High resolution He I{alpha} photoelectron spectroscopy of formaldehyde and ketene and their deuterated compounds, are reported. The combination of a (H2CO) double-pass high-resolution electron-energy analyzer and effective rotational cooling of the sample by supersonic expansion enable the spectroscopy of these molecular cations. The vibrational autocorrelation functions are calculated from the high-resolution photoelectron spectra, shedding light on the ultrafast intramolecular dynamics of the molecular cations. This study reveals much more vibrational structural detail in the first electronic excited state of H2CO cations. The first electronic excited state of H2CO cations may have nonplanar equilibrium geometry. Strong isotope effects on vibronic (vibrational) coupling are observed in the second electronic excited state of H2CO. Vibrational autocorrelation functions are calculated for all four observed electronic states of H2CO. The correlation function of the first electronic excited state of H2CO shows a slow decay rate on the femtosecond time scale. The ultrafast decay of the H2CO cations in the third electronic excited state implies that dissociation and intramolecular processes are the main decay pathways. The present spectra of the ground states of ketene cations have more fine structure than before. The AIEs of the first and fifth excited states are determined unambiguously more accurately. The …

This report discusses: a brief introduction to storage rings; crystalline beams; laser cooling of ion beams; description of astrid-the experimental setup; first experiments with lithium 7 ion beam; experiments with erbium 166 ion beams; further experiments with lithium 7 ion beams; beam dynamics, laser cooling,and crystalline beams in astrid; possibilities for further study in astrid.

Modern nodal methods are currently available which can accurately and efficiently solve the static and transient neutron diffusion equations. Most of the methods, however, are limited to two energy groups for practical application. The objective of this research is the development of a static and transient, multidimensional nodal method which allows more than two energy groups and uses a non-linear iterative method for efficient solution of the nodal equations. For both the static and transient methods, finite-difference equations which are corrected by the use of discontinuity factors are derived. The discontinuity factors are computed from a polynomial nodal method using a non-linear iteration technique. The polynomial nodal method is based upon a quartic approximation and utilizes a quadratic transverse-leakage approximation. The solution of the time-dependent equations is performed by the use of a quasi-static method in which the node-averaged fluxes are factored into shape and amplitude functions. The application of the quasi-static polynomial method to several benchmark problems demonstrates that the accuracy is consistent with that of other nodal methods. The use of the quasi-static method is shown to substantially reduce the computation time over the traditional fully-implicit time-integration method. Problems involving thermal-hydraulic feedback are accurately, and efficiently, solved by …

The room temperature rate (TR) constants for fluorescence quenching fluorescence of H{sub 2}, HD, and D{sub 2} B {sup 1}{Sigma}{sub u}{sup +} by {sup 4}He were measured as a function of the initially excited rotational and vibrational level of the hydrogen molecule, and the RT rate constants for molecular angular momentum reorientation of H{sub 2}, HD and D{sub 2} (B {sup 1}{Sigma}{sub u}{sup +}. v{prime}=0, J{prime}=1, M{sub J}=0) in collisions with He, Ne, Ar and H{sub 2}(X {sup 1}{Sigma}{sub g}{sup +}) were also measured. Vibrational state dependence of the quenching cross sections fits a vibrationally adiabatic model of the quenching process. From the vibrational state dependence of the quenching cross section, the barrier height for the quenching reaction is found to be 250{plus_minus}40 cm{sup {minus}1}, and the difference in the H-H stretching frequencies between H{sub 2}(B) and the H{sub 2}-He complex at the barrier to reaction is 140{plus_minus}80 cm{sup {minus}1}. The effective cross sections for angular momentum reorientation in collisions of H{sub 2}, HD, D{sub 2} with He and Ne were found to be about 30 {Angstrom}{sup 2} and were nearly the same for each isotope and with He and Ne as collision partners. Cross sections forreorientation of HD and …

The effect of humidity, particle hygroscopicity and size on the mass loading capacity of glass fiber HEPA filters has been studied. At humidifies above the deliquescent point, the pressure drop across the HEPA filter increased non-linearly with the areal loading density (mass collected/filtration area) of NaCl aerosol, thus significantly reducing the mass loading capacity of the filter compared to dry hygroscopic or non-hygroscopic particle mass loadings. The specific cake resistance, K{sub 2}, has been computed for different test conditions and used as a measure of the mass loading capacity. K. was found to decrease with increasing humidity for the non-hygroscopic aluminum oxide particles and the hygroscopic NaCl particles (at humidities below the deliquescent point). It is postulated that an increase in humidity leads to the formation of a more open particulate cake which lowers the pressure drop for a given mass loading. A formula for predicting K{sub 2} for lognormally distributed aerosols (parameters obtained from impactor data) is derived. The resistance factor, R, calculated using this formula was compared to the theoretical R calculated using the Rudnick-Happel expression. For the non-hygroscopic aluminum oxide the agreement was good but for the hygroscopic sodium chloride, due to large variation in the cake …

High purity KMF{sub 6} and K{sub 2}MF{sub 6} salts (M = Mo,Re, Ru, Os, Ir, Pt) are obtained from reduction hexafluorides. A rhombohedral unit cell is observed for KReF{sub 6}. Fluoride ion capture by Lewis acids from the hexafluorometallate (IV) salts affords high purity tetrafluorides for M = Mo, Re, Ru, Os, and Pd. The structure of RuF{sub 4} is determined from X-ray synchrotron and neutron powder data. Unit cells based on theorthorhombic PdF{sub 4} type cell are derived from X-ray powder data for ReF{sub 4} and OsF{sub 4}. Fluoride ion capture from KAgF{sub 4} provides the thermally unstable trifluoride as a bright, red, diamagnetic solid. The structure solution of AgF{sub 3} and redetermination of the AuF{sub 3} structure from X-ray synchrotron and neutron powder data demonstrate that the two are isostnictural. Thermal decomposition product of AgF{sub 3} is the mixed valence compound Ag{sup II}Ag{sub 2}{sup III}F{sub 8}. Several new salts containing the (Ag - F){sub n}{sup n+} chain cation are prepared. The first linear (Ag - F){sub n}{sup n+} chain is observed in AgF{sup +}BF{sub 4 {sup {minus}}} which crystallizes in a tetragonal unit. AgFAuF{sub 4} has a triclinic unit cell and is isostructural with CuFAuF{sub 4}. AgFAuF{sub 6} …

The EQCM was used to study the deposition and composition of electrodeposited pure PbO{sub 2} and Bi-doped PbO{sub 2} active toward anodic oxygen-transfer reactions. Within the doped films, Bi is incorporated as Bi{sup +5} in the form of BiO{sub 2}A, where A is ClO{sub 4}{sup {minus}} or NO{sub 3}{sup {minus}}. For deposition of these 2 materials, changes in hydration between the Au oxide and the depositing film resulted in higher mass-to-charge ratios. XRD and XPS were used to study the films; the rutile structure of PbO{sub 2} is retained even with the Bi doping. The EQCM was also used to study the formation and dissolution of Au oxide and preoxide structures formed on the Au substrate electrodes in acidic media. The preoxide structures were AuOH and increased the surface mass. For the formation of stable Au films on quartz wafers, Ti interlayers between Au and quartz was found to be very effective.

The main goal of the work presented in this thesis is produce highly spin-polarized xenon to create much greater signal intensities (up to 54,000 times greater) so as to allow studies to be made on systems with low surface area and long spin-lattice relaxation times. The spin-exchange optical pumping technique used to create high nuclear spin polarization is described in detail in chapter two. This technique is initially applied to some multiple-pulse optically detected NMR experiments in low magnetic field (50G) that allow the study of quadrupoler interactions with a surface of only a few square centimeters. In chapter three the apparatus used to allow high field {sup 129}Xe NMR studies to be performed with extremely high sensitivity is described and applied to experiments on diamagnetic susceptibility effects in thin ({approximately}2000 layers) films of frozen xenon. Preliminary surface investigations of laser polarized {sup 129}Xe adsorbed an a variety of materials (salts, molecular crystals, amorphous carbon, graphite) are then discussed. A full detailed study of the surface of a particular polymer, poly(acrylic acid), is presented in chapter four which shows the kind of detailed information that can be obtained from this technique. Along with preliminary results for several similar polymers, a …

As the field of computational fluid dynamics (CFD) continues to mature, algorithms are required to exploit the most recent advances in approximation theory, numerical mathematics, computing architectures, and hardware. Meeting this requirement is particularly challenging in incompressible fluid mechanics, where primitive-variable CFD formulations that are robust, while also accurate and efficient in three dimensions, remain an elusive goal. This dissertation asserts that one key to accomplishing this goal is recognition of the dual role assumed by the pressure, i.e., a mechanism for instantaneously enforcing conservation of mass and a force in the mechanical balance law for conservation of momentum. Proving this assertion has motivated the development of a new, primitive-variable, incompressible, CFD algorithm called the Continuity Constraint Method (CCM). The theoretical basis for the CCM consists of a finite-element spatial semi-discretization of a Galerkin weak statement, equal-order interpolation for all state-variables, a 0-implicit time-integration scheme, and a quasi-Newton iterative procedure extended by a Taylor Weak Statement (TWS) formulation for dispersion error control. Original contributions to algorithmic theory include: (a) formulation of the unsteady evolution of the divergence error, (b) investigation of the role of non-smoothness in the discretized continuity-constraint function, (c) development of a uniformly H{sup 1} Galerkin weak statement …

In this dissertation the possibility that chaos and simple determinism are governing the dynamics of reversed field pinch (RFP) plasmas is investigated. To properly assess this possibility, data from both numerical simulations and experiment are analyzed. A large repertoire of nonlinear analysis techniques is used to identify low dimensional chaos in the data. These tools include phase portraits and Poincare sections, correlation dimension, the spectrum of Lyapunov exponents and short term predictability. In addition, nonlinear noise reduction techniques are applied to the experimental data in an attempt to extract any underlying deterministic dynamics. Two model systems are used to simulate the plasma dynamics. These are the DEBS code, which models global RFP dynamics, and the dissipative trapped electron mode (DTEM) model, which models drift wave turbulence. Data from both simulations show strong indications of low dimensional chaos and simple determinism. Experimental date were obtained from the Madison Symmetric Torus RFP and consist of a wide array of both global and local diagnostic signals. None of the signals shows any indication of low dimensional chaos or low simple determinism. Moreover, most of the analysis tools indicate the experimental system is very high dimensional with properties similar to noise. Nonlinear noise reduction …

The development of new ion sources is important in the area of surface analysis to make it easier to perform more sensitive and accurate analyses. In surface analysis a primary ion beam composed of a single species can help when predicting and interpreting the results. Therefore, much interest and effort has been focused on producing pure ion emitters. An instrument has been designed and constructed to view the current densities of the ions being emitted from pure ion emitters. The instrument electrostatically accelerates and focuses the ion beam onto a microchannel plate detector equipped with a phosphor screen for viewing the images. These images are used to identify areas of enhanced ion emission. Once these areas are identified, the investigator can use other instruments to analyze them, and hopefully develop a better understanding of the chemistry and physics involved in the ion emission process. A computer based control system has been integrated into the system to simplify the operation of the instrument and provide safety features to protect the hardware from damage. A closed-circuit video camera system is used to allow the images to be remotely viewed during imaging procedures. Experiments show that the instrument has a lower detection limit …

Complex fragment emission has been studied in the 60 MeV/A {sup 197}Au + {sup 12}C, {sup 27}Al, {sup 51}V, {sup nat}Cu, and {sup 197}Au reactions. Velocity spectra, angular distributions and cross sections have been constructed for each target from the inclusive data. Coincidence data including 2-, 3-, 4-, and 5-fold events have also been examined. Furthermore neutron multiplicity distributions have been obtained for the above reactions by utilizing a novel neutron calorimetric approach.

Because of the ubiquitous nature of turbulence and the vast array of different systems which have turbulent solutions, the study of turbulence is an area of active research. Much present day understanding of turbulence is rooted in the well established properties of homogeneous Navier-Stokes turbulence, which, due to its relative simplicity, allows for approximate analytic solutions. This work examines a group of turbulent systems with marked differences from Navier-Stokes turbulence, and attempts to quantify some of their properties. This group of systems represents a variety of drift wave fluctuations believed to be of fundamental importance in laboratory fusion devices. From extensive simulation of simple local fluid models of long wavelength drift wave turbulence in tokamaks, a reasonably complete picture of the basic properties of spectral transfer and saturation has emerged. These studies indicate that many conventional notions concerning directions of cascades, locality and isotropy of transfer, frequencies of fluctuations, and stationarity of saturation are not valid for moderate to long wavelengths. In particular, spectral energy transfer at long wavelengths is dominated by the E {times} B nonlinearity, which carries energy to short scale in a manner that is highly nonlocal and anisotropic. In marked contrast to the canonical self-similar cascade …

In this dissertation, we present some of the recent advances made in solving two-stage stochastic linear programming problems of large size and complexity. Decomposition and sampling are two fundamental components of techniques to solve stochastic optimization problems. We describe improvements to the current techniques in both these areas. We studied different ways of using importance sampling techniques in the context of Stochastic programming, by varying the choice of approximation functions used in this method. We have concluded that approximating the recourse function by a computationally inexpensive piecewise-linear function is highly efficient. This reduced the problem from finding the mean of a computationally expensive functions to finding that of a computationally inexpensive function. Then we implemented various variance reduction techniques to estimate the mean of a piecewise-linear function. This method achieved similar variance reductions in orders of magnitude less time than, when we directly applied variance-reduction techniques directly on the given problem. In solving a stochastic linear program, the expected value problem is usually solved before a stochastic solution and also to speed-up the algorithm by making use of the information obtained from the solution of the expected value problem. We have devised a new decomposition scheme to improve the convergence …

Subcritical fatigue crack growth, from cyclic tensile loading, was demonstrated in warm pressed Polycrystalline lithium hydride. Experiments were performed with cyclic tension-tension crack opening (mode I) loads applied to a pre-cracked compact type specimen in an argon environment at a temperature of 21C (70F). The fatigue crack growth was found to occur between 7.56 {times} 10{sup {minus}ll} M/cycle (2.98 {times} l0{sup {minus}9} in/cycle) and 2.35 {times} l0{sup {minus}8} m/cycle (9.24{times}10{sup {minus}7} in/cycle) for a range of stress intensity factors between 1.04 MPa{center_dot}{radical}m (0.95 ksi{center_dot}{radical}in) and 1.49 MPa{center_dot}{radical}m (1.36 ksi{center_dot}{radical}in). The rate of fatigue crack growth from cyclic tensile loading was found to be in excess of crack growth from sustained loading at an equivalent stress intensity factor. Furthermore, a fatigue threshold was not evident from the acquired data.

The melting and solidification was studied using in-situ high temperature XRD from melting point to 900{degree}C in 0.2, 0.1, 0.02 atm O{sub 2} and pure N{sub 2}. The incongruent melting point of Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8} was lowered by decreasing the partial O{sub 2} pressure from 870C (in .2 atm O{sub 2}) to 830C (in pure N{sub 2} atmosphere). As temperature was increased the incongruent melting of Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8} followed a phase sequence in which (Ca, Sr)CuO{sub 2} {r_arrow} (Ca, Sr)CuO{sub 2} {r_arrow} (Ca,Sr)O occur in presence of Bi-rich liquid. At 900C, the only crystalline phase present in the melt was (Ca,Sr)O. This phase sequence remained the same for all four different partial O{sub 2} pressures. During the solidification of Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8}, from 10C below the melting point to 760C, the major phases that form depend on the partial O{sub 2} pressure. As partial O{sub 2} pressures was lowered from 0.2 to 0 atm, the major second phase formation out of the melt follows the sequence of (Ca, Sr)CuO{sub 2} {r_arrow} (Ca, Sr)CuO{sub 2} {r_arrow} (Ca,Sr)O respectively. At 0.1 Atm partial O{sub 2} pressure and below, Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8} solidified out …

A wide range of research has been published on the problem of estimating the parameters of electromagnetic and acoustical sources from measurements of signals measured at an array of sensors. In the quasi-static electromagnetic cases examined here, the signal variation from a point source is relatively slow with respect to the signal propagation and the spacing of the array of sensors. As such, the location of the point sources can only be determined from the spatial diversity of the received signal across the array. The inverse source localization problem is complicated by unknown model order and strong local minima. The nonlinear optimization problem is posed for solving for the parameters of the quasi-static source model. The transient nature of the sources can be exploited to allow subspace approaches to separate out the signal portion of the spatial correlation matrix. Decomposition techniques are examined for improved processing, and an adaptation of MUtiple SIgnal Characterization (MUSIC) is presented for solving the source localization problem. Recent results on calculating the Cramer-Rao error lower bounds are extended to the multidimensional problem here. This thesis focuses on the problem of source localization in magnetoencephalography (MEG), with a secondary application to thunderstorm source localization. Comparisons are …

Ion-induced conductivity has been used to investigate the detector characteristics of diamond detectors. Both integrated-charge, and time-resolved current measurements were performed to examine the mean carrier transport properties of diamond and the dynamics of charge collection under highly-localized and high-density excitation conditions. The integrated-charge measurements were conducted with a standard pulse-counting system with {sup 241}Am radioactivity as the excitation source for the detectors. The time-resolved current measurements were performed using a 70 GHz random sampling oscilloscope with the detectors incorporated into high-speed microstrip transmission lines and the excitation source for these measurements was an ion beam of either 5-MeV He{sup +} or 10-MeV Si{sup 3+}. The detectors used in both experiments can be described as metal-semiconductor-metal (MSM) devices where a volume of the detector material is sandwiched between two metal plates. A charge collection model was developed to interpret the integrated-charge measurements which enabled estimation of the energy required to produce an electron-hole pair ({epsilon}{sub di}) and the mean carrier transport properties in diamond, such as carrier mobility and lifetime, and the behavior of the electrical contacts to diamond.

The Mirrortron is a concept in which heavy ions are accelerated by a large local transient space potential that is produced in a hot electron plasma. The purpose of this experiment is to begin a proof of principle experiment to investigate the feasibility of producing this space potential and its associated electric field. If a large magnetic field is suddenly generated in a hot electron plasma with a loss-cone distribution, then potentials on the order of the electron temperature are expected. This potential lasts a few tens of nanoseconds. The investigation begins with a theoretical analysis of this phenomenon giving the space potential as a function of the applied magnetic field. The theory is further extended to cases of relativistic electron distributions. This is then followed by design work on a mirror confinement system for hot electrons. In this experiment a 50--100 keV electron temperature plasma is created with electron cyclotron resonance heating using two frequencies of relatively low microwave power. The microwaves are coupled to resonant frequencies of the vacuum chamber. The volume averaged plasma density is measured to be in the 10{sup 9} cm{sup {minus}3} range. A strap coil and a flat Blumlein transmission line pulse generator were …

Semiconductor nanocrystals, small biomolecules, and {sup 13}C enriched solids were studied through the relaxation in NMR spectra. Surface structure of semiconductor nanocrystals (CdS) was deduced from high resolution {sup 1}H and {sup 13}C liquid state spectra of thiophenol ligands on the nanocrystal surfaces. The surface coverage by thiophenol was found to be low, being 5.6 and 26% for nanocrystal radii of 11.8 and 19.2 {angstrom}. Internal motion is estimated to be slow with a correlation time > 10{sup {minus}8} s{sup {minus}1}. The surface thiophenol ligands react to form a dithiophenol when the nanocrystals were subjected to O{sub 2} and ultraviolet. A method for measuring {sup 14}N-{sup 1}H J-couplings is demonstrated on pyridine and the peptide oxytocin; selective 2D T{sub 1} and T{sub 2} experiments are presented for measuring relaxation times in crowded spectra with overlapping peaks in 1D, but relaxation effects interfere. Possibility of carbon-carbon cross relaxation in {sup 13}C enriched solids is demonstrated by experiments on zinc acetate and L-alanine.

Quantum manifestation of classical chaos has been one of the extensively studied subjects for more than a decade. Yet clear understanding of its nature still remains to be an open question partly due to the lack of a canonical definition of quantum chaos. The classical definition seems to be unsuitable in quantum mechanics partly because of the Heisenberg quantum uncertainty. In this regard, quantum chaos is somewhat misleading and needs to be clarified at the very fundamental level of physics. Since it is well known that quantum mechanics is more fundamental than classical mechanics, the quantum description of classically chaotic nature should be attainable in the limit of large quantum numbers. The focus of my research, therefore, lies on the correspondence principle for classically chaotic systems. The chaotic damped driven pendulum is mainly studied numerically using the split operator method that solves the time-dependent Schroedinger equation. For classically dissipative chaotic systems in which (multi)fractal strange attractors often emerge, several quantum dissipative mechanisms are also considered. For instance, Hoover`s and Kubo-Fox-Keizer`s approaches are studied with some computational analyses. But the notion of complex energy with non-Hermiticity is extensively applied. Moreover, the Wigner and Husimi distribution functions are examined with an equivalent …

This technique worked well for determining the thickness and densities for composite components having the higher linear attenuation coefficient; it accurately determined thickness of epoxy-resin and Al metal, and the denisty of bone, to {le} 4% in the graphite-epoxy, bone-plexiglas, and Al-Al corrosion composites. Accuracy is dictated by the magnitude and uncertainty of the linear attenuation coefficient. Use of Ge detector and multichannel analyzer are limited by inspection time (1 day for point measurement) and access limitation. Immediate development of a rapid in-service inspection tool is limited by the amplifier and MCA systems. The MCA should be replaced with a single-channel analyzer, and an electronic device should be built for monitoring the incoming signal for Pile-Up-Rejection.

A desolvation scheme for introducing aqueous and organic samples into an argon inductively coupled plasma is described; the aerosol generated by nebulizer is heated (+140 C) and cooled ({minus}80 C) repeatedly, and the dried aerosol is then injected into the mass spectrometer. Polyatomic ions are greatly suppressed. This scheme was validated with analysis of seawater and urine reference samples. Finally, the removal of organic solvents by cryogenic desolvation was studied.

Bolometry was used obtain accurate submillimeter residual loss data for epitaxial films of YBa{sub 2}Cu{sub 3}O{sub 7} (YBCO), Tl{sub 2}Ca{sub 2}Ba{sub 2}Cu{sub 3}O{sub 10}, Tl{sub 2}CaBa{sub 2}Cu{sub 2}O{sub 8} (TCBCO), and Ba{sub 0.6}K{sub 0.4}BiO{sub 3} (BKBO). We were able to fit the absorptivity measured for Nb films to an Eliashberg strong coupling calculation; excellent agreement resulted between parameters from best fits and measured Residual Resistivity Ratio. Microwave surface resistance measurements made on the same YBCO and TCBCO films are in excellent agreement with submillimeter measurements. Absorptivities for all YBCO films studied are qualitatively similar, increasing smoothly with frequency, with no gap-like features below the well known absorption edge at 450 cm{sup {minus}1}. Losses in YBCO films were fit to a weakly coupled grain model for the a-b plane conductivity. Strong phonon structure was observed in TCBCO films between 60 and 700 cm{sup {minus}1} (2 THz and 23 THz); these losses could not be fitted to the simple weakly coupled grain model, in contrast to the case for other high-{Tc} superconductors where phonon structure observed in ceramics are is absent in epitaxial oriented films and crystals because of electronic screening due to high conductivity of a-b planes. Absorptivity data for the …