Physics Commons^™

Atomic-Level Mechanisms Of Fast Relaxation In Metallic Glasses, Leo W. Zella

Doctoral Dissertations

Glasses are ubiquitous in daily life and have unique properties which are a consequence of the underlying disordered structure. By understanding the fundamental processes that govern these properties, we can modify glasses for desired applications. Key to understanding the structure-dynamics relationship in glasses is the variety of relaxation processes that exist below the glass transition temperature. Though these relaxations are well characterized with macroscopic experimental techniques, the microscopic nature of these relaxations is difficult to elucidate with experimental tools due to the requirements of timescale and spatial resolution. There remain many questions regarding the microscopic nature of relaxation in glass …

Chirality, Symmetry-Breaking, And Chemical Substitution In Multiferroics, Kiman Park

Doctoral Dissertations

Multiferroic materials attract significant attention due to their potential utility in a broad range of device applications. The inclusion of heavy metal centers in these materials enhances their magnetoelectric properties, yielding fascinating physical phenomena such as the Dzyaloshinskii–Moriya interaction, nonreciprocal directional dichroism, enhancement of spin-phonon coupling, and spin-orbit-entangled ground states. This dissertation provides a comprehensive survey of magnetoelectric multiferroics containing heavy metal centers and explores spectroscopic techniques under extreme conditions. A microscopic examination of phase transitions, symmetry-breaking, and structure-property relationships enhances the fundamental understanding of coupling mechanisms.

In A2Mo3O8 (A = Fe, Zn, Ni, and Mn), we use optical spectroscopy …

Exploring Skyrmions Dynamics And Structure Using Neutron Scattering, W-L-Namila Chandula Liyanage

Doctoral Dissertations

Magnetic skyrmions are topologically protected chiral spin textures with great potential for next-generation consumer technologies. These magnetic structures can be described as spins continuously wrapping into a closed coplanar loop, featuring a core and fencing perimeter with opposite out-of-plane orientations. While conventional depictions of magnetic skyrmions use a two-dimensional projection, recent research underscores the importance of their three-dimensional structure in determining their topology and stability. Magnetic skyrmions typically emerge just below the curie temperature of a magnetic material, creating what is known as a skyrmion pocket. In most materials the stability pocket is at low temperatures and finite fields, however …

Imaging Normal Fluid Flow In He Ii With Neutrons And Lasers — A New Application Of Neutron Beams For Studies Of Turbulence, Xin Wen

Doctoral Dissertations

Turbulence is ubiquitous in life —from biology to astrophysics. The best direct numeric simulations (DNS) have only been benchmarked against low resolution, time-averaged experimental configurations—partly because of limitations in computing power. With time, computing power has greatly increased, so there is need for higher quality data of turbulent flow. In this dissertation, we explore a solution that enables quantitative visualization measurement of the velocity field in liquid helium, which has the potential of breaking new ground for high Reynolds number turbulence research and model testing.

Our technique involves creation of clouds of molecular tracers using 3He-neutron absorption reaction in liquid …

Understanding Liquid Dynamics Using The Van Hove Function From Inelastic Neutron Scattering Measurements, Yadu Krishnan Sarathchandran

Doctoral Dissertations

Liquid state physics remains relatively unexplored compared to solid-state physics, which achieved massive progress over the last century. The theoretical and experimental methodologies used in solid-state physics are not suitable to study the liquid state due to the latter's strong time dependence and the lack of periodicity in structure. The approaches based on phonon dynamics break down when phonons are over-damped and localized in liquids. The microscopic nature of atomic dynamics and many-body interactions leading to liquid state properties such as viscosity and dielectric loss in liquids remain unclear. Inelastic neutron scattering measurements were done to study the microscopic origins …

Studying Electron Dynamics For Quantum Materials With Real Space Resolution: A Wannier Orbital Approach To Spectroscopy Using High-Performance Supercomputers, Casey J. Eichstaedt

Doctoral Dissertations

Quantum materials have a promising future for energy and security applications which will lay the bedrock for material science research for decades to follow. Partic- ularly, ‘one-dimensional’ Mott-insulating cuprates such as SrCuO 2 and (Ca)Sr 2 CuO 3 have been deemed to fall under a ‘fractionalization’ paradigm in which the electrons disintegrate into bosonic collective excitations of their fundamental constituents— spin, charge, and ‘orbital’ degrees of freedom— due to the anisotropic crystalline structure, deeming them outside the band theory of solids. Here, I provide ab initio theory for the ‘one-dimensional’ cuprates SrCuO 2 and (Ca)Sr 2 CuO 3 using no …

Topological States In Matter, Hasitha W. Suriya Arachchige

Doctoral Dissertations

Topologically nontrivial spin textures, mesoscopic spin configurations that cannot be continuously transformed to an elementary magnetic configuration such as a ferromagnet or antiferromagnet, are of interest due to their ability to exhibit magnetic solitons, with topological protection. Such properties have the potential for applications in future data storage and communication devices. For example, spin textures found in materials such as MnSi, Cu2OSe3, Co-Zn-Mn alloys, and GaV4S8, commonly known as skyrmions, are driven by the interplay of atomic-scale exchange interactions, single-ion anisotropy, and an applied magnetic field. Of particular importance to this class of materials is the presence of a Dyaloshinski …

Semi-Classical Theories Of Quantum Magnets, Hao Zhang

Doctoral Dissertations

Recent progress in magnetism has been driven by embracing the complexity associated with entangled spin, orbital, and lattice degrees of freedom and by understanding the emergent quantum behaviors of magnetic systems. Over the past decades, intense efforts have been devoted to “extreme quantum materials” comprising low-dimensional lattices of spin S = 1/2 degrees of freedom, that are candidates to host quantum spin liquid phases with no classical counterpart. Finite-spin (S ≥ 1) systems that exhibit ground states with short-ranged entanglement have not been the center of much attention because they are expected to behave semi-classically. However, as we will demonstrate …

Numerical Studies Of Correlated Topological Systems, Rahul Soni

Doctoral Dissertations

In this thesis, we study the interplay of Hubbard U correlation and topological effects in two different bipartite lattices: the dice and the Lieb lattices. Both these lattices are unique as they contain a flat energy band at E = 0, even in the absence of Coulombic interaction. When interactions are introduced both these lattices display an unexpected multitude of topological phases in our U -λ phase diagram, where λ is the spin-orbit coupling strength. We also study ribbons of the dice lattice and observed that they qualitative display all properties of their two-dimensional counterpart. This includes flat bands near …

Quantum Computational Simulations For Condensed Matter Systems, Trevor Alan Keen

Doctoral Dissertations

In condensed matter physics, and especially in the study of strongly correlated electron systems, numerical simulation techniques are crucial to determine the properties of the system including interesting phases of matter that arise from electron-electron interactions. Many of these interesting phases of matter, including but not limited to Mott-insulating materials and possibly high-temperature superconducting systems, can be modeled by the Hubbard model. Although it is one of the simplest models to include electron-electron interactions, it cannot be solved analytically in more than one dimension and thus numerical techniques must be employed. Although there have been great strides in classical numerical …

Emergent Phenomenon In Jeff=1/2 Iridate, Junyi Yang

Doctoral Dissertations

Recent work on various quantum materials has led to fruitful result including unconventional magnetic states, topological properties, and exotic emergent phenomenon. High T_c superconductivity is one of the prominent properties discovered in quantum materials like strong correlated systems. Though the efforts on understanding this exotic behavior have lasted for years, the mechanism remains elusive owing to the many-body nature of the system and the research scope limitation within cuprates. Recent unravel of J_eff=1/2 state in the iridate square lattice offers alternative to study the complicated many body physics and potentially achieve high T_c superconductivity. In addition, …

Local Dynamics And Atomic-Level Structures In Metallic Liquids And Glasses, Zengquan Wang

Doctoral Dissertations

Structure and dynamics at the atomic level in metallic glasses and liquids are poorly understood when compared to the crystalline solids. For instance, even though viscosity is the basic property of liquids, its atomistic origin is not well elucidated. Also, the physics of the fragility of liquids and the crossover phenomenon is far from full understanding. Earlier, through molecular dynamics (MD) simulations a direct connection was found between the timescale describing the macroscopic viscous behavior, the Maxwell relaxation time (t_M = h/G_∞, h is the shear viscosity and G_∞ is the high-frequency shear modulus) and …

Spectroscopic Properties Of Ferroic Superlattices, Shiyu Fan

Doctoral Dissertations

The interplay between charge, structure, magnetism, and orbitals leads to rich physics and exotic cross-coupling in multifunctional materials. Superlattices provide a superb platform to study the complex interactions between different degrees of freedom. In this dissertation, I present a spectroscopic investigation of natural and engineered superlattices including Fe_xTaS₂ and (LuFeO₃)_m/(LuFe₂O₄)₁ under external stimuli of temperature and magnetic field as well as chemical substitution. Studying the phase transitions, symmetry-breaking, and complex interface interactions from a microscopic viewpoint enhances fundamental understanding of coupling mechanism between different order parameters and the …

Numerical Studies Of Superconductivity And Charge-Density-Waves: Progress On The 2d Holstein Model And A Superconductor-Metal Bilayer, Philip M. Dee

Doctoral Dissertations

The problem of superconductivity has been central in many areas of condensed matter physics for over 100 years. Despite this long history, there is still no theory capable of describing both conventional and unconventional superconductors. Recent experimental observations such as the dilute superconductivity in SrTiO₃ and near room-temperature superconductivity in hydride compounds under extreme pressure have renewed interest in electron-phonon systems. Adding to this is evidence that electron-phonon coupling may play a supporting role in unconventional systems like the cuprates and monolayer FeSe on SrTiO₃.

One way to make sense of these observations is to construct simple …

Exploring Structural And Electronic Properties Of Triangular Adatom Layers On The Silicon Surface Through Adsorbate Doping, Tyler S. Smith

Doctoral Dissertations

The analysis of the electronic structure and morphology of 1/3 monolayers (ML) of Sn or Pb on Si(111) and Ge(111) has played an important role in understanding the role of electronic correlations in two dimensions. Specifically, the two-dimensional lattice of partially filled dangling bonds of these so-called α-phases has been an important testbed for studying structural phase transitions and correlated electronic phenomena ever since the discovery of a surface charge density wave in the Pb/Ge(111) system more than two decades ago. With the exception of the novel Sn/Si(111) system, all $\alpha$-phases undergo a charge ordering transition at low temperature. The …

Numerical Studies Of Multi-Orbital Hubbard Models, Nitin Kaushal

Doctoral Dissertations

This thesis examines the emergence of exotic phases in multi-orbital Hubbard models due to competition between Coulomb interaction, spin-orbit coupling and kinetic energy. Exact diagonalization and numerically accurate density matrix renormalization group methods are used to study small clusters and one dimensional chains. Two dimensional lattices are solved using unrestricted real-space Hartree-Fock approximation. Novel excitonic insulators, due to condensation of spin-orbit excitons, are found in the spin-orbit coupling vs Coulomb interation phase diagrams of (t_2g)ⁿ systems for n = 4 and 3.5. Moreover, the presence of a BCS-BEC crossover in the (t_2g)4 excitonic insulator is …

Theoretical Modeling Of Metallic Compounds With Versatile Properties By Combining First-Principles Calculations And Global Structure Prediction Algorithms, Jinseon Park

Doctoral Dissertations

Improving the target properties of existing materials or finding new materials with enhanced functionality for practical applications is at the heart of the materials research. In this respect, the first-principles approaches, which have been successfully integrated into modern high- performance computers, have become an indispensable part of the materials research, providing a better understanding of existing materials and guidance on the design of new materials. Using state-of-the-art computational/theoretical approaches that couple global structure prediction with ab initio density functional theory calculations, we investigate structural and electronic properties of Cs_xO [cesium oxides], Li_1+xMn₂O₄ [lithium …

From Pyrochlore To The Tripod Kagome Lattice: Magnetism Of New Compound Family A2re3sb3o14 (A = Mg, Zn; Re = Pr, Nd, Gd, Tb, Dy, Ho, Er, Yb), Zhiling Dun

Doctoral Dissertations

Geometrical frustration refers to the inability of a complex system to satisfy all its competing interactions within an underlying topological constrained lattice. The two-dimensional kagome lattice is one of the most frustrated lattices and has been a favorite in the theoretical condensed matter community. However, the large variety of exotic states predicted in kagome lattices lies in contrast to a paucity of experimental systems, making new kagome lattice compounds highly desired.

In this dissertation, I shall provide a systematic study of the structural and magnetic properties of a new compounds family, A2RE3Sb3O14 (A = Mg, Zn; RE = Pr, Nd, …

Numerical Studies Of Iron Based Superconductors Using Spin-Fermion Models, Christopher Brian Bishop

Doctoral Dissertations

The iron pnictide and iron chalchogenide superconductors are studied numerically using classical Monte Carlo techniques to reproduce experimental data and make predictions about the nature of the relevant interactions. The focus will be using Spin-Fermion models in a classical approximation to explore the phase diagram and calculate important physical properties of these materials over a wide range of temperatures.

Local Moments And Itinerant Electrons: Gaining New Insights Through Investigating Electronic And Dynamical Properties, Nicholas Steven Sirica

Doctoral Dissertations

Magnetic materials are often categorized in terms of either a purely local or a purely itinerant picture despite the fact that the vast majority actually fall within a spectrum that ranges between these two extremes. It is from such a starting point that this thesis aims at developing an understanding of how the complex interplay between local moments and itinerant electrons ultimately affects the electronic and dynamical properties. Such ideas are explored in greater detail using two materials as case studies: the chiral helimagnet Cr_1/3NbS₂ [Cr intercalated Niobium Disulfide] and YFe₂Ge₂ [Yttrium Iron Germanide] …

First-Principles Study Of Point Defect Behavior At Interfaces And In-Plane Strain Fields, Jianqi Xi

Doctoral Dissertations

Interfaces in solid materials are the so-called boundaries, separating crystals with the same structure and chemistry but different orientations, e.g. grain boundaries (GBs), different stacking sequences, e.g. stacking faults (SFs), or crystals with different structures and/or chemistries as well as orientations, e.g. the interface between substrate and thin film. In this study, first-principles calculations are used to investigate the defect behavior at different interfaces and in-plane strain fields, such as stacking fault (SF) in silicon carbide (SiC), in-plane strain field near interfaces in potassium tantalate (KTaO₃), and grain boundary in ceria (CeO₂).

Results show that the …

Electronic And Magnetic Materials Under External Stimuli, Kenneth Robert O'Neal

Doctoral Dissertations

The interaction between spin, charge, and lattice degrees of freedom leads to exotic and useful properties in multifunctional materials. This delicate balance of energy scales allows external stimuli such as temperature, magnetic field, or pressure to drive to novel phases. As a local probe technique, spectroscopy can provide insight into the microscopic mechanism of the phase transitions. In this dissertation I present spectroscopic studies of functional materials under extreme conditions.

Nanomaterials have attracted attention because nanoscale confinement affects various material properties and often reduces energy scales or suppress phase transitions. Combining Raman and infrared spectroscopies reveals that the breakdown mechanism …

Unveiling Quantum Critical Phenomena In Selected Rare Earth Intermetallic Compounds, Lekhanath Poudel

Doctoral Dissertations

The quantum critical phenomenon of CeCu_6-xAu_x (x =0.1) [gold-doped cerium copper six] presents a host of intriguing puzzles: In particular, the dynamic susceptibility showing E/T-scaling with a fractional exponent of 0.75 is a surprise and is clearly inconsistent with the established approach developed by Hertz, Millis, and Moriya (HMM). Interestingly, the phase diagram of CeCu_6-xAu_x [gold-doped cerium copper six] also suggests a zero temperature structural phase transition, raising the possibility of a structural quantum critical point (QCP). To provide a further insight into the unconventional quantum criticality and to investigate the possibility of …

Properties And Manipulation Of Ionic Liquid-Solid Interfaces In Complex Oxide Materials, Anthony Thomas Wong

Doctoral Dissertations

Ionic liquids are liquid salts that are bringing rapid changes to the field of solid electronic materials. The implementation of ionic liquids in conjunction with these solid materials produces interfacial effects, especially when a bias is applied across the ionic liquid, forming an electric double layer. Electric double layers in ionic liquids are unique in their formation and the interfacial charges that are orders of magnitude higher than conventional techniques they can impart, providing new techniques for device design and implementation. In chapter 1, the fundamentals of the solid state electronic and magnetic materials are introduced, along with ionic liquids, …

Understanding Three-Body Interactions In Hexagonal Close Packed Solid He-4, Ashleigh Locke Barnes

Doctoral Dissertations

The ground state properties of hexagonal close packed (hcp) solid ⁴He [He-4] are dominated by large atomic zero point motions which make the primary contribution to the solid’s low-temperature Debye-Waller (DW) factors. Preliminary investigations have also suggested that three-body interactions can play an important role in this system, particularly at higher densities. However, due to their computational cost, these interactions are not generally incorporated into theoretical models of solid ⁴He [He-4]. In order to accurately treat both zero point motion and three-body interactions, we have developed a perturbative treatment in which the three-body energy is added as a …

Investigating The Properties Of Superfluid He-4 Through Density Functional Calculations, Matthew Francis Dutra

Doctoral Dissertations

We present a study of isotopically pure He-4 systems evaluated using helium density functional theory (He-DFT) with the intent of better understanding their ground state structural and energetic properties, particularly within the scope of singularly-doped helium droplets. We self-consistently solve for the density profiles and chemical potentials for a wide range of pure helium droplet sizes (up to 9500 atoms) via an imaginary time propagation method, and fit the resultant energetic data to a power law formula to be able to extrapolate values for even larger droplets. Subsequent calculations on singularly-doped droplets within the same size range yield accurate binding …

Optical Spectroscopy And The Contruction Of An Optimal Wannier Basis With Application To The Development Of Ab Initio Models, Robert Gerard Van Wesep

Doctoral Dissertations

Understanding the role of local orbital degrees of freedom in the behavior of solid state systems has long been understood as a key to unraveling the mysteries presented by complex transition metal compounds. A general approach to the many-body problem is density functional theory (DFT) and its time-dependent extension (TDDFT), which provide a realistic representation of the material-dependent symmetry and chemistry of a compound. Calculation of quantities in (TD)DFT are most often performed using the basis of Bloch states, which is not natural for investigating local degrees of freedom. The Wannier basis provides localized orbitals that retain all of the …

Characterizing Local Order And Physical Properties Of Rare Earth Complex Oxides, Thomas Jacob Shamblin

Doctoral Dissertations

With more than 500 compositions, materials possessing the pyrochlore structure have a myriad of technological applications and physical phenomena. Three of the most noteworthy properties are the structure’s ability to resist amorphization making it a possible host matrix for spent nuclear fuel, its exotic magnetic properties arising from geometric frustration, and fast ionic conductivity for solid-oxide fuel cell applications. This work focuses on these three aspects of the pyrochlore’s many potential uses. Structural characterization revealed that pyrochlore-type oxides have a tendency to disorder from a high symmetry cubic structure to a lower symmetry orthorhombic arrangement in response to a variety …

Spontaneously Generated Inhomogeneous Phases Via Holography, Kübra Yeter Aydeniz

Doctoral Dissertations

We discuss a holographic model consisting of a U(1) gauge field and a scalar field coupled to a charged AdS (anti-de Sitter) black hole under a spatially homogeneous chemical potential. By turning on a higher-derivative interaction term between the U(1) gauge field and the scalar field, a spatially dependent profile of the scalar field is generated spontaneously. We calculate the critical temperature at which the transition to the inhomogeneous phase occurs for various values of the parameters of the system. We solve the equations of motion below the critical temperature, and show that the dual gauge theory on the boundary …

Crystal Growth And Physical Property Characterization Of Complex Perovskite Oxides, Ling Li

Doctoral Dissertations

Bulk EuTiO₃ [europium titanate], a quantum paraelectric antiferromagnet, is shown to exhibit multiferroic behavior in strained thin film form, which highlights the spin-phonon coupling in this system. We have investigated the structural, elastic, magnetic, thermal and transport properties of single crystals of EuTiO₃ as well as doped system EuTi_1-xB_xO₃ (B = Zr, Nb) [Zr and Nb doped europium titanate] utilizing various experimental techniques and theoretical calculations.

The cubic to tetragonal structural transition in pure EuTiO₃ is characterized by a pronounced step-like softening of the elastic moduli near 288 K [kelvin], which resembles …