The muon is a useful probe of magnetic fields in superconductors, but knowing the field seen by the muon is often of limited value until we know where the muon is in the crystal lattice. In this thesis I employ two independent theoretical methods to search for candidate muon sites: the potential energy field method, which seeks the minimum of the electrostatic potential of the μ⁺, and the magnetic dipolar field method, which compares the calculated magnetic field (due to the host electronic, atomic or nuclear dipolar fields) with the observed local fields at the muon. / Science, Faculty of / Physics and Astronomy, Department of / Graduate

Redfield's theory and the theory of master equations have been reviewed and their applications to muonium spin dynamics discussed. It was found that both theories are equivalent in the Markov limit. In some cases, analytical expressions for relaxation rates are found. In addition, Redfield's theory was applied to describe spin relaxation of muonium-substituted free radicals near level-crossing resonances. Theoretical predictions were compared with experimental data for the C₆F₆-Mu radical and the results suggest there are several relaxation mechanisms involved. / Science, Faculty of / Physics and Astronomy, Department of / Graduate

The first half of the thesis presents our experimental study of a helical magnet MnGe. We apply μSR technique to study the dynamic as well as the static magnetism in MnGe. Our key findings are as follows. From the muon dynamic relaxation 1/T1 results, no apparent critical behavior or anomaly was observed at the boundary between param- agnetic and the induced-ferromagnetic regions. Our study revealed linear relation between the transverse field relaxation rate and the static magnetization. Furthermore, their ratio, which can be regarded a form of hyperfine coupling constant, is very similar in the induced ferromagnetic region and the paramagnetic region. This suggest that the Z component of the Mn moment is static in both regions. On the other hand, the single relaxation rate in the transverse spectra suggest that the internal field is highly homogeneous in the induced ferromagnetic region. We therefore speculate that the induced ferromagnetic region and the paramagnetic region are not separate phases, but rather a single phase with different tendencies as temperature decrease. With decreasing temperature, the paramagnetic region is marked with the winning of the tendency towards ferromagnetic ordering over random ordering, and the induced ferromagnetic region is marked with the winning of the tendency towards the helical order over ferromagnetic order.At lower temperature, we observed dynamic critical behavior in the boundary between the induced ferromagnetic region and the Skyrmion region. Specifically, in low fields, the 1/T1 relaxation rate behaves qualitatively different from the prediction of SCR theory for itinerant ferromagnet for large temperature regime above Tc. In high fields, on the other hand, the system recovers the SCR itinerant ferromagnetic behavior. Through analyzing field effect on spin fluctuation and phase transition in the low and high field regimes, we speculate that this could be due to the suppression of helical fluctuation into ferromagnetic-like fluc- tuation by large magnetic fields. Our μSR results, which show 2nd order signature for the transition between the induced ferromagnetic region into the Skyrmion region, is consistent with considerations based on the topology of the magnetic structure in each phase. At low temperatures within the Skyrmion region of MnGe, our analysis of the transverse field data shows that all the three components of the Mn moment is frozen. The quadratic tempera- ture dependence of 1/T1 at low temperatures suggest the two-magnon spin wave to be the dominant spin excitation in the Skyrmion region. This is similar to those seen in local- ized moment magnets and is qualitatively different from the linear temperature dependence predicted from SCR theory for itinerant ferromagnets. The second half of the thesis present our derivation of the structure function and the pair distribution function (PDF) for textured materials. We also derive the analytical form of the PDF for a few special cases of texture. In this study, we start from the general form of a 3D structure function and derive the general and orientationally averaged form of the structure function and PDF for textured samples. In particular for a thin film sample with fibre texture, our formalism gives the result known as the 2 dimensional PDF. We developed open-software that calculates the 2 dimensional PDF for a textured thin film, and showed that the experimental PDF was well fitted using the model. On the other hand, the PDF method could be extended to an energy-dependent form, which could reveal explicitly the effect of lattice dynamics on the local arrangement of the atoms. This is usually called the dynamic PDF method. In this thesis we derive the analytical form of the dynamic PDF for a simple molecule that contains two identical atoms. And we interpret the mathematical results with physical consideration of the lattice dynamics. In addition, we also propose a new definition for the dynamic PDF which can be shown to reduce to the atomic PDF by integrating over energy. This new definition of the dynamic PDF incorporates the contribution from multi-phonon scattering effects, and can be computed conveniently from inelastic neutron scattering.

This thesis presents a study on several series of unconventional Fe-based superconductors; namely, derivatives of NaFeAs and LiFeAs, as well as molecular-intercalated FeSe. Primarily using muon spin rotation (SR), but also x-ray diffraction (XRD) and magnetic susceptibility measurements, the nature of both magnetic and superconducting phases within these systems is studied. Particular attention is focussed on how these states compete or coexist with one another. The aforementioned experimental techniques are first used to explore the phase diagram of NaFe1xCoxAs. This phase diagram includes regions of long-range antiferromagnetism and short-range order, that both coexist with superconductivity. Magnetism is gradually destroyed, primarily through a diminishment of the size of the ordered moment, as superconductivity is enhanced by Co substitution. This interplay is explored in detail. By contrast, superconductivity in LiFeAs cannot be enhanced by transition metal substitution, suggesting that it is intrinsically optimally-doped. I investigate this conclusion by studying the evolution of the penetration depth in superconducting compositions of LiFe1xCoxAs and LiFe1xNixAs, and comparing these data to those from other electron-doped systems. I also study an unusual and emergent magnetic phase in Li1yFe1+yAs. This work suggests that LiFeAs supports a superconducting phase that resembles those in other Fe-pnictides, but is uniquely close to an additional magnetic instability. I then move on to the study of a recently discovered series, based on FeSe intercalated with ammonia and various metals. I study both the penetration depth and the intrinsic magnetic phases in these systems using SR and compare them with other compounds based on FeSe. I find that these intercalated systems support spacially separated regions of dynamic magnetism and superconductivity and I discuss how much these phases depend on the precise chemical details of the intercalated layer. Finally, I return to the experimental study of NaFe1xCoxAs, extending the range of techniques employed by using high-field magnetometry and high-pressure SR. These studies reveal new features of this system that were not accessible using low-field and ambient-pressure methods. In particular, I show that the magnetic moment size in NaFeAs unexpectedly increases with pressure, suggesting that the electronic structure of this compound may be unique amongst known Fe-based superconductors.

This thesis is concerned with how the physical properties of transition metal oxides change due to chemical substitution or intercalation. Experiments using the muon-spin relaxation and rotation (μSR) techniques were carried out at the ISIS Facility (UK) and the Paul Scherrer Institute (CH). In conjunction with the μSR results, the results of heat capacity and magnetic susceptibility experiments are used to provide complementary information on the same samples. Investigations of the properties of the layered triangular lattice magnets NaNiO2 and LiNiO2 are presented. For NaNiO2, all three experimental techniques are used to provide a full survey of the thermodynamic and magnetic properties of this compound. For LiNiO2, μSR studies of notionally stoichiometric and Mg-doped samples were carried out. These showed that Mg doping causes a significant change in the magnetic dynamics of the material, but neither sample exhibits long-range magnetic order. The magnetic ordering of the extensively studied perovskite compounds LaTiO3 and YTiO3 is investigated using μSR. The results were in agreement with previous neutron diffraction studies of the two compounds, but clarified the orientation of the magnetic moments in LaTiO3. It was also possible to make a detailed comparison between the μSR results and those of dipole field calculations of the magnetic field at possible muon stopping sites, allowing these to be deduced and compared with results in other well characterized transition metal oxides. The two titanium chain compounds NaTiSi2O6 and TiOCl exhibit spin gap formation at unusually high temperatures due to unconventional dimerization mechanisms. A model allowing the comparison of X-ray diffraction data, dimerization, and the magnitude of the spin gap is proposed. This is tested against both magnetic susceptibility and μSR data for both compounds. For NaTiSi2O6 both experimental techniques are in reasonable agreement, whereas in TiOCl the results are conclusively different. The origin of this disparity in TiOCl is explored. The intercalation of organic chain molecules into Bi based high-temperature superconductors has previously been demonstrated to extend the interlayer spacing by a factor of up to three without changing the superconducting transition temperature. μSR is used to investigate the London penetration depth, as a function of interlayer spacing, of two series of such samples. The results show a simple trend corresponding to a constant density of superconducting electron pairs in each layer. The consequences of this result are discussed in the context of previously identified scaling relations between superconducting parameters. Results of experiments excluding the possibility of magnetic order and muon-organic radical formation in these samples are presented, as well a preliminary study of the field distributions in a mosaic of intercalated crystallites.

Thesis (Ph. D.)--University of California, Riverside, 2009. / Includes abstract. Includes bibliographical references (leaves 121-123). Issued in print and online. Available via ProQuest Digital Dissertations.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第22235号 / 理博第4549号 / 新制||理||1654(附属図書館) / 京都大学大学院理学研究科物理学・宇宙物理学専攻 / (主査)教授 前野 悦輝, 教授 松田 祐司, 教授 佐藤 昌利 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DFAM

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

No description available.

Pyrochlore iridates have received considerable attention for the past few years as they possess strong electron correlations and spin orbit coupling, giving rise to a finite temperature metal-insulator transition (MIT). The nature of this MIT transition is related to the magnetic order of the Ir atoms which also experience frustration as they are part of a pyrochore structure. The aim of this study is to elucidate the magnetic configuration of the magnetic iridium ions by doping Y2Ir2O7 with Bi. Here we present a study on the magnetic properties of the Y2−xBixIr2O7 (x = 0, 0.2, 0.4, 0.9, 1.3, 2) system using μSR and DC susceptibility. Our results show that pure Y2Ir2O7 has a magnetic transition to a long- range ordered state. Substituting Bi by Y results in a lower temperature transition with increasing amount of bismuth. When the system goes into the ordered state a weak ferromagnetic moment is seen. This is in agreement with the belief that the system orders in an canted antiferromagnetic fashion with all-in all-out spins in the tetrahedron of the pyrochlore structure. However the addition of bismuth into the sample does not change the internal magnetic field measured at low temperatures with μSR, but only changes the transition temperature and the ordered volume fraction. For the Bi2Ir2O7 system two magnetic transitions had been measured previously counter to the belief that this material did not order magnetically. In this work, our μSR measurements show no evidence of such a transition. In the transverse field μSR set up a small Knight shift is measured due to the local susceptibility of Bi2Ir2O7. / Thesis / Master of Science (MSc)