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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
121

Magnetism and Superconductivity in Iron-based Superconductors as Probed by Nuclear Magnetic Resonance

Hammerath, Franziska 15 December 2011 (has links)
Nuclear Magnetic Resonance (NMR) has been a fundamental player in the studies of superconducting materials for many decades. This local probe technique allows for the study of the static electronic properties as well as the low energy excitations of the electrons in the normal and the superconducting state. On that account it has also been widely applied to Fe-based superconductors from the very beginning of their discovery in February 2008. This dissertation comprises some of these very first NMR results, reflecting the unconventional nature of superconductivity and its strong link to magnetism in the investigated compounds LaO(1-x)F(x)FeAs and LiFeAs.:1. Introduction 2. Basic Principles of NMR 3. NMR in the Superconducting State 4. Iron-based Superconductors 5. Experimental Setup 6. NMR on LaO(1-x)F(x)FeAs in the Normal State 7. MR and NQR on LaO(1-x)F(x)FeAs in the Superconducting State 8. NMR and NQR on LiFeAs 9. Conclusions
122

Thermische Tieftemperatureigenschaften von Seltenerd-Übergangsmetall-Borkarbiden

Lipp, Dieter 12 April 2002 (has links)
The present work reports on thermal low-temperature properties of rare earth transition metal borocarbides such as specific heat, thermal conductivity and thermopower. The influence of structural disorder, caused by stoichiometric variations and substitutions of the rare earth element or the transition metal, on the thermal and superconducting low-temperature properties is investigated. The structural disorder results in the reduction of the superconducting transition temperature Tc, of the Sommerfeld value gamma, of the upper critical magnetic field Hc2(0), of the negative curvature of the H-dependence of the T-linear specific heat contribution gamma(H), and in the reduction of the positive curvature of Hc2(T) near Tc. But isoelectronic rare earth substitutions do not result in the transition from clean to dirty limit. Due to Pt-substitutions similar reductions of thermal and superconducting properties are observed. The behaviour of Hc2(0) and the concentration dependence of the positive curvature of Hc2(T) near Tc point to the transition from clean to quasi-dirty limit in the case of Pt-substitutions. / In der vorliegenden Arbeit werden Untersuchungen zu thermischen Tieftemperatureigenschaften, wie der spezifischen Wärmekapazität, der Wärmeleitfähigkeit und der Thermokraft, an supraleitenden Seltenerd-Übergangsmetall-Borkarbiden vorgestellt. Es wurde der Einfluß von gezielt hervorgerufener Unordnung im kristallographischen Aufbau, die durch isoelektronische Substitutionen des Seltenerd-Elements und des Übergangsmetalls sowie durch Söchiometrievariationen erzeugt wurde, auf die thermischen und supraleitenden Tieftemperatureigenschaften untersucht. Folge der strukturellen Unordnung ist eine Reduzierung der charakteristischen Eigenschaften, wie der Sprungtemperatur der Supraleitung Tc, der Sommerfeldkonstanten gamma, des oberen kritischen Magnetfelds Hc2(0), der negativen Krümmung in der Feldabhängigkeit des T-linearen Beitrags zur spezifischen Wärme gamma(H) sowie eine Reduzierung der positiven Krümmung in der Temperaturabhängigkeit von Hc2(T). Isoelektronische Substitutionen auf dem Seltenerd-Platz führen aber nicht zum Erreichen des dirty limit. Eine Reduzierung der relevanten supraleitenden und thermischen Eigenschaften durch Pt-Beimengungen wird ähnlich wie im Falle der Lu-Substitution festgestellt. Die Konzentrationsabhängigkeit von Hc2(0) sowie die Krümmung von Hc2(T) weisen hier auf einen Übergang vom clean limit zum quasi-dirty limit durch die Pt-Substitution hin.
123

Interplay of magnetic, orthorhombic, and superconducting phase transitions in iron-based superconductors

Schmiedt, Jacob 29 October 2014 (has links) (PDF)
The physics of iron pnictides has been the subject of intense research for half a decade since the discovery of superconductivity in doped LaFeAsO in 2008. By now there exists a large number of different materials that are summarized under the term "pnictides'' with significant differences in their crystal structure, electronic properties, and their phase diagrams. This thesis is concerned with the investigation of the various phase transitions that are observed in the underdoped compounds of the pnictide subgroups RFeAsO, where R is a rare-earth element, and AFe_2As_2, where A is an alkaline-earth element. These compounds display two closely bound transitions from a tetragonal to an orthorhombic phase and from a paramagnetic to an antiferromagnetic metal. Both symmetry-broken phases are suppressed by doping or pressure and close to their disappearance superconductivity sets in. The superconducting state is stabilized until some optimal doping or pressure is reached and gets suppressed thereafter. The central goal of this thesis is to improve our understanding of the interplay between these three phases and to describe the various phase transitions. We start from an itinerant picture that explains the magnetism as a result of an excitonic instability and show how the other phases can be included into this picture. This approach is based on the the observation that the compounds we are interested in have a Fermi surface with multiple nested electron and hole pockets and that they have small to intermediate interaction strengths. The thesis starts with a study of the doping dependence of the antiferromagnetic phase transition in four different five-orbital models. We use the random-phase approximation to determine the transition temperature, the dominant ordering vector, and the contribution of the different orbitals to the ordering. This allows us to identify the more realistic models, which give results that are in good agreement with experimental observations. In addition to the frequently made assumption of orbital-independent interaction potentials we study the effect of a reduction of the interaction strengths that involve the d_{xy} orbital. We find that this tunes the system between two different nesting instabilities. A reduction of the interactions that involve the d_{xy} orbital also enhances the tendency towards incommensurate (IC) order. For a weak reduction this tendency is compensated by the presence of the orthorhombic phase. However, for a reduction of 30%, as it is suggested by constrained random-phase-approximation calculations, we always find large doping ranges, where a state with IC order has the highest transition temperature. We continue the investigation of the magnetic phase transition by studying the competition of different possible types of antiferromagnetic order that arises from the presence of two degenerate nesting instabilities with the ordering vectors (pi,0) and (0,pi). We derive a Ginzburg-Landau free energy from a microscopic two-band model and find that the presence of the experimentally observed stripe phase strongly depends on the number and size of the hole pockets in the system and on the doping. We show that within the picture of a purely magnetically driven nematic phase transition, which breaks the C_4 symmetry and induces the orthorhombic distortion, the nematic phase displays exactly the same dependence on the model parameters as the magnetic stripe phase. We propose that in addition to the purely magnetically driven nematic instability there is a ferro-orbital instability in the system that stabilizes the nematic transition and, thus, explains the experimentally observed robustness of the orthorhombic transition. We argue that including a ferro-orbital instability into the picture may also be necessary to reproduce the transition from simultaneous first-order transitions into an orthorhombic antiferromagnetic state to two separate second-order transitions, which is observed as a function of doping. Finally, a study of the superconducting phase transition inside the antiferromagnetic phase that is observed in some pnictide compounds is presented. We present an approach to calculate the fluctuation-mediated pairing interaction in the spin-density-wave phase of a multiband system, which is based on the random-phase approximation. This approach is applied to a minimal two-band model for the pnictides to study the effect of the various symmetry-allowed bare on-site interactions on the gap symmetry and structure. We find a competition between various even- and odd-parity states and over a limited parameter range a p_x-wave state is the dominant instability. The largest part of the parameter space is dominated by even parity states but the gap structure sensitively depends on the bare interactions. We propose that the experimentally observed transition from a nodeless to a nodal gap can be due to changes in the on-site interaction potentials.
124

On the electronic phase diagram of Ba1-xKx(Fe1-yCoy)2As2 and EuFe2(As1-xPx)2 superconductors: A local probe study using Mössbauer spectroscopy and Muon Spin Relaxation

Goltz, Til 28 October 2015 (has links)
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.
125

Wachstum, Pinningeigenschaften und Granularität von dicken YBa2Cu3O7-δ-Schichten auf texturierten metallischen Substraten

Pahlke, Patrick 29 January 2018 (has links)
In der vorliegenden Arbeit wurden Schichten des Hochtemperatursupraleiters YBa2Cu3O7-δ (YBCO) untersucht, die epitaktisch mittels gepulster Laserabscheidung auf texturierten metallischen Templaten abgeschieden wurden. Dabei kamen ionenstrahltexturiertes ABAD-YSZ-Band und walztexturiertes NiW-Band zum Einsatz. Für Anwendungen solcher sogenannten Bandleiter ist die Fähigkeit zum Transport möglichst hoher kritischer Ströme Ic essentiell. Dies kann durch das Wachstum möglichst dicker Schichten, eine Verbesserung der Flussschlauchverankerung (Pinning), sowie die Reduzierung der durch Korngrenzen verursachten Stromlimitierung erreicht werden. Im ersten Teil der Arbeit wurden strukturelle und supraleitende Eigenschaften in bis zu 5 µm dicken YBCO-Schichten auf ABAD-YSZ-Band untersucht. Dazu wurden neben nicht-fremdphasendotierten (undotierten) YBCO-Schichten auch BaHfO3- und BaY(NbTa)O6-dotierte YBCO-Schichten herangezogen. Die Untersuchungen erfolgten mittels Röntgenbeugungs-methoden (XRD), Rasterelektronen- und Rasterkraftmikroskopie (REM, AFM), sowie resistiver und induktiver Methoden zur Bestimmung der Sprungtemperatur Tc und der kritischen Stromdichte Jc. Schichtdickenabhängige Messungen konnten u. a. zeigen, dass Ic in undotierten YBCO-Schichten bei einer Dicke oberhalb von 2,8 µm nicht weiter anstieg, während Ic in den dotierten Schichten bis zu einer Dicke von 5 µm nicht limitiert war. Darüber hinaus konnte in temperatur- und feldabhängigen Jc-Messungen ein verbessertes Pinningverhalten bei tiefen Temperaturen und in hohen äußeren Magnetfeldern gefunden werden. Mit Hilfe von transmissionselektronenmikroskopischen Untersuchungen (TEM) und Messungen der Jc-Anisotropie wurde zusätzlich ein Strukturschema herausgearbeitet, das eine Verknüpfung von Herstellungsparametern, Mikrostruktur und Pinningeigenschaften ermöglicht. Der zweite Teil befasste sich mit der Analyse der Mikrostruktur und der lokalen Textur von undotierten YBCO-Schichten auf ABAD-YSZ- und NiW-Band. Die lokale Textur wurde dabei mittels Rückstreuelektronenbeugung (EBSD) aufgelöst. Die Ergebnisse wurden mit orts-aufgelösten Magnetisierungsmessungen (Raster-Hall-Sonden-Mikroskopie) korreliert, mit denen der lokale Stromfluss untersucht werden kann. Auf beiden Templaten zeigte sich eine granulare Struktur, die durch gegeneinander verkippte bzw. verdrehte YBCO-Körner gekennzeichnet war. Während die granulare Struktur auf ABAD-YSZ-Band durch hauptsächlich in-plane missorientierte YBCO-Bereiche mit einem Durchmesser < 1 µm charakterisiert war, konnten auf NiW-Band hauptsächlich out-of-plane missorientierte Bereiche mit einer typischen Größe von 20-50 µm nachgewiesen werden. Auf NiW-Band hing die YBCO-Mikrostruktur und die Schärfe der lokalen Textur von der individuellen out-of-plane Missorientierung des darunter-liegenden NiW-Korns ab, was auf eine bereits im unbeschichteten NiW-Band vorhandene Facettierung zurückgeführt werden konnte. Zu deren Beschreibung wurde ein Facettenmodel entwickelt, das durch TEM-Untersuchungen bestätigt werden konnte. Abschließend wurde auf einkristallinen Substraten und auf ABAD-YSZ-Band ein homogener Stromfluss nachgewiesen, während die supraleitenden Eigenschaften in YBCO-Schichten auf NiW-Band von der lokalen Mikrostruktur und Textur bestimmt wurden. Damit konnte gezeigt werden, dass die globalen Eigenschaften der Bandleiter vom Zusammenspiel eines über Korngrenzen miteinander verbundenen Ensembles von Körnern mit individuellen Eigenschaften bestimmt werden.
126

Crystal growth and perfection of selected intermetallic and oxide compounds

Souptel, Dmitri 21 January 2005 (has links)
The aim of the present work is to clarify the interplay between the complex technological chain of crystal preparation, chemical and structural perfection of grown crystals of intermetallic compounds and oxides and their physical properties. This technological chain includes detailed studies of unknown or insufficiently known phase diagrams, their correlation with growth conditions and optimisation of process parameters for obtaining single crystals with high chemical and physical perfection. The measurements of the physical properties of the grown crystals such as superconductivity, thermoelectric or dielectric properties not only show new features and properties for application of the materials obtained, but also allow conclusions of the crystal perfection. The studies are focused on the following systems: RENi2B2C borocarbides (RE=Y, Tb or Ho) displaying superconductivity, magnetic order and a strong interplay between magnetic and superconducting properties for YNi2B2C, TbNi2B2C, HoNi2B2C, respectively; CeSi2-?Ô and Ru2Si3 as examples of systems with magnetic and promising thermoelectric properties, respectively; MgB2 and LiBC to test of theoretical predictions of the new superconducting intermetallic compounds discovered in the last years; SrTiO3 and SrZrO3 oxide compounds with special dielectric and optical properties. For this wide spectrum of substances necessarily different growth techniques were applied. That is mainly the floating zone (FZ) or travelling solvent floating zone (TSFZ) techniques with optical heating. Flux techniques were used if the vapour pressure of composing elements is high such as for Mg and Li. The crucible free FZ technique is very attractive for the crystal growth of these intermetallic and oxide compounds to avoid contamination with the crucible material, if the melts have very high chemical reactivity, high melting temperatures and if a large crystal size (at least 3-5 mm) is desired for corresponding physical measurements. One special aim in the presented work is the optimisation of the preparation and growth process features with respect to crystal perfection, establishing new relationships between process parameters, crystal perfection, crystallographic structure, composition of grown crystals and the related physical properties. Optimisation of crystal growth process requires own constitutional studies of growth relevant parts of corresponding multicomponent phase diagrams. Therefore, parts of the phase diagrams were experimentally revealed by differential thermal analysis (DTA), optical metallography and EPMA and partially combined with CALPHAD calculations.
127

Investigation of renormalization effects in high temperature cuprate superconductors

Zabolotnyy, Volodymyr B. 16 April 2008 (has links)
While in conventional superconductors coupling between electrons and phonons is known to be responsible for the electron pairing, for the high temperature superconductors the pairing media remains under debates. Since the interactions of electrons with other degrees of freedom (phonons, magnetic excitations, etc) manifest themselves by an additional renormalization in the electronic dispersion, they can be investigated by means of Angle Resolved Photoelectron Spectroscopy. In the work renormalization in two families of high Tc cuprates have been studied. Along the diagonal of the two-dimensional BZ, the renormalization effects are represented by an unusual band dispersion that develops a so-called ‘‘kink’’. In the vicinity of the (pi, 0) point of the BZ, where the order parameter reaches its maximum, the renormalization is noticeably stronger and makes itself evident even in the shape of a single spectral line measured for a fixed momentum. It was shown that for the Bi-2212 samples substitution of Cu atoms in Cu-O plane changes renormalization features in ARPES spectra both in nodal and antinodal parts of the Brillouin zone. The smearing of the dip in the in the spectral line shape measured at (pi; 0) point can be well explained by coupling of electrons to the magnetic resonance mode. The effect of Zn and Ni substitution on the antinodal ARPES spectra was shown to be in good agreement with the influence of these impurities on magnetic resonance mode seen in inelastic neutron scattering experiments. This, in addition to the previous ARPES studies of temperature and doping dependence of peak-dip-hump structure, mass renormalization near antinodal region and a kink in the nodal part of Brillouin zone, provides further evidence that the coupling to magnetic excitations, rather than to phonons, is responsible for the observed unusual renormalization. Unlike the well studied Bi-2212 family of cuprates, photoemission on YBCO-123 turns out to be much more complicated. The observed spectra have a strong contribution from a heavily overdoped surface component with the hole doping level of about x~0.30, which is weakly dependent on the sample stochiometry. Absence of any signs of superconductivity in the spectra of the overdoped component was argued to result from the unusually high doping level. This conclusion is supported by the fact that the overdoped bands give rise to the Fermi surface and band structure consistent with the predictions of the LDA calculations, as well as, by the dependence of the photoemission matrix element on the excitation energy, which closely follows that of the superconducting bulk component. Specific experimental geometry was used to enhance the signal coming from the superconducting component. In particular, experiments with circularly polarized light bundled with simple theoretical considerations enabled better separation of the surface and the bulk components. This type of experiments also suggests that the overdoped component is mainly localized in the topmost CuO2 bilayer, while the next bilayers in the YBCO-123 structure already represent bulk properties and retain superconductivity. Using partially Ca substituted samples it was possible to obtain spectra with a suppressed overdoped component. The likely reason for the suppression is a shift of the most probable cleavage plane from the Ba–O interface to the Y layer. Spectra from the Ca substituted sample clearly reveal a sizable superconducting gap, and strong renormalization effects in the vicinity of the antinodal point. The fact that the renormalization vanishes above Tc and has strong momentum dependence, diminishing away from the (pi; 0)/(0; pi) point, strongly suggests that the reason for this renormalization in YBCO-123 is coupling of the electronic subsystem to spin resonance, similar to the case of Bi-2212.
128

Ladungsanregungen im ungeordneten t-t’-t”-J-Modell

Kühnert, Christian 13 January 2009 (has links)
Für die theoretische Beschreibung verschiedener Substanzen, so z.B. für diverse Kuprate die Anwendungen als Hochtemperatur-Supraleiter finden, spielt das t-J-Modell eine wichtige Rolle. In vielen Fällen kann man Abweichungen der Verbindungen vom idealen translationsinvarianten Festkörper vernachlässigen, für bestimmte Eigenschaften ist jedoch der Einfluß von Störstellen,z.B. Dotieratomen, bedeutsam. Um solche Verunreinigungen einzubeziehen, behandelt die vorliegende Arbeit das t-J-Modell mit einer zusätzlichen on-site-Energie mit über die Gitterpläte zufallsverteilten Werten. Um für dieses Modell die Einteilchen-Greensfunktion zu bestimmen, wird ein Verfahren entwickelt, welches auf der Projektionstechnik basiert und die Einbeziehung des Unordnungsterms ermöglicht. Die notwendige Mittelung über die möglichen Unordnungskonfigurationen erfolgt näherungsweise durch Faktorisierung und ist verwandt mit der sogenannten average T-matrix approximation, wird hier jedoch auf ein stark korreliertes System erweitert. Zur Illustration wird der Grundzustand von La2−xSrxCuO4 und Nd2−xCexCuO4 bei einem zusätzlichen Ladungsträger über Halbfüllung untersucht. Wie Bandstrukturrechnungen zeigen, ruft die Dotierung der elektronendotierten Substanz gerade einen solchen Zufallsterm hervor. Dies wurde in der bisherigen Literatur meist vernachlässigt. Bei der Übertragung der Bandstrukturergebnisse in die Modellparameter des t-t′-t′′-J-Modells zeigt sich, daß der Einfluß der Dotieratome bei La2−xSrxCuO4 um etwa eine Größenordnung geringer ist als in Nd2−xCexCuO4 . Als wichtige Ursache hierfür wird der Einfluß der Apex-Sauerstoffatome angesehen, die im Fall von La2−xSrxCuO4 die Seltenerd- Dotieratome gegenüber der Kupferoxidebene abschirmen. Für das mit diesen Parametern belegte Modell wird anschließend die Einteilchen- Greensfunktion berechnet, die Ausgangspunkt der Berechnung verschiedener Observablen ist. Die für die elektronendotierte Substanz auftretende lokale Mode gibt zu dem Vorschlag Anlaß, daß die unterschiedliche Stabilität der antiferromagnetischen Phase für die beiden betrachteten Substanzen nicht nur auf die Art der Ladungsträger zurückzuführen ist, sondern auch auf die Struktur der Elementarzelle. / The t-J-Modell can be applied to several classes of materials, e.g. high-Tc cuprate superconductors. Often translational invariance can be assumed, but sometimes it is necessary to take into account the effects of the doping atoms at randomly distributed sites. Therefore a t-J-Modell with an additional randomly distributed on-site energy is investigated. To calculate the one-particle Green’s function considering this term of disorder, a method is developed which bases on projection technique. The average over the possible configurations of the dopand atoms is approximated by factorization and is similar to the so-called average T-matrix approximation. Here it is extended to a model with strong correlations. In order to illustrate the methode the single-particle ground state of La2−xSrxCuO4 and Nd2−xCexCuO4 is analyzed. Band-structure calculations exhibit that for the electron-doped case the doping atoms (in first approximation) induce indeed a term of disordered on-site energies. The transformation of the values of this energies at the copper sites into the parameters in the t − t′ − t′′ − J-model shows that the influence of doping in La2−xSrxCuO4 is by about an order of magnitude smaller than in Nd2−xCexCuO4 . The existence of apex oxygen atoms between the rare-earth plane and the copper-oxygen plane in La2−xSrxCuO4 is one important reason for that effect. The single-particle Greens function for the t-t′-t′′-J-model with these parameters is calculated. A local mode appears in the electron-doped case, which suggests that the differences of the stability of the antiferromagnetic phases in both compounds are not only due to the type of charge carriers but also due to the structure of the unit cell.
129

Electronic Structure Investigation of Novel Superconductors / Elektronische Struktur neuartiger Supraleiter

Buling, Anna 14 August 2014 (has links)
The discovery of superconductivity in iron-based pnictides in 2008 gave rise to a high advance in the research of high-temperature superconductors. But up to now there is no generally admitted theory of the non-BCS mechanism of these superconductors. The electron and hole doped Ba122 (BaFe2As2) compounds investigated in this thesis are supposed to be suitable model systems for studying the electronic behavior in order to shed light on the superconducting mechanisms. The 3d-transiton metal doped Ba122 compounds are investigated using the X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), X-ray emission spectroscopy (XES) and X-ray magnetic circular dichroism (XMCD), while the completely hole doped K122 is observed using XPS. The experimental measurements are complemented by theoretical calculations. A further new class of superconductors is represented by the electride 12CaO*7Al2O3: Here superconductivity can be realized by electrons accommodated in the crystallographic sub-nanometer-sized cavities, while the mother compound is a wide band gap insulator. Electronic structure investigations, represented by XPS, XAS and resonant X-ray photoelectron spectroscopy (ResPES), carried out in this work, should help to illuminate this unconventional superconductivity and resolve a debate of competing models for explaining the existence of superconductivity in this compound.
130

Einfluß der magnetischen Ordnung auf Supraleitung und Kristallstruktur in Seltenerd-Nickel-Borkarbid-Verbindungen / Influence of the magnetic order on superconductivity and crystal structure in rare earth nickel borocarbides

Kreyßig, Andreas 05 September 2001 (has links) (PDF)
Rare-earth nickel borocarbids RNi2B2C are particularly suitable for investigations on one of the most interesting problems in modern solid-state physics: these compounds display competition and coexistence of superconductivity and magnetism. Depending on the R3+ ion, the transition temperatures are in an experimentally easy accessible range of 1 K to 25 K. This thesis presents experimental studies on the interplay of both ordering phenomena. Neutron diffraction is used to determine the magnetic order and the resulting changes of the crystal structure. Experiments are performed on polycrystalline and single crystal samples in dependence on temperature and external magnetic fields. The Ni-B stoichiometry of the tetragonal RNi2B2C compounds is systematically varied and the magnetic R3+ ions are partially substituted by other magnetic or nonmagnetic R?3+ ions. The experimental results are compared with macroscopic magnetic and electrical properties. For HoNi2B2C three different magnetic structures are found in a narrow temperature range. While for two magnetic structures the Ho3+ moments are modulated along the c axis, a third magnetic structure with a modulation in a direction is observed. Both, partial substitution of Ho3+ ions and variation of the Ni-B stoichiometry, strongly modify the formation of these different types of magnetic order. The comparison with the concomitant changes of the superconducting properties yields the following scenario for HoNi2B2C-based compounds: superconductivity coexists with both magnetic structures with modulations in c direction. However, the onset of magnetic order weakens the superconductivity. For the magnetic structure with modulation along the a axis, components of the magnetic moments arise in c direction. The resulting local magnetic fields on Ni sites yield a strong suppression of the superconductivity. The observed competition between superconductivity and the magnetic structure with modulation along the a axis strongly suggests that the modification of the electronic structure due to the superconducting state influences the magnetic ordering. As a further impact of the magnetism in RNi2B2C compounds with R = Ho, Dy, Tb and Er changes of the crystal structure are investigated. Using high-resolution neutron diffraction, tetragonal-to-orthorhombic lattice distortions are found. They are induced by those magnetic structures with either parallel or anti-parallel alignement of R3+ magnetic moments. The direction of the lattice distortions, the dependence of their size on the square of the effective ordered magnetic moment and on the type of the R3+ ions indicate that the magneto-elastic interactions are determined by crystal-field effects. This fact also facilitates the elucidation of the magnetic phase diagrams by neutron diffraction experiments in external magnetic fields. For a given phase, absence or presence of magneto-elastic lattice distortions restrict the set of possible magnetic structures. For HoNi2B2C the magnetic phases reported in literature are confirmed. The experimental results for DyNi2B2C are interpreted using a simple model to determine the magnetic structures. Based on mean field calculations, the differences in the magnetic structures for increasing and decreasing magnetic fields can be understood as very strong hysteresis effects in connection with first-order phase transitions. / Seltenerd-Nickel-Borkarbid-Verbindungen RNi2B2C sind bestens zur Untersuchung eines der interessantesten Probleme der modernen Festkörperphysik geeignet: Diese Substanzen weisen Konkurrenz und Koexistenz von Supraleitung und Magnetismus auf, wobei die vom R3+-Ion abhängigen Übergangstemperaturen in einem experimentell gut zugänglichen Bereich von 1 K bis 25 K liegen. Die vorliegende Dissertation stellt experimentelle Arbeiten zum Wechselspiel der beiden Ordnungsphänomene vor. Für poly- und einkristalline Proben werden die magnetischen Ordnungen und resultierende Veränderungen der Kristallstruktur mittels Neutronendiffraktion in Abhängigkeit von der Temperatur und vom äußeren Magnetfeld bestimmt und mit den makroskopischen magnetischen und elektrischen Eigenschaften verglichen. Hierbei werden die tetragonalen RNi2B2C-Verbindungen gezielt in ihrer Ni-B-Stöchiometrie variiert sowie die magnetischen R3+-Ionen partiell durch andere magnetische als auch unmagnetische R?3+-Ionen substituiert. Für HoNi2B2C werden in einem engen Temperaturbereich drei verschiedene magnetische Strukturen nachgewiesen. Während in zwei magnetischen Ordnungen die Ho3+-Momente entlang der c-Achse moduliert sind, wird für die dritte magnetische Ordnung eine Modulation in a-Richtung beobachtet. Sowohl durch die partielle Substitution der Ho3+-Ionen als auch durch die Ni-B-Stöchiometrievariation wird die Ausprägung der magnetischen Strukturen stark modifiziert. Der Vergleich mit den ebenfalls veränderten supraleitenden Eigenschaften ergibt das folgende Bild für die HoNi2B2C-Verbindungen: Die Supraleitung koexistiert mit den beiden c-Achsen-modulierten magnetischen Strukturen, das Einsetzen der magnetischen Ordnung führt jedoch zu einer Schwächung der Supraleitung. Die a-Achsen-modulierte magnetische Struktur weist Momentkomponenten in c-Richtung auf, die auf Grund der resultierenden lokalen Magnetfelder an den Ni-Plätzen eine starke Unterdrückung der Supraleitung bewirken. Die beobachtete Konkurrenz zwischen der Supraleitung und der a-Achsen-modulierten magnetischen Struktur gibt andererseits einen starken Hinweis darauf, daß die Modifizierung der elektronischen Struktur im supraleitenden Zustand auf das magnetische System rückwirkt. Als weitere Auswirkung des Magnetismus kommt es in RNi2B2C-Verbindungen mit R = Ho, Dy, Tb und Er zu Veränderungen der Kristallstruktur. Mittels hochauflösender Neutronendiffraktion werden magnetisch induzierte, tetragonal-zu-orthorhombische Gitterverzerrungen für diejenigen magnetischen Ordnungen nachgewiesen, bei denen die magnetischen Momente der R3+-Ionen parallel bzw. antiparallel ausgerichtet sind. Die Richtung der Gitterverzerrung, die Abhängigkeit ihrer Größe vom Quadrat des geordneten magnetischen Momentes als auch von der Art der R3+-Ionen deuten darauf hin, daß die magneto-elastischen Wechselwirkungen durch Kristallfeldeffekte bestimmt werden. Diese Einsicht unterstützt auch die Aufklärung der magnetischen Phasendiagramme mittels magnetfeldabhängiger Neutronenbeugungsexperimente. Für eine magnetische Phase schränkt das Auftreten bzw. Fehlen der magneto-elastischen Effekte die Vielfalt der möglichen magnetischen Strukturen ein. Die aus der Literatur bekannten magnetischen Phasen von HoNi2B2C werden bestätigt. Für DyNi2B2C werden die experimentellen Ergebnisse unter Nutzung eines einfachen Modelles interpretiert und die magnetischen Strukturen bestimmt. Anhand von Molekularfeldrechnungen können die Unterschiede in den magnetischen Strukturen für ansteigendes und für abnehmendes Magnetfeld als sehr starke Hystereseeffekte in Zusammenhang mit Phasenübergängen erster Ordnung gedeutet werden.

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