Thesis (Ph. D.)--University of California, San Diego, 1981. / Vita. Includes bibliographical references (leaves 87-94).

Thesis (Ph. D.)--University of California, San Diego, 1981. / Vita. Includes bibliographical references (leaves 87-94).

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In his programmatic article More Is Different (1972), Nobel laureate P. W. Anderson captured the fundamental interest in quantum matter in a nutshell. The central motive in this field is emergence. In the inaugural volume of the homonymous journal, J. Goldstein defined this as "the arising of novel and coherent structures, patterns and properties during the process of self-organization in complex systems". Famously, the idea that the "the whole is greater than the sum of its parts" goes back to Aristotle's metaphysics, and it has served as a stimulating concept in 19th century biology, economics and philosophy. The study of emergence in condensed matter physics is unique in that the underlying complex systems are sufficiently "simple" to be modelled from first principles. Notably, the emergent phenomena discovered in this field, such as high-temperature superconductivity, giant magnetoresistance, and strong permanent magnetism have had an enormous impact on technology, and thus, society. Historically, there has been a distinction between materials with localized, strongly interacting (or correlated) electrons - and non-interacting, itinerant electronic states. In the last decade, several new states of matter have been discovered, which emerge not from correlations, but from peculiar symmetries (or topology) of itinerant electronic states. The term quantum materials has therefore become popular to subsume these two strands of condensed matter physics: Electronic correlations and topology. In this thesis, I report investigations of four quantum materials which each illustrate present key interests in the field: The mechanism of high temperature superconductivity, the search for materials that combine both electronic correlations and non-trivial topology and novel emergent phenomena that arise from the synergy of electronic correlations and a strong coupling of spin- and orbital degrees of freedom. The common factor and potential key to understanding these materials is magnetism. My experimental work is focused on neutron and x-ray scattering techniques, which are able to determine both order and dynamics of magnetic states at the atomic scale. I illustrate the full scope of these methods with experimental studies at neutron and synchrotron radiation facilities. This includes both diffraction and spectroscopy, of either single- or polycrystalline samples. My in-depth analysis of each dataset is aided by structural, magnetic and charge transport experiments. Thus, I provide a quantitative characterization of magnetic fluctuations in an iron-based superconductor and in two Dirac materials, and determine the magnetic order in a Dirac semimetal candidate and a complex oxide. As a whole, these results demonstrate the elegant complementarity of modern scattering techniques. Although such methods have a venerable history, they are presently developing at a rapid pace. Several results of this thesis have only been enabled by very recent instrumental advances.

Superconductivity and ferromagnetism are two antagonistic physical phenomena which their coexistence in a uniform material can be resolved only under extraordinary conditions. The reason for that is the phonon-mediated attraction energy between electrons which results in the formation of the so-called Cooper pairs, is usually smaller that the exchange (Zeeman) interaction between electrons which tend to align the electron spins. However, non-zero total momentum Cooper pairs can be accomplished even in the presence of an exchange field as surprisingly! predicted first by Fulde and Ferrel [1] and independently by Larkin and Ovchinikov [2] nearly 50 years ago. This coexistence has already been observed experimentally in both bulk samples [3, 4] and in thin films [5-7] which result from a different type of electron-pairing mechanism which electrons with spin pointing in the same direction team up to form Cooper pairs with one unit of spin, resulting in the so-called triplet superconductivity. Apart from this so-called ferromagnetsuperconductors which both superconducting and ferromagnetism order parameters are present in a uniform material, hybrid systems [8] are made form materials with different or even mutually exclusive properties. Therefore the overall property can be strongly affected by the interaction between constituent materials. The present work, concerns such a hybrid system where Nb, a superconducting metal having transition temperature below 9.5K, is placed in contact with a ferromagnetic metal, Gd with bulk Curie temperature of around 290 K in a form of a nanocomposite. The mutual immiscibility of these two elements gives us the opportunity to take advantage of both the superconduction and ferromagnetism properties of the constituents and further study the transport and magnetic behavior of the system and their effects on each other specially on the critical current of the superconductor which is expected to be modified by the proximity of the ferromagnetic metal.

This work reports on physical properties of a novel CeCo0.715Si2.285 compound. The compound crystallizes in the I-4m2 space group structure with extremely elongated unit cell (a = 4.13˚A , c = 32.84˚A) containing BaAl4 structural patterns. In zero magnetic field it orders antiferromagnetically at TN = 10.0K. Under application of magnetic field along the c-axis it manifests numerous magnetic transitions in small fields (B < 0.5T), resembling the so-called 'devil's staircase' behaviour (e.g. CeSb, CeCoGe3). The magnetization is almost constant from 1T up to 45T for H||c but considerably reduced (0.3µB/Ce) with respect to the free Ce3+ ion. For fields applied along the a-axis typical behaviour for a hard axis in a material with uniaxial anisotropy is observed. The performed single crystal neutron diffraction experiment did not allow complete determination of magnetic structure. 1

<p> The interplay between superconductivity, magnetism and crystal structure is a central issue in the study of the high Tc cuprates. The transition metal compound La2-xBaxCuO4 (LBCO) was the very first high Tc superconductor, discovered by J. G. Bednorz and K. A. Muller in 1986. However, it has been much less extensively studied than other high Tc materials, due to the difficulty of growing large single crystals. With our Image Furnace facility, we have successfully grown high quality, large LBCO crystals (with x~0.095 , 0.08, 0.05 and 0.025) on the underdoped side of the well known 1/8 (x=0.125) anomaly in this material's phase diagram.</p> <p> Using our rotating anode X-ray source at McMaster University we have performed high-resolution X-ray diffraction studies on our x=0.095 and 0.08 samples and on a 1/8 doped LBCO (x=0.125) crystal grown by our collaborators. The X-ray study mapped out a sequence of tetragonal and orthorhombic crystal structures with temperature, which were known from earlier measurements.</p> <p>We have also performed neutron scattering studies at several Laboratories on x=0.095 , 0.08, 0.05 and 0.025 samples. We observed elastic spin incommensurate Bragg peaks in all samples, and inelastic measurements on the x=0.095 sample allowed us to explore the material's low energy spin fluctuations. The elastic neutron scattering results of higher doped samples (x=0.095 and 0.08) indicate that "collinear" static incommensurate magnetic ordering develops below the low temperature structural phase transition, and this order persists into the superconducting state. Static incommensurate magnetic order is also observed in the La2-xBaxCuO4 (x=0.05 and 0.025) compounds with ordering wavevectors which are rotated by 45° about the commensurate (0.5 ,0.5 ,0) position, with respect to that in the superconducting x=0.095 and 0.08 samples. These spin modulations are one dimensional in the x=0.05 and 0.025 samples, with ordering wavevectors lying along the orthorhombic b* direction. Such a rotation in the orientation of the static spin ordering as a function of increasing Ba doping, from diagonal to collinear is roughly coincident with the transition from an insulating to a superconducting ground state and is similar to that observed in the related La2-xSrxCuO4 system. The low energy, inelastic neutron scattering studies show that the dynamic spin susceptibility for x=0.095 is constant within the superconducting state and decreases as the temperature rises above Tc. </p> / Thesis / Doctor of Philosophy (PhD)

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.

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.

This thesis describes neutron scattering experiments on strongly correlated systems exhibiting a range of emergent phenomena: antiferromagnetism, charge order, superconductivity and multiferroicity. I have examined the La_{2}CoO_{4} compound which is a Mott insulator and orders antiferromagnetically near room temperature. The La_{2}CoO_{4} sample was studied using spherical neutron polarimetry and I present magnetic structure models to describe the two antiferromagnetic phases of the compound. Furthermore, the magnetic fluctuations have been investigated using neutron time-of-flight technique. This has allowed us to extract the dominant exchange interactions in the system. More interestingly, the work on La_{2}CoO_{4} presented in this thesis provides a basis for the experimental evidence of an hourglass dispersion in La_{5/3}Sr_{1/3}CoO_{4}, previously only observed in the copper oxide based superconductors. This dispersion has been understood in terms of a stripe ordered magnetic phase and was found to be well described by a linear spin-wave model. Neutron scattering experiments were also carried out on the new iron-based high-temperature superconductors, FeSe_{x}Te_{1−x}. A range of compositions were studied, including both antiferromagnetically ordered and superconducting. Below the superconducting phase transition temperature, a spin resonance mode was found centred on the antiferromagnetic wavevector. This is an important feature shared by many unconventional superconductors. The spin resonance intensity was found to reflect the order parameter of the superconducting state. Polarised inelastic neutron scattering experiments have revealed a small anisotropy between the in-plane and out-of-plane magnetic fluctuations at the resonance. This anisotropy cannot be readily explained by the usual anisotropic terms in the Hamiltonian. This could be evidence of new physics in the FeSe_{x}Te_{1−x} superconductors. Finally, I have studied CuO – a high-temperature multiferroic. Analysis of polarised neutron diffraction experiments shows that the magnetic domain population can be varied using an externally applied electric field. This unambiguously demonstrates coupling between the magnetic and ferroelectric degrees of freedom. Using representation analysis I derive the incommensurate magnetic structure in the multiferroic phase. The origin of the magnetoelectric coupling is consistent with models based on the inverse Dzyaloshinskii-Moriya interaction.