<p> Due to high specific capacity for lithiation, molybdenum dichalcogenides such as MoO₂ and MoS₂ are potential replacements for graphite anodes in Li-ion batteries. However, in bulk form these materials exhibit poor rate capability and lose capacity with each cycle. While the performance can be improved by changes to morphology, the details of the lithium intercalation mechanism are not fully understood. </p><p> In this work, X-ray absorption spectroscopy (XAS) is employed to investigate this mechanism, including X-ray absorption near-edge spectroscopy (XANES) and X-ray absorption fine-structure spectroscopy (XAFS). For MoS₂, modeling of the local structure supports the metallic conversion reaction model by the second lithiation.</p><p>

This thesis presents a study of two basic modes of deformation of a thin sheet: wrinkling and crumpling, viewed primarily in the context of an elastic sheet confined by capillary forces on a drop of liquid. First, it provides a brief conceptual background in the relevant physics of thin sheet mechanics and capillarity and introduces the general principles of wrinkling and crumpling. The problem of confining a circular sheet on an increasingly curved spherical drop is presented as a vehicle to explore these principles. At finite curvature, the sheet is seen to wrinkle around its outer edge. At large confinement, characteristic features of crumpling gradually dominate the pattern. The experimental observations in both regimes are analyzed separately. Analysis of images of the sheet in the wrinkled regime yield data for the number and length of the wrinkled zone, as a function of the experimental control parameter, the pressure. The length of the wrinkles is correctly described by a far-from-threshold theory, which describes a limiting regime in thin-sheet mechanics, distinguished by high 'bendability'. The validity of this theory is verified by the data for highly bendable, ultrathin sheets for the first time. The theory is based on the assumption that the wrinkles completely relax compressive stresses and therefore preserve the cylindrical symmetry of the stress field. The emergence of crumpling from the wrinkled shape is explored via evolution of visible features in the sheet as well as gaussian curvature measurements obtained by analyzing height maps from optical profilometry. The emergence of several length scales, increasing asymmetry in curvature distribution, the failure of wrinkle extent prediction and formation of d-cones associated with crumpling are all measured to locate the transition to a crumpled state. The value of gaussian curvature at the center of the sheet appears to follow the cylindrically symmetric prediction over the whole range of the experiment, suggesting that the onset of crumpling events does not affect the global shape of the sheet. Finally, analogous wrinkling and crumpling behavior of particle-laden interfaces is discussed. The spontaneous formation of conical defects in a curved 2D crystal is compared to the crumpling of a sheet on a drop, and insight from thin sheet mechanics is applied to the mysterious wrinkling of particle rafts. Some future directions for measuring wrinkling of sheets on negative curvature surfaces and deformations of fluid interfaces are proposed.

<p> This dissertation is an account of the first calorimetric detection of individual He*₂ excimers within a bath of superfluid ⁴He. When superfluid helium is subject to ionizing radiation, diatomic He molecules are created in both the singlet and triplet states. The singlet He molecules decay within nanoseconds, but due to a forbidden spin-flip the triplet molecules have a relatively long lifetime of 13 seconds in superfluid He. When He*₂ molecules decay, they emit a ~15 eV photon. Nearly all matter is opaque to these vacuum-UV photons, although they do propagate through liquid helium. The triplet state excimers propagate ballistically through the superfluid until they quench upon a surface; this process deposits a large amount of energy into the surface. The prospect of detecting both excimer states is the motivation for building a detector immersed directly in the superfluid bath.</p><p> The detector used in this work is a single superconducting titanium transition edge sensor (TES). The TES is mounted inside a hermetically sealed chamber at the baseplate of a dilution refrigerator. The chamber contains superfluid helium at 100 mK. Excimers are created during the relaxation of high-energy electrons, which are introduced into the superfluid bath either in situ via a sharp tungsten tip held above the field-emission voltage, or by using an external gamma-ray source to ionize He atoms. These excimers either propagate through the LHe bath and quench on a surface, or decay and emit vacuum-ultraviolet photons that can be collected by the detector.</p><p> This dissertation discusses the design, construction, and calibration of the TES-based excimer detecting instrument. It also presents the first spectra resulting from the direct detection of individual singlet and triplet helium excimers.</p>

<p> Engineered quantum systems are poised to revolutionize information science in the near future. A persistent challenge in applied quantum technology is creating controllable, quantum interactions while preventing information loss to the environment, decoherence. In this thesis, we realize mesoscopic superconducting circuits whose macroscopic collective degrees of freedom, such as voltages and currents, behave quantum mechanically. We couple these mesoscopic devices to microwave cavities forming a cavity quantum electrodynamics (QED) architecture comprised entirely of circuit elements. This application of cavity QED is dubbed Circuit QED and is an interdisciplinary field seated at the intersection of electrical engineering, superconductivity, quantum optics, and quantum information science. Two popular methods for taming active quantum systems in the presence of decoherence are discrete feedback conditioned on an ancillary system or quantum reservoir engineering. Quantum reservoir engineering maintains a desired subset of a Hilbert space through a combination of drives and designed entropy evacuation. Circuit QED provides a favorable platform for investigating quantum reservoir engineering proposals. A major advancement of this thesis is the development of a quantum reservoir engineering protocol which maintains the quantum state of a microwave cavity in the presence of decoherence. This thesis synthesizes strongly coupled, coherent devices whose solutions to its driven, dissipative Hamiltonian are predicted a <i>priori</i>. This work lays the foundation for future advancements in cavity centered quantum reservoir engineering protocols realizing hardware efficient circuit QED designs. </p>

<p> This work contributes to the study of magnetic interactions in the low-dimensional antiferromagnets <i>M</i>(Sb,Ta)₂O₆, where <i> M</i> is a transition metal. By virtue of the trirutile structure, <i> M-O-O-M</i> chains propagate along [110] at <i>z</i> = 0 and [1<span style="text-decoration:overline">1</span>0] at <i>z</i> = 1/2 of the unit cell. These chains are separated along [001] by sheets of weakly-interacting diamagnetic ions. The spin-exchange coupling perpendicular to the chains is weak, permitting the low-dimensional classification. Single crystals have been grown using chemical vapor deposition and the floating zone method. Magnetization, in-field heat capacity, and high-resolution thermal expansion measurements have been performed along various axes, revealing significant anisotropy due to the peculiar magnetic structures and low dimensionality.</p><p> The Neel temperature, <i>T_N,</i> at which long-range order occurs is found to be unstable against the application of magnetic field above 2 T. Large fields tend to lower <i>T_N</i> of the set of moments with projections along the applied field. Moments which are aligned perpendicular to the field are significantly less affected. This can lead to the formation of a secondary peak in heat capacity when magnetic field is along either [110] or [1<span style="text-decoration:overline">1</span>0]. The change in heat capacity at the location of the newly formed peak means there is a change in entropy, which depends upon the direction of applied field with respect to the magnetic moments. Consequently, an anisotropic magnetocaloric effect arises due to the unique magnetic structure. The anisotropic nature of this effect has potential applications in magnetic refrigeration.</p>

<p> For a broad class of two-dimensional (2D) materials, the transition from isotropic fluid to crystalline solid is described by the theory of melting due to Kosterlitz, Thouless, Halperin, Nelson and Young (KTHNY). According to this theory, long-range order is achieved via elimination of the topological defects which proliferate in the fluid phase. However, many natural and man-made 2D systems posses spatial curvature and/or non-trivial topology, which require the presence of topological defects, even at T=0. In principle, the presence of these defects could profoundly affect the phase behavior of such a system. In this thesis, we develop and characterize an experimental system of charged colloidal particles that bind electrostatically to the interface between an oil and an aqueous phase. Depending on how we prepare the sample, this fluid interface may be flat, spherical, or have a more complicated geometry. Focusing on the cases where the interface is flat or spherical, we measure the interactions between the particles, and probe various aspects of their phase behavior. On flat interfaces, this phase behavior is well-described by KTHNY theory. In spherical geometries, however, we observe spatial structures and inhomogeneous dynamics that cannot be captured by the measures traditionally used to describe flat-space phase behavior. We show that, in the spherical system, ordering is achieved by a novel mechanism: sequestration of topological defects into freely-terminating grain boundaries (&ldquo;scars&rdquo;), and simultaneous spatial organization of the scars themselves on the vertices of an icosahedron. The emergence of icosahedral order coincides with the localization of mobility into isolated &ldquo;lakes&rdquo; of fluid or glassy particles, situated at the icosahedron vertices. These lakes are embedded in a rigid, connected &ldquo;continent&rdquo; of locally crystalline particles.</p><p>

<p> Originally proposed in high energy physics as particles, which are their own anti-particles, Majorana fermions have never been observed in experiments. However, possible signatures of their condensed matter analog, zero energy, charge neutral, quasiparticle excitations, known as Majorana zero modes (MZMs), are beginning to emerge in experimental data. The primary method of engineering topological superconductors capable of supporting MZMs is through proximity-coupled semiconductor nanowires with strong Rashba spin-orbit coupling and an applied magnetic field. Recent tunneling transport experiments involving these materials, known as semiconductor-superconductor heterostructures, were capable for the first time of measuring quantized zero bias conductance plateaus, which are robust over a range of control parameters, long believed to be the smoking gun signature of the existence of MZMs. The possibility of observing Majorana zero modes has garnered great excitement within the field due to the fact that MZMs are predicted to obey non-Abelian quantum statistics and therefore are the leading candidates for the creation of qubits, the building blocks of a topological quantum computer. In this work, we first give a brief introduction to Majorana zero modes and topological quantum computing (TQC). We emphasize the importance that having a true topologically protected state, which is not dependent on local degrees of freedom, has with regard to non-Abelian braiding calculations. We then introduce the concept of partially separated Andreev bound states (ps-ABSs) as zero energy states whose constituent Majorana bound states (MBSs) are spatially separated on the order of the Majorana decay length. Next, through numerical calculation, we show that the robust 2<i> e²/h</i> zero bias conductance plateaus recently measured and claimed by many in the community to be evidence of having observed MZMs for the first time, can be identically created due to the existence of ps-ABSs. We use these results to claim that all localized tunneling experiments, which have been until now the main way researchers have tried to measure MZMs, have ceased to be useful. Finally, we outline a two-terminal tunneling experiment, which we believe to be relatively straight forward to implement and fully capable of distinguishing between ps-ABSs and true topologically protected MZMs.</p><p>

Thesis (Ph.D.)--Brown University, 2008. / Advisor: Xinsheng S. Ling. Includes bibliographical references (leaves 111-125).

<p> The Mott metal-insulator transition (MIT) in transition-metal complex oxides results from strong electron-electron interactions and is accompanied by a rich spectrum of phenomena, including magnetic, charge, and orbital ordering, superconductivity, structural distortions, polarons, and very high-density 2-dimensional interface electron liquids. Recent advances in oxide heteroepitaxy allow interface control as a promising new approach to tuning the exotic properties of materials near the quantum critical point, with potential application to technologies including phase-change electronics, high power transistors, and sensors. The dynamical conductivity of oxide heterostructures is measured using a combination of terahertz time-domain spectroscopy, Fourier transform infrared spectroscopy, and dc magnetotransport. The rare-earth nickelates <i> R</i>NiO₃ (<i>R</i> = La, Nd...) exhibit a temperature and bandwidth controlled MIT in bulk. Measurements of the Drude response in epitaxial thin films provide quantification of the strain-dependent mass enhancement in the metallic phase due to strong correlations. Reduction of LaNiO₃ film thickness leads to additional mass renormalization attributed to structural distortions at the heteroepitaxial interface, and an MIT is observed depending on the interfacing materials in coherent perovskite heterostructures. The rare-earth titanates <i>R</i>TiO₃ exhibit a bandwidth and band filling controlled Mott MIT. Furthermore, the heterointerface between Mott insulating GdTiO₃ and band insulating SrTiO₃ exhibits a 2-dimensional itinerant electron liquid, with extremely high sheet densities of 3 &times; 10¹⁴ cm^-2. The dynamical conductivity of the interface electrons is analyzed in terms of subband-dependent electron mobility and the established large polaron dynamics in bulk SrTiO₃. Additional confinement of the electron liquids is achieved by decreasing the SrTiO₃ layer thickness, with attendant increase in the dynamical mass. Taking the confinement to its extreme limit, a single (GdO)⁺ plane in Mott insulating GdTiO₃ is replaced with a (SrO)⁰ plane. This is equivalent to "delta-doping" the Mott insulator with an extremely high density sheet of holes. The transport and absorption in the resulting two-dimensional insulator are consistent with a simple model of small polaron hopping. A comparison is made to similar features in the conductivity of randomly doped Sr_1-xGd_xTiO₃ films.</p>

Thesis (Ph.D.)--Indiana University, Dept. of Physics, 2007. / Title from PDF t.p. (viewed Nov. 20, 2008). Source: Dissertation Abstracts International, Volume: 68-03, Section: B, page: 1688. Adviser: David V. Baxter.