This thesis determines what, if any, measurements of aerosol properties made at the Earth surface are representative of those within the entire air column. Data from the Atmospheric Radiation Measurement site at the Southern Great Plains, the only location in the world where ground-based and in situ airborne measurements are routinely made. Flight legs during the one-year period from March 2000 were categorized as either within or above the atmospheric boundary layer (ABL) by use of an objective mixing height determination technique. Correlations between aerosol properties measured at the surface and those within and above the ABL were computed. Aerosol extensive and intensive properties measured at the surface were found representative of values within the ABL, but not of within the free atmosphere.

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 …

The Neel temperatures, T{sub N}, of Tb{sub x}Er{sub 1-x}Ni{sub 2}B{sub 2}C samples have been determined from the temperature dependence of magnetization measurements. A breakdown of the de Gennes scaling of T{sub N} with a clear turning point around x = 0.45 has been observed. The T{sub N} values of Tb{sub x}Er{sub 1-x}Ni{sub 2}B{sub 2}C do not change much within the range of O < x < 0.45 and then, for larger x they increase almost linearly with concentration until T{sub N} = 14.9K is reached for x = 1, TbNi{sub 2}B{sub 2}C. The clear change in the x-dependence of T{sub N} around x = 0.45 can be linked to a change in the local moment ordering direction from transverse to longitudinal, a change which is consistent with recent resonant X-ray scattering data. These features in T{sub N}(x) can be explained using a mean field model.

In the fit part, the Compact Muon Solenoid (CMS) forward calorimeter design studies are presented. The forward calorimeter consists of quartz fibers embedded in a steel absorber. Radiation damage studies of the quartz fiber and the absorber as well as the results of the first pre-production prototype PPP-I are presented. In the second part, the {Omega}{sub c}{sup 0}search studies at the SELEX (E781) experiment at FermiLab are presented. 107 {+-} 22 {Omega}{sub c}{sup 0} events are observed in three decay modes. The relative branching ratio ({Omega}{sub c}{sup 0} {yields} {Omega}{sup -}{pi}{sup -}{pi}{sup +}{pi}{sup +})/{Beta}({Omega}{sub c}{sup 0} {yields} {Omega}{sup -}{pi}{sup +}) is measured as 2.00 {+-} 0.45(stat) {+-} 0.32(sys).

This thesis reports the results from the theoretical investigations, both numerical and analytical, of collisionless relaxation phenomena in beam-plasma systems. Many results of this work can also be applied to other lossless systems of plasma physics, beam physics and astrophysics. Different aspects of the physics of collisionless relaxation and its modeling are addressed. A new theoretical framework, named Coupled Moment Equations (CME), is derived and used in numerical and analytical studies of the relaxation of second order moments such as beam size and emittance oscillations. This technique extends the well-known envelope equation formalism, and it can be applied to general systems with nonlinear forces. It is based on a systematic moment expansion of the Vlasov equation. In contrast to the envelope equation, which is derived assuming constant rms beam emittance, the CME model allows the emittance to vary through coupling to higher order moments. The CME model is implemented in slab geometry in the absence of return currents. The CME simulation yields rms beam sizes, velocity spreads and emittances that are in good agreement with particle-in-cell (PIC) simulations for a wide range of system parameters. The mechanism of relaxation is also considered within the framework of the CME system. It …

Neutron generators based on the {sup 2}H(d,n){sup 3}He and {sup 3}H(d,n){sup 4}He fusion reactions are the most commonly available neutron sources. The applications of current commercial neutron generators are often limited by their low neutron yield and their short operational lifetime. A new generation of D-D/D-T fusion-based neutron generators has been designed at Lawrence Berkeley National Laboratory (LBNL) by using high current ion beams hitting on a self-loading target that has a large surface area to dissipate the heat load. This thesis describes the rationale behind the new designs and their potential applications. A survey of other neutron sources is presented to show their advantages and disadvantages compared to the fusion-based neutron generator. A prototype neutron facility was built at LBNL to test these neutron generators. High current ion beams were extracted from an RF-driven ion source to produce neutrons. With an average deuteron beam current of 24 mA and an energy of 100 keV, a neutron yield of >10{sup 9} n/s has been obtained with a D-D coaxial neutron source. Several potential applications were investigated by using computer simulations. The computer code used for simulations and the variance reduction techniques employed were discussed. A study was carried out to …

The goal of this thesis is to determine under what conditions, if any, measurements of aerosol properties made at the Earth's surface are representative of aerosol properties within the column of air above the surface. This thesis will use data from the Atmospheric Radiation Measurement (ARM) site at the Southern Great Plains (SGP) which is the only location in the world where ground-based and in situ airborne measurements are made on a routine basis. All flight legs in the one-year period from March 2000-March 2001 were categorized as either within or above the atmospheric boundary layer using an objective mixing height determination technique. The correlations between the aerosol properties measured at the surface and the measured within and above the ABL were then computed. The conclusion of this comparison is that the aerosol extensive and intensive properties measured at the surface are representative of values within the ABL, but not within the free atmosphere.

GAMESS, a quantum chetnistry program for electronic structure calculations, has been freely shared by high-performance application scientists for over twenty years. It provides a rich set of functionalities and can be run on a variety of parallel platforms through a distributed data interface. While a chemistry computation is sophisticated and hard to develop, the resource sharing among different chemistry packages will accelerate the development of new computations and encourage the cooperation of scientists from universities and laboratories. Common Component Architecture (CCA) offers an enviromnent that allows scientific packages to dynamically interact with each other through components, which enable dynamic coupling of GAMESS with other chetnistry packages, such as MPQC and NWChem. Conceptually, a cotnputation can be constructed with "plug-and-play" components from scientific packages and require more than componentizing functions/subroutines of interest, especially for large-scale scientific packages with a long development history. In this research, we present our efforts to construct cotnponents for GAMESS that conform to the CCA specification. The goal is to enable the fine-grained interoperability between three quantum chemistry programs, GAMESS, MPQC and NWChem, via components. We focus on one of the three packages, GAMESS; delineate the structure of GAMESS computations, followed by our approaches to its component …

This dissertation contains five papers in the format required for journal publication which describe (in part) my research accomplishments as a graduate student at Iowa State University. This work can be broadly categorized as the binding of weakly-coordinating ligands to cationic organometallic ruthenium fragments, and consists of two main areas of study. Chapters 2-4 are investigations into factors that influence the binding of dibenzothiophenes to {l_brace}Cp'Ru(CO){sub 2}{r_brace}{sup +} fragments, where Cp' = {eta}{sup 5}-C{sub 5}H{sub 5} (Cp) and {eta}{sup 5}-C{sub 5}Me{sub 5} (Cp*). Chapters 5 and 6 present the synthesis and structural characterization of complexes containing corannulene buckybowls that are {eta}{sup 6}-coordinated to {l_brace}Cp*Ru{r_brace}{sup +} fragments. The first chapter contains a brief description of the difficulty in lowering sulfur levels in diesel fuel along with a review of corannulene derivatives and their metal complexes. After the final paper is a short summary of the work herein (Chapter 7). Each chapter is independent, and all equations, schemes, figures, tables, references, and appendices in this dissertation pertain only to the chapter in which they appear.

Photonic band gap (PBG) crystals are periodic dielectric structures that manipulate electromagnetic radiation in a manner similar to semiconductor devices manipulating electrons. Whereas a semiconductor material exhibits an electronic band gap in which electrons cannot exist, similarly, a photonic crystal containing a photonic band gap does not allow the propagation of specific frequencies of electromagnetic radiation. This phenomenon results from the destructive Bragg diffraction interference that a wave propagating at a specific frequency will experience because of the periodic change in dielectric permitivity. This gives rise to a variety of optical applications for improving the efficiency and effectiveness of opto-electronic devices. These applications are reviewed later. Several methods are currently used to fabricate photonic crystals, which are also discussed in detail. This research involves a layer-by-layer micro-transfer molding ({mu}TM) and stacking method to create three-dimensional FCC structures of epoxy or titania. The structures, once reduced significantly in size can be infiltrated with an organic gain media and stacked on a semiconductor to improve the efficiency of an electronically pumped light-emitting diode. Photonic band gap structures have been proven to effectively create a band gap for certain frequencies of electro-magnetic radiation in the microwave and near-infrared ranges. The objective of this …

The top quark is by far the heaviest known fundamental particle with a mass nearing that of a gold atom. Because of this strikingly high mass, the top quark has several unique properties and might play an important role in electroweak symmetry breaking - the mechanism that gives all elementary particles mass. Creating top quarks requires access to very high energy collisions, and at present only the Tevatron collider at Fermilab is capable of reaching these energies. Until now, top quarks have only been observed produced in pairs via the strong interaction. At hadron colliders, it should also be possible to produce single top quarks via the electroweak interaction. Studies of single top quark production provide opportunities to measure the top quark spin, how top quarks mix with other quarks, and to look for new physics beyond the standard model. Because of these interesting properties, scientists have been looking for single top quarks for more than 15 years. This thesis presents the first discovery of single top quark production. An analysis is performed using 2.3 fb{sup -1} of data recorded by the D0 detector at the Fermilab Tevatron Collider at centre-of-mass energy {radical}s = 1.96 TeV. Boosted decision trees are …

Longitudinal compression of space-charge dominated beams can be achieved by imposing a head-to-tail velocity tilt on the beam. This tilt has to be carefully tailored, such that it is removed by the longitudinal space-charge repulsion by the time the beam reaches the end of the drift compression section. The transverse focusing lattice should be designed such that all parts of the beam stay approximately matched, while the beam smoothly expands transversely to the larger beam radius needed in the final focus system following drift compression. In this thesis, several drift compression systems were designed within these constraints, based on a given desired pulse shape at the end of drift compression systems were designed within these constraints, based on a given desired pulse shape at the end of drift compression. The occurrence of mismatches due to a rapidly increasing current was analyzed. In addition, the sensitivity of drift compression to errors in the initial velocity tilt and current profile was studied. These calculations were done using a new computer code that accurately calculates the longitudinal electric field in the space-charge dominated regime.

Current theories have been successful in explaining many nonlinear optical experiments in undoped semiconductors. However, these theories require a ground state which is assumed to be uncorrelated. Strongly correlated systems of current interest, such as a two dimensional electron gas in a high magnetic field, cannot be explained in this manner because the correlations in the ground state and the low energy collective excitations cause a breakdown of the conventional techniques. We perform ultrafast time-resolved four-wave mixing on $n$-modulation doped quantum wells, which contain a quasi-two dimensional electron gas, in a large magnetic field, when only a single Landau level is excited and also when two levels are excited together. We find evidence for memory effects and as strong coupling between the Landau levels induced by the electron gas. We compare our results with simulations based on a new microscopic approach capable of treating the collective effects and correlations of the doped electrons, and find a good qualitative agreement. By looking at the individual contributions to the model, we determine that the unusual correlation effects seen in the experiments are caused by the scattering of photo-excited electron-hole pairs with the electron gas, leading to new excited states which are not …

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 …

Electrochemically modulated liquid chromatography (EMLC) employs a conductive material as both a stationary phase for chromatographic separations and as a working electrode for performing electrochemistry experiments. This dual functionality gives EMLC the capacity to manipulate chromatographic separations by changing the potential applied (E{sub app}) to the stationary phase with respect to an external reference. The ability to monitor retention as a function of E{sub app} provides a means to chromatographically monitor electrosorption processes at solid-liquid interfaces. In this dissertation, the retention mechanism for EMLC is examined from the perspective of electrical double layer theory and interfacial thermodynamics. From the chromatographic data, it is possible to determine the interfacial excess ({Lambda}) of a solute and changes in interfacial tension (d{gamma}) as a function of both E{sub app} and the supporting electrolyte concentration. Taken together, these two experimentally manipulated parameters can be examined within the context of the Gibbs adsorption equation to delineate the contribution of a variety of interfacial properties, including the charge of solute on the stationary phase and the potential of zero charge (PZC), to the mechanism behind EMLC-based retention. The chromatographic probing of interfacial phenomena is complemented by electroanalytical experiments that exploit the ability to monitor the electronic …

The case-hardening process modifies the near-surface permeability and conductivity of steel, as can be observed through changes in alternating current potential drop (ACPD) along a rod. In order to evaluate case depth of case hardened steel rods, analytical expressions are derived for the alternating current potential drop on the surface of a homogeneous rod, a two-layered and a three-layered rod. The case-hardened rod is first modeled by a two-layer rod that has a homogeneous substrate with a single, uniformly thick, homogeneous surface layer, in which the conductivity and permeability values differ from those in the substrate. By fitting model results to multi-frequency ACPD experimental data, estimates of conductivity, permeability and case depth are found. Although the estimated case depth by the two-layer model is in reasonable agreement with the effective case depth from the hardness profile, it is consistently higher than the effective case depth. This led to the development of the three-layer model. It is anticipated that the new three-layered model will improve the results and thus makes the ACPD method a novel technique in nondestructive measurement of case depth. Another way to evaluate case depth of a case hardened steel rod is to use induction coils. Integral form …

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 …

Selecting the model is an important and essential step in model based fault detection and diagnosis (FDD). Several factors must be considered in model evaluation, including accuracy, training data requirements, calibration effort, generality, and computational requirements. All modeling approaches fall somewhere between pure first-principles models, and empirical models. The objective of this study was to evaluate different modeling approaches for their applicability to model based FDD of vapor compression air conditioning units, which are commonly known as chillers. Three different models were studied: two are based on first-principles and the third is empirical in nature. The first-principles models are the Gordon and Ng Universal Chiller model (2nd generation), and a modified version of the ASHRAE Primary Toolkit model, which are both based on first principles. The DOE-2 chiller model as implemented in CoolTools{trademark} was selected for the empirical category. The models were compared in terms of their ability to reproduce the observed performance of an older chiller operating in a commercial building, and a newer chiller in a laboratory. The DOE-2 and Gordon-Ng models were calibrated by linear regression, while a direct-search method was used to calibrate the Toolkit model. The ''CoolTools'' package contains a library of calibrated DOE-2 curves …

This dissertation describes a test of the Standard Model (SM) of particle physics by measuring the probability, or cross section, of simultaneously producing a W boson and a Z boson from proton-antiproton collisions. The SM predicts the cross section of WZ production to be 3.68 {+-} 0.25 pb. The SM and physics of WZ production are described in Chapter 2 of this dissertation. The 1.96 TeV center-of-mass energy proton-antiproton collisions are provided by the Fermi National Accelerator Laboratory (FNAL) Tevatron Collider. The W and Z particles are detected using the D0 detector, which is described in Chapter 3. The data were collected by the detector during 2002-2006 corresponding to 1 fb{sup -1} of p{bar p} collisions. This data set is described in Chapter 6. The measurement uses the trilepton (e{nu}ee, {mu}{nu}ee, e{nu}{mu}{mu}, and {mu}{nu}{mu}{mu}) decay channels, in which a W decays to a charged lepton plus a neutrino and a Z decays to a pair of charged leptons. The W and Z particle selection criteria, detection efficiency, and background determination are described in Chapter 7. We observe 13 candidate events in 1 fb{sup -1} of p{bar p} collisions. In this data set we expect to see 4.5 {+-} 0.6 background …

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 …

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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, …

Motor vehicles are a significant source of population exposure to air pollution. Focusing on California's South Coast Air Basin as a case study, the author combines ambient monitoring station data with hourly time-activity patterns to determine the population intake of motor vehicle emissions during 1996-1999. Three microenvironments are considered wherein the exposure to motor vehicle emissions is higher than in ambient air: in and near vehicles, inside a building that is near a freeway, and inside a residence with an attached garage. Total motor vehicle emissions are taken from the EMFAC model. The 15 million people in the South Coast inhale 0.0048% of primary, nonreactive compounds emitted into the basin by motor vehicles. Intake of motor vehicle emissions is 46% higher than the average ambient concentration times the average breathing rate, because of microenvironments and because of temporal and spatial correlation among breathing rates, concentrations, and population densities. Intake fraction (iF) summarizes the emissions-to-intake relationship as the ratio of population intake to total emissions. iF is a population level exposure metric that incorporates spatial, temporal, and interindividual variability in exposures. iFs can facilitate the calculation of population exposures by distilling complex emissions-transport-receptor relationships. The author demonstrates this point by predicting …

The authors develop a family of fast methods approximating the solution to a wide class of static Hamilton-Jacobi partial differential equations. These partial differential equations are considered in the context of control-theoretic and front-propagation problems. In general, to produce a numerical solution to such a problem, one has to solve a large system of coupled non-linear discretized equations. The techniques use partial information about the characteristic directions to de-couple the system. Previously known fast methods, available for isotropic problems, are discussed in detail. They introduce a family of new Ordered Upwinding Methods (OUM) for general (anisotropic) problems and prove convergence to the viscosity solution of the corresponding Hamilton-Jacobi partial differential equation. The hybrid methods introduced here are based on the analysis of the role played by anisotropy in the context of front propagation and optimal trajectory problems. The performance of the methods is analyzed and compared to that of several other numerical approaches to these problems. Computational experiments are performed using test problems from control theory, computational geometry and seismology.