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Ion exchange column elution methods for the separation of americium and curium using tartrate and lactate solutions have been developed which are superior to citrate elutions. Tartrate elutions are suitable for slow separations and lactate elutions are satisfactory for general use where rapid separations are required. Fission and spallation products were isolated from Pu{sup 239} targets which had been bombarded with alpha particles of 21 to 37 Mev energy. Fission yield curves as well as fission and spallation excitation functions are presented and discussed in terms of odd-even and Z{sup 2}/A effects. The high cross sections observed for the (a, 2n) and (a, p2n) reactions were surprising results from this investigation. In the course of the Pu{sup 239} bombardments, studies of the decay schemes of Am{sup 240}, Cm{sup 240}, and Cm{sup 241} were undertaken. Decay energy and half-1ife information on all of the transmercury nuclides has been collected and systematized. Trends on the energy surface for alpha energies, beta energies, nucleon binding energies, and Bohr-Wheeler parameters are presented. These energy systematics have led to a complete tabulation of the masses of the isotopes of the elements above mercury. Predictions of nuclear properties are included for some isotopes of elements 99 …

The development of rapid, selective, and sensitive methods for the determination of osmium in liquid samples is reported. The specific application of primary interest was the estimation of microgram or milligram quantities of osmium in homogeneous reactcr fuel solutions which contain uranyl sulfate as the major component and corrosion products of stainless steel as minor components. (W.L.H.)

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The effects of certain pulse-shaping networks on the signal-to-noise ratio of a nuclear pulse amplifier were considered. The shaping networks discussed are: equal RC-integrating and RC-differentiating time constant, single- delay-line clipper and RC integrator, and doubledelay-line clipper and RC integrator. The effects of these networks on the signal, when high count rates and overload pulses are present, were also considered. Equations and curves were developed for the energy resolution (signal-tonoise ratio) and resolving time (related to the ability to operate at high counting rates) of the networks. Experimental results are shown for the energy resolution of the types of pulse- shaping networks considered. (auth)

Experimental studies of the relative atomic mu --meson capture probabilities in the constituents of chemical compounds are described. Fermi and Teller had predicted that the atomic-capture probability is proportional to the nuclear charge of the atomic species weighted by its atomic concentration. This is sometimes referred to as the Fermi-Teller Z law.'' Previous experiments indicated no clear systematics to this capture process, and there are conflicts between the results of several measurements made with the same or similar compounds. In these experiments the capturing atom was identified by detection of either mesic x rays or decay electrons from mu /sup -/ mesons bound in the mesic K shell in the atomic species, In these experiments oxides and sulfides of some medium- and high-Z elements as well as two metallic solutions were used, and a nuclear capture product (neutron) rather than the decay electrons was detected. Results show that among the substances examIned, namely CuO, Sb/sub 2/O/sub 3, PbO, CuS, Sb/sub 2/S/sub 3/, PbS AgLi, and CuAu, the Z law'' behavior is not indicated either in insulators or in metals, although in all cases there is a preference for capturing in the atom of higher Z. If the atomic-capture probability is …

The nuclear radiations of nuclides: U{sup 233}, Pu{sup 239}, Bk{sup 243}, Bk{sup 244}, Bk{sup 245}, Bk{sup 246}, Bk{sup 249}, Cf{sup 249}, and Fm{sup 255} were investigated with high-resolution spectrometers. The {alpha}-particle spectra of all nuclides except Bk{sup 249} were measured with 6 mm diameter surface-barrier detectors. Bk{sup 249} {alpha}-particles were analyzed with a double-focusing magnetic spectrograph. The {gamma}-singles were examined with the recently developed Ge(Li) and Si(Li) detectors coupled with very-low noise 'internal FET' preamplifiers. Weak alpha groups were observed in coincidence with {gamma}-rays, detected with a NaI(Tl) scintillation spectrometer. To improve the over-all coincidence efficiency a new coincidence apparatus was designed and built. This instrument consisted of a cooled 4.5 cm diameter semiconductor detector for {alpha}-particle detection and a 3 cm diameter by 2.7 cm long Ge(Li) detector for {gamma}-ray analysis. The Ge(Li) detector could also be replaced with a NaI(Tl) detector. Cf{sup 249} conversion electrons were measured with a cooled Si(Li) detector coupled with an internal FET preamplifier. On the basis of the present work and previous information, energy-level diagrams of the daughter nuclei have been constructed. The levels have been grouped into rotational bands built on Nilsson single-particle states. Because of identification of several rotational members of …

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The formation constants for the reactions PuO{sub 2}{sup +} + H{sub 2}O = PuO{sub 2}(OH) + H{sup +} and PuO{sub 2}{sup +} + CO{sub 3}{sup 2} = PuO{sub 2}(CO{sub 3}){sup {minus}} were determined in aqueous sodium perchlorate solutions by laser-induced photoacoustic spectroscopy. The molar absorptivity of the PuO{sub 2}{sup +} band at 569 nm decreased with increasing hydroxide concentration. Similarly, spectral changes occurred between 540 and 580 nm as the carbonate concentration was increased. The absorption data were analyzed by the non-linear least-squares program SQUAD to yield complexation constants. Using the specific ion interaction theory, both complexation constants were extrapolated to zero ionic strength. These thermodynamic complexation constants were combined with the oxidation-reduction potentials of Pu to obtain Eh versus pH diagrams. 120 refs., 35 figs., 12 tabs.

The series of projects described in this dissertation was stimulated by the discovery of high temperature superconductivity. Our goal was to develop useful applications which would be competitive with the current state of technology. The high-{Tc} microbolometer was developed into the most sensitive direct detector of millimeter waves, when operated at liquid nitrogen temperatures. The thermal boundary resistance of thin YBa{sub 2}Cu{sub 3}0{sub 7-{delta}} films was subsequently measured and provided direct evidence for the bolometric response of high-{Tc} films to fast (ns) laser pulses. The low-{Tc} microbolometer was developed and used to make the first direct measurements of the frequency dependent optical efficiency of planar lithographed antennas. The hot-electron microbolometer was invented less than a year prior to the writing of this dissertation. Our analysis, presented here, indicates that it should be possible to attain up to two orders of magnitude higher sensitivity than that of the best available direct detectors when operated at the same temperature. The temperature readout scheme for this device could also be used to measure the intrinsic interaction between electrons and phonons in a metal with a sensitivity that is five orders of magnitude better than in previous measurements. Preliminary measurements of quasiparticle trapping effects …

The morphology of craters resulting from high irradiance laser ablation of silicon was measured using a white light interferometry microscope. The craters show a dramatic increase in their depth and volume at a certain irradiance, indicating a change in the primary mechanism for mass removal. Laser shadowgraph imaging was used to characterize and differentiate the mass ejection processes for laser irradiances above and below the threshold value. Time-resolved images show distinct features of the mass ejected at irradiances above the threshold value including the presence of micron-sized particulates; this begins at approximately 300 {approx} 400 ns after the start of laser heating. The analysis of the phenomena was carried out by using two models: a thermal evaporation model and a phase explosion model. Estimation of the crater depth due to the thermally evaporated mass led to a large underestimation of the crater depth for irradiances above the threshold. Above the threshold irradiance, the possibility of phase explosion was analyzed. Two important results are the thickness of the superheated liquid layer that is close to the critical temperature and the time for vapor bubbles that are generated in the superheated liquid to achieve a critical size. After reaching the critical size, …

A laboratory investigation was undertaken to determine the effect of microbe generated gas bubbles in controlled, saturated sediment columns utilizing a novel technique involving acoustic wave propagation. Specifically, the effect of denitrifying bacteria on saturated flow conditions was evaluated in light of the stimulated production of N{sub 2} gas and the resulting plugging of the pore throats. The propagation of high frequency acoustic waves through the sediment columns was used to locate those regions in the column where gas accumulation occurred. Over a period of six weeks, regions of gas accumulation resulted in the attenuation of acoustic wave energies with the decreases in amplitude typically greater than one order of magnitude.

This document is the third sub-report of the EUV AIM design study being conducted at LLNL on behalf of International Sematech (ISMT). The purpose of this study as identified in section 1.2 of the statement of work is to research the basic user requirements of an actinic defect characterization tool, potential design configurations and top-level specifications. The objectives of this design study specifically identified in section 1.3 of the statement of work were to: (1) Determine the user requirements of an actinic defect characterization tool; (2) Determine if an EUV AIM tool is an appropriate platform for actinic defect characterization; (3) Determine possible design configurations and top-level performance specifications; (4) Identify potential technical issues and risks of different technical approaches; (5) Provide estimates of cost relating to different technical approaches; and (6) Provide simulated performance for key subsystems and the entire system. The sub-sections of the study to be addressed were accordingly defined in the statement of work as being: (1) Formulation of top-level specifications; (2) Identification of system configurations suitable for meeting the top-level specifications; (3) Preliminary design of imaging systems; (4) Preliminary design of illumination systems; (5) Prediction and comparison of performance through aerial image calculation; (6) Identification …

Rapid developments in time-resolved optical spectroscopy have led to renewed interest in the nonequilibrium state of superconductors and other highly correlated electron materials. In these experiments, the nonequilibrium state is prepared by the absorption of short (less than 100 fs) laser pulses, typically in the near-infrared, that perturb the density and energy distribution of quasiparticles. The evolution of the nonequilibrium state is probed by time resolving the changes in the optical response functions of the medium that take place after photoexcitation. Ultimately, the goal of such experiments is to understand not only the nonequilibrium state, but to shed light on the still poorly understood equilibrium properties of these materials. We report nonequilibrium experiments that have revealed aspects of the cup rates that have been inaccessible by other techniques. Namely, the diffusion and recombination coefficients of quasiparticles have been measured in both YBa{sub 2}Cu{sub 3}O{sub 6.5} and Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8+x} using time-resolved optical spectroscopy. Dependence of these measurements on doping, temperature and laser intensity is also obtained. To study the recombination of quasiparticles, we measure the change in reflectivity {Delta}R which is directly proportional to the nonequilibrium quasiparticle density created by the laser. From the intensity dependence, we estimate …

Better devices are needed for the detection of aerosolized biological warfare agents. Advances in the ongoing development of one such device, the BioAerosol Mass Spectrometry (BAMS) system, are described here in detail. The system samples individual, micrometer-sized particles directly from the air and analyzes them in real-time without sample preparation or use of reagents. At the core of the BAMS system is a dual-polarity, single-particle mass spectrometer with a laser based desorption and ionization (DI) system. The mass spectra produced by early proof-of-concept instruments were highly variable and contained limited information to differentiate certain types of similar biological particles. The investigation of this variability and subsequent changes to the DI laser system are described. The modifications have reduced the observed variability and thereby increased the usable information content in the spectra. These improvements would have little value without software to analyze and identify the mass spectra. Important improvements have been made to the algorithms that initially processed and analyzed the data. Single particles can be identified with an impressive level of accuracy, but to obtain significant reductions in the overall false alarm rate of the BAMS instrument, alarm decisions must be made dynamically on the basis of multiple analyzed particles. …

The goal of this dissertation is twofold. The first part concerns the development of a numerical method for solving Maxwell's equations on unstructured hexahedral grids that employs both high order spatial and high order temporal discretizations. The second part involves the use of this method as a computational tool to perform high fidelity simulations of various electromagnetic devices such as optical transmission lines and photonic crystal structures to yield a level of accuracy that has previously been computationally cost prohibitive. This work is based on the initial research of Daniel White who developed a provably stable, charge and energy conserving method for solving Maxwell's equations in the time domain that is second order accurate in both space and time. The research presented here has involved the generalization of this procedure to higher order methods. High order methods are capable of yielding far more accurate numerical results for certain problems when compared to corresponding h-refined first order methods , and often times at a significant reduction in total computational cost. The first half of this dissertation presents the method as well as the necessary mathematics required for its derivation. The second half addresses the implementation of the method in a parallel …

YBa{sub 2}Cu{sub 3}O{sub 7-{delta}} (YBCO) coated conductors are promising materials for large-scale superconductivity applications. One version of a YBCO coated conductor is based on ion beam assisted deposition (IBAD) of magnesium oxide (MgO) onto polycrystalline metal substrates. SrTiO{sub 3} (STO) is often deposited by physical vapor deposition (PVD) methods as a buffer layer between the YBCO and IBAD MgO due to its chemical stability and lattice mismatch of only {approx}1.5% with YBCO. In this work, some aspects of the stability of STO with respect to copper (Cu) and chemical solution deposition of STO on IBAD MgO templates were examined. Solubility limits of Cu in STO were established by processing Cu-doped STO powders by conventional bulk preparation techniques. The maximum solubility of Cu in STO was {approx}1% as determined by transmission electron microscopy (TEM) and Rietveld refinements of x-ray diffraction (XRD) data. XRD analysis, performed in collaboration with NIST, on powder compositions on the STO/SrCuO{sub 2} tie line did not identify any ternary phases. SrCu{sub 0.10}Ti{sub 0.90}O{sub y} buffer layers were prepared by pulsed laser deposition (PLD) and CSD on IBAD MgO flexible metallic textured tapes. TEM analysis of a {approx}100 nm thick SrCu{sub 0.10}Ti{sub 0.90}O{sub y} buffer layer deposited by …

Ulrich in the forward to the Zenger and Folkman (2002) book, ''The Extraordinary Leader'', wrote about the importance of character in leadership stating, ''Everything about great leaders radiates from character. Character improves the probability of exhibiting strong interpersonal skill. Some of this perceived character is innate . . . but more is driven by the leader's self-awareness and interactions with others'' (p. ix). The purpose of this study was to explore the relationship between leadership effectiveness and character using leader-managers of knowledge workers as the subject sample. Findings indicated that character, particularly those factors associated with honesty, setting the example, and valuing and strengthening others, were what set the most effective leader-managers apart from their peers. Technical competence and self-efficacy were found to be common characteristics of the study sample as was a drive for results. Who a leader-manager is, his/her substance, was found in this study to differentiate the ''best'' leader-managers at the Lawrence Livermore National Laboratory. By their character, leader-managers establish the environment in which knowledge workers contribute and grow. As found by Pfeiffer (2000), Leaders of companies that experience smaller gaps between what they know and what they do (to turn knowledge into action), understand that their …

Over the past ten years, methods have been developed to construct discrete nanostructures using nanocrystals and biomolecules. While these frequently consist of gold nanocrystals and DNA, semiconductor nanocrystals as well as antibodies and enzymes have also been used. One example of discrete nanostructures is dimers of gold nanocrystals linked together with complementary DNA. This type of nanostructure is also known as a nanocrystal molecule. Discrete nanostructures of this kind have a number of potential applications, from highly parallel self-assembly of electronics components and rapid read-out of DNA computations to biological imaging and a variety of bioassays. My research focused in three main areas. The first area, the refinement of electrophoresis as a purification and characterization method, included application of agarose gel electrophoresis to the purification of discrete gold nanocrystal/DNA conjugates and nanocrystal molecules, as well as development of a more detailed understanding of the hydrodynamic behavior of these materials in gels. The second area, the development of methods for quantitative analysis of transmission electron microscope data, used computer programs written to find pair correlations as well as higher order correlations. With these programs, it is possible to reliably locate and measure nanocrystal molecules in TEM images. The final area of …

Surfactant-coated cobalt nanocrystals can be prepared with areasonable degree of control over particle size and shape using athermolytic route. The small crystallite size, enhanced reactivity andtunable interparticle interactions enable use of this material asstarting material for demonstration of achievement of novel structuresusing extremely simple solution-based approaches. In particular,formation of hollow cobalt sulfide nanocrystals upon chemicalmodification and emergence of long-range orientational order upondrying-mediated assembly of cobalt nanocrystals is reportedhere.Colloidal preparation of Co nanocrystals has been well-studied.Here, we emphasize general principles and crystallographic/morphologicalcharacterization of disk-shaped hcp-Co nanocrystals. Use of surfactantmolecules enables achievement of multiple morphologies in one syntheticsystem.Formation of hollow structures upon in-solution sulfidation of Conanocrystals is presented and discussed. A Kirkendall-type effect,involving dominant outward mass transport during formation of the ionicshell material explains the results naturally. It is expected that thisphenomenon will generalize extensively to formation of hollow structuresof an enormous variety of compositions. Detailed study of particlemorphology as a function of reaction conditions suggest phenomena likelyto be generally relevant to use of this approach. A short report ofcrystallographic co-alignment into vortex-like structures is alsoprovided. Our current best picture of this process involves an interplayof packing and magnetic interactions between facetedparticles.

Guest-host interaction has long been a subject of interest in many disciplines. Emphasis is often on how a small amount of guest substance could significantly affect the properties of a host material. This thesis describe our work in studying a guest-host effect where dye-doping of liquid crystalline materials greatly enhances the optical Kerr nonlinearity of the material. The dye molecules, upon excitation and via intermolecular interaction, provides an extra torque to reorient the host molecules, leading to the enhanced optical Kerr nonlinearity. We carried out a comprehensive study on the dynamics of the photoexcited dye-doped liquid crystalline medium. Using various experimental techniques, we separately characterized the dynamical responses of the relevant molecular species present in the medium following photo-excitation, and thus were able to follow the transient process in which photo-excitation of the dye molecules exert through guest-host interaction a net torque on the host LC material, leading to the observed enhanced molecular reorientation. We also observed for the first time the enhanced reorientation in a pure liquid crystal system, where the guest population is created through photoexcitation of the host molecules themselves. Experimental results agree quantitatively with the time-dependent theory based on a mean-field model of the guest-host interaction.

In order to better understand the fundamental components that govern catalytic activity, two-dimensional model platinum nanocatalyst arrays have been designed and fabricated. These catalysts arrays are meant to model the interplay of the metal and support important to industrial heterogeneous catalytic reactions. Photolithography and sub-lithographic techniques such as electron beam lithography, size reduction lithography and nanoimprint lithography have been employed to create these platinum nanoarrays. Both in-situ and ex-situ surface science techniques and catalytic reaction measurements were used to correlate the structural parameters of the system to catalytic activity.

We are becoming dependent on energy more today than we were a century ago, and with increasing world population and booming economies, sooner or later our energy sources will be exhausted. Moreover, our economy and welfare strongly depends on foreign oil and in the shadow of political uncertainties, there is an urgent need for a reliable, safe, and cheap energy source. Thermonuclear fusion, if achieved, is that source of energy which not only will satisfy our demand for today but also for centuries to come. Today, there are two major approaches to achieve fusion: magnetic confinement fusion (MFE) and inertial confinement fusion (ICF). This dissertation explores the inertial confinement fusion using the fast ignition concept. Unlike the conventional approach where the same laser is used for compression and ignition, in fast ignition separate laser beams are used. This dissertation addresses three very important topics to fast ignition inertial confinement fusion. These are laser-to-electron coupling efficiency, laser-generated electron beam transport, and the associated isochoric heating. First, an integrated fast ignition experiment is carried out with 0.9 kJ of energy in the compression beam and 70 J in the ignition beam. Measurements of absolute K{sub {alpha}} yield from the imploded core revealed …

Much of the previous work in the large data visualization area has solely focused on handling the scale of the data. This task is clearly a great challenge and necessary, but it is not sufficient. Applying standard visualization techniques to large scale data sets often creates complicated pictures where meaningful trends are lost. A second challenge, then, is to also provide algorithms that simplify what an analyst must understand, using either visual or quantitative means. This challenge can be summarized as improving the legibility or reducing the complexity of massive data sets. Fully meeting both of these challenges is the work of many, many PhD dissertations. In this dissertation, we describe some new techniques to address both the scale and legibility challenges, in hope of contributing to the larger solution. In addition to our assumption of simultaneously addressing both scale and legibility, we add an additional requirement that the solutions considered fit well within an interoperable framework for diverse algorithms, because a large suite of algorithms is often necessary to fully understand complex data sets. For scale, we present a general architecture for handling large data, as well as details of a contract-based system for integrating advanced optimizations into a …