Thesis (Ph. D.)--University of Wisconsin--Madison, 1967. / Typescript. Vita. eContent provider-neutral record in process. Description based on print version record. Includes bibliographical references.

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.

Neutron reflectivity offers the opportunity for non-destructive characterisation of buried polymer interfaces. Specular neutron reflectivity is commonly used to characterise the structure of conjugated polymer interfaces found in organic electronic devices. However, detecting specularly reflected neutrons only allows the measurement of the root-mean-square (RMS) roughness of the interface averaged over a macroscopic lateral distance. There are two contributions to the RMS roughness of a polymer/polymer interface; i) the so-called 'intrinsic interfacial width' due to mixing of the polymers at a molecular level and ii) lateral roughness due to deviations of the interface position from the plane of the substrate. In this work a numerical model is developed to analyse experimental off specular reflectivity. The model is based on the distorted wave Born approximation (DWBA). Specular and off specular neutron reflectivity data is collected from a model conjugated polymer/amorphous polymer interface (poly(9,9-dioctylfluorene) (F8) on deuterated PMMA) and a conjugated poly- mer/fullerene interface (poly(3-hexylthiophene) (P3HT) polymer on [6,6]-phenyl C61-butyric acid methylester (PCBM)). This allows probing of the structure in the plane of the interfaces to distinguish the intrinsic interfacial width from the lateral roughness. The structure of the F8/dPMMA interface is studied by systematically varying the film thickness, which strongly impacts on the amplitude of the lateral interface roughness, and allows more complete analysis of the relative contributions of intrinsic mixing and lateral roughness. For comparison off specular measurements on amorphous/amorphous polymer (PMMA/polystyrene) interfaces are performed, which have been studied previously using specular neutron reflectivity and self consistent held theory. Fitting specular reflectivity using standard techniques and off specular reflectivity data using the model developed allow intrinsic and lateral roughness contributions for the F8/dPMMA system to be separated by direct measurement. The P3HT/PCBM interface exhibits no lateral roughness as the materials are found to be miscible.

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Accurately collimated monoenergetic fast neutron beams of small angular width were produced by bombarding heavy ice targets with deuterons, and operating the neutron detector in coincidence with a semiconductor detector detecting the He³ recoil nuclei. Using a bombarding energy of E[subscript d] 50 keV a neutron beam of energy 2.55 MeV and known absolute intensity was produced. The measured beam profile agreed with the theoretically calculated profile. The beam was used to measure the absolute neutron detection efficiency and the pulse spectrum of a plastic scintillation counter bombarded by 2.55 MeV neutrons. Using a bombarding energy of E[subscript d] = 2 MeV a neutron beam of energy 5.08 MeV was produced and the bearers profile was measured. / Science, Faculty of / Physics and Astronomy, Department of / Graduate

Measurements of the angular distribution and total reaction rate in neutron-proton scattering are described. The emphasis of this work has been to obtain an accurate normalization of the distribution, which is difficult to achieve with neutral beams. Nearly monoenergetic neutrons from the d(p,n)pp reaction were scattered from a liquid hydrogen target. The neutron beam energy was determined from the time of flight with respect to the radio frequency signal of the TRIUMF cyclotron. The differential cross section was measured at 319 and 493 MeV from 10 to 180 degrees in the centre of mass (CM.). Calibrated neutron beam monitors upstream of the scattering target provided an absolute normalization over the whole angular range. Between 10 and 100 degrees CM. a neutron detector consisting of a charged particle veto, a carbon convertor and two trigger scintillators sandwiching 7 multiwire proportional chambers was used to select elastic neutrons by time of flight techniques. The neutron angular distribution was measured with an average precision of 5% and an uncertainty on the normalization of 1.3%. An associated particle experiment (neutrons and recoil protons detected in coincidence) determined the efficiency of the neutron detector and the monitors were calibrated by measuring the incident neutron flux with the neutron detector in the beam, i.e. at zero degrees. The recoil protons were detected in the angular range between 60 and 180 degrees CM. with a precision of 1% to 2% and an error on the normalization of 2.8% at 319 MeV and 3.7% at 493 MeV. Elastic events were selected by time of flight and by either a measurement of magnetic rigidity (momentum) or total energy. The absolute normalization of the two experimental techniques is verified by the overlap of the two measurements and by comparing the integrated differential cross section with the measured total cross section. The neutron-proton total cross section was measured at six energies between 200 and 500 MeV by a transmission type experiment to a precision of 1% to 3%. The systematic corrections were small, of the order of 1%, and the statistical errors were increased to include monitor and beam instabilities. The measurements show a smooth quadratic energy dependence. The data was included in a phase shift analysis and a dispersion relation analysis along with the previous world data. Agreement between the real part of the forward scattering amplitude predicted by the phase shift analysis and by the dispersion relation analysis is improved. The errors on the 1=0 (isoscalar) phase shifts are decreased and to a lesser extent on the 1=1 phase shifts. There is a marked improvement in the smooth variation with energy of the 1=0 phase shifts and a better agreement of the higher partial waves with the theoretical predictions of the Paris potential. / Science, Faculty of / Physics and Astronomy, Department of / Graduate

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The purpose of this experiment was to make positive assignment of the Cs133 energy levels excited by the inelastic scattering of neutrons.

The alkali metal graphite intercalates and the conducting polymers polyacetylene and polypyrrole are reviewed and compared. Polyacetylene was synthesized by Luttinger's method and doped by exposure to caesium vapour. The doped and undoped polyacetylene were characterized by neutron powder diffraction. Hydrogen absorption and subsequent pyrolysis of caesium doped polyacetylene were studied. Mass spectrum analysis of the gases evolved at 300°C showed methane and other alkanes, indicating H₂ addition to the polymer chain followed by methane elimination. The graphite intercalates C₈Cs and C₂₄Cs reacted irreversibly with acetylene, neutron powder diffraction indicating graphite and two new substances. Mass spectrum analysis of gases evolved on heating showed ethylene, butene and butadiene, suggesting a polymerization. Polypyrrole was synthesized electrochemically and characterized by cyclic voltammetry. Gram quantities of polypyrrole doped with BF^-₄ and C10^-₄ were prepared electrochemically under high vacuum conditions to achieve high purity and avoid oxygen doping. Perchlorate doped polypyrrole prepared in an oxygen-free environment proved dangerously unstable, especially when dry. The neutron scattering law for a harmonic oscillator and the energy level splitting pattern of a 1-D rotor in a cos3θ hindering potential are reviewed and applied to solid acetonitrile. Intense lines in the neutron spectrum at 140 and 190 cm^-1 are assigned to methyl group torsions with barriers to rotation of 400 and 734 cm^-1. Hydrogen is reversibly physisorbed by intercalates C₂₄K, C₂₄Rb and C₂₄Cs at 100K to form compounds C₂₄M(H₂)₂. Neutron spectra of H₂, HD and D₂ physisorbed by C₂₄Rb and C₂₄Cs at energy transfers between 0.3-3 meV and 10-200 meV (1 meV = 8.065 cm^-1) were measured and assigned to rotational tunnelling and librations of hydrogen molecules in two sites of different dimensions. The cos2θ barriers to rotation were 57 and 78 meV respectively in C₂₄Rb(H₂)_x and 51 and 78 meV in C₂₄Cs(H₂)_x. A structural model is proposed for the metal layers with the hydrogen molecules in the layers and perpendicularly oriented.