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Title: Structural Studies of Degradation Mechanism of Lithium Rich Manganese, Nickel, and Iron Based Cathodes
Creator: Aryal, Shankar
Date: 2018
Description: Layered oxide compounds are superior with respect to discharge voltage and discharge specific capacity compared to other families of cathodes....
Show moreLayered oxide compounds are superior with respect to discharge voltage and discharge specific capacity compared to other families of cathodes. Therefore, LiCoO2 and LiMnxNiyCozO2, are the most commonly used cathodes since the commercialization of lithium ion battery. Recently, Li rich Ni, Mn, and Co oxide composite cathodes have been introduced with some improvements. As Co is toxic and expensive, attempts have been made to replace Co with cheap and environmentally friendly Fe. This dissertation reports that comparable discharge specific capacity and discharge voltage can be achieved by replacing Co with Fe and optimizing the composition of Mn, Ni, and Fe. However, the capacity and voltage fading on cycling are still remaining challenges. Structural change on electrochemical cycling is the main reason behind this fading. X-ray absorption spectroscopy (XAS), the specific element probe technique to study local structure and X-ray diffraction (XRD) to study the crystallographic phase information are utilized to understand the degradation/aging mechanism. A series of Li rich Mn, Ni, and Fe oxide composite cathode materials Li1.2Mn(0.30+x)Ni(0.40-x)Fe0.10O2 for x = 0, 0.05, 0.10, 0.15, 0.20 and 0.25 were prepared using a sol-gel synthesis method. Rhombohedral and monoclinic crystal phases are found in Li rich Mn, Ni, and Fe composite oxide materials, but pure rhombohedral phase cannot be obtained without excess Li in the stoichiometric LiMO2 form. The pure monoclinic phase Li2MnO3 is also synthesized to confirm its presence in the composite oxide cathodes. Particle size and surface morphology are studied with scanning electron microscopy. The composite cathodes are cycled to over 100 cycles at 0.3C, for C = 250 mAhg-1 rate. XAS before and after 100 electrochemical cycles of Li rich Mn-Ni-Fe based cathodes is reported for the first time. The determination of fractional contents of monoclinic and rhombohedral phases in the composite oxide cathodes is not possible by powder XRD analysis, however, Li2MnO3 content decreases on decreasing Mn content and on increasing Ni content. The composition with higher Ni content has a higher degree of cation mixing. The synergistic effect of rhombohedral and monoclinic phases in Li rich Mn, Ni, and Fe based cathode is critical for stable electrochemical performance. The Li1.2Mn0.50Ni0.20Fe0.10O2 cathode showed the most stable cyclability performance (194 mAhg-1 first discharge capacity with 94 % capacity retention after 100 cycles at 0.3C rate) however, Li1.2Mn0.40Ni0.30Fe0.10O2 (220 mAhg-1 first discharge capacity with 57 % capacity retention) and Li1.2Mn0.55Ni0.15Fe0.10O2 (241 mAhg-1 first discharge capacity with 68 % capacity retention) cathodes showed higher 1st discharge capacity but poor cyclability under the same charge/discharge cycling.The XAS at Mn K-edge is used to explain the mechanism of Li2MnO3 activation for the improved electrochemical performance of Li rich Mn, Ni, and Fe oxide composite cathode, however Li2MnO3 contributed differently in different compositions. Synchrotron XRD and XAS measurements probed the lattice size expansion, which decreases the chemical potential of Li ions in the cathode on cycling leading to lower discharge voltage after cycling.
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Title: A Novel Non-parametric Density Estimation Approach to Measuring Muon Ionization Cooling and Reverse Emittance Exchange in the MICE Experiment
Creator: Mohayai, Tanaz Angelina
Date: 2018
Description: The Muon Ionization Cooling Experiment (MICE) located at Rutherford Appleton Laboratory in the U.K. has demonstrated muon ionization beam...
Show moreThe Muon Ionization Cooling Experiment (MICE) located at Rutherford Appleton Laboratory in the U.K. has demonstrated muon ionization beam cooling for the first time. A beam of muons in MICE is produced from high-energy proton beam collision with a fixed target, generating pions which in turn decay into muons. Pion-decay muons, thus, are tertiary particles and, as a result, occupy a large volume in position‒momentum phase space. To fit the muon beam into smaller and more cost-effective accelerating devices, muon beam phase‒space volume needs to be reduced (beam cooling). Ionization beam cooling, which before MICE has never been demonstrated experimentally for muons, is the only technique fast enough to be used for muons within their short lifetime. Ionization cooling occurs when muons traverse an absorbing material and lose momentum through ionization energy loss. The cooling effect in MICE is measured using two scintillating-fiber tracking detectors. These trackers, one upstream and one downstream of the absorber, reconstruct and measure the position and momentum coordinates of each muon. Given the precision MICE needed to demonstrate beam cooling, it is necessary to develop analysis tools that can account for any effects that may lead to inaccurate measurement of cooling, such as non‒linear effects in beam optics. Non‒parametric density estimation techniques, such as kernel density estimation (KDE), provide a basis for creating analysis tools that are robust against these effects, directly calculating the muon beam phase-space density and volume for demonstrating beam cooling. This thesis focuses on the application of KDE to the measurement of beam cooling in MICE. The KDE technique is validated using known distributions and is applied to simulated and experimental MICE data corresponding to the various magnet, optics, and absorber configurations. Using the KDE technique, muon beam cooling in the four‒dimensional transverse phase space, as well as reverse emittance exchange using MICE data have been demonstrated.
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Title: Physicochemical Characterization of the SiC Barrier Layer of Irradiated TRISO Fuel
Creator: Seibert, Rachel
Date: 2018
Description: Tristructural-isotropic (TRISO) nuclear fuel is designed to be an inherently safe microencapsulated fuel for use in advanced nuclear reactors...
Show moreTristructural-isotropic (TRISO) nuclear fuel is designed to be an inherently safe microencapsulated fuel for use in advanced nuclear reactors. TRISO fuel is comprised of an uranium-carbide/uranium-oxide mixed kernel, surrounded subsequently by a porous carbon buffer layer, pyrolytic carbon, silicon carbide, and pyrolytic carbon. The silicon carbide layer acts as both the structural backbone and the main barrier to non-gaseous fission product release from the kernel. During operation, fission products are known to release from intact fuel (silver) and to locally corrode the silicon carbide layer (palladium). Release of silver can pose a threat to safety and maintenance workers due to plate-out on reactor components, while palladium corrosion leads the possibility of failure of the SiC layer. An understanding of the silver release mechanism, the diffusion of palladium and fuel kernel components, and their possible correlation is necessary to understand envelopes for safe operation using these fuels.This work focuses on analysis of the reactivity of silver, palladium, and fissile inventory with silicon carbide to determine potential mechanisms and interactions. Irradiated TRISO particles and model thin film cubic silicon carbide (3C-SiC) surfaces were studied to compare and understand the reaction mechanisms of these fission products. Analysis on both systems involved X-ray Absorption Fine Structure Spectroscopy (XAFS) measurements to determine the local atomic structure of the bulk material and electron microscopy studies to observe the microstructure and fission product location. Additionally, x-ray photoelectron spectroscopy (XPS) was used to study the fundamental surface science of silver and palladium in the 3C-SiC thin films. From the comparative studies in this work, the interaction of silver, palladium, and fuel kernel products has been observed. Palladium silicides are preferentially formed, but silver remains metallic and diffuses through both bulk SiC, through material defects, and through grain boundary diffusion. Uranium preferentially forms carbides with increasing temperature. Plutonium primarily forms silicides, but with short carbon bonds. All fission products and fissile inventory were observed to be segregated along grain boundaries in the SiC. This work did not measure a single release mechanism, but suggests multiple mechanisms work together simultaneously. It also presents the first evidence of uranium carbide formation at elevated temperatures and of silver as a metal in irradiated TRISO fuel, to the best of the author's knowledge.
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Title: IRREGULAR GROWTH AND INTERFACIAL EFFECT IN THIN FILM MULTILAYER STRUCTURES FOR USES IN PHOTOCATHODE APPLICATIONS
Creator: Lee, ZhengRong
Date: 2021
Description: Improving photocathode performance by increasing the electron density while lowering the angular spread of emitted electrons can improve...
Show moreImproving photocathode performance by increasing the electron density while lowering the angular spread of emitted electrons can improve particle accelerator performance, expanding the reach of both fundamental and applied science. Materials science expertise is needed to design new photocathodes with these desired properties. Nemeth, et al, determined that a multilayered photocathode structure consisting of MgO/Ag/MgO could be engineered for higher brightness and lower dispersion [Nemeth, et al, Phys. Rev. Lett. 104, 046801 (2010)]. The dispersion of the surface bands impacts the angular spread of the emitted beam, and the model predicted that the bands could be tuned by precisely controlling the layer thicknesses of the multilayer structure. We synthesized and probed this MgO/Ag/MgO system experimentally. We measured the work function, emittance, and quantum efficiency of multilayer photocathodes with different MgO layer thicknesses to compare with theoretical predictions. We observed that although the general trend was as predicted, the measurements and the model were not in exact agreement [Velasquez, et al, Appl. Surf. Sci. 360, 762 (2016)]. In this work, we have undertaken a study of the electronic structure of the interfaces to explore how these observed deviations may have originated. It is possible that the fabrication process leads to non-ideal interfaces compared to those constructed in the simulations. To study how the fabrication affects the interfaces, hard X-ray photoemission spectroscopy(HAXPES) was used to probe the chemistry of the buried interfaces within the thin film multilayer structure of Ag and MgO. In these multilayer structures, we observed that the silver layers were predominantly metallic. A small high binding energy (ΔE = 0.69 eV) peak was also observed in the Ag 3d core level in the samples. This peak is shifted in the opposite direction of the binding energy shift in silver oxides, suggesting that this peak is not due to the formation of silver oxides at the interfaces with the MgO. Two possible explanations for the origin of this peak then are charge transfer at the interface from the Ag to the oxide monolayer or the formation of silver nanoparticles during the growth process. Based upon simple depth profiling analysis, we postulate the former is the more likely explanation. In addition, the O 1s and Mg 1s core level indicated the presence of Mg(OH)2. The MgO layers react with H2O in the vacuum chamber or ideal gas used as a buffer during sample transfer. Since the theory predicts a strong dependence upon the number of MgO layers surrounding the Ag, the formation of Mg(OH)2 likely contributes to the non- ideal behavior, even given the similarity in the electronic structure to MgO (large band gap insulator) and Mg(OH)2. The speed at which this reaction occurs would significantly limit the lifetime and the utility of the MgO/Ag multilayer photocathodes. In order to custom engineer multilayer photocathodes, complete control over the growth process will be needed to ensure that the ideal surfaces are formed. Using non-reactive materials would greatly increase the lifetime of the engineered photocathodes.
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Title: INVESTIGATION OF STRUCTURE AND PROCESSING EFFECTS ON THE ELECTROCHEMICAL PERFORMANCE OF COBALT-FREE, LITHIUM- AND MANGANESE-RICH LAYERED OXIDE CATHODE FOR LIBS
Creator: Kucuk, Kamil
Date: 2021
Description: Rechargeable Li-ion batteries (LIBs) have been widely used in a diverse range of energy storage systems because of their high energy and power...
Show moreRechargeable Li-ion batteries (LIBs) have been widely used in a diverse range of energy storage systems because of their high energy and power density, low self-discharge, and tolerable memory effect, compared to the conventional alkaline, lead acid, and nickel-cadmium (Ni/Cd) batteries. [2] Since not only cathodes materials control the energy density of a cell, but also the capacity of cathode material characteristically restricts the cell capacity (as well as about 40% of the cell cost results from the cost of cathode raw materials), the majority of studies on LIBs have been carried out on developing alternative cathodes with higher energy, lower cost, and more environmentally friendliness. [2], [3] From this perspective, both Co-free and lithium- & manganese-rich (LMRO) layered oxide MNF cathodes, Li1.2(MnxNiyFez)O2, have recently attracted great attention in lithium-ion battery (LIB) research for electric vehicles and energy storage devices due to their high capacities of over 250 mAhg−1 and being eco-friendly and inexpensive compared to the cobalt-based Li-rich Li1.2(NixMnyCoz)O2 and Ni-rich Li(NixMnyCoz)O2 (NMC), and LiCoO2 commercial cathodes. Replacing toxic and expensive Co in the LMRO cathodes with environmentally friendly and much cheaper Fe element has been extensively studied over the last two decades. It was suggested by Aryal, S. et. al., in 2018. [4] that the Li1.2(Mn0.50Ni0.20Fe0.10)O2 (MNF502010) Co-free LMRO MNF cathodes seem better in terms of capacity-retention with higher discharge capacity and less voltage fade compared to other MNF compositions. However, the MNF502010 cathode still suffers from its lower experimental capacity, compared to its expected theoretical capacity (270-455 mAhg−1), as well as capacity decay, voltage fade, poor rate capability, and thermal instability. In this dissertation, it is reported that comparable specific discharge capacity with less amount of voltage fading and capacity decay can be achieved by fluorine doping, synthesizing materials in large amounts (0.1 mol synthesis at least) with two-step firing, and then washing the obtained nanocomposites with H3PO4 to create Li3PO4 layer on the surface of bulk MNF composites. The specific discharge capacity and cycling performance of the Co-free MNF502010 cathodes were studied and enhanced by using and optimizing these approaches in this work for the first time. However, voltage fading and capacity decay are still remaining challenges, even if they are remarkably mitigated by applying these approaches. Structural changes due to layered to spinel transformation, less amount of monoclinic phase activation leading to structural deformation occurring after 1st charge, dissolution of the transition metals (TM), and oxygen release (loss of lattice oxygen) from the MNF material upon following electrochemical cycling at higher voltage (≥ 4.5V ) seem the main reasons behind these challenges, specifically the voltage fading and capacity decay.A series of fluorine-doped/undoped, Co-free MNF502010 nanocomposite cathode materials (Li1.2(Mn0.50Ni0.20Fe0.10)O2(1−x)F2x, briefly F-doped MNF) were synthesized by using a sol-gel technique. Firstly (Chapter 4), the fluorine was substituted for oxygen in the parent MNF compound in different fractions (0.00, 0.025, 0.05,0.075, 0.10, which means 0%, 2.5%, 5.0%, 7.5%, and 10%), in order to optimize the amount of fluorine for better performance; secondly (Chapter 5), a large batch (0.1mol, 10 times more than the previous batch) of 5%F-doped material was prepared by a modified sol-gel synthesis which is modified by heating at 700 ◦C for different time-periods; 7.5 hours (7.5h), 15 hours (15h, two-step firing, 7.5h + rest for 12h + 7.5h), instead of heating directly 15 hours (d15h), as done in the first chapter; finally (Chapter 6), H3PO4 treatment resulting in a non-uniform Li3PO4 layer on the bulk surface. These approaches were respectively applied on doped/undoped MNF502010 nano-composites, in order to overcome the challenges already mentioned above. Finally, the effects of these approaches on the structural, morphological, and electrochemical properties of MNF cathode materials were investigated by means of powder X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM) with energy dispersive X-ray (EDS) analysis, X-ray photoelectron spectroscopy (XPS), cyclic voltammetry (CV), galvanostatic charge-discharge cycling, and X-ray absorption spectroscopy (XAS, an element specific probe technique). Specifically, ex-situ XAS was performed at the Mn, Ni, and Fe K-edge and used to detect the changes both in the oxidation state of the transition metal (TM) ions and their local environments in order to get a better understanding of the improved performance of the composite materials, as well as their failure mechanism. Moreover, the EXAFS data were modeled to gain insight into the influence of these approaches on the electrochemical performance of both pristine (uncycled) and cycled electrodes (after the 100th discharge). From correlating the electrochemical performance of the modified/unmodified MNF nano-composite cathodes to their XANES and EXAFS analysis, the ability to achieve higher specific capacity is strongly dependent on the formation of a well-ordered layered structure and the amount of monoclinic component (Li2MnO3) activation resulting in higher redox-activity of the Mn cations. The long-term cyclability or capacity retention can be enhanced by heating the resulting powders with a two-step firing (instead of directly 15 hours) and washing them with 1wt%H3PO4 solution to create a Li3PO4 conductive and protective layer.
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Title: FIELD EMISSION MITIGATION VIA IN-SITU PLASMA PROCESSING IN 1.3 GIGAHERTZ 9-CELL LCLS-II CAVITIES
Creator: Giaccone, Bianca
Date: 2021
Description: Field emission (FE) is one of the limiting factors in superconducting radiofrequency cavities' performance. It is known that even a few...
Show moreField emission (FE) is one of the limiting factors in superconducting radiofrequency cavities' performance. It is known that even a few monolayers of surface adsorbed contaminants can lower the niobium work function and increase the FE. In order to address the field emission that may arise once the accelerator is already assembled, it was decided to develop plasma processing for the Linac Coherent Light Source II, a method to mitigate field emission in-situ. Starting from Doleans's successful experience with plasma processing for high beta cavities, Fermi National Accelerator Laboratory is developing plasma cleaning for TESLA shaped 1.3 GHz 9-cell cavities. A new method of ignition based on the higher order modes and couplers was developed, along with a detection procedure that allows to identify the location of the plasma inside the cavity. In this work are presented the results of plasma processing applied to 1.3 GHz cavities, both single-cell and 9-cells. The cavities were contaminated with multiple sources, naturally or artificially, and their performance was measured through cryogenic RF tests before and after plasma cleaning. These experiments proved that plasma processing successfully removed hydrocarbon-related field emission from cavities artificially contaminated, but also from a cavity with natural and unknown FE source. In some cases of more extreme contamination through vacuum failure simulation conducted in air (not in a cleanroom), plasma processing was not able to recover the cavity's performance. An ongoing analysis of the cavity contaminants is presented here, explaining the reason why some contaminated cavities showed little improvement after plasma processing. A microscopic study of the effect of plasma processing on the niobium surface is also presented. Niobium samples prepared with different surface treatments were analyzed using X-ray photoelectron spectroscopy, scanning electron microscopy and energy-dispersive X-ray spectroscopy. The samples were subjected to plasma processing and analyzed again, in order to draw a comparison and identify possible surface changes caused by the reactive oxygen contained in the glow discharge. The samples were prepared with different surface treatments in order to understand if plasma processing may affect them differently. This study showed a possible increase in the oxide thickness after plasma processing and a reduction of the energy difference between the pentoxide and the metal peaks. In preparation for this study, the near-surface region of one niobium sample was investigated with X-ray photoelectron spectroscopy at various steps of sputtering and subsequent oxide regrowth in air. The results showed that the majority of the oxide is composed of Nb2O5, however, the presence of two suboxides (NbO, NbO2) is observed, plus an additional peak (attributed to Nb2O) measured both during sputtering and oxide regrowth.
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Title: Computational study on the heme scavenging ability of Staphylococcus aureus IsdH receptor: Utilizing molecular dynamics to understand an unknown mechanism
Creator: Clayton, Joseph Alan
Date: 2021
Description: Methicillin-resistant Staphylococcus aureus (MRSA) has become an infamous pathogen with infection rates that have declined slowly in recent...
Show moreMethicillin-resistant Staphylococcus aureus (MRSA) has become an infamous pathogen with infection rates that have declined slowly in recent years. S. aureus requires iron as a metabolic nutrient during infection and obtains this nutrient through an iron-regulated surface-determinant (Isd) system that extracts iron from the host’s heme stored in hemoglobin (Hb) through near iron transporter (NEAT) domains. This work concentrates on studying the second and third NEAT domains of IsdH by utilizing atomistic molecular dynamics to probe the heme scavenging process; in collaboration with the Clubb Group at UCLA, we discover key functional regions of IsdH and describe fundamental interdomain dynamics. In addition, I investigate a conventional computational method to describe protein dynamics and propose an alternative that aims to alleviate computational effort by incorporating experimental data.
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Title: Electron Cloud studies at Fermilab
Creator: Ji, Yichen
Date: 2019
Description: The presence of unwanted electrons in an accelerator vacuum chamber, known as E-cloud (E-cloud) can potentially cause operational problems in...
Show moreThe presence of unwanted electrons in an accelerator vacuum chamber, known as E-cloud (E-cloud) can potentially cause operational problems in the Fermilab Main Injector (MI) and Recycler Ring (RR). E-cloud has caused instability in the RR in the past, and although it is not currently a problem, there is measurable E-cloud in the MI accelerator. There are planned beam intensity increases due to upgrades of the Fermilab accelerator complex, so E-cloud could become a problem. Some work has been done by others previously to understand how low SEY (Secondary Electron Yield coefficient) coatings might mitigate production of E-cloud, and to model the mechanism whereby E-cloud causes beam instability. Using previous studies as a base, this research took several approaches toward understanding the risk of E-cloud at Fermilab. The evolution of the SEY of the SS316L (stainless steel), TiN coated SS316L, and amorphous carbon coated SS316L were measured in-situ using a SEY measurement station in the MI tunnel. The SEY of these materials change over time either due to bombardment of the E-cloud, or disruption of vacuum conditions. The SEY evolution was tracked over a several year period to find out how long it takes for the SEY of each material to reach its lowest level, and how much the SEY rises during deconditioning periods of poor vacuum. The SEY measurement results can be used to determine whether the SS316L will be a problem at upgrade intensities, and if so, whether or not TiN and A-Carbon coatings can mitigate E-cloud related problems sufficiently. Direct measurements of the E-cloud were done as well, and compared to simulation. The E-cloud bombardment rate was measured at different beam intensities and bunch lengths. It was possible to get detailed information on how the E-cloud varies over the acceleration cycle, where sensitivity to bunch length is reflected in the evolution of the E-cloud. The Retarding Field Analyzer (RFA) measuring the E-cloud bombardment rate was near the instrument that is used to measure the SEY of the beam pipe material. This proximity provided an accurate SEY value for simulations, so that the simulated E-cloud bombardment rate could be better compared to measurement. Bunch length measurements and computations generated accurate bunch length information also needed as input for simulations. After this careful control of the input parameters, the POSINST simulations of E-cloud were a good match to direct measurements. This gave confidence that predictions could be made concerning the E-cloud densities at upgrade intensities. These densities were compared against corresponding proton densities to predict the SEY required to avoid instabilities. That prediction and the information provided by the SEY measurements provide helpful information regarding the risks of E-cloud effects at future beam intensities at Fermilab.
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Title: Energy Scale Study for PROSPECT's Measurement of the Antineutrino Spectrum of 235U
Creator: Zhang, Xianyi
Date: 2019
Description: Neutrinos from nuclear fission reactors have been widely studied in particle and nuclear physics. In the last ten years, the antineutrino flux...
Show moreNeutrinos from nuclear fission reactors have been widely studied in particle and nuclear physics. In the last ten years, the antineutrino flux and spectrum were measured independently by short baseline reactor experiments. Both flux and spectrum measurements showed discrepancies compared to theoretical models based on historical measurements and nuclear databases. These discrepancies hint at sterile neutrino oscillation at the eV mass scale, as well as an incomplete theoretical model. PROSPECT, the Precision Reactor Oscillation and Spectrum experiment, was built to probe for sterile neutrino oscillations and precisely measure the reactor antineutrino spectrum from a highly 235U enriched reactor. The PROSPECT antineutrino detector is an optically segmented liquid scintillator detector deployed at seven meters to nine meters from the High Flux Isotope Reactor at Oak Ridge National Laboratory. This dissertation details the analysis to calibrate the energy scale of the PROSPECT antineutrino detector, an essential step for both the oscillation and spectrum measurements. To characterize the nonlinear detector energy response, a unique calibration and analysis strategy was developed to overcome challenges brought on by particle multi-segment scattering within the PROSPECT detector. With the calibrated scale for energy reconstruction, PROSPECT measured of the antineutrino spectrum from a 235U-burning reactor.
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Title: Physics at the MeV-Scale in Liquid Argon Time Projection Chambers
Creator: Lepetic, Ivan Thomas
Date: 2020
Description: The liquid argon time projection chamber (LArTPC) is the detection technology chosen for several Fermilab-based neutrino experiments. This...
Show moreThe liquid argon time projection chamber (LArTPC) is the detection technology chosen for several Fermilab-based neutrino experiments. This technology will be used in studies of neutrino cross-sections and oscillations, neutrinos from supernovae as well as a variety of studies of beyond the Standard Model physics. This thesis explores the use of these detectors to study MeV-scale activity. MeV-scale electrons arising from Compton scatters of deexcitation photons and photons from inelastic neutron scattering in neutrino-nucleus interactions are reconstructed using novel methods presented here. This work represents the first demonstration of MeV-scale physics capabilities in a LArTPC neutrino experiment as well as the first observation of neutrino-produced photons from nuclear de-excitation and inelastic neutron scattering. A search for millicharged particles, postulated by theories of beyond the standard model physics, is also performed using data from a LArTPC and the low-energy reconstruction techniques developed. The results set world-leading bounds on the parameter space of millicharged particles. The work in this thesis demonstrates that studies of MeV-scale activity and new physics are possible with LArTPC technology and provides the foundation for future LArTPC studies of low energy neutrinos and new physics.
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Title: IN SITU X-RAY ABSORPTION SPECTROSCOPY STUDY OF TIN-BASED GRAPHITE COMPOSITE ANODES FOR LITHIUM-ION BATTERIES
Creator: Ding, Yujia
Date: 2019
Description: Sn-based anode materials such as Sn, SnO2, Sn4P3, and SnS2 that exhibit large theoretical capacities are promising alternatives to traditional...
Show moreSn-based anode materials such as Sn, SnO2, Sn4P3, and SnS2 that exhibit large theoretical capacities are promising alternatives to traditional graphite anodes for Li-ion batteries. However, their capacities fade drastically in a few cycles due to substantial volume changes during the lithiation/delithiation process resulting in cracking and pulverization of the electrode. A graphite matrix is introduced by high-energy ball milling to obtain a graphite composite and enhance the electrochemical performance. Indeed, Sn4P3/graphite composite exhibits a reversible capacity of 651 mA h g-1 in the 100th cycle, and SnS2/graphite composite shows 591 mA h g-1 in the 50th cycle.To obtain a better understanding of the improved performance of the composite materials and the reason for the more gradual capacity fading, in situ EXAFS is used to investigate these mechanisms using in situ coin cells and in situ vacuum-sealed pouch cells. The collected EXAFS data were analyzed by modeling to extract detailed local environment changes during the lithiation/delithiation process.In the crystalline phases of Sn-based materials, the conversion reaction forming metallic Sn is partially reversible and partially irreversible, and the subsequent alloying/dealloying reaction forming LiSn alloys is reversible. Introducing the graphite matrix increases electrical conductivity and prevents aggregation of intermediate Sn clusters. The graphite matrix also plays a significant role in transforming composites into highly dispersed amorphous phases. These amorphous phases, formed in the first few cycles of Sn4P3/graphite and SnS2/graphite composites, exhibit excellent reversibility in both conversion and alloying/dealloying reactions, which is the main reason for the significant improvements in electrochemical performance. The slow growth of metallic Sn clusters and the slight reduction in amorphous phases result in gradual capacity loss over long-term cycling. Introducing the graphite matrix and creating highly dispersed composite samples are the successful strategies that can be scaled up to develop new battery materials in the future.
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Title: Proceedings of the XLIII International Symposium on Multiparticle Dynamics
Creator: Chekanov, Sergei, Sullivan, Zack
Date: 2013, 2013-09-15
Publisher: IIT Press
Description: This Proceedings of the XLIII International Symposium on Multiparticle Dynamics (ISMD 2013) contains summaries of some of the outstanding...
Show moreThis Proceedings of the XLIII International Symposium on Multiparticle Dynamics (ISMD 2013) contains summaries of some of the outstanding research presented at the 2013 meeting. The 2013 Symposium was held at the Illinois Institute of Technology (IIT) in Chicago, Illinois over September 15–20. The Symposium was jointly organized by the IIT College of Science and the High Energy Physics Division of Argonne National Laboratory. More than 100 participants from nearly 20 countries participated in the Symposium to review progress and discuss upcoming issues in the fields of high-energy physics, nuclear physics and astrophysics. The International Symposium on Multiparticle Dynamics (ISMD) is a major international high-energy conference which attracts participants with a common interest in reactions involving a large number of particles. From the beginning, the goal was to bring experimentalists and theorists together to discuss all aspects multiparticle dynamics, from new analysis techniques to the latest discoveries.
Sponsorship: IIT College of Science, High Energy Physics Division of Argonne National Laboratory
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Title: Simulation and Experimental Testing of High-Gradient Dielectric Disk Accelerating Cavities
Creator: Weatherly, Sarah K.
Date: 2022
Description: Structure-based wakefield acceleration can be accomplished using either Collinear Wakefield Acceleration (CWA) where the drive beam and the...
Show moreStructure-based wakefield acceleration can be accomplished using either Collinear Wakefield Acceleration (CWA) where the drive beam and the witness beam are located on the same beamline or Two Beam Acceleration (TBA) where the RF power generated by the drive beam is extracted and transferred to the witness beam line. A Dielectric Disk Accelerator (DDA) is an accelerating structure that is utilized by TBA that uses dielectric disks to improve the structure's shunt impedance and accelerate the witness beam. Dielectric based accelerators studied in this thesis are X-Band structures (have a working frequency between 8 and 12 GHz) that can use any pulse length but in this study utilize short (<20 ns) traveling wave pulses. Short pulse lengths are used to decrease breakdown probability and allow for a large gradient. DDAs have a higher group velocity and a larger shunt impedance compared to traditional metallic accelerating structures while maintaining a large accelerating gradient. DDAs are a strong candidate for use in the Argonne Wakefield Accelerator’s 500 MeV Demonstrator. Recent experimental results of a clamped single cell structure demonstrated a >100 MV/m accelerating gradient with no evidence of breakdown in the RF volume. Additional structures, including a brazed single cell model and a multicell structure, have been designed and are now being fabricated for high power testing.
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Title: Advanced methods for storage ring nonlinear beam dynamics design and implementation
Creator: Song, Minghao
Date: 2022
Description: To meet the increasing demands of scientific researchers for brighter photonbeams, storage ring beam emittance is continually pushed down to a...
Show moreTo meet the increasing demands of scientific researchers for brighter photonbeams, storage ring beam emittance is continually pushed down to a new ultra-low level. It, therefore, becomes correspondingly more challenging to ensure such storage rings have good nonlinear beam dynamics performance. This thesis work is focused on developing advanced methods for low emittance storage ring nonlinear beam dynamics design and implementation.Nonlinear beam dynamics optimization is essential to low emittance storagering design. A highly efficient multi-objective optimization algorithm is needed to simultaneously achieve a large dynamic aperture and a large local momentum aperture. Work was done to improve and test a machine learning-based algorithm called multi-generation Gaussian process optimizer (MG-GPO). This advanced method uses constructed GP models to pre-select solutions, and benchmarking of results on toy problems shows that MG-GPO converges significantly faster than traditional algorithms. The MG-GPO algorithm was successfully applied to nonlinear lattice design optimization, for example, to the SPEAR3 upgrade 7-nm lattice, and it was demonstrated to converge faster than NSGA-II and MOPSO. This was due to its capability of selecting candidates that tend to have better performance. This algorithm will help accelerate nonlinear lattice studies.Correction of nonlinear beam dynamics is also important for low emittancestorage ring commissioning and operation. In order to measure and correct features relevant to the nonlinear beam dynamics, an effective method is needed to excite sustained beam oscillations to large amplitude. A method based on the concept of autoresonance was proposed. This advanced technique excites nonlinear transverse beam motion in storage rings by sweeping the drive frequency. The theory for the autoresonance threshold was derived for the nonlinear optics systems in storage rings, both with and without damping effects, using Hamiltonian dynamics. The theoretical predictions for the drive amplitude threshold were found to agree well with simulations for a simple storage ring model, as well as for simulations with the actual SPEAR3 and APS lattices. The theory was also compared favorably to historical data from experiments on SPEAR3. Simulations verified that an oscillation driven by autoresonant excitation matches the character of a free oscillation, so that beam oscillation data taken during the ramping process can confidently be used to characterize the nonlinear beam dynamics performance. The precision of measurements can be improved by using autoresonant excitation since large amplitude beam oscillations are sustained significantly longer. Simulations of autoresonant excitation demonstrated the measurements of the detuning coefficients and resonance driving terms. The use of autoresonant excitation for the detection of faulty magnets and correction of resonance driving terms was also demonstrated.Online optimization is an alternative way to effectively improve nonlinear beamdynamics performance in a real storage ring. The greater efficiency of an advanced optimization algorithm is also needed to find globally optimal solutions in the limited experimental time that is typically available. The MG-GPO algorithm was implemented for SPEAR3 vertical emittance minimization and injection efficiency optimization. Again, the optimized solutions demonstrate that MG-GPO is more efficient than the commonly used PSO algorithm. SPEAR3 performance was successfully improved during the online optimization runs with MG-GPO.
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Title: SYSTEMATIC ANALYSIS OF THE MCENTER BEAMLINE AT THE FERMILAB TEST BEAM FACILITY FOR THE NOVA TEST BEAM EXPERIMENT
Creator: Temizel, Buse Naz
Date: 2021
Description: This thesis presents a systematic analysis of the MCenter beamline at the Fermilab Test Beam Facility to help to generate improved beam...
Show moreThis thesis presents a systematic analysis of the MCenter beamline at the Fermilab Test Beam Facility to help to generate improved beam profiles for the NOvA Test Beam Experiment. Several studies were carried out to understand beam transport to the experiment, including optics calculations and computer simulations using a novel procedure for incorporating the acceptance of the channel. Data from beam profile monitors was used to trace the beam phase space and compared to simulation results. Detailed analysis revealed that the beam sizes on the NOvA target were large compared to its transverse size. New tunes were proposed for a detailed beam optics study. Analysis of the new tunes shows that the new optics produce two components corresponding to two different peaks at different energies in the horizontal profile at the NOvA target.
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Title: Quantum Computation for the Understanding of Mass: Simulating Quantum Field Theories
Creator: Rivero Ramírez, Pedro
Date: 2021
Description: This thesis demonstrates the production of hadron mass on a quantum computer. Working in the Nambu–Jona-Lasinio model in 1+1 dimensions and 2...
Show moreThis thesis demonstrates the production of hadron mass on a quantum computer. Working in the Nambu–Jona-Lasinio model in 1+1 dimensions and 2 flavors, I show a separation of the contribution of quark masses and interactions to the mass. Along the way I develop a new tool called Quantum Sampling Regression (QSR) that allows for an optimal sampling of low qubit quantum computers when using hybrid variational eigenvalue solving techniques. I demonstrate the regime where QSR dominates the current standard Variational Eigensolver Technique, and benchmark it by improving the calculation of deuteron binding energy. Finally, I developed QRAND — a multiprotocol and multiplatform quantum random number generation framework — in support of the quantum computing community.
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Title: MEASUREMENT OF ELECTRON NEUTRINO AND ANTINEUTRINO APPEARANCE WITH THE NOνA EXPERIMENT
Creator: Yu, Shiqi
Date: 2020
Description: As a long-baseline neutrino oscillation experiment, the NuMI Off-axis $\nu_e$ Appearance (NOvA) experiment aims at studying neutrino physics...
Show moreAs a long-baseline neutrino oscillation experiment, the NuMI Off-axis $\nu_e$ Appearance (NOvA) experiment aims at studying neutrino physics by measuring neutrino oscillation parameters using the neutrino flux from the Main Injector (NuMI) beam. It has two functionally identical detectors. The near detector is onsite at Fermi National Accelerator Laboratory. The far detector is 810 km away from the source of neutrinos and antineutrinos, at Ash River, Minnesota. At the near detector, muon neutrinos or antineutrinos, before significant oscillations take place, are used to correct the Monte Carlo simulation. At the far detector, the neutrino and antineutrino fluxes after significant oscillations have happened are measured and analyzed to study neutrino oscillation. The NOvA experiment is sensitive to the values of $\sin^2\theta_{23}$, $\Delta m^2_{32}$, and $\delta_{CP}$. The latest values from the NOvA 2020 analysis are as follows: $\sin^2\theta_{23}=0.57^{+0.03}_{-0.04}$, $\Delta m^2_{32}=(2.41\pm0.07)\times10^{-3}$ eV$^2$/c$^4$, and $\delta_{CP}=0.82\pi$ with a wide 1$\sigma$ interval of uncertainty. My study is focused on the neutrino oscillation analysis with NOvA, including detector light model tuning, particle classification with convolutional neural network, electron neutrino and antineutrino energy reconstruction, and oscillation background estimation. Most of my studies have been used in the latest NOvA publication and the NOvA 2020 analysis.
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Title: Development of a novel ultra-nanocrystalline diamond (UNCD) based photocathode and exploration of its emission mechanisms
Creator: Chen, Gongxiaohui
Date: 2020
Description: High quality electron sources are one of the most commonly used probing tools used for the study of materials. Photoemission cathodes, capable...
Show moreHigh quality electron sources are one of the most commonly used probing tools used for the study of materials. Photoemission cathodes, capable of producing ultra-short and ultra-high intensity beams, are a key component of accelerator based light sources and some microscopy tools. High quantum efficiency (QE), low intrinsic emittance, and long lifetime (or good vacuum tolerance) are three of the most critical features for a photocathode; however, these are difficult to achieve simultaneously and trade-offs need to be made for different applications. In this work, a novel semi-metallic material of nitrogen-incorporated ultrananocrystalline diamond ((N)UNCD) has been studied as a photocathode. (N)UNCD has many of the unique diamond properties, such as low intrinsic as-grown surface roughness (at the order of 10~nm) due to its nanometer scale crystalline size, relatively long lifetime in air, high electrical conductivity with nitrogen doping, and potentially high QE performance due to the high grain boundary densities where most of electron emission occurs. High contrast interference of incident and reflected radiation within (N)UNCD thin films was observed, and this feature allows fast thickness determination based on an analytical optics methodology. This method has been extended to study and calculate the etching rates of two commonly used O$_2$ and H$_2$ plasmas for use with future (N)UNCD microfabrication processes. The mean transverse energy (MTE) of (N)UNCD was determined over a wide UV range in a DC photogun. Unique MTE behavior was observed; it did not scale with photon energy unlike most metals. This behavior is associated with emission from spatially-confined states in the graphite regions (with low electron effective mass) between the diamond grains. Such behavior suggests that beam brightness many be increased by the simple mechanism of increasing the photon energy so that the QE increases, while the MTE remains constant.Two individual (N)UNCD photocathodes synthesized two years apart have been characterized in a realistic RF photogun. Both the QE and intrinsic emittance were characterized. It was found that the QE of $\sim4.0\times 10^{-4}$, is more than an order of magnitude higher than that of most commonly used metal cathodes (such as Cu and Nb). The intrinsic emittance (0.997~$\mu$m/mm) is comparable to that of photocathodes now deployed in research accelerators. The most impressive feature is the excellent robustness of (N)UNCD material; there was no evidence of performance degradation, even after years-long atmospheric exposure. The results of this work demonstrate that a cathode made of (N)UNCD material is able to achieve balanced performance of three of the primary critical photocathode figures-of-merit.
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Title: Systematic Serendipity: A Study in Discovering Anomalous Astrophysics
Creator: Giles, Daniel K
Date: 2020
Description: In the present era of large scale surveys, big data presents new challenges to the discovery process for anomalous data. Advances in astronomy...
Show moreIn the present era of large scale surveys, big data presents new challenges to the discovery process for anomalous data. Advances in astronomy are often driven by serendipitous discoveries. Such data can be indicative of systematic errors, extreme (or rare) forms of known phenomena, or most interestingly, truly novel phenomena which exhibit as-of-yet unobserved behaviors. As survey astronomy continues to grow, the size and complexity of astronomical databases will increase, and the ability of astronomers to manually scour data and make such discoveries decreases. In this work, we introduce a machine learning-based method to identify anomalies in large datasets to facilitate such discoveries, and apply this method to long cadence light curves from NASA's Kepler Mission. Our method clusters data based on density, identifying anomalies as data that lie outside of dense regions in a derived feature space. First we present a proof-of-concept case study and we test our method on four quarters of the Kepler long cadence light curves. We use Kepler's most notorious anomaly, Boyajian's Star (KIC 8462852), as a rare `ground truth' for testing outlier identification to verify that objects of genuine scientific interest are included among the identified anomalies. Additionally, we report the full list of identified anomalies for these quarters, and present a sample subset of identified outliers that includes unusual phenomena, objects that are rare in the Kepler field, and data artifacts. By identifying <4% of each quarter as outlying data, under 6k individual targets for the dataset used, we demonstrate that this anomaly detection method can create a more targeted approach in searching for rare and novel phenomena.We further present an outlier scoring methodology to provide a framework of prioritization of the most potentially interesting anomalies. We have developed a data mining method based on k-Nearest Neighbor distance in feature space to efficiently identify the most anomalous light curves. We test variations of this method including using principal components of the feature space, removing select features, the effect of the choice of k, and scoring to subset samples. We evaluate the performance of our scoring on known object classes and find that our scoring consistently scores rare (<1000) object classes higher than common classes, meaning that rarer objects are successfully prioritized over common objects. The most common class, categorized as miscellaneous stars without any major variability, and rotational variables compose well over two-thirds of the KIC, yet are considerably underrepresented in the top outliers. We have applied scoring to all long cadence light curves of quarters 1 to 17 of Kepler's prime mission and present outlier scores for all 2.8 million light curves for the roughly 200k objects.
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Title: In situ EXAFS studies of novel Palladium-based anode catalysts for direct ethanol and formic acid fuel cells
Creator: Su, Ning
Date: 2024
Description: In this work we made nanoscale uniform deposition of Pd based anode catalyst on the transition metal Au (with atomic ratio Pd:Au=1:10) support...
Show moreIn this work we made nanoscale uniform deposition of Pd based anode catalyst on the transition metal Au (with atomic ratio Pd:Au=1:10) support of direct liquid ethanol fuel cells (DLEFCs) and direct liquid formic acid fuel cells (DLFAFCs). Synthesizing with uniform dispersion and catalyst nanoparticle dimensions understand the role of Pd reaction on its support in the direct EOR (ethanol oxidation reaction) and FOR (formic acid reaction) pathways, we performed in situ Pd K-edge X-ray absorption spectroscopy measurements as a function of potential using a custom-designed flow cell with the catalyst deposited on the glassy carbon window. We did in-situ EXAFS to better understand the reaction mechanism of Pd1@Au10 anode catalyst with EOR and AOR in nanoscale. Compared EOR with FOR electrochemical performance showed Pd@Au&C played better in ethanol than HCOOH and more stable which the the current density can reach up to 1216.25 mA·mg-1 Pd of EOR with Pd1@Au10&C in 1M KOH+1M EtOH (CH3CH2OH) on the ethanol fuel cells (DLEFCs), and 3.56 times higher of the EOR current compared with commercial Pd@C
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