This thesis presents the search for neutral Minimal Supersymmetric extension of Standard Model (MSSM) Higgs bosons decaying to tau pairs where one of the taus decays leptonically, and the other one hadronically. CDF Run II data with L{sub int} = 310 pb{sup -1} are used. There is no evidence of MSSM Higgs existence, which results in the upper limits on {sigma}(p{bar p} {yields} {phi}) x BR({phi} {yields} {tau}{tau}) in m{sub A} range between 115 and 250 GeV. These limits exclude some area in tan {beta} vs m{sub A} parameter space.

Magnetic refrigeration is a promising technology that offers a potential for high energy efficiency. The giant magnetocaloric effect of the R{sub 5}(Si{sub x}, Ge{sub 1-x}){sub 4} alloys (where R=rare-earth and O {le} x {le} 1), which was discovered in 1997, make them perfect candidates for magnetic refrigeration applications. In this study the microstructures of Gd{sub 5}(Si{sub x}Ge{sub 1-x}){sub 4} alloys have been characterized using electron microscopy techniques, with the focus being on distinctive linear features first examined in 1999. These linear features have been observed in R{sub 5}(Si{sub x}, Ge{sub 1-x}){sub 4} alloys prepared from different rare-earths (Gd, Tb, Dy and Er) with different crystal structures (Gd{sub 5}Si{sub 4}-type orthorhombic, monoclinic and Gd{sub 5}Ge{sub 4}-type orthorhombic). Systematic scanning electron microscope studies revealed that these linear features are actually thin-plates, which grow along specific directions in the matrix material. The crystal structure of the thin-plates has been determined as hexagonal with lattice parameters a=b=8.53 {angstrom} and c=6.40 {angstrom} using selected area diffraction (SAD). Energy dispersive spectroscopy analysis, carried out in both scanning and transmission electron microscopes, showed that the features have a composition approximating to R{sub 5}(Si{sub x},Ge{sub 1-x}){sub 3}.phase. Orientation relationship between the matrix and the thin-plates has been calculated …

Applications augmented with adaptive capabilities are becoming common in parallel computing environments. For large-scale scientific applications, dynamic adjustments to a computationally-intensive part may lead to a large pay-off in facilitating efficient execution of the entire application while aiming at avoiding resource contention. Application-specific knowledge, often best revealed during the run-time, is required to initiate and time these adjustments. In particular, General Atomic and Molecular Electronic Structure System (GAMESS) is a program for ab initio quantum chemistry that places significant demands on the high-performance computing platforms. Certain electronic structure calculations are characterized by high consumption of a particular resource, such as CPU, main memory, or disk I/O. This may lead to resource contention among concurrent GAMESS jobs and other programs in the dynamically changing environment. Thus, it is desirable to improve GAMESS calculations by means of dynamic adaptations. In this thesis, we show how an application- or algorithm-specific knowledge may play a significant role in achieving this goal. The choice of implementation is facilitated by a module-driven middleware easily integrated with GAMESS that assesses resource consumption and invokes GAMESS adaptations to the system environment. We show that the throughput of GAMESS jobs may be improved greatly as a result of such …

Our explorations of rare-earth, transition metal intermetallics have resulted in the synthesis and characterization, and electronic structure investigation, as well as understanding the structure-bonding-property relationships. Our work has presented the following results: (1) Understanding the relationship between compositions and properties in LaFe{sub 13-x}Si{sub x} system: A detailed structural and theoretical investigation provided the understanding of the role of a third element on stabilizing the structure and controlling the transformation of cubic NaZn{sub 13}-type structures to the tetragonal derivative, as well as the relationship between the structures and properties. (2) Synthesis of new ternary rare-earth iron silicides RE{sub 2-x}Fe{sub 4}Si{sub 14-y} and proposed superstructure: This compound offers complex structural challenges such as fractional occupancies and their ordering in superstructure. (3) Electronic structure calculation of FeSi{sub 2}: This shows that the metal-semiconductor phase transition depends on the structure. The mechanism of band gap opening is described in terms of bonding and structural distortion. This result shows that the electronic structure calculations are an essential tool for understanding the relationship between structure and chemical bonding in these compounds. (4) Synthesis of new ternary rare-earth Zinc aluminides Tb{sub 3}Zn{sub 3.6}Al{sub 7.4}: Partially ordered structure of Tb{sub 3}Zn{sub 3.6}Al{sub 7.4} compound provides new insights into …

Electroanalytical chemistry is often utilized in chemical analysis and Fundamental studies. Important advances have been made in these areas since the advent of chemically modified electrodes: the coating of an electrode with a chemical film in order to impart desirable, and ideally, predictable properties. These procedures enable the exploitation of unique reactivity patterns. This dissertation presents studies that investigate novel reaction mechanisms at self-assembled monolayers on gold. In particular, a unique electrochemical current amplification scheme is detailed that relies on a selective electrode to enable a reactivity pattern that results in regeneration of the analyte (redox recycling). This regenerating reaction can occur up to 250 times for each analyte molecule, leading to a notable enhancement in the observed current. The requirements of electrode selectivity and the resulting amplification and detection limit improvements are described with respect to the heterogeneous and homogeneous electron transfer rates that characterize the system. These studies revealed that the heterogeneous electrolysis of the analyte should ideally be electrochemically reversible, while that for the regenerating agent should be held to a low level. Moreover, the homogeneous reaction that recycles the analyte should occur at a rapid rate. The physical selectivity mechanism is also detailed with respect to …

This thesis presents two exclusive production processes in p{bar p} collisions at {radical}s = 1.96 TeV, using the Collider Detector Facility at Fermi National Accelerator Laboratory. An observation of exclusive e{sup +}e{sup -} production through {gamma}{gamma} {yields} e{sup +}e{sup -} is presented, as well as evidence for exclusive production of {gamma}{gamma} through gg {yields} {gamma}{gamma} (via a quark loop). The exclusive e{sup +}e{sup -} production observation is based on 16 candidate events, with a background estimate of 2.1{sub -0.3}{sup +0.7}. Each event has an e{sup +}e{sup -} pair (E{sub T} (e) > 5 GeV, |{eta}(e)| < 2) and nothing else observable in the CDF detector. The measured cross section is 1.6{sub -0.3}{sup +0.5}(stat) {+-} 0.3(sys) pb, while the predicted cross section is 1.711 {+-} 0.008 pb. The kinematic properties of the events are consistent with the predictions of the LPAIR Monte Carlo. The evidence for exclusive {gamma}{gamma} production consists of 3 candidate events, with a background estimate of 0.0{sub -0.0}{sup +0.2} events. Each event has two photons (E{sub T}{gamma}) > 5 GeV, |{eta}({gamma})| < 1 and nothing else observable in the CDF detector. The measured cross section for these events is 0.14{sub -0.04}{sup +0.14}(stat) {+-} (sys) pb. It agrees with …

Sum frequency generation (SFG) vibrational spectroscopy, atomic force microscopy (AFM), and quartz crystal microbalance (QCM) have been used to study the molecular surface structure, surface topography and mechanical properties, and quantitative adsorbed amount of biological molecules at the solid-liquid interface. The molecular-level behavior of designed peptides adsorbed on hydrophobic polystyrene and hydrophilic silica substrates has been examined as a model of protein adsorption on polymeric biomaterial surfaces. Proteins are such large and complex molecules that it is difficult to identify the features in their structure that lead to adsorption and interaction with solid surfaces. Designed peptides which possess secondary structure provide simple model systems for understanding protein adsorption. Depending on the amino acid sequence of a peptide, different secondary structures ({alpha}-helix and {beta}-sheet) can be induced at apolar (air/liquid or air/solid) interfaces. Having a well-defined secondary structure allows experiments to be carried out under controlled conditions, where it is possible to investigate the affects of peptide amino acid sequence and chain length, concentration, buffering effects, etc. on adsorbed peptide structure. The experiments presented in this dissertation demonstrate that SFG vibrational spectroscopy can be used to directly probe the interaction of adsorbing biomolecules with a surface or interface. The use of …

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The use of n-alkanethiolate self-assembled monolayers on gold has blossomed in the past few years. These systems have functioned as models for common interfaces. Thiolate monolayers are ideal because they are easily modified before or after deposition. The works contained within this dissertation include interfacial characterization (inbred reflection absorption spectroscopy, ellipsometry, contact angle, scanning probe microscopy, and heterogeneous electron-transfer kinetics) and various modeling scenarios. The results of these characterizations present ground-breaking insights into the structure, function, and reproducible preparation of these monolayers. Surprisingly, three interfacial properties (electron-transfer, contact angle, and ellipsometry) were discovered to depend directly on the odd-even character of the monolayer components. Molecular modeling was utilized to investigate adlayer orientation, and suggests that these effects are adlayer structure specific. Finally, the electric force microscopy and theoretical modeling investigations of monolayer samples are presented, which show that the film dielectric constant, thickness, and dipole moment directly affect image contrast. In addition, the prospects for utilization of this emerging technique are outlined.

In the process of exploring and understanding the influence of crystal structure on the system of compounds with the composition Gd{sub 5}(Si{sub x}Ge{sub 1-x}){sub 4} several new compounds were synthesized with different crystal structures, but similar structural features. In Gd{sub 5}(Si{sub x}Ge{sub 1-x}){sub 4}, the main feature of interest is the magnetocaloric effect (MCE), which allows the material to be useful in magnetic refrigeration applications. The MCE is based on the magnetic interactions of the Gd atoms in the crystal structure, which varies with x (the amount of Si in the compound). The crystal structure of Gd{sub 5}(Si{sub x}Ge{sub 1-x}){sub 4} can be thought of as being formed from two 3{sup 2}434 nets of Gd atoms, with additional Gd atoms in the cubic voids and Si/Ge atoms in the trigonal prismatic voids. Attempts were made to substitute nonmagnetic atoms for magnetic Gd using In, Mg and Al. Gd{sub 2}MgGe{sub 2} and Gd{sub 2}InGe{sub 2} both possess the same 3{sup 2}434 nets of Gd atoms as Gd{sub 5}(Si{sub x}Ge{sub 1-x}){sub 4}, but these nets are connected differently, forming the Mo{sub 2}FeB{sub 2} crystal structure. A search of the literature revealed that compounds with the composition R{sub 2}XM{sub 2} (R=Sc, Y, Ti, …

In this thesis, we discuss applications of first principles methods to x-ray resonant spectra and elastic properties calculation. We start with brief reviews about theoretical background of first principles methods, such as density functional theory, local density approximation (LDA), LDA+U, and the linear augmented plane wave (LAPW) method to solve Kohn-Sham equations. After that we discuss x-ray resonant scattering (XRMS), x-ray magnetic circular dichroism (XMCD) and the branching problem in the heavy rare earths Ledges. In the last chapter we discuss the elastic properties of the second hardest material AlMgB{sub 14}.

The explorations of rare-earth, transition metal intermetallics have resulted in the synthesis and characterization, and electronic structure investigation, as well as understanding the structure-bonding property relationships. The work has presented the following results: (1) Understanding the relationship between compositions and properties in LaFe{sub 13-x}Si{sub x} system: A detailed structural and theoretical investigation provided the understanding of the role of a third element on stabilizing the structure and controlling the transformation of cubic NaZn{sub 13}-type structures to the tetragonal derivative, as well as the relationship between the structures and properties. (2) Synthesis of new ternary rare-earth iron silicides Re{sub 2-x}Fe{sub 4}Si{sub 14-y} and proposed superstructure: This compound offers complex structural challenges such as fractional occupancies and their ordering in superstructure. (3) Electronic structure calculation of FeSi{sub 2}: This shows that the metal-semiconductor phase transition depends on the structure. The mechanism of band gap opening is described in terms of bonding and structural distortion. This result shows that the electronic structure calculations are an essential tool for understanding the relationship between structure and chemical bonding in these compounds. (4) Synthesis of new ternary rare-earth Zinc aluminides Tb{sub 3}Zn{sub 3.6}Al{sub 7.4}: Partially ordered structure of Tb{sub 3}Zn{sub 3.6}Al{sub 7.4} compound provides new insights …

The research presented and discussed within involves the development of novel biological applications of mesoporous silica nanoparticles (MSN) and an investigation of mesoporous material by transmission electron microscopy (TEM). Mesoporous silica nanoparticles organically functionalized shown to undergo endocytosis in cancer cells and drug release from the pores was controlled intracellularly and intercellularly. Transmission electron microscopy investigations demonstrated the variety of morphologies produced in this field of mesoporous silica nanomaterial synthesis. A series of room-temperature ionic liquid (RTIL) containing mesoporous silica nanoparticle (MSN) materials with various particle morphologies, including spheres, ellipsoids, rods, and tubes, were synthesized. By changing the RTIL template, the pore morphology was tuned from the MCM-41 type of hexagonal mesopores to rotational moire type of helical channels, and to wormhole-like porous structures. These materials were used as controlled release delivery nanodevices to deliver antibacterial ionic liquids against Escherichia coli K12. The involvement of a specific organosiloxane function group, covalently attached to the exterior of fluorescein doped mesoporous silica nanoparticles (FITC-MSN), on the degree and kinetics of endocytosis in cancer and plant cells was investigated. The kinetics of endocystosis of TEG coated FITC-MSN is significantly quicker than FITC-MSN as determined by flow cytometry experiments. The fluorescence confocal microscopy investigation …

Superconducting high resolution fast-neutron calorimetric spectrometers based on {sup 6}LiF and TiB{sub 2} absorbers have been developed. These novel cryogenic spectrometers measure the temperature rise produced in exothermal (n, {alpha}) reactions with fast neutrons in {sup 6}Li and {sup 10}B-loaded materials with heat capacity C operating at temperatures T close to 0.1 K. Temperature variations on the order of 0.5 mK are measured with a Mo/Cu thin film multilayer operated in the transition region between its superconducting and its normal state. The advantage of calorimetry for high resolution spectroscopy is due to the small phonon excitation energies k{sub B}T on the order of {mu}eV that serve as signal carriers, resulting in an energy resolution {Delta}E {approx} (k{sub B}T{sup 2}C){sup 1/2}, which can be well below 10 keV. An energy resolution of 5.5 keV has been obtained with a Mo/Cu superconducting sensor and a TiB{sub 2} absorber using thermal neutrons from a {sup 252}Cf neutron source. This resolution is sufficient to observe the effect of recoil nuclei broadening in neutron spectra, which has been related to the lifetime of the first excited state in {sup 7}Li. Fast-neutron spectra obtained with a {sup 6}Li-enriched LiF absorber show an energy resolution of 16 …

In recent years, semiconductor nanocrystal quantum dots havegarnered the spotlight as an important new class of biological labelingtool. Withoptical properties superior to conventional organicfluorophores from many aspects, such as high photostability andmultiplexing capability, quantum dots have been applied in a variety ofadvanced imaging applications. This dissertation research goes along withlarge amount of research efforts in this field, while focusing on thedesign and development of new nanoprobes from semiconductor nanocrystalsthat are aimed for useful imaging or sensing applications not possiblewith quantum dots alone. Specifically speaking, two strategies have beenapplied. In one, we have taken advantage of the increasing capability ofmanipulating the shape of semiconductor nanocrystals by developingsemiconductor quantum rods as fluorescent biological labels. In theother, we have assembled quantum dots and gold nanocrystals into discretenanostructures using DNA. The background information and synthesis,surface manipulation, property characterization and applications of thesenew nanoprobes in a few biological experiments are detailed in thedissertation.

The G0 (G-Zero) forward angle experiment completed in Hall C of the Thomas Jefferson National Accelerator Facility (TJNAF) has measured the parity violating asymmetries in elastic electron-proton scattering over a Q2 range of 0.12 < Q2 < 1.0 (GeV/c)2. A linear combination of the strange electric (GsE) and magnetic (GsM) form factors calculated from these asymmetries indicate a non-zero contribution of the strange quark to the charge and magnetization structure of the proton in the above kinematic range at a 89% confidence level. The results show a previously unmeasured Q2 dependence of the strange form factors. Combining the G0 results with previous parity violating experiments show that at Q2 = 0.1 (GeV/c)2 GsM = 0.62+-0.31 GsE = -0.013+-0.028 At intermediate Q2 of about 0.23 (GeV/c)2, a consistent value of GsM is seen compared to previous experiments, together with a measurement that may imply a negative value of GsE. For Q2 above 0.5 (GeV/c)2 a consistently positive value for the linear combination of the strange form factors is seen.

In order to understand the physical processes associated with fs-laser waveguide writing in glass, the effects of the laser repetition rate, the material composition and feature size were studied. The resulting material changes were observed by collecting Raman and fluorescence spectra with a confocal microscope. The guiding behavior of the waveguides was evaluated by measuring near field laser coupling profiles in combination with white light microscopy. Waveguides and Bragg gratings were fabricated in fused silica using pulse repetition rates from 1 kHz to 1 MHz and a wide range of scan speeds and pulse energies. Two types of fluorescence were detected in fused silica, depending on the fabrication conditions. Fluorescence from self trapped exciton (E{prime}{sub {delta}}) defects, centered at 550 nm, were dominant for conditions with low total doses, such as using a 1 kHz laser with a scan speed of 20 {micro}m/s and pulse energies less than 1 {micro}J. For higher doses a broad fluorescence band, centered at 650 nm, associated with non-bridging oxygen hole center (NBOHC) defects was observed. Far fewer NBOHC defects were formed with the 1 MHz laser than with the kHz lasers possibly due to annealing of the defects during writing. We also observed an …

This dissertation describes magnetic resonance imaging (MRI) of protons performed in a precession field of 132 {micro}T. In order to increase the signal-to-noise ratio (SNR), a pulsed 40-300 mT magnetic field prepolarizes the sample spins and an untuned second-order superconducting gradiometer coupled to a low transition temperature superconducting quantum interference device (SQUID) detects the subsequent 5.6-kHz spin precession. Imaging sequences including multiple echoes and partial Fourier reconstruction are developed. Calculating the SNR of prepolarized SQUID-detected MRI shows that three-dimensional Fourier imaging yields higher SNR than slice-selection imaging. An experimentally demonstrated field-cycling pulse sequence and post-processing algorithm mitigate image artifacts caused by concomitant gradients in low-field MRI. The magnetic field noise of SQUID untuned detection is compared to the noise of SQUID tuned detection, conventional Faraday detection, and the Nyquist noise generated by conducting biological samples. A second-generation microtesla MRI system employing a low-noise SQUID is constructed to increase SNR. A 2.4-m cubic, eddy-current shield with 6-mm thick aluminum walls encloses the experiment to attenuate external noise. The measured noise is 0.75 fT Hz{sup -1/2} referred to the bottom gradiometer loop. Solenoids wound from 30-strand braided wire to decrease Nyquist noise and cooled by either liquid nitrogen or water polarize the …

Similar to elastic electron scattering, Compton Scattering on the proton at high momentum transfers(and high p⊥) can be an effective method to study its short-distance structure. An experiment has been carried out to measure the cross sections for Real Compton Scattering (RCS) on the proton for 2.3-5.7 GeV electron beam energies and a wide distribution of large scattering angles. The 25 kinematic settings sampled a domain of s = 5−11(GeV/c)2,−t = −7(GeV/c)2 and −u = 0.5−6.5(GeV/c)2. In addition, a measurement of longitudinal and transverse polarization transfer asymmetries was made at a 3.48 GeV beam energy and a scattering angle of θcm = 120o. These measurements were performed to test the existing theoretical mechanisms for this process as well as to determine RCS form factors. At the heart of the scientific motivation is the desire to understand the manner in which a nucleon interacts with external excitations at the above listed energies, by comparing and contrasting the two existing models – Leading Twist Mechanism and Soft Overlap “Handbag” Mechanism – and identify the dominant mechanism. Furthermore, the Handbag Mechanism allows one to calculate reaction observables in the framework of Generalized Parton Distributions (GPD), which have the function of bridging the wide …

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.

Many chemical reactions utilize organometallic complexes as catalysts. These complexes find use in reactions as varied as bond activation, polymerization, and isomerization. This thesis outlines the construction of a new ultrafast laser system with an emphasis on the generation of tunable mid-infrared pulses, data collection, and data analysis.

The shrinking of IC devices has followed the Moore's Law for over three decades, which states that the density of transistors on integrated circuits will double about every two years. This great achievement is obtained via continuous advance in lithography technology. With the adoption of complicated resolution enhancement technologies, such as the phase shifting mask (PSM), the optical proximity correction (OPC), optical lithography with wavelength of 193 nm has enabled 45 nm printing by immersion method. However, this achievement comes together with the skyrocketing cost of masks, which makes the production of low volume application-specific IC (ASIC) impractical. In order to provide an economical lithography approach for low to medium volume advanced IC fabrication, a maskless ion beam lithography method, called Maskless Micro-ion-beam Reduction Lithography (MMRL), has been developed in the Lawrence Berkeley National Laboratory. The development of the prototype MMRL system has been described by Dr. Vinh Van Ngo in his Ph.D. thesis. But the resolution realized on the prototype MMRL system was far from the design expectation. In order to improve the resolution of the MMRL system, the ion optical system has been investigated. By integrating a field-free limiting aperture into the optical column, reducing the electromagnetic interference …

Sum frequency generation (SFG) surface vibrational spectroscopy was used to characterize interfaces pertinent to current surface engineering applications, such as thin film polymers and novel catalysts. An array of advanced surface science techniques like scanning probe microscopy (SPM), x-ray photoelectron spectroscopy (XPS), gas chromatography (GC) and electron microscopy were used to obtain experimental measurements complementary to SFG data elucidating polymer and catalyst surface composition, surface structure, and surface mechanical behavior. Experiments reported in this dissertation concentrate on three fundamental questions: (1) How does the interfacial molecular structure differ from that of the bulk in real world applications? (2) How do differences in chemical environment affect interface composition or conformation? (3) How do these changes correlate to properties such as mechanical or catalytic performance? The density, surface energy and bonding at a solid interface dramatically alter the polymer configuration, physics and mechanical properties such as surface glass transition, adhesion and hardness. The enhanced sensitivity of SFG at the buried interface is applied to three systems: a series of acrylates under compression, the compositions and segregation behavior of binary polymer polyolefin blends, and the changes in surface structure of a hydrogel as a function of hydration. In addition, a catalytically active thin …

Our research focuses on taking advantage of the ability of scanning tunneling microscopy (STM) to operate at high-temperatures and high-pressures while still providing real-time atomic resolution images. We also utilize high-pressure x-ray photoelectron spectroscopy (HPXPS) to monitor systems under identical conditions thus giving us chemical information to compare and contrast with the structural and dynamic data provided by STM.