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Nanoscale chemical and mechanical characterization of thin films:sum frequency generation (SFG) vibrational spectroscopy at buriedinterfaces

Description: 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 film of polymer coated nanoparticles is investigated to evaluate the efficacy of SFG to provide in situ information for catalytic reactions involving small mass adsorption and/or product development. Through the use of SFG, in situ total internal reflection (TIR) was used to increase the sensitivity of SFG and provide the necessary specificity to investigate interfaces of thin polymer films and nanostructures previously considered unfeasible. The dynamic nature of thin film surfaces is examined and it is found that the non-equilibrium states contribute to practical applications of acrylates, blends and hydrogels. Lastly, nanoparticle surfaces and the catalytic activity and selectivity of ...
Date: May 19, 2006
Creator: Kweskin, S.J.
Partner: UNT Libraries Government Documents Department

Inclusive Rates and Spectra of the Lambda, Cascade, and Omega Hyperons atBaBar

Description: We employ Runs 1-4 off-peak data sample (about 21.5 fb{sup -1}) to produce the current world-best spectra and production rates measurements for three strangely-flavored baryons: the {Lambda} hyperon, the cascade hyperon, and the {Omega} hyperon. These improved measurements shall enable theoretical and phenomelogical workers to generate more realistic models for the hadronization process, currently one of the unresolved problem areas in the standard model of particle physics. This analysis was conducted using codes from release 16 series. We report the production rate at 10.54 GeV for the {Lambda} as 0.0900 {+-} 0.0006(stat.) {+-} 0.0039(sys.) per hadronic event. Our measured production rate at the same energy for the cascade hyperon is 0.00562 {+-} 0.00013(stat.) {+-} 0.00045(sys.) per hadronic event, while that for the {Omega} hyperon is 0.00027 {+-} 0.00004(stat.) {+-} 0.0008(sys.) per hadronic event. The spectral measurements for the respective particles also constitute current world-best measurements.
Date: May 19, 2008
Creator: Chien, Andrew L.
Partner: UNT Libraries Government Documents Department

Search for the Production of Gluinos and Squarks with the CDF II Experiment at the Tevatron Collider

Description: This thesis reports on two searches for the production of squarks and gluinos, supersymmetric partners of the Standard Model (SM) quarks and gluons, using the CDF detector at the Tevatron √s = 1.96 TeV p$\bar{p}$ collider. An inclusive search for squarks and gluinos pair production is performed in events with large E<sub>T</sub> and multiple jets in the final state, based on 2 fb<sup>-1</sup> of CDF Run II data. The analysis is performed within the framework of minimal supergravity (mSUGRA) and assumes R-parity conservation where sparticles are produced in pairs. The expected signal is characterized by the production of multiple jets of hadrons from the cascade decays of squarks and gluinos and large missing transverse energy E<sub>T</sub> from the lightest supersymmetric particles (LSP). The measurements are in good agreement with SM predictions for backgrounds. The results are translated into 95% confidence level (CL) upper limits on production cross sections and squark and gluino masses in a given mSUGRA scenario. An upper limit on the production cross section is placed in the range between 1 pb and 0.1 pb, depending on the gluino and squark masses considered. The result of the search is negative for gluino and squark masses up to 392 GeV/c<sup>2</sup> in the region where gluino and squark masses are close to each other, gluino masses up to 280 GeV/c<sup>2</sup> regardless of the squark mass, and gluino masses up to 423 GeV=c<sup>2</sup> for squark masses below 378 GeV/c<sup>2</sup>. These results are compatible with the latest limits on squark/gluino production obtained by the D0 Collaboration and considerably improve the previous exclusion limits from direct and indirect searches at LEP and the Tevatron. The inclusive search is then extended to a scenario where the pair production of sbottom squarks is dominant. The new search is performed in a generic MSSM scenario with ...
Date: May 19, 2010
Creator: De Lorenzo, Gianluca
Partner: UNT Libraries Government Documents Department

Ultrafast Magnetization Dynamics of SrRuO3 Thin Films

Description: Itinerant ferromagnet SrRuO3 has drawn interest from physicists due to its unusual transport and magnetic properties as well as from engineers due to its low resistivity and good lattice-matching to other oxide materials. The exact electronic structure remains a mystery, as well as details of the interactions between magnetic and electron transport properties. This thesis describes the use of time-resolved magneto-optical Kerr spectroscopy to study the ferromagnetic resonance of SrRuO3 thin films, where the ferromagnetic resonance is initiated by a sudden change in the easy axis direction in response to a pump pulse. The rotation of the easy axis is induced by laser heating, taking advantage of a temperature-dependent easy axis direction in SrRuO3 thin films. By measuring the change in temperature of the magnetic system in response to the laser pulse, we find that the specific heat is dominated by magnons up to unusually high temperature, ~;;100 K, and thermal diffusion is limited by a boundary resistance between the film and the substrate that is not consistent with standard phonon reflection and scattering models. We observe a high FMR frequency, 250 GHz, and large Gilbert damping parameter, alpha ~;; 1, consistent with strong spin-orbit coupling. We observe a time-dependent change in the easy axis direction on a ps time-scale, and we find that parameters associated with the change in easy axis, as well as the damping parameter, have a non-monotonic temperature dependence similar to that observed in anomalous Hall measurements.
Date: May 19, 2009
Creator: Langner, Matthew C.
Partner: UNT Libraries Government Documents Department

Steric and electronic effects of 1,3-disubstituted cyclopentadienyl ligands on metallocene derivatives of Cerium, Titanium, Manganese, and Iron

Description: Sterically demanding 1,3-disubstituted cyclopentadienyl ligands were used to modify the physical properties of the corresponding metallocenes. Sterically demanding ligands provided kinetic stabilization for trivalent cerium compounds. Tris(di-t-butylcyclopentadienyl)cerium was prepared and anion competition between halides and cyclopentadienyl groups which had complicated synthesis of the tris(cyclopentadienyl)compound was qualitatively examined. Bis(di-t-butylcyclopentadienyl)cerium methyl was prepared and its rate of decomposition, by ligand redistribution, to tris(di-t-butylcyclopentadienyl)cerium was shown to be slower than the corresponding rate for less sterically demanding ligands. Asymmetrically substituted ligands provided a symmetry label for examination of chemical exchange processes. Tris[trimethylsilyl(t-butyl)cyclopentadienyl]cerium was prepared and the rate of interconversion between the C1 and C3 isomers was examined. The enthalpy difference between the two distereomers is 7.0 kJ/mol. The sterically demanding cyclopentadienyl ligands ansa-di-t-butylcyclopentadiene (Me2Si[(Me3C)2C5H3]2), ansa-bis(trimethylsilyl)cyclopentadiene (Me2Si[(Me3Si)2C5H3]2) and tetra-t-butylfulvalene and metallocene derivatives of the ligands were prepared and their structures were examined by single crystal X-ray crystallography. The effect that substituents on the cyclopentadienyl ring have on the pi-electron system of the ligand was examined through interaction between ligand and metal orbitals. A series of 1,3-disubstituted manganocenes was prepared and their electronic states were determined by solid-state magnetic susceptibility, electron paramagnetic resonance, X-ray crystallography, and variable temperature UV-vis spectroscopy. Spin-equilibria in [(Me3C)2C5H3]2Mn and [(Me3C)(Me3Si)C5H3]2Mn were examined and indicate an enthalpy difference of 15 kJ/mol between the high-spin and low-spin forms. Cyclopentadienyl groups resistant to intramolecular oxidative addition allowed isolation of compounds susceptible to intramolecular decomposition. A kinetically stable, base-free titanocene was prepared using di-t-butylcyclopentadienyl ligands and the reactivity of the compound toward small molecules was investigated. The titanocene reacts reversibly with hydrogen to form the titanocene dihydride and the equilibrium in solution between titanocene dihydride, and titanocene and hydrogen, was examined.
Date: May 19, 2000
Creator: Sofield, C.D.
Partner: UNT Libraries Government Documents Department

Synthesis, Structure, and Reactivity ofbis(1,2,4-tri-t-butylcyclopentadienyl) Complexes of Cerium

Description: The sterically demanding 1,2,4-tri-t-butylcyclopentadienylligand (1,2,4-(Me3C)3C5H2, hereafter Cp') has been used to preparemonomeric cerium metallocenes, Cp 2CeX (X = Cl, I, OSO2CF3), which areused to synthesize the benzyl, Cp'2CeCH2C6H5. The benzyl is a usefulstarting material for preparing other complexes in the Cp'2CeZ system (Z= BF4, F, NH2, C6H5, H). X-ray crystal structures of Cp'2CeOSO2CF3,Cp'2CeF, Cp'2CeCH2C6H5, and Cp'2CeH are presented. The benzyl slowlydecomposes in solution to toluene and a metallacycle,[Cp'][(Me3C)2C5H2(CMe2CH2)]Ce. The ring CMe3 groups of both themetallacycle and the hydride, Cp'2CeH, can be fully deuterated byprolonged exposure to C6D6, providing a useful labeling tool inmechanistic studies.The hydride activates C-F and/or C-H bonds influorobenzenes, C6HxF6-x , x = 0-5. The reactions are selective, with theselectivity depending on the presence of two fluorines ortho to thereaction site more than on the type of bond activated. Complexes of thetype Cp'2CeC6HxF5-x , x = 0-4, are formed as intermediates, which slowlydecompose in solution to Cp'2CeF and fluorobenzynes, C6HxF4-x, x = 0-4,which are trapped. The rate at which Cp'2CeC6HxF5-x complexes decomposeincreases as the number of fluorines decreases. Complexes with oneortho-fluorine decompose much faster than those with two ortho-fluorines.The metallacycle activates only C-H bonds in fluorobenzenes, permittingthe synthesis of specific Cp'2CeC6HxF5-x complexes. The crystal structureof Cp'2CeC6F5 is presented. The hydride and the metallacycle react withfluoromethanes, CH4-xFx, x = 1-3, through postulated Cp'2CeCH3-xFxintermediates to generate Cp'2CeF and other products. The other products,CH4, tri-t-butylbenzenes, tri-t-butylfluorobenzenes, and a presumedmetallocene cerium fluoride with one Cp' and one (Me2EtC)(Me3C)2C5H2ligand, suggest a decomposition pathway for Cp'2CeCH3-xFx , x = 1-3, thatinvolves carbenes or carbenoids, which are trapped. The hydridepolymerizes ethylene, but hydrogenates other olefins. The metallacycleactivates C-H bonds in olefins and aromatics to generate new complexeswith Ce-C bonds. The hydride reacts with one equivalent of CO in pentaneto generate (Cp'2Ce)2CH2O, whose crystal structure shows the presence ofa bridging dianionic formaldehyde ligand. (Cp'2Ce)2CH2O reacts H2 ...
Date: May 19, 2005
Creator: Werkema, Evan L.
Partner: UNT Libraries Government Documents Department