The study of the co-existence of singlet superconductivity and ferromagnetism in bulk materials has been a long standing and intriguing problem in condensed matter physics since the superconductivity and ferromagnetism are quantum mechanically antagonistic to each other (i.e. parallel alignment of spins in the ferromagnet and Cooper pairs with oppositely aligned spins in the superconductor).Though it is incompatible to have the coexistence of singlet superconductivity and ferromagnetism in bulk compound, it is highly possible to artificially fabricate superconductor (S)/ferromagnet (F) heterostructures using various thin film deposition techniques and to study the interplay between the two antagonistic quantum phases over their characteristic length scales. The mutual interaction between the two competing order parameters at the interface in hybrid S/F heterostructures give rise to a variety of novel exotic physical phenomena. Moreover, the spin polarized transport and tunneling experiments in S/F heterostructures seem to be very much useful for providing important information on the spin dependent electronic properties of high Tc superconductors below and above the transition temperature. This can help a lot to understand the long debated unusual electronic properties and pairing mechanism of high Tc superconductors. In addition to the rich fundamental aspects buried in the study of S/F heterostructures, one can also use the spin dependent properties of high Tc superconductors in S/F heterostructures to design new spintronics devices from the application point of view. In this thesis an attempt is made to understand the spin polarized electron transport across S/F heterostructures where the superconductor used is YBa2Cu3O7-δand the ferromagnets are La0.5Sr0.5CoO3, La0.7Sr0.3MnO3, and La0.7Ca0.3MnO3. In addition, the magnetic properties of the La1-x SrxCoO3 system is also investigated in detail. The thesis is organized in six chapters and a brief summary of each chapter is given below. Chapter1 gives a brief introduction to the superconductivity, ferromagnetism and the interplay between superconductivity and ferromagnetism at the interface of S/F heterostructures. It also describes various exotic phenomena and the proximity effect that emerges at the S/F interface due to competing interactions. In addition, it also includes a discussion on various types of indirect magnetic interactions and basic idea about the spin glass ordering in magnetic materials. Chapter 2 outlines the basic principles of various experimental techniques employed for the work presented in this thesis. Chapter 3 describes an extensive magnetic and magnetotransport study of the La1-xSrxCoO3 system to understand the manifestation of various magnetic phases associated with it. The first section of this chapter aims at understanding the phase separation scenario in La0.85Sr0.15CoO3. Since the magnetic behavior of La0.85Sr0.15CoO3 is in the border area of spin glass (SG) and ferromagnetic (F) region in the x-T phase diagram; it has been subjected to a controversial debate for the last several years; while some groups show evidence for magnetic phase separation (PS), others show SG behavior. However, the experimental results presented in this thesis clearly demonstrate that the instability towards PS with inhomogeneous states or competing phases in La0.85Sr0.15CoO3 is not inherent or intrinsic to this compound; rather it is a consequence of the heat treatment condition during the preparation method. It is realized that low temperature annealed sample shows PS whereas the high temperature annealed sample shows the characteristics of canonical SG behavior. The second section of this chapter deals with a detailed study about the possible existence of various magnetic phases of La1-xSrxCoO3 in the range 0 ≤x ≤0.5. The dc magnetization study for x ≥0.18 exhibits the characteristic of ferromagnetic like behavior and for x<0.18, the SG behavior. More strikingly, the dc magnetization studies for x<0.18 rules out the existence of any ferromagnetic correlation that gives rise to irreversible line in the spin glass regime. The ac susceptibility study for x<0.18, exhibits a considerable frequency dependent peak shift, time-dependent memory effect, and the characteristic spin relaxation time scale τo ~10-13s, all pointing towards the characteristics of SG behavior. On the other hand, the ac susceptibility study in the higher doping ferromagnetic side exhibits the coexistence of glassy and ferromagnetic behavior. The glassiness is interpreted in terms of inter-cluster interaction. The reciprocal susceptibility vs. T plot in the paramagnetic side adheres strictly to Curie-Weis behavior and does not provide any signature for the pre-formation of ferromagnetic clusters well above the Curie temperature. The magnetotransport study reveals a cross over from metallic behavior to semiconducting like behavior for x ≤0.18 and the system exhibits a peak in MR in the vicinity of Tc on the metallic side and a large value of MR at low temperature on the semiconducting side. Such high value of MR in the semiconducting spin glass regime is strongly believed due to spin dependent part of random potential distribution. Based on the present experimental findings, a revised phase diagram has been constructed and each phase has been characterized with its associated properties. Chapter 4 deals with a comprehensive study of thickness dependent structural, magnetic and magnetotransport properties of oriented La0.5Sr0.5CoO3 thin films grown on LaAlO3 by pulsed laser deposition. The films are found to undergo a reduction in Curie temperature with decrease in film thicknesses and it is primarily caused by the finite size effect since the finite scaling law holds good over the studied thickness range. The contribution from strain induced suppression of the Curie temperature with decreasing film thickness is ruled out since all the films exhibit a constant out of plane tensile strain (0.5%) irrespective of their thickness. The coercivity of the films is observed to be an order of magnitude higher than that of the bulk. This is attributed to the local variation of the internal strain that introduces strong pinning sites (via. magnetoelastic interaction) for the magnetization reversal. In addition, an increase in the electrical resistivity and coercivity is observed with decrease in film thickness and it is strongly believed to be due to the interface effect. Chapter5 reports on the investigation of the effect of ferromagnetic layer on (i) pair breaking effect and (ii) vortex dynamics in different superconducting(S)/ ferromagnetic (F) bi-layers grown by pulsed laser deposition. The current (I) dependent electrical transport studies in the S/F bi-layers exhibit a significant reduction in the superconducting transition temperature with the increase in applied current as compared to single YBa2Cu3O7-δlayer and it follows I2/3 dependence in accordance with the pair breaking effect. Moreover, the superconducting transition temperature in YBa2Cu3O7-δ/ La0.7Sr0.3MnO3 bilayer is surprisingly found to be much larger than the YBa2Cu3O7-δ/La0.5Sr0.5CoO3. It appears that the current driven from a material with low spin polarization (-11%) like La0.5Sr0.5CoO3 can also suppress the superconductivity to a larger extent. This indicates that the degree of spin polarization of the ferromagnetic electrode is not the only criteria to determine the suppression of superconductivity by pair breaking effect in superconductor/ferromagnet hybrid structures; rather the transparency of the interface for the spin polarization, the formation of vortex state due to the stray field of ferromagnetic layer and the ferromagnetic domain patterns might play significant roles to determine such effect. More interestingly, the spin diffusion length in YBa2Cu3O7-δis found have a much longer length scale than that reported earlier in the study of F/ S heterostructures. The activation energy (U) for the vortex motion in S/F bilayers is reduced remarkably by the presence of the F layers. In addition, the U exhibits a logarithmic dependence on the applied magnetic field in the S/F bilayers suggesting the existence of decoupled 2D pancake vortices. This result is discussed in terms of the reduction in the effective S layer thickness and the weakening of the S coherence length due to the presence of F layers. Chapter 6 deals with the magnetotransport study on two different kind of F/S/F trilayers viz. La0.7Sr0.3MnO3/YBa2Cu3O7-δ/La0.7Sr0.3MnO3 and La0.5Sr0.5CoO3/YBa2Cu3O7-δ/La0.7Ca0.3MnO3 with changes in superconducting and ferromagnetic layer thickness. The activation energy for the vortex motion in F/S/F trilayer is found to decrease considerably as compared to S/F bilayer and it also exhibits a logarithmic dependence on magnetic field which gives the signature of existence of decoupled 2D pancake vortices. The magnetotransport study reveals that a much lower magnetic field is required to suppress the superconductivity in trilayer as compared to single YBCO layer. Moreover, the transport study also reveals that a threshold thickness of YBCO is required for the onset of superconductivity in trilayer structure and the onset of superconducting Tc increases with increase in YBCO thickness. More strikingly, a remarkable unconventional anisotropic superconducting Tc (Tc H║c-axis<Tc H⊥c-axis) is observed in La0.5Sr0.5CoO3/YBa2Cu3O7-δ/La0.7Ca0.3MnO3 trilayer for the magnetic field applied parallel and perpendicular to c-axis. The trilayer system also exhibits a huge positive magnetoresistance (MR) below superconducting Tc and it could arise due to vortex dissipation in liquid state of superconductor in the tri-layer structure. Finally, the thesis concludes with a general conclusion and an outlook in this area of research.

Les supraconducteurs à hautes températures sont considérablement utilisés dans des applications telles que des machines électriques. La conception de telles machines requiert une évaluation précise des pertes AC générées par leurs bobinages de câbles supraconducteurs multifilamentaires torsadés. Ainsi, des outils numériques robustes et précis sont indispensables afin de modéliser rapidement en 3D le comportement de tels câbles. Dans ce manuscrit, deux approches numériques dont une approche de type galerkin discontinue furent développées afin de simplifier considérablement la modélisation 3D de ce type de câbles. Elles furent appliquées à la formulation en H couplée aux effets thermiques. La modélisation de cas simples a permis de valider ces approches en les comparant à celle des éléments finis implémentée sur Comsol. Puis, une transformation géométrique fut proposée afin de modéliser de façon équivalente en 3D, quelque soit la configuration en champ magnétique, des câbles à filaments supraconducteurs droits à la place de filaments torsadés. De cette transformation, un modèle d'ordre réduit fut développé et validé afin de simplifier considérablement la modélisation 3D de ce type de câbles. À partir de ce modèle réduit, l'influence du champ elliptique sur les pertes par aimantation d'un échantillon de 100 câbles de 54 filaments de MgB ₂ torsadés fut modélisé en moins d'une journée. Par ailleurs, des premières études empiriques montrant la faisabilité d'une homogénéisation furent brièvement présentées et validées pour des câbles ayant une seule couche de filament. / High temperature superconductors are increasingly being used for several applications such as electrical machines. Thus the design of suchdevices ultimately requires an accurate evaluation of AC losses generated by superconducting coils sometimes made of twisted multifilamentary wires.The development of robust numerical tools geared towards the 3 D modeling of such wires is therefore needed. In this manuscript, the main objective isto develop numerical approaches allowing considerable simplifications of the modelling of twisted multi-filamentary superconducting wires in 3 D. First, two numerical approaches such as the discontinuous galerkin method applied on the thermally coupled H -formulation were developed. They were compared and validated on simple cases using the finite element method implemented in Com-sol. Then, a well-defined mapping was proposed to simply model in 3 D, for any magnetic field configuration, straight multifilamentary wires instead oftwisted ones. An application of this mapping allowed the development of a model-order reduction approach which simplify considerably the mod-elling of twisted wires in 3 D. Thus, the elliptical magnetic fields impact on magnetization losses was accurately modeled in less than a day with the reduced approach applied on 100 MgB ₂ wires with 54 twisted filaments. As a research perspective on the reduced model advanced applications, an homogenization, empirically defined, was briefly presented for wires with single layer only.

This master thesis is focused on temperature dependence of magnetization curves and susceptibility of thin films of type-I superconductor. A model for susceptibility of type-I superconductor in intermediate state is presented. This model is compared with experimental data yielding temperature dependence of critical magnetic field of superconductor. Furthermore it is shown that sufficiently thin film of superconductor which is type-I in bulk can exhibit type-II behaviour in perpendicular magnetic field. Susceptibility measured on such a film is therefore compared to susceptibility calculated for Bean model for type-I superconductors.

Ziel dieser Arbeit war die Untersuchung des Einflusses epitaktischer Verspannung auf die Eigenschaften von dünnen Schichten eisenbasierter Supraleiter. Dafür wurden erstmalig epitaktische Schichten des Materials Ba(Fe1−xNix)2As2 mit unterschiedlichem Nickelgehalt mithilfe der gepulsten Laserdeposition hergestellt und ihre strukturellen und elektrischen Transporteigenschaften charakterisiert. Die Ergebnisse wurden mit Massivproben, sowie mit Dünnschichten des verwandten Systems Ba(Fe1−xCox)2As2 verglichen. Dabei wurde ein maximales Tc von 21,6K gemessen, was die entsprechenden Werte für Massivproben dieses Materials übersteigt. Je nach verwendetem Substrat führt die induzierte stauchende oder dehnende mechanische Verspannung zu einer Verschiebung des elektronischen Phasendiagrammes. Die Wechselwirkung mit magnetischen Fluktuationen nahe des antiferromagnetischen Phasenübergangs führt zudem in Dünnschichten zu einer starken Erhöhung des Anstieges des oberen kritischen Magnetfeldes nahe der Sprungtemperatur. Untersuchungen des magnetischen Phasendiagrammes in hohen Magnetfeldern zeigen für Ba(Fe1−xNix)2As2 ein ähnliches Verhalten wie im Co-dotierten System. Die Messungen ergaben bei niedrigen Temperaturen eine geringe Anisotropie des oberen kritischen Feldes, während die Anisotropie des Irreversibilitätsfeldes aufgrund der vorherrschenden Defektstruktur erhöht ist. Des Weiteren wurden epitaktische Dünnschichten des Supraleiters FeSe1−xTex erstmalig auf dem Halbleitersubstrat GaAs abgeschieden. Dabei wurden Sprungtemperaturen von bis zu 17,4K erreicht. Das Wachstum auf speziellen mehrlagigen GaAs-Architekturen ermöglichte zudem die Realisierung dreidimensionaler Mikroobjekte, bei denen sich die Dünnschicht aufgrund von Relaxation epitaktischer Verspannung des Substrates zu Helices aufrollt. Mechanische Defekte führten jedoch dazu, dass keine supraleitenden Eigenschaften gemessen werden konnten. In diesem Fall ist eine weitere Optimierung der Mikrostrukturierungsprozesse notwendig. / In this work, we studied the influence of epitaxial strain on the properties of iron based superconducting thin films grown by pulsed laser deposition. Epitaxial films of Ba(Fe1-xNix)2As2 have been realised for the first time using different nickel doping contents. Afterwards their structural and superconducting properties have been characterised. The results were compared to bulk samples as well as to thin films of the related compound Ba(Fe1-xCox)2As2. A maximum Tc of 21,6 K was measured, which exeeds the highest reported values of bulk samples. Depending on the used substrate, the phase diagram is shifted due to the induced tensile or compressive strain in the films. Compared to bulk samples, the slope of the upper critical field is strongly enhanced near the critical temperature due to antiferromagnetic fluctuations. The magnetic phase diagram measured in high fields shows simularities with the isostructural Co-doped system. The measurements reveal a small anisotropy of the upper critical field for low temperatures, while the anisotropy of the irreversibility field is increased due to the defect structure in the film. Furthermore, epitaxial thin FeSe1-xTex films have been deposited on GaAs as a new substrate material for iron based superconducting thin films achieving a critical temperature of up to 17,4 K. The self-organised formation of threedimensional micro helices by strain relaxation was realised by the preparation of epitaxial films on customized GaAs-based multilayer achitectures. However, mechanical defects prevented the superconducting characterisation. Therefore, a further improvement of the involved processes for microstructuring is necessary.

Organic materials with fascinating/intriguing electronic properties have been the driving force for many research activities in the past, and in particular for important progress in materials science covering both new functional materials as well as theoretical developments. In addition, charge transfer, i. e., the addition or removal of charges to or from molecules in organic solids is one route to modify and control their electronic properties. Recently, the discovery of superconductivity in several alkali metal intercalated hydrocarbon systems (picene, phenanthrene, coronene and 1,2;8,9-dibenzopentacene) with rather high transition temperatures has opened a new chapter in organic material science as well as solid-state physics. The search for a microscopic understanding of the mechanism that drives materials superconducting always has initiated a large number of scientific activities, and there are numerous examples where these activities have provided major advancement. A basic foundation of this understanding is the knowledge of the electronic properties of the material under investigation. In this context, this thesis reports first, very detailed insight into the electronic structure of both undoped as well as potassium doped picene, coronene and 1,2;8,9-dibenzopentacene using electron energy-loss spectroscopy (EELS) as main experimental method. Additionally, also photoemission spectroscopy experiments have been performed to investigate the occupied electronic density of states close to the chemical potential. In order to learn more about the electronic structure we have compared the results we obtained from EELS and photoemission spectroscopy with theoretical calculations based on Density functional theory (DFT) using the local-density approximation (LDA). We identify the peculiar case of very close lying conduction bands that upon doping harbour the electrons that form the Cooper-pairs in the superconducting state. Moreover, the presented data display substantial changes in the electronic excitation spectrum upon doping, whereas in the doped case the appearance of one new peak (for picene) and several new peaks (for coronene and 1,2;8,9-dibenzopentacene) in the former optical gap is reported. By using a Kramers–Kronig analysis (KKA) it is possible to gain information about the nature of this doping introduced excitations. In particular, in case of picene, the new low energy feature can be assigned to a charge carrier plasmon. Interestingly, this plasmon disperses negatively upon increasing momentum transfer, which deviates significantly from the traditional picture of metals based on the homogeneous electron gas. The comparison with calculations of the loss function of potassium intercalated picene shows how this finding is the result of the competition between metallicity and electronic localization on the molecular units. Furthermore, core level excitation measurements show the reduction of the lowest lying C 1s excitation feature, which clearly demonstrates that potassium intercalation leads to a filling of the conduction bands with electrons. Additionally, the measurements of potassium intercalated 1,2;8,9-dibenzopentacene clearly indicate the formation of particular doped phases with compositions K_xdibenzopentacene (x = 1, 2, 3), whereas the data suggest that K_1dibenzopentacene has an insulating ground state with an energy gap of about 0.9 eV, while K_2dibenzopentacene and K_3dibenzopentacene might well be metallic, because of the absent of an energy gap in the electronic excitation spectra. Interestingly, a comparison of the photoemission as well as EELS spectra of undoped 1,2;8,9-dibenzopentacene and pentacene reveal that the electronic states close to the Fermi level and the electronic excitation spectra of the two materials are extremely similar, which is due to the fact, that the additional two benzene rings in 1,2;8,9-dibenzopentacene virtually do not contribute to the delocalized pi molecular orbitals close to the Fermi level. This close electronic similarity is in contrast to the behavior upon potassium doping, where evidence for a Mott state has been reported in the case of pentacene. A comparison of the low energy excitation spectra of chrysene with picene (phenacenes) as well as tetracene with pentacene (acenes) crystals reveal a significant difference between the former and the latter two materials. While for the phenacenes (zigzag arrangement) the excitation onset is characterized by up to five weak excitation features with only small anisotropy and without visible Davydov splitting within the a*, b*-planes, the acene (linear arrangement) spectra are dominated by a large excitation close to the onset and a sizable Davydov splitting. The presented data show further that the spectral shape of the pentacene excitation spectrum provides clear evidence for a large admixture of molecular Frenkel-type excitons with charge-transfer excitations resulting in excited states with a significantly mixed character. This conclusion is in good agreement with recent advanced calculations which predicted a charge-transfer admixture to the lowest singlet excitation which is significantly dependent upon the length of the acene molecules. Moreover, also for picene and chrysene we observe differences which point towards an increased charge-transfer contribution to the singlet excitation spectrum in the former. Finally, investigations of the electronic properties of undoped and potassium doped chrysene, a close relative of picene, show that the doping introduced changes are in a similar range such as observed in case of picene. Interestingly, due to the analogy between the observed changes in the electronic structure upon potassium doping between chrysene and picene and further similarity in the crystal structure we speculate that chrysene is a promising candidate for another aromatic hydrocabon superconductor.

This work gives insight in some key aspects for the understanding of the origin of high-temperature superconductivity in the newly discovered class of iron-based materials. In particular, thermodynamic methods, such as SQUID magnetometry, specific heat and dilatometry were used, in order to (i) assess the evolution of electronic correlations in a series of transition metal substitutions of the well-known BaFe2As2 as a function of 3d band filling and (ii) to re-investigate the phase diagram of Co-doped LaFeAsO on single crystals, with particular interest in the interplay between the nematic/magnetic phase of the parent compound and superconductivity induced by in-plane electron doping. In the first part of this work, the Sommerfeld coefficient (γ_exp) was extracted from the low temperature specific heat data and compared with the theoretical values obtained by band theory calculations, in order to obtain the mass enhancement (m∗/mb) in the series BaT2As2 (T = Cr, Mn, Fe, Co, Ni, Cu). The results clearly show an overall decrease of the electronic correlations while departing from the half-filled (3d5) to the fully filled configuration (3d10), thus suggesting a highly correlated 3d5 state. The evolution of electronic correlations as a function of 3d band filling for n > 5 is in agreement with previous theoretical calculations, underlining the importance of Hund’s coupling in describing the normal-state properties of iron-based superconductors. In addition, it was found that the decrease in m∗/mb for n > 5 follows an increase of the crystal field splitting (Δ), determined by the progressive distortion of the As-T-As angle (α_bond) from the ideal tetrahedral environment. This study reveals a complex interplay between electronic correlations, band filling and crystal structure in determining the physical properties of 122 systems. In the second part, the phase diagram of Co-doped LaFeAsO was re-investigated using single crystals by thermodynamic methods. From magnetic susceptibility studies we track the doping evolution of the antiferromagnetic phase, revealing a continuous decrease of T_N up to 5% Co doping. In order to study the evolution of the so-called nematic phase, the temperature dependence of the length changes along the a and b orthorhombic directions, ΔL/L_0, was determined by high-resolution capacitance dilatometry. The results clearly show a gradual reduction of the orthorhombic distortion δ and of T_S with increasing Co content up to 4.5%, while it is completely suppressed for 7.5% Co. Bulk superconductivity with T_c = 10.5 K was found in a small doping region around 6% Co content, while both T_c and the superconducting volume fraction rapidly drop in the neighbouring doping regime. Ultimately, no microscopic coexistence between the superconducting and magnetic phases can be assessed within our resolution limit, in sharp contrast with other iron-pnictide families, e.g., electron- and hole-doped BaFe2As2.

We study the unusual phases seen in charge transfer salts (CTS) at 1/2 and 1/4 filling. We use the Holstein-Hubbard model (HHM) and the Peierls extended Hubbard model (PEH) to study competing phases in CTS. In the 1/2illed HHM the Holstein coupling promotes a Peierls charge-density wave phase while the on-site Coulomb repulsion U gives rise to antiferromagnetic correlations and a Mott insulating state. Takada et al. have shown possibility of a third metallic phase between the Mott and the Peierls phase. We investigate the presence of an intermediate phase between the Mott and Peierls phase using Stochastic Series Expansion (SSE) method. We used charge and spin susceptibilities to determine the phase boundaries. As the coupling is increased a spin gap opens followed by the Peierls transition. The intermediate phase is metallic and has a spin gap but no charge gap. Transitions from the Mott to intermediate and intermediate to Peierls state are Kosterlitz-Thouless type (KT). As the coulomb repulsion is increaed beyond certain value the two KT transitions fuse to give a single first order transition. Similar behavior is seen at 1/4illed HHM. We also studied the temperature dependence of charge ordering (CO) in 1/4illed CTS. Most previous theoretical studies of the on CTS have concentrated on ground state or T=0 properties. Here we show the evolution of charge ordered (CO) state with temperature and directly related the experimental phase diagram with our theoretical results. Our calculations show that as temperature is lowered the Wigner crystal state gives way to spin-Peierls state with a different pattern of CO. Also we show that the critical value of nearest neighbor Coulomb repulsion is depends on the total spin and is different for different spin subspace.

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No description available.

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