Time variability analyses have been applied to data composed of event times of X-rays emitted from the binary system Cygnus X-1 to search for unique black hole signatures. The X-ray data analyzed was collected at ten microsecond time resolution or better from two instruments, the High Energy Astrophysical Observatory (HEAO) A-1 detector and the Rossi X-ray Timing Explorer (XTE) Proportional Counter Array (PCA). HEAO A-1 and RXTE/PCA collected data from 1977--79 and from 1996 on with energy sensitivity from 1--25 keV and 2--60 keV, respectively. Variability characteristics predicted by various models of an accretion disk around a black hole have been searched for in the data. Drop-offs or quasi-periodic oscillations (QPOs) in the Fourier power spectra are expected from some of these models. The Fourier spectral technique was applied to the HEAO A-1 and RXTE/PCA data with careful consideration given for correcting the Poisson noise floor for instrumental effects. Evidence for a drop-off may be interpreted from the faster fall off in variability at frequencies greater than the observed breaks. Both breaks occur within the range of Keplerian frequencies associated with the inner edge radii of advection-dominated accretion disks predicted for Cyg X-1. The break between 10--20 Hz is also …

The syntheses of silicon-containing compounds and the studies of their rearrangements have been active research areas in the Barton research group. Previously, the addition of disilanes to acetylenes was studied in the group and an intramolecular 2S + 2A mechanism has been proposed. In this thesis, the work is focused on the addition of disilanes to cumulenes. The syntheses of the precursors are discussed and the possible mechanisms for their thermal, photochemical and catalytic rearrangements are proposed. Conjugated organic polymers have been studied in the group since 1985 because of their potential for exhibiting high electroconductivity, photoconductivity, strong non-linear optical response and intense fluorescence. In the second section of this dissertation, the synthesis and property studies of poly(phenylene vinylene) analogues are discussed.

An escaping alpha collector probe has been developed for TFTR`s DT phase. Energy distributions of escaping alphas have been determined by measuring the range of {alpha}-particles implanted into nickel foils located within the alpha collector. Results at 1.0 MA of plasma current are in good agreement with predictions for first orbit alpha loss. Results at 1.8 MA, however, show a significant anomalous loss of partially thermalized alphas (in addition to the expected first orbit loss), which is not observed with the lost alpha scintillator detectors in DT plasmas, but does resemble the anomalous delayed loss seen in DD plasmas. None of the candidate explanations proposed thus far are fully consistent with the anomalous loss observations. An experiment designed to study the effect of plasma major radius shifts on {alpha}-particle loss has led to a better understanding of {alpha}-particle dynamics in tokamaks. Intuitively, one might suppose that confined marginally passing {alpha}-particles forced to move toward higher magnetic field during an inward major radius shift (i.e., compression) would mirror and become trapped particles, leading to increased alpha loss. Such an effect was looked for during the shift experiment, however, no significant changes in alpha loss to the 90{degree} lost alpha scintillator detector …

Gabor first proposed holography in 1948 as a means to experimentally record the amplitude and phase of scattered wavefronts, relative to a direct unscattered wave, and to use such a {open_quotes}hologram{close_quotes} to directly image atomic structure. But imaging at atomic resolution has not yet been possible in the way he proposed. Much more recently, Szoeke in 1986 noted that photoexcited atoms can emit photoelectron of fluorescent x-ray wavefronts that are scattered by neighboring atoms, thus yielding the direct and scattered wavefronts as detected in the far field that can then be interpreted as holographic in nature. By now, several algorithms for directly reconstructing three-dimensional atomic images from electron holograms have been proposed (e.g. by Barton) and successfully tested against experiment and theory. Very recently, Tegze and Faigel, and Grog et al. have recorded experimental x-ray fluorescence holograms, and these are found to yield atomic images that are more free of the kinds of aberrations caused by the non-ideal emission or scattering of electrons. The basic principles of these holographic atomic imaging methods are reviewed, including illustrative applications of the reconstruction algorithms to both theoretical and experimental electron and x-ray holograms. The author also discusses the prospects and limitations of these …

Effective on March 15, 1990, the Environmental Protection Agency established regulations controlling the emission of radionuclides to the air from Department of Energy facilities to limit the dose to the public to 10 mrem/yr. These regulations are detailed in 40 CFR 61, Subpart H, {open_quotes}National Emission Standards for Emissions of Radionuclides Other Than Radon from Department of Energy Facilities{close_quotes}. Part of these regulations require the operation of sampling systems on stacks meeting certain requirements. Although Los Alamos National Laboratory has a long history of stack sampling, the systems in place at the time the regulation became effective did not meet the specific design requirements of the new regulation. In addition, certain specific program elements did not exist or were not adequately documented. The Los Alamos National Laboratory has undertaken a major effort to upgrade its compliance program to meet the requirements of USEPA. This effort involved: developing new and technically superior sampling methods and obtaining approval from the Environmental Protection Agency for their use; negotiating specific methodologies with the Environmental Protection Agency to implement certain requirements of the regulation: implementing a complete, quality assured, compliance program; and upgrading sampling systems. After several years of effort, Los Alamos National Laboratory now …

Photosynthesis is a complex process which results in the conversion of solar radiation into chemical energy. This chemical energy is then used as the free energy source for all living organisms. In its basic form, photosynthesis can be described as the light-activated synthesis of carbohydrates from the simple molecules of water and carbon dioxide: 6H{sub 2}O + 6 CO{sub 2} light C{sub 6}H{sub 12}O{sub 6} + 6 O{sub 2} This basic mechanism actually requires numerous reaction steps. The two primary steps being: the capture of light by pigment molecules in light-harvesting antenna complexes and the transfer of this captured energy to the so-called photochemical reaction center. While the preferred pathway for energy absorbed by the chromophores in the antenna complexes is transfer to the reaction center, energy can be lost to competing processes such as internal conversion or radiative decay. Therefore, the energy transfer must be rapid, typically on the order of picoseconds, to successfully compete. The focus of the present work is on the construction of light-harvesting antenna complexes incorporating modular pigment-proteins.

A conceptual management framework is developed and applied in a science and engineering organization located within a non-profit, public institution. The goal of this research is to select a set of projects whose combined contributions to the organization`s strategic interests satisfy sponsor desires and can be completed within existing time and resource constraints. The development of the rationale for project selection and implementation within the plutonium facility at Los Alamos National Laboratory is studied. This includes the integration of prioritization decision tools, optimization techniques, and advanced planning and scheduling tools. The Nuclear Materials Technology Division is the custodian of the plutonium facility, whose mission is to develop, demonstrate, and deploy technologies necessary to address the nation`s and world`s plutonium problems. This includes management of nuclear weapon stockpile components, stabilization of plutonium residues, clean-up of contaminated soils and facilities, support to non-proliferation and arms control initiatives, and the eventual disposition of surplus plutonium. In this study, projects are evaluated against selection criteria deemed to be of critical program importance. The Analytic Hierarchy Process is used to evaluate and rank the importance of the suite of candidate projects. Because individual projects may be of interest to a number of business sectors and …

After introducing the subject of conjugated polymers, the thesis has three sections each containing a literature survey, results and discussion, conclusions, and experimental methods on the following: synthesis, characterization of electroluminescent polymers containing conjugated aryl, olefinic, thiophene and acetylenic units and their studies for use in light-emitting diodes; synthesis, characterization and study of conjugated polymers containing silole unit in the main chain; and synthesis, characterization and study of silicon-bridged and butadiene-linked polythiophenes.

A main research interest is the characterization of monolayers formed by the spontaneous adsorption of organosulfur compounds at gold. This dissertation describes the development and application of long optical pathlength thin-layer spectroelectrochemistry in an attempt to address key issues regarding the reactivity of surface-immobilized molecules. The first section of this introductory chapter briefly describes the general approach to the preparation and characterization of these films. The last section provides an overview of the main principles and advantages of thin-layer spectroelectrochemistry for studying surface-adsorbed species. The body of this dissertation is divided into four chapters. Chapter 2 consists of a paper describing the design, construction, and characterization of a cuvette-based LOPTLC. Chapter 3 is a paper which examines the reductive desorption process using thin-layer spectroelectrochemistry to monitor and identify the desorption product. Chapter 4 is a paper describing the characterization of monolayers functionalized with a catechol terminal group which serves as a redox transformable coordination site for metal ion binding. Chapter 5 discusses the application of thin-layer spectroelectrochemistry to acid-base reactivity studies of surface-immobilized molecules. The final section provides some general conclusions and a prospectus for future studies. These chapters have been processed separately for inclusion on the data base. This …

There has been continuing development of generic classes of microstrip gas chambers (MSGCs), microgap gas chambers (MGCs) and microdot gas chambers (MDOTs) at Lawrence Berkeley National Laboratory (LBNL) over the past few years, to improve such detectors beyond their present capabilities, to produce detectors suitable for use in current or upcoming experiments, and to allow a basis for new R&D developments which may incorporate these detectors as part of the system. All of these new detectors are collectively referred to as {open_quotes}gas avalanche microdetectors{close_quotes}. The MSGC, which was motivated by the pioneering work of A. Oed, has many attractive features, especially excellent spatial resolution ({approximately}30 {mu}m rms at normal incidence) and high rate capability ({approximately}10{sup 6} mm{sup -2}{center_dot}s{sup -1}). Moreover, the MGC seems to have certain advantages over the MSGC in speed, stability and simplicity, and the MDOT has larger gain (>10{sup 4}) and the intrinsic advantages of two-dimensional readout. Because of these attractive properties, they have received a great deal of attention for nuclear and high energy physics experiments, medical X-ray imaging and many other fields requiring radiation detection and measurement.

Potassium tantalate niobate (KTN) pyroelectric detectors are expected to provide detectivities, of 3.7 x 10{sup 11} cmHz {sup {1/2}}W{sup {minus}1} for satellite-based infrared detection at 90 K. The background limited detectivity for a room-temperature thermal detector is 1.8 x 10{sup 10} cmHz{sup {1/2}}W{sup {minus}1}. KTN is a unique ferroelectric for this application because of the ability to tailor the temperature of its pyroelectric response by adjusting its ratio of tantalum to niobium. The ability to fabricate high quality KTN thin films on Si-based substrates is crucial to the development of KTN pyroelectric detectors. Si{sub x}N{sub y} membranes created on the Si substrate will provide the weak thermal link necessary to reach background limited detectivities. The device dimensions obtainable by thin film processing are expected to increase the ferroelectric response by 20 times over bulk fabricated KTN detectors. In addition, microfabrication techniques allow for easier array development. This is the first reported attempt at growth of KTN films on Si-based substrates. Pure phase perovskite films were grown by pulsed laser deposition on SrRuO{sub 3}/Pt/Ti/Si{sub x}N{sub y}/Si and SrRuO{sub 3}/Si{sub x}N{sub y}/Si structures; room temperature dielectric permittivities for the KTN films were 290 and 2.5, respectively. The dielectric permittivity for bulk grown, …

This paper presents a review of the Direct Stator Flux Field Orientation control method. This method can be used to control an induction motor`s torque and flux directly and is the application of interest for this thesis. This control method is implemented without the traditional feedback loops and associated hardware. Predictions are made, by mathematical calculations, of the stator voltage vector. The voltage vector is determined twice a switching period. The switching period is fixed throughout the analysis. The three phase inverter duty cycle necessary to control the torque and flux of the induction machine is determined by the voltage space vector Pulse Width Modulation (PWM) technique. Transient performance of either the flux or torque requires an alternate modulation scheme which is also addressed in this thesis. A block diagram of this closed loop system is provided. 22 figs., 7 tabs.

Microscale separation and detection methods for real-time monitoring of dynamic cellular processes (e.g., secretion) by capillary electrophoresis (CE) and microscopic imaging were developed. Ultraviolet laser-induced native fluorescence (LINF) provides simple, sensitive and direct detection of neurotransmitters and proteins without any derivatization. An on-column CE-LINF protocol for quantification of the release from single cell was demonstrated. Quantitative measurements of both the amount of insulin released from and the amount remaining in the cell ({beta}TC3) were achieved simultaneously. Secretion of catecholamines (norepinephrine (NE) and epinephrine (E)) from individual bovine adrenal chromaffin cells was determined using the on-column CE-LINF. Direct visualization of the secretion process of individual bovine adrenal chromaffin cells was achieved by LINF imaging microscopy with high temporal and spatial resolution. The secretion of serotonin from individual leech Retzius neurons was directly characterized by LINF microscopy with high spatial resolution.

In this thesis the author discusses the methodology for doing photometry: from procedure of extracting supernova counts from images that contain combined supernova plus galaxy flux, to standard star calibration, to additional instrumental corrections that arise due to the multiple telescopes used for observations. He discusses the different sources of photometric error and their correlations, and the construction of the covariance matrix for all the points in the light curve. He then describes the K corrections which account for the redshifting of spectra that are necessary to compare the photometry of the high-redshift data with those from nearby (z < 0.1) supernovae. Finally, he uses the first seven of the supernovae to test the hypothesis that they live in an under-dense bubble where the locally measured Hubble constant differs significantly from the true Hubble constant. He also uses the data to place limits on the value of the Hubble constant. Discussions of several other important aspects of the data analysis are or will be included in other papers. These topics include a description of how the covariance matrix is used to generate light-curve fits, a discussion of non-photometric systematic errors that also effect the measurements, and a discussion of the …

MiniMax (Fermilab T-864) was a small test/experiment at the Tevatron designed to search for disoriented chiral condensates (DCC) in the forward direction. Relativistic quantum field theory treats the vacuum as a medium, with bulk properties characterized by long-range order parameters. This has led to suggestions that regions of {open_quotes}disoriented vacuum{close_quotes} might be formed in high-energy collision processes. In particular, the approximate chiral symmetry of QCD could lead to regions of vacuum which have chiral order parameters disoriented to directions which have non-zero isospin, i.e. disoriented chiral condensates. A signature of DCC is the resulting distribution of the fraction of produced pions which are neutral. The MiniMax detector at the C0 collision region of the Tevatron was a telescope of 24 multi-wire proportional chambers (MWPC`s) with a lead converter behind the eighth MWPC, allowing the detection of charged particles and photon conversions in an acceptance approximately a circle of radius 0.6 in pseudorapidity-azimuthal-angle space, centered on pseudorapidity {eta} {approx} 4. An electromagnetic calorimeter was located behind the MWPC telescope, and hadronic calorimeters and scintillator were located in the upstream anti-proton direction to tag diffractive events.

In the first part of this work, the author describes studies of donors in AlSb and in GaAs at large hydrostatic pressures, two materials in which the conduction band minimum is not parabolic, but has a camel`s back shape. These donors were found to display only one or two absorption lines corresponding to ground to bound excited state transitions. It is shown that due to the non-parabolic dispersion, camel`s back donors may have as few as one bound excited state and that higher excited states are auto-ionized. Thus, it is possible that transitions to these other states may be lost in the continuum. In the second part, calculations of mobilities in GaN and other group III-Nitride based structures were performed. GaN is interesting in that the carriers in nominally undoped material are thought to originate from impurities which have an ionization energy level resonant with the conduction band, rather than located in the forbidden gap. These donors have a short range potential associated with them which can be effective in scattering electrons in certain situations. It was found that effects of these resonant donors can be seen only at high doping levels in III-Nitride materials and in Al{sub x}Ga{sub 1{minus}x}N …

Three-dimensional creeping flow around single, axisymmetric protrusions is studied numerically using the boundary-integral technique. Emphasis is placed upon cylindrical protrusions on plane walls for various height-to-radius (h-to-a) aspect ratios, but cones and sections of spheres protruding from plane walls are also briefly examined. The presented items include shear-stress distributions, shear-stress contours, extents of the fluid-flow disturbance, total forces and torques on the cylinders, streamlines, and skin-friction lines. Also included is a discussion of flow topology around axisymmetric geometries. No flow reversal is observed for cylindrical protrusions with aspect ratios greater than 2.4 to 2.6. At higher aspect ratios, the fluid tends to be swept around cylindrical protrusions with little vertical motion. At lower aspect ratios, the strength of the recirculation increases, and the recirculation region becomes wider in the transverse direction and narrower in the flow direction. Also, the recirculation pattern begins to resemble the closed streamline patterns in two-dimensional flow over square ridges. However, unlike two-dimensional flow, closed streamline patterns are not observed. For arbitrary axisymmetric geometries, the extent of the fluid-flow disturbance can be estimated with the total force that is exerted on the protrusion. When the same force is exerted on protrusions with different aspect ratios, the …

This work describes the continued development of a new separation technique, electrochemically-modulated liquid chromatography (EMLC), from column design, retention mechanisms to pharmaceutical applications. The introduction section provides a literature review of the technique as well as a brief overview of the research in each of the chapters. This section is followed by four chapters which investigate the issues of EMLC column design, the retention mechanism of monosubstituted aromatic compounds, and the EMLC-based applications to two important classes of pharmaceutical compounds (i.e., corticosteroids and benzodiazepines). These four sections have been removed to process separately for inclusion on the database. The dissertation concludes with a general summary, a prospectus, and a list of references cited in the General Introduction. 32 refs.

The author`s group has previously shown that isocyanides are readily adsorbed from solutions to Au powder and bind to the Au surface in an end-on fashion through the terminal carbon. Later work demonstrated that the equilibrium constants for the reversible adsorption of electronically inequivalent isocyanides could be obtained using the Langmuir isotherm technique. This dissertation describes two projects completed which complement the initial findings of this group. Initially, several alkylisocyanides were synthesized to examine the effect of tail length on Au powder adsorption. It was observed that the length of the alkyl chain affected not only the Au surface binding affinity, but also the rate of surface saturation and saturation coverage values. Direct competition studies were also studied using a {sup 13}C-labeled isocyanide. These studies demonstrated the stabilization afforded by substrate-substrate packing forces in SAM`s formed by the longer chain isocyanides. In a second study, di and triisocyanides were synthesized to determine the effect that the length of the connecting link and the number of isocyanide groups (as points of attachment) have on Au adsorption stability. The work in this area describes the binding modes, relative binding affinities and surface coverage values for a series of flexible alkyl and xylyldiisocyanides …

The equilibrium motion of vortices in two- and three-dimensional superconductors has been studied with a dc Superconducting QUantum Interference Device (SQUID). This technique has the advantage of probing the system in a non-invasive manner as well as providing dynamic information over many decades in frequency. Through measurements of the spectral density of magnetic flux noise, S{sub {Phi}}({omega}), as a function of temperature and applied magnetic field, the effects of proton and heavy ion irradiation on flux noise in crystals of YBa{sub 2}Cu{sub 3}O{sub 7{minus}{delta}} have been measured and compared with the effects on the critical current, J{sub c}. Both proton and heavy ion irradiation proved effective at reducing S{sub {Phi}}({omega}), with proton irradiation having a larger effect. Measurement of S{sub {Phi}}({omega}) due to the equilibrium Kosterlitz-Thouless-Berezinskii transition in two-dimensional Josephson Junction Arrays (JJAs) was studied as a function of temperature for three different arrays and using three different sensors. S{sub {Phi}} is shown to obey dynamic scaling over as many as five decades in frequency, and estimates are made for the dynamic critical exponent z. An analytic theory for the high- and low-frequency behavior of S{sub {Phi}}({omega}) is presented and compared to the measured data, with the result that the …

EUV lithography is a promising and viable candidate for circuit fabrication with 0.1-micron critical dimension and smaller. In order to achieve diffraction-limited performance, all-reflective multilayer-coated lithographic imaging systems operating near 13-nm wavelength and 0.1 NA have system wavefront tolerances of 0.27 nm, or 0.02 waves RMS. Owing to the highly-sensitive resonant reflective properties of multilayer mirrors and extraordinarily tight tolerances set forth for their fabrication, EUV optical systems require at-wavelength EUV interferometry for final alignment and qualification. This dissertation discusses the development and successful implementation of high-accuracy EUV interferometric techniques. Proof-of-principle experiments with a prototype EUV point-diffraction interferometer for the measurement of Fresnel zoneplate lenses first demonstrated sub-wavelength EUV interferometric capability. These experiments spurred the development of the superior phase-shifting point-diffraction interferometer (PS/PDI), which has been implemented for the testing of an all-reflective lithographic-quality EUV optical system. Both systems rely on pinhole diffraction to produce spherical reference wavefronts in a common-path geometry. Extensive experiments demonstrate EUV wavefront-measuring precision beyond 0.02 waves RMS. EUV imaging experiments provide verification of the high-accuracy of the point-diffraction principle, and demonstrate the utility of the measurements in successfully predicting imaging performance. Complementary to the experimental research, several areas of theoretical investigation related to the novel …

Semiconductor and metallic nanocrystals exhibit interesting electronic transport behavior as a result of electrostatic and quantum mechanical confinement effects. These effects can be studied to learn about the nature of electronic states in these systems. This thesis describes several techniques for the electronic study of nanocrystals. The primary focus is the development of novel methods to attach leads to prefabricated nanocrystals. This is because, while nanocrystals can be readily synthesized from a variety of materials with excellent size control, means to make electrical contact to these nanocrystals are limited. The first approach that will be described uses scanning probe microscopy to first image and then electrically probe surfaces. It is found that electronic investigations of nanocrystals by this technique are complicated by tip-sample interactions and environmental factors such as salvation and capillary forces. Next, an atomic force microscope technique for the catalytic patterning of the surface of a self assembled monolayer is described. In principle, this nano-fabrication technique can be used to create electronic devices which are based upon complex arrangements of nanocrystals. Finally, the fabrication and electrical characterization of a nanocrystal-based single electron transistor is presented. This device is fabricated using a hybrid scheme which combines electron beam lithography …

We develop a polarization-sensitive femtosecond pump probe technique, Raman induced polarization spectroscopy (RIPS), to study coherent rotation in molecular fluids. By observing the collisional dephasing of the coherently prepared rotational states, we are able to extract information concerning the effects of molecular interactions on the rotational motion. The technique is quite sensitive because of the zero background detection method, and is also versatile due to its nonresonant nature.

Highly dispersed transition metal catalysts are used in numerous commercial processes such as hydrocarbon conversions. For example, the use of Pt supported on acidic alumina or silica-alumina for reforming of naphtha in the production of gasoline is well known. Another use of supported catalysts is in automobile emission control where supported Pt-Rh bimetallic catalysts are used. Supported Ru can be used in Fischer-Tropsch synthesis for the production of higher hydrocarbons from synthesis gas. While many of these catalyst systems have been in commercial operation for several decades there is still a lack of consensus regarding the exact role of the catalyst on a molecular level. In particular, little is known about the mechanisms operating on the catalyst surface at the high pressure and high temperature conditions typically used in commercial operations. This report contains the general introduction and conclusions and an appendix containing the operating instructions for a microcalorimeter. Three chapters have been processed separately. They are: the effect of K on the kinetics and thermodynamics of hydrogen adsorption on Ru/SiO{sub 2}; hydrogen adsorption states on silica supported Ru-Ag and Ru-Cu bimetallic catalysts investigated via microcalorimetry; a comparative study of hydrogen chemisorption on silica supported Ru, Rh, and Pt.