Studies of phonon anharmonicity in solids

Today our understanding of the vibrational thermodynamics of materials at low temperatures is emerging nicely, based on the harmonic model in which phonons are independent. At high temperatures, however, this understanding must accommodate how phonons interact with other phonons or with other excitations. We shall see that the phonon-phonon interactions give rise to interesting coupling problems, and essentially modify the equilibrium and non-equilibrium properties of materials, e.g., thermodynamic stability, heat capacity, optical properties and thermal transport of materials. Despite its great importance, to date the anharmonic lattice dynamics is poorly understood and most studies on lattice dynamics still rely on the harmonic or quasiharmonic models. There have been very few studies on the pure phonon anharmonicity and phonon-phonon interactions. The work presented in this thesis is devoted to the development of experimental and computational methods on this subject.

Modern inelastic scattering techniques with neutrons or photons are ideal for sorting out the anharmonic contribution. Analysis of the experimental data can generate vibrational spectra of the materials, i.e., their phonon densities of states or phonon dispersion relations. We obtained high quality data from laser Raman spectrometer, Fourier transform infrared spectrometer and inelastic neutron spectrometer. With accurate phonon spectra data, we obtained the energy shifts and lifetime broadenings of the interacting phonons, and the vibrational entropies of different materials. The understanding of them then relies on the development of the fundamental theories and the computational methods.

We developed an efficient post-processor for analyzing the anharmonic vibrations from the molecular dynamics (MD) calculations. Currently, most first principles methods are not capable of dealing with strong anharmonicity, because the interactions of phonons are ignored at finite temperatures. Our method adopts the Fourier transformed velocity autocorrelation method to handle the big data of time-dependent atomic velocities from MD calculations, and efficiently reconstructs the phonon DOS and phonon dispersion relations. Our calculations can reproduce the phonon frequency shifts and lifetime broadenings very well at various temperatures.

To understand non-harmonic interactions in a microscopic way, we have developed a numerical fitting method to analyze the decay channels of phonon-phonon interactions. Based on the quantum perturbation theory of many-body interactions, this method is used to calculate the three-phonon and four-phonon kinematics subject to the conservation of energy and momentum, taking into account the weight of phonon couplings. We can assess the strengths of phonon-phonon interactions of different channels and anharmonic orders with the calculated two-phonon DOS. This method, with high computational efficiency, is a promising direction to advance our understandings of non-harmonic lattice dynamics and thermal transport properties.

These experimental techniques and theoretical methods have been successfully performed in the study of anharmonic behaviors of metal oxides, including rutile and cuprite stuctures, and will be discussed in detail in Chapters 4 to 6. For example, for rutile titanium dioxide (TiO₂), we found that the anomalous anharmonic behavior of the B_1g mode can be explained by the volume effects on quasiharmonic force constants, and by the explicit cubic and quartic anharmonicity. For rutile tin dioxide (SnO₂), the broadening of the B_2g mode with temperature showed an unusual concave downwards curvature. This curvature was caused by a change with temperature in the number of down-conversion decay channels, originating with the wide band gap in the phonon dispersions. For silver oxide (Ag₂O), strong anharmonic effects were found for both phonons and for the negative thermal expansion.

Measurement of the neutron beta decay asymmetry using ultracold neutrons

The free neutron beta decay correlation A₀ between neutron polarization and electron emission direction provides the strongest constraint on the ratio λ = g_A/g_V of the Axial-vector to Vector coupling constants in Weak decay. In conjunction with the CKM Matrix element V_ud and the neutron lifetime τ_n, λ provides a test of Standard Model assumptions for the Weak interaction. Leading high-precision measurements of A₀ and τ_n in the 1995-2005 time period showed discrepancies with prior measurements and Standard Model predictions for the relationship between λ, τ_n, and V_ud. The UCNA experiment was developed to measure A₀ from decay of polarized ultracold neutrons (UCN), providing a complementary determination of λ with different systematic uncertainties from prior cold neutron beam experiments. This dissertation describes analysis of the dataset collected by UCNA in 2010, with emphasis on detector response calibrations and systematics. The UCNA measurement is placed in the context of the most recent τ_n results and cold neutron A₀ experiments.

Ferromagnetic Resonance Force Microscopy

A new approach to magnetic resonance was introduced in 1992 based upon detection of spin-induced forces by J. Sidles [1]. This technique, now called magnetic resonance force microscopy (MRFM), was first demonstrated that same year via electron paramagnetic resonance (EPR) by D. Rugar et al. [2]. This new method combines principles of magnetic resonance with those of scanned probe technology to detect spin resonance through mechanical, rather than inductive, means. In this thesis the development and use of ferromagnetic resonance force microscopy (FMRFM) is described. This variant of MRFM, which allows investigation of ferromagnetic samples, was first demonstrated in 1996 by Z. Zhang et al. [3]. FMRFM enables characterization of (a) the dynamic magnetic properties of microscale magnetic devices, and (b) the spatial dependence of ferromagnetic resonance within a sample. Both are impossible with conventional ferromagnetic resonance techniques.

Ferromagnetically coupled systems, however, pose unique challenges for force detection. In this thesis the attainable spatial resolution - and the underlying physical mechanisms that determine it - are established. We analyze the dependence of the magnetostatic modes upon sample dimensions using a series of microscale yttrium iron garnet (YIG) samples. Mapping of mode amplitudes within these sample is attained with an unprecedented spatial resolution of 15μm. The modes, never before analyzed on this scale, fit simple models developed in this thesis for samples of micron dimensions. The application of stronger gradient fields induces localized perturbation of the ferromagnetic resonance modes. The first demonstrations of this effect are presented in this study, and a simple theoretical model is developed to explain our observations. The results indicate that the characteristics of the locally-detected ferromagnetic modes are still largely determined by the external fields and dimensions of the entire sample, rather than by the localized interaction volume (i.e., the locale most strongly affected by the local gradient field). Establishing this is a crucial first step toward understanding FMRFM in the high gradient field limit where the dispersion relations become locally determined. In this high gradient field regime, FMRFM imaging becomes analogous with that of EPR MRFM.

FMRFM has also been employed to characterize magnetic multilayers, similar to those utilized in giant magnetoresistance (GMR) devices, on a lateral scale 40 x 40μm. This is orders of magnitude smaller than possible via conventional methods. Anisotropy energies, thickness, and interface qualities of individual layers have been resolved.

This initial work clearly demonstrates the immense and unique potential that FMRFM offers for characterizing advanced magnetic nanostructures and magnetic devices.

Radiative tau production and decay

A study of the muon decay channel of the τ lepton with the presence of a photon has been carried out to verify theoretical predictions for the production rate of e⁺e^- → τ⁺τ^-γ and for the branching ratio of τ^- → ν_τ µ^-ν_µγ. Included in this study is the first direct measurement of radiative tau decay. Using e⁺e^- annihilation data taken at 29 GeV center-of-mass energy with the Mark II detector, we find the ratio of the measured τ^- → ν_τ µ^-ν_µγ branching fraction to the expected value from QED to be 1.03 ± 0.42. The ratio of measured-to-predicted number of events from radiative T production, e⁺e^- → τ⁺τ^-γ, where one of the τ's decay to μνν is found to be 0.91 ± 0.20. We have not seen an indication of anomalous behavior in radiative tau events.

Plasma loop and strapping field dynamics: reproducing solar eruptions in the laboratory

Coronal mass ejections (CMEs) are dramatic eruptions of large, plasma structures from the Sun. These eruptions are important because they can harm astronauts, damage electrical infrastructure, and cause auroras. A mysterious feature of these eruptions is that plasma-filled solar flux tubes first evolve slowly, but then suddenly erupt. One model, torus instability, predicts an explosive-like transition from slow expansion to fast acceleration, if the spatial decay of the ambient magnetic field exceeds a threshold.

We create arched, plasma filled, magnetic flux ropes similar to CMEs. Small, independently-powered auxiliary coils placed inside the vacuum chamber produce magnetic fields above the decay threshold that are strong enough to act on the plasma. When the strapping field is not too strong and not too weak, expansion force build up while the flux rope is in the strapping field region. When the flux rope moves to a critical height, the plasma accelerates quickly, corresponding to the observed slow-rise to fast-acceleration of most solar eruptions. This behavior is in agreement with the predictions of torus instability.

Historically, eruptions have been separated into gradual CMEs and impulsive CMEs, depending on the acceleration profile. Recent numerical studies question this separation. One study varies the strapping field profile to produce gradual eruptions and impulsive eruptions, while another study varies the temporal profile of the voltage applied to the flux tube footpoints to produce the two eruption types. Our experiment reproduced these different eruptions by changing the strapping field magnitude, and the temporal profile of the current trace. This suggests that the same physics underlies both types of CME and that the separation between impulsive and gradual classes of eruption is artificial.

Excitation energies and decay properties of T = 3/2 states in ^(17)O, ^(17)F and ^(21)Na

The two lowest T = 3/2 levels in ²¹Na have been studied in the ¹⁹F(³He, n), ²⁰Ne (p,p) and ²⁰Ne (p,p’) reactions, and their excitation energies, spins, parities and widths have been determined. In a separate investigation, branching ratios were measured for the isospin-nonconserving particle decays of the lowest T = 3/2 levels in ¹⁷O and ¹⁷F to the ground state and first two excited states of ¹⁶O, by studying the ¹⁵N(³He,n) ¹⁷F*(p) ¹⁶O and ¹⁸O(³He, α)¹⁷O*(n) ¹⁶O reactions.

The ¹⁹F(³He,n) ²¹Na reaction was studied at incident energies between 4.2 and 5.9 MeV using a pulsed-beam neutron-time-of-flight spectrometer. Two T = 3/2 levels were identified at excitation energies of 8.99 ± 0.05 MeV (J > ½) and 9.22 ± 0.015 MeV (J ^π = ½⁺, Γ ˂ 40 keV). The spins and parities were determined by a comparison of the measured angular distributions with the results of DWBA calculations.

These two levels were also obsesrved as isospin-forbidden resonances in the ²⁰Ne(p,p) and ²⁰Ne(p,p’) reactions. Excitation energies were measured and spins, parities, and widths were determined from a single level dispersion theory analysis. The following results were obtained:

E_x = 8.973 ± 0.007 MeV, J ^π = 5/2 ⁺ or 3/2⁺, Γ ≤ 1.2 keV,

^Γp_o = 0.1 ± 0.05 keV; E_x = 9.217 ± 0.007 MeV, J^π = ½ ⁺,

Γ = 2.3 ± 0.5 keV, ^Γp_o = 1.1 ± 0.3 keV.

Isospin assignments were made on the basis of excitation energies, spins, parities, and widths.

Branching ratios for the isospin-nonconserving proton decays of the 11.20 MeV, T = 3/2 level in ¹⁷F were measured by the ¹⁵N(³He,n) ¹⁷ F*(p) ¹⁶O reaction to be 0.088 ± 0.016 to the ground state of ¹⁶O and 0.22 ± 0.04 to the unresolved 6.05 and 6.13 MeV levels of ¹⁶O. Branching ratios for the neutron decays of the analogous T = 3/2 level, at 11.08 MeV in ¹⁷O, were measured by the ¹⁶O(³He, α)¹⁷O*(n)¹⁶O reaction to be 0.91 ± 0.15 to the ground state of ¹⁶O and 0.05 ± 0.02 to the unresolved 6.05 and 6.13 MeV states. By comparing the ratios of reduced widths for the mirror decays, the form of the isospin impurity in the T = 3/2 levels is shown to depend on T_z.

Force chains, friction, and flow: Behavior of granular media across length scales

We study the behavior of granular materials at three length scales. At the smallest length scale, the grain-scale, we study inter-particle forces and "force chains". Inter-particle forces are the natural building blocks of constitutive laws for granular materials. Force chains are a key signature of the heterogeneity of granular systems. Despite their fundamental importance for calibrating grain-scale numerical models and elucidating constitutive laws, inter-particle forces have not been fully quantified in natural granular materials. We present a numerical force inference technique for determining inter-particle forces from experimental data and apply the technique to two-dimensional and three-dimensional systems under quasi-static and dynamic load. These experiments validate the technique and provide insight into the quasi-static and dynamic behavior of granular materials.

At a larger length scale, the mesoscale, we study the emergent frictional behavior of a collection of grains. Properties of granular materials at this intermediate scale are crucial inputs for macro-scale continuum models. We derive friction laws for granular materials at the mesoscale by applying averaging techniques to grain-scale quantities. These laws portray the nature of steady-state frictional strength as a competition between steady-state dilation and grain-scale dissipation rates. The laws also directly link the rate of dilation to the non-steady-state frictional strength.

At the macro-scale, we investigate continuum modeling techniques capable of simulating the distinct solid-like, liquid-like, and gas-like behaviors exhibited by granular materials in a single computational domain. We propose a Smoothed Particle Hydrodynamics (SPH) approach for granular materials with a viscoplastic constitutive law. The constitutive law uses a rate-dependent and dilation-dependent friction law. We provide a theoretical basis for a dilation-dependent friction law using similar analysis to that performed at the mesoscale. We provide several qualitative and quantitative validations of the technique and discuss ongoing work aiming to couple the granular flow with gas and fluid flows.

Electromagnetic decay of the 1.7- and 2.43-MeV levels in ^9Be

The 1.7- and 2.43-MeV levels in ⁹Be were populated with the reaction ¹¹B(d, α)⁹Be* by bombarding thin boron on carbon foils with 1.7-MeV deuterons. The alpha particles were analyzed in energy with a surface-barrier counter set at the unique kinematically determined angle and the recoiling ⁹Be nuclei at 90^o were analyzed in rigidity with a magnetic spectrometer, in energy by a surface-barrier counter at the spectrometer focus, and in velocity by the time delay between an alpha and a ⁹Be count. When a pulse from the spectrometer counter was in the appropriate delayed coincidence with a pulse from the alpha counter, the two pulses were recorded in a two-dimensional pulse height analyzer. Most of the ⁹Be* decay by particle breakup. Only those that gamma decay are detected by the spectrometer counter. Thus the experiment provides a direct measurement of Γ_rad/Γ. Analysis of 384 observed events gives Γ_rad/Γ = (1.16 ± 0.14) X 10^-4 for the 2.43-MeV level. Combining this ratio with the value of Γ_rad = 0.122 ± 0.015 eV found from inelastic electron scattering gives Γ = (1.05 ± 0.18) keV. For the 1.7-MeV level, an upper limit, Γ_rad/Γ ≤ 2.4 = 10^-5, was determined.

Particle fluid mechanics in shear flows, acoustic waves, and shock waves

Three different categories of flow problems of a fluid containing small particles are being considered here. They are: (i) a fluid containing small, non-reacting particles (Parts I and II); (ii) a fluid containing reacting particles (Parts III and IV); and (iii) a fluid containing particles of two distinct sizes with collisions between two groups of particles (Part V).

Part I

A numerical solution is obtained for a fluid containing small particles flowing over an infinite disc rotating at a constant angular velocity. It is a boundary layer type flow, and the boundary layer thickness for the mixture is estimated. For large Reynolds number, the solution suggests the boundary layer approximation of a fluid-particle mixture by assuming W = W_p. The error introduced is consistent with the Prandtl’s boundary layer approximation. Outside the boundary layer, the flow field has to satisfy the “inviscid equation” in which the viscous stress terms are absent while the drag force between the particle cloud and the fluid is still important. Increase of particle concentration reduces the boundary layer thickness and the amount of mixture being transported outwardly is reduced. A new parameter, β = 1/Ω τ_v, is introduced which is also proportional to μ. The secondary flow of the particle cloud depends very much on β. For small values of β, the particle cloud velocity attains its maximum value on the surface of the disc, and for infinitely large values of β, both the radial and axial particle velocity components vanish on the surface of the disc.

Part II

The “inviscid” equation for a gas-particle mixture is linearized to describe the flow over a wavy wall. Corresponding to the Prandtl-Glauert equation for pure gas, a fourth order partial differential equation in terms of the velocity potential ϕ is obtained for the mixture. The solution is obtained for the flow over a periodic wavy wall. For equilibrium flows where λ_v and λ_T approach zero and frozen flows in which λ_v and λ_T become infinitely large, the flow problem is basically similar to that obtained by Ackeret for a pure gas. For finite values of λ_v and λ_T, all quantities except v are not in phase with the wavy wall. Thus the drag coefficient C_D is present even in the subsonic case, and similarly, all quantities decay exponentially for supersonic flows. The phase shift and the attenuation factor increase for increasing particle concentration.

Part III

Using the boundary layer approximation, the initial development of the combustion zone between the laminar mixing of two parallel streams of oxidizing agent and small, solid, combustible particles suspended in an inert gas is investigated. For the special case when the two streams are moving at the same speed, a Green’s function exists for the differential equations describing first order gas temperature and oxidizer concentration. Solutions in terms of error functions and exponential integrals are obtained. Reactions occur within a relatively thin region of the order of λ_D. Thus, it seems advantageous in the general study of two-dimensional laminar flame problems to introduce a chemical boundary layer of thickness λ_D within which reactions take place. Outside this chemical boundary layer, the flow field corresponds to the ordinary fluid dynamics without chemical reaction.

Part IV

The shock wave structure in a condensing medium of small liquid droplets suspended in a homogeneous gas-vapor mixture consists of the conventional compressive wave followed by a relaxation region in which the particle cloud and gas mixture attain momentum and thermal equilibrium. Immediately following the compressive wave, the partial pressure corresponding to the vapor concentration in the gas mixture is higher than the vapor pressure of the liquid droplets and condensation sets in. Farther downstream of the shock, evaporation appears when the particle temperature is raised by the hot surrounding gas mixture. The thickness of the condensation region depends very much on the latent heat. For relatively high latent heat, the condensation zone is small compared with Ʌ_D.

For solid particles suspended initially in an inert gas, the relaxation zone immediately following the compression wave consists of a region where the particle temperature is first being raised to its melting point. When the particles are totally melted as the particle temperature is further increased, evaporation of the particles also plays a role.

The equilibrium condition downstream of the shock can be calculated and is independent of the model of the particle-gas mixture interaction.

Part V

For a gas containing particles of two distinct sizes and satisfying certain conditions, momentum transfer due to collisions between the two groups of particles can be taken into consideration using the classical elastic spherical ball model. Both in the relatively simple problem of normal shock wave and the perturbation solutions for the nozzle flow, the transfer of momentum due to collisions which decreases the velocity difference between the two groups of particles is clearly demonstrated. The difference in temperature as compared with the collisionless case is quite negligible.

CP and the three pion decay of the K°

The time distribution of the decays of an initially pure K° beam into π+π-π° has been analyzed to determine the complex parameter W (also known as Ƞ^+-° and (x + iy)). The K° beam was produced in a brass target by the interactions of a 2.85 GeV/c π- beam which was generated on an internal target in the Lawrence Radiation Laboratory (LRL) Bevatron. The counters and hodoscopes in the apparatus selected for events with a neutral (K°) produced in the brass target, two charged secondaries passing through a magnet spectrometer and a ɣ-ray shower in a shower hodoscope.

From the 275K apparatus triggers, 148 K → π+π-π° events were isolated. The presence of a ɣ-ray shower in the optical shower chambers and a two-prong vee in the optical spark chambers were devices used to isolate the events. The backgrounds were further reduced by reconstructing the momenta of the two charged secondaries and applying kinematic constraints.

The best fit to the final sample of 148 events distributed between .3 and 7.0 K_S lifetimes gives:

ReW = -.05 ±.17

ImW = +.39 +.35/-.37

This result is consistent with both CPT invariance (ReW = 0) and CP invariance (W = 0). Backgrounds are estimated to be less than 10% and systematic effects have also been estimated to be negligible.

An analysis of the present data on CP violation in this decay mode and other K° decay modes has estimated the phase of ɛ to be 45.3 ± 2.3 degrees. This result is consistent with the super weak theories of CP violation which predicts the phase of ɛ to be 43°. This estimate is in turn used to predict the phase of Ƞ°° to be 48.0 ± 7.9 degrees. This is a substantial improvement on presently available measurements. The largest error in this analysis comes from the present limits on W from the world average of recent experiments. The K → πuʋ mode produces the next largest error. Therefore further experimentation in these modes would be useful.