great importance. This calls for an unique scenario in regard to our understanding of unconventional superconductivity, as the presence of chirality in Sr2RuO4 might imply a new form of pairing, which is yet to be firmly determined. Chiral superconductors break time reversal symmetry by definition, and in general time-reversal-symmetry breaking (TRSB) superconductivity indicates complex two component order parameters. Probing Sr2RuO4 under uniaxial pressure offers the possibility to lift the degeneracy between such components. However, despite strenuous efforts, a splitting of the superconducting and TRSB transitions under uniaxial pressure has not been observed so far. In this thesis, I report muon spin relaxation measurements on Sr2RuO4 samples, placed under uniaxial stress. The relatively large sample size suitable for μSR demanded for a customized uniaxial pressure cell in order to perform our experiments. It has been a technically challenging task to have a fully fledged uniaxial pressure cell with stringent requirements, that is suitable for time restricted facility experiments like μSR. The technical advancement has been documented thoroughly in this thesis. Using the dedicated uniaxial pressure cell, we observed the much awaited stress induced splitting between the onset temperatures of superconductivity and time reversal symmetry breaking, consistent with the qualitative expectations for a chiral order parameter in Sr2RuO4. In addition to that, we report the appearance of a bulk magnetic order in Sr2RuO4 under higher uniaxial stress for the first time, above the critical pressure at which a Lifshitz transition is known to occur. The signal in the state appearing at high stress qualitatively differs from that in the TRSB state in unstressed Sr2RuO4, which provides evidence that the enhanced muon spin relaxation at lower stresses is not a consequence of conventional magnetism. As a whole, our results strongly support the idea of two-component superconducting order parameter in Sr2RuO4, that breaks time-reversal symmetry.

Magnetic nanoparticles have received extensive attention in the biomedical research, e.g. as prospective contrast agents for T2-weighted magnetic resonance imaging. The ability of a contrast agent to enhance the relaxation rate of 1 H in its vicinity is quantified by relaxivity. The main aim of this thesis is to evaluate the transversal re- laxivity of ε-Fe2−x Alx O3 nanoparticles coated with amorphous silica or citrate - its dependence on external magnetic field, temperature and thickness of silica coating - by means of nuclear magnetic resonance. The aluminium content x = 0.23(1) was determined from XRF, the material was further characterised by XRPD, Möss- bauer spectroscopy, DLS, TEM and magnetic measurements. The size of magnetic cores was ∼ 21 nm, the thickness of silica coating ∼ 6,10,17 and 21 nm. Magne- tization of the ε-Fe2−x Alx O3 nanoparticles increased by ∼ 30 % when compared to ε-Fe2O3. The saturating dependence of relaxivity on external magnetic field and on the linear decrease with increase of thickness of silica coating contravene the theo- retical model of motional averaging regime (MAR); nevertheless, the temperature dependence acquired in 0.47 T and 11.75 T may be explained by MAR. In compari- son to ε-Fe2O3 nanoparticles, the relaxivity of examined samples was higher for par-...

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