Thesis (MScEng (Electrical and Electronic Engineering))--University of Stellenbosch, 2010. / ENGLISH ABSTRACT: This thesis presents an attempt at creating a fully functional SQUID for the purposes of a predefined application. The goal of the work is to provide a method of development, primarily utilising the facilities of the Engineering Faculty of the University of Stellenbosch, with minimal assistance from other departments. This method is then analysed and the successes and failures discussed in order to provide guidelines and recommendations for future research. The device consists of a gradiometric SQUID, as well as electronics which provide the SQUID bias current, output linearisation and output signal filtering. YBCO is used for the superconducting material, allowing the use of liquid nitrogen as coolant which eases the operation and portability of the device. Various methods of creating Josephson junctions are tested, such as constriction bridges using AFM lithography and step-edge junctions, with and without different buffer layers. Proof of concept simulations demonstrate the viability of the device. Unfortunately, a functional device could not be constructed, mostly due to the design requiring higher levels of resolution and process control than some of the available facilities can provide. Recommendations are provided for future researchers. / AFRIKAANSE OPSOMMING: Hierdie tesis beskryf ’n poging om ’n volledige funksionele SQUID te vervaardig vir die doeleindes van ’n vasgestelde toepassing. Die doel van die werk is om ’n metode te voorsien wat hoofsaaklik gebruik maak van die fasiliteite van die Ingenieurswese Fakulteit van die Universiteit van Stellenbosch, met minimale hulp van ander departemente. Hierdie metode word dan ondersoek en die suksesse en mislukkings bespreek om riglyne en voorstellings te voorsien vir toekomstige navorsing. Die toestel bestaan uit ’n gradiometriese SQUID, sowel as elektronika wat voorsiening maak vir voorspanning, uittree-linearisering en ’n uittree-filter. YBCO is as supergeleidende materiaal gebruik, wat die gebruik van vloeibare stikstof as verkoeler moontlik maak en dus die hantering en draagbaarheid van die toestel vergemaklik. Verskillende metodes om Josephson-vlakke te vervaardig is getoets, onder andere vernouingsbrugvlakke deur middel van AFM litografie en stapvlakke met en sonder bufferlae. Bewys van konsep simulasies demonstreer die lewensvatbaarheid van die toestel. Ongelukkig kon ’n funksionele weergawe van die toestel nie vervaardig word nie, hoofsaaklik as gevolg van die ontwerp wat hoër resolusievlakke en beter prosesbeheer benodig as wat sekere van die beskikbare fasiliteite kan voorsien. Aanbevelings word voorsien vir toekomstige navorsers.

One of the challenges facing condensed matter physics nowadays is to understand the electronic structure of high temperature superconductors. This dissertation compiles our contribution to the experimental information concerning this subject. Tunneling conductance spectroscopy a technique capable of probing the electronic density of states in hybrid structures was used to study the current and spin transport properties across junctions between metallic counterelectrodes and Bi2Sr2CaCu2O8- (BSCCO) crystals. Since in these structures the transport is mediated by transmission channels depending on superconductive characteristics, the energy resolved density of states is a signature of the mechanism of superconductivity. For instance, one can observe the superconductive energy gap and the behavior of subgap bound states due to phase sensitive Andreev reflections at the junction interface. In particular, tunneling spectroscopy makes possible the observation of the LOFF state characterized by the coexistence of superconductivity and magnetism. Cuprates like BSCCO are highly anisotropic materials and their superconductivity is almost two dimensional, being confined in the CuO2 planes. Therefore, our junctions combine monocrystals of underdoped samples of BSCCO with various thin film counterelectrodes normal metal (Ag), conventional superconductor (Pb) and ferromagnetic metal (Fe) deposited perpendicular onto the cuprate ab-plane (CuO2 plane). We performed measurements on Ag/BSCCO junctions for two current injection directions into the same crystal. We observed that, near the 110 crystal surface, the conductance spectra show a high zero bias peak (ZBCP) which is a manifestation of zero energy Andreev bound states due to an anisotropic superconductive order parameter. Near the 100 surface, the ZBCP is largely suppressed. This is consistent with a predominantly 2 2 x y d - -wave pairing symmetry. In some cases, the ZBCP splits or decreases in amplitude at low temperatures. This is consistent with the existence of a subdominant s-wave (or xy d ) resulting in a mixed d is + state which breaks time reversal symmetry (BTRS). Since we observe this phenomenon in the underdoped case, we do not confirm the possibility of a quantum critical point close to the optimal doping. Our Pb/BSCCO spectra contradict the theory explaining the BTRS by proximity effect. The Fe/BSCCO junctions measure the effect of spin polarization. We explain the recorded 4-peak asymmetric structure by the combined effect of a spin independent BTRS state and a spin filtering exchange energy in the barrier responsible for a large ZBCP splitting. The LOFF state was observed in the proximity region induced on the ferromagnetic side of multilayered-Fe/Ag/BSCCO structures. As expected for the LOFF order parameter, the spectra develops coherent damped oscillations with the Fe layer thickness probing different regions. The magnitude and sign of the oscillation depends on the energy. The conductances at energy zero or equal to the superconductive gap are modulated in antiphase proving that the order parameters takes successively positive and negative values. Changing the junction orientation with 4 p , results in an opposite behavior for the same distance. The maximal amplitudes in one direction is replaced by minima, showing that, besides space, the LOFF state modulation depends on the phase of the high temperature order parameter inducing the proximity

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Strong electron-electron correlations and lattice frustration are two physical interactions that pose serious challenges to condensed matter physics. A variety of exotic physical phenomena, for example, charge ordering, spin liquid, and unconventional superconductivity, are believed to arise from the interplay of the two interactions. In this dissertation, I examine two families of systems which exhibit both electron-electron correlations and lattice frustration – charge transfer solids and layered cobaltates. The half-filled band Hubbard model on the triangular lattice has been proposed by mean-field theories as the minimal model for the superconductivity in the charge transfer solids. In the first part of this dissertation, by using exact calculations, I prove the absence of superconductivity in this model. This result calls for a new theoretical approach to describe the rich physics in charge transfer solids. In the second part of this dissertation, I study charge transfer solids by focusing on its real bandfilling ¼. I show that a new kind of insulating phase, paired electron crystal, emerges from antiferromagnetism as the frustration is increased. The paired electron crystal state can explain the various insulating states adjacent to the superconducting state, thus provides a new avenue towards the understanding of the unconventional superconductivity in charge transfer solids and other ¼ filled systems. In the third part of this dissertation, I investigate the carrier concentration-dependent electronic behavior in layered cobaltates. I provide a natural yet simple explanation for this behavior. I show that it can be described within correlated-electron Hamiltonians with finite on-site and significant nearest neighbor hole-hole Coulomb repulsions. I also point out the similarities between organic charge transfer solids and layered cobaltates, which may involve superconductivity.

High-pressure techniques have become increasingly important in the synthesis of ceramic and metallic solids allowing the discovery of new materials with interesting properties. In this research dense solid oxides have been synthesised at high pressures, and structural investigations have been conducted using x-ray and neutron diffraction. The perovskite LaPdO3 has been synthesised at pressures of 6{10GPa. Neutron diffraction studies have been carried out from 7{260K to investigate any structural distortions, particularly related to the possibility of charge order at low temperatures. No reduction in symmetry associated with charge ordering has been observed; the material appears to remain metallic with only one unique Pd site down to 7K. LaPdO3 adopts the GdFeO3-type Pbnm structure. The PdO6 octahedra exhibit a tetragonal distortion throughout the temperature range with a shortening of the apical Pd{O bonds of 2:5% relative to the equatorial bonds. Attempts to prepare analogues of the perovskite containing smaller rare earths have resulted in multi-phase samples, and further RPdO3 perovskites remain inaccessible although there is evidence for a small amount of the perovskite phase in the products of synthesis attempts with neodymium. Three new oxypnictide superconductors, RFeAsO1 xFx (R = Tb, Dy and Ho) have been synthesised at 7{12GPa. The materials are isostructural with other recently discovered iron arsenide superconductors and have Tc's of 52:8 K, 48:5K and 36:2K respectively, demonstrating a downturn in Tc in the series for smaller R. Systematic studies on TbFeAsO0.9F0.1 and HoFeAsO0.9F0.1 show negative values of dTc=dV in contrast to those reported for early R containing materials. Low-temperature neutron diffraction measurements on both materials, and synchrotron studies on HoFeAsO0.9F0.1 reveal no tetragonal to orthorhombic transitions as observed in early R-containing materials with lower doping levels. Magnetic reflections are evident but they are shown to be from R2O3 and RAs impurities with TN's of 5:5K for Tb2O3, 6:5K for HoAs and 1:7K < TN < 4K for Ho2O3. The implications of these results for superconductivity in the iron arsenides are discussed.

This thesis describes inelastic neutron scattering (INS) experiments on several iron-based materials. The experiments were primarily designed to investigate the link between magnetic dynamics and superconductivity. The work contributes to evidence that magnetic fluctuations influence or are influenced by superconductivity. It is demonstrated that the INS response of a material, in conjunction with theoretical models, can provide valuable information about both superconductivity and magnetism. I measured the magnetically ordered parent-compound SrFe2As2 to investigate the nature of magnetism in iron-based systems. Comparison of the data to models based on both itinerant and localised magnetism showed that an itinerant model offers the best description of the data. LiFeAs is a superconductor that shows no magnetic order, however I was able to distinguish a magnetic signal in its INS spectrum. The signal is consistent with the magnetic resonance observed in several other iron-based superconductors. This indicates that LiFeAs likely hosts an s± gap symmetry. I investigated two iron-phosphide systems, LaFePO and Sr2ScO3FeP, and in this case I was unable to identify any magnetic scattering. Comparison to LiFeAs showed that any signal in LaFePO is at least 7 times weaker. These results suggest that magnetic fluctuations are not as influential to the electronic properties of iron-phosphide systems as they are in other iron-based superconductors. In CsxFe2−ySe2 I found two independent signals that appear to be related to phase-separated magnetic and superconducting regions of the sample. I showed that fluctuations associated with the magnetically ordered phase are consistent with localised magnetism, and do not respond to superconductivity. The second signal, however, increases in intensity below the superconducting transition temperature Tc = 27K, consistent with a magnetic resonance. This could be indicative of a pairing symmetry in CsxFe2−ySe2 that is distinct from most other iron-based superconductors. Finally, the molecular intercalated FeSe compound Li0.6(ND2)0.2(ND3)0.8Fe2Se2 revealed strong magnetic fluctuations. Again the signal was consistent with a magnetic resonance responding to Tc = 43 K. The results suggest that Lix(ND2)y(ND3)1−yFe2Se2 is similar to the superconducting phase of CsxFe2−ySe2, placing constraints on theoretical models to describe the molecular intercalated FeSe compounds.

One of the most central concepts in condensed matter physics is the electronic band structure. Although band theory was established more than 80 years ago, recent developments have led to new insights that are formulated in the framework of topological band theory. In this thesis a subset of topological band theory is presented, with particular focus on topological supercon- ductors and accompanying Majorana fermions. While simple models are used to introduce basic concepts, a physically more realistic model is also studied intensely in the papers. Through self- consistent tight-binding calculations it is confirmed that Majorana fermions appear in vortex cores and at wire end points when the superconductor is in the topologically non-trivial phase. Many other properties such as the topological invariant, experimental signatures in the local density of states and spectral function, unconventional and odd-frequency pairing, the precense of spin-polarized currents and spin-polarization of the Majorana fermions, and a local π-phase shift in the order parameter at magnetic impurities are also investigated.

The physics of the series Pr_yY_1-yBa₂Cu₃O_6&plus;x, and ability of Pr to suppress superconductivity, has been a subject of frequent discussions in the literature for more than a decade. This thesis describes a polarised neutron diffraction (PND) experiment performed on PrBa₂Cu₃O_6.24 designed to find out something about the electron structure. This experiment pushed the limits of what can be done using the PND technique. The problem is one of a limited number of measured Fourier components that need to be inverted to form a real space image. To accomplish this inversion the maximum entropy technique has been employed. In some cases, the maximum entropy technique has the ability to increase the resolution of ‘inverted’ data immensely, but this ability is found to depend critically on the choice of constants used in the method. To investigate this a Bayesian robustness analysis of the maximum entropy method is carried out, resulting in an improvement of the maximum entropy technique for analysing PND data. Some results for nickel in the literature have been re-analysed and a comparison is made with different maximum entropy algorithms. Equipped with an improved data analysis technique and carefully measured PND data for PrBa₂Cu₃O_6.24 a number of new interesting features are observed, putting constraints on existing theoretical models of Pr_yY_1-yBa₂Cu₃O_6&plus;x and leaving room for more questions to be answered.

This thesis reports the synthesis and characterisation of the layered oxypnictides Sr₂MO₃FeAs (M = Sc, V and Cr) and CeOMnAs. In these materials the choice of transition metal cation at the tetrahedral site in the arsenide layer chiefly dictates the physical properties that are observed. The bulk of this work has focussed on the development of a new family of iron arsenide superconductor with the general formula Sr₂MO₃FeAs (M = Sc, V, Cr). This structure is comprised of anti-PbO-type [FeAs]^- layers which alternate with insulating [Sr₂MO₃]⁺ oxide fragments that resemble a portion of the K₂NiF₄ structure. In contrast to other FeAs parent materials, no member of the Sr₂MO₃FeAs family exhibits any strong evidence for long range Fe order or a tetragonal to orthorhombic distortion upon cooling. Attempts to electron and hole dope Sr₂ScO₃FeAs into the superconducting regime have as yet been unsuccessful. Although Sr₂ScO₃FeAs shows no evidence for Fe ordering, a checkerboard arrangement of Cr³⁺ spins in the ab-plane is observed below 40 K (k = (½, ½, 0)) analogous to that seen in Pr₂CuO₄. The partial substitution of Fe²⁺ (d⁶) by Co²⁺ (d⁷) in Sr₂CrO₃Fe_1-xCo_xAs has been shown to be a fruitful strategy for electron-doping this material into the superconducting regime with T_c maximised at 18 K in Sr₂CrO₃Fe_0.92Co_0.08As. It is also established that this substitution influences the ordering on the Cr sub-lattice with a doubling in the size of the magnetic cell along the c axis (k = (½, ½, ½)). Sr₂VO₃FeAs, a rare example of an “undoped” superconductor (T_c = 25 K), is shown to be electron-doped by mixed valence vanadium +3.13(5). Magnetometry measurements also reveal a series of magnetic transitions in Sr₂VO₃FeAs, however μSR and powder neutron diffraction studies suggest that this system is some way from commensurate long range order. In contrast to Sr₂CrO₃FeAs, electron-doping strategies in Sr₂VO₃FeAs have the effect of decreasing T_c and ultimately suppressing superconductivity entirely as Sr₂V_1-xTi_xO₃FeAs and Sr₂VO₃Fe_1-xCo_xAs materials are over electron-doped. Sr₂V_1-xMg_xO₃FeAs samples were also prepared, but rather than this strategy hole-doping the FeAs layer it preferentially oxidises vanadium towards V⁴⁺. This substitution also has a considerable effect on the superconducting critical temperature (T_c) which is raised as high as 31 K in Sr₂V_0.775Mg_0.225O₃FeAs. The isovalent substitution of Sr²⁺ by Ca²⁺ in Sr_2-xCa_xVO₃FeAs has been shown to strongly influence the superconducting properties of this material and a clear correlation between the evolution of T_c and the shape of the FeAs₄ tetrahedron has been established. These results demonstrate that superconductivity in iron-based superconductors is extremely sensitive to both electron count and the crystal structure. Finally, investigations into the manganese oxide arsenide CeOMnAs reveal room temperature ordering of Mn²⁺ spins and a spin reorientation transition of Mn moments at 36 K. This transition is concomitant with Ce ordering and an apparent weak structural distortion, demonstrating that f electrons are able to dictate the orientation of Mn moments.