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Title: High-Entropy Stabilization as a Designing Tool for Li-Ion Electrodes
Creator: Bandeira Jovino Marques, Otavio Jose
Date: 2023
Description: High-Entropy oxides (HEOs) form a new class of materials where the configurational entropy plays the stabilizing role of multicomponent...
Show moreHigh-Entropy oxides (HEOs) form a new class of materials where the configurational entropy plays the stabilizing role of multicomponent systems at high temperatures. Recently, it raised much attention for energy storage applications, especially on Li-ion batteries, where the combination of several different elements in a single solid solution can synergistically act to overcome some of its main drawbacks, improving the battery’s performance. The entropy stabilization opens new boundaries on electrode’s design by increasing the compositional space available for different structures and compounds. Not long ago, the high-entropy oxide (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O demonstrated a big potential as anode material in Li-ion batteries. Its high capacity and long cycling stability raised a lot of questions about the role of the transition metals in the conversion reaction, and the configurational entropy contribution to the electrochemical reaction, further supporting the electrode’s stability. In order to investigate the structural evolution, the role of the multicomponent oxides and structures on the battery’s performance, and the entropic contribution to the electrode’s stability, this research proposes a systematic and robust methodology around the (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O high-entropy oxide (HEO). The project heavily relies on the EXAFS ability to determine the short-range structure and the chemical sensitivity to isolate the elemental contribution of the compound at different cycling and charging states. First, the role of different metallic cations on the electrochemical reaction mechanism of the HEO was analyzed by the change in local structure during different charging steps of a Li-ion battery (Chapter 3). Secondly, the entropy contribution and tunability effects on electrochemical performance were tested in a series of medium and high-entropy oxides derived from the seminal HEO. Mg, Co, Ni, Cu, and Zn were individually removed from the HEO’s composition at a time and tested as Li-ion electrode. Fe was also added to the HEO’s composition (HEO+Fe) in order to prove the tunability effects and entropy contribution (Chapter 4). Operando x-ray absorption spectroscopy (XAS) was used to capture the short lived phases and the transient nature of the conversion reaction, to explain the origins of the extra storage capacity encountered on entropy stabilized systems (Chapter 5). Finally, the role of the high-entropy oxide initial structure was investigated and compared, to check versatility of the elements that can be used on a high-entropy system (Chapter 6).
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Title: Using Niobium surface encapsulation and Rhenium to enhance the coherence of superconducting devices
Creator: Crisa, Francesco
Date: 2024
Description: In recent decades, the scientific community has grappled with escalating complexity, necessitating a more advanced tool capable of tackling...
Show moreIn recent decades, the scientific community has grappled with escalating complexity, necessitating a more advanced tool capable of tackling increasingly intricate simulations beyond the capabilities of classical computers. This tool, known as a quantum computer, features processors composed of individual units termed qubits. While various methods exist for constructing qubits, superconducting circuits have emerged as a leading approach, owing to their parallels with semiconductor technology.In recent years, significant strides have been made in optimizing the geometry and design of qubits. However, the current bottleneck in the performance of superconducting qubits lies in the presence of defects and impurities within the materials used. Niobium, owing to its desirable properties, such as high critical temperature and low kinetic inductance, stands out as the most prevalent superconducting material. Nonetheless, it is encumbered by a relatively thick oxide layer (approximately 5 nm) exhibiting three distinct oxidation states: NbO, NbO$_2$, and Nb$_2$O$_5$. The primary challenge with niobium lies in the multitude of defects localized within the highly disordered Nb$_2$O$_5$ layer and at the interfaces between the different oxides. In this study, I present an encapsulation strategy aimed at restraining surface oxide growth by depositing a thin layer (5 to 10 nm) of another material in vacuum atop the Nb thin film. This approach exploits the superconducting proximity effect, and it was successfully employed in the development of Josephson junction devices on Nb during the 1980s.In the past two years, tantalum and titanium nitride have emerged as promising alternative materials, with breakthrough qubit publications showcasing coherence times five to ten times superior to those achieved in Nb. The focus will be on the fabrication and RF testing of Nb-based qubits with Ta and Au capping layers. With Ta capping, we have achieved the best T1 (not average) decay time of nearly 600 us, which is more than a factor of 10 improvements over the bare Nb. This establishes the unique capping layer approach as a significant new direction for the development of superconducting qubits.Concurrently with the exploration of materials for encapsulation strategies, identifying materials conducive to enhancing the performance of superconducting qubits is imperative. Ideal candidates should exhibit a thin, low-loss surface oxide and establish a clean interface with the substrate, thereby minimizing defects and potential sources of losses. Rhenium, characterized by an extremely thin surface oxide (less than 1 nm) and nearly perfect crystal structure alignment with commonly used substrates such as sapphire, emerges as a promising material platform poised to elevate the performance of superconducting qubits.
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Title: Laser Powder Bed Fusion Of Cost-Effective Non-Spherical Ti-6Al-4V Powder
Creator: Asherloo, Mohammadreza
Date: 2023
Description: This comprehensive research delves into the intricate dynamics of Laser Powder Bed Fusion (L-PBF) of Ti-6Al-4V powders, emphasizing the...
Show moreThis comprehensive research delves into the intricate dynamics of Laser Powder Bed Fusion (L-PBF) of Ti-6Al-4V powders, emphasizing the potential of non-spherical, hydride-dehydride (HDH) powders as a cost-efficient alternative to traditional spherical powders. The study systematically explores the interplay between powder morphology, granulometry, and various post-processing treatments in shaping the resultant microstructure, porosity, and mechanical properties of L-PBF fabricated Ti-6Al-4V components.Initial investigations focused on the flowability, packing density, and resultant density of L-PBF parts using HDH powders with varying size distributions. Through meticulous optimization of laser parameters, parts with a relative density exceeding 99.5% were achieved, even at production rates 1.5–2 times higher than conventional LPBF processes. Dynamic synchrotron X-ray imaging provided insights into laser-powder interactions, revealing key mechanisms of porosity formation associated with HDH powders. Further microstructural examinations highlighted the formation of columnar β grains with acicular α/α′ phases in the as-built condition. Mechanical tests, including fatigue assessments under fully-reversed tension-compression conditions, revealed the critical role of surface roughness in fatigue performance. Notably, mechanical grinding significantly improved fatigue strength, especially in the high cycle fatigue region, by eliminating surface micro-notches. X-ray diffraction analyses further elucidated the stress and micro-strain profiles, offering insights into the material's deformation mechanisms. A pivotal discovery was the presence of α/α′ on prior β/β grain boundaries, challenging the prevailing notion that high cooling rates in L-PBF preclude β/β grain boundary variant selection. Electron backscatter diffraction and synchrotron X-ray imaging illuminated the role of powder characteristics in locally modulating cooling rates, leading to β/β grain boundary α′ lath growth. Lastly, the research underscored the multifaceted interdependencies among contouring, powder granulometry, Hot Isostatic Pressing (HIP), and mechanical surface treatments. A pronounced increase in sub-surface porosities was identified when contouring was combined with fine powder granulometry. However, post-HIP treatments induced a phase transformation from martensitic α′ to a basket-weave α+β microstructure, enhancing the material's fatigue resistance to levels comparable to wrought Ti-6Al-4V. In summation, this doctoral research offers a holistic understanding of the L-PBF process for Ti-6Al-4V, emphasizing the viability of non-spherical HDH powders and providing a roadmap for parameter optimization, defect minimization, and mechanical property enhancement in L-PBF-fabricated Ti-6Al-4V structures.
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Title: Investigation of Electrochemical Properties and Fabrication of Lithium- and Sodium-ion Batteries
Creator: Chen, Changlong
Date: 2023
Description: Since the successful commercialization of Li-ion battery, the opportunity in creating a sustainable world with evenly-distributed energy...
Show moreSince the successful commercialization of Li-ion battery, the opportunity in creating a sustainable world with evenly-distributed energy supply and less environmental concerns has been significantly increased. This triggered tremendous efforts from both academy and industry in building better Li-ion batteries. Along the research and development over past 30 years, the performance of current Li-ion batteries has met some basic needs in our daily life, such as powering electronic devices and electric vehicles for a short time, while superior capabilities, like extended operating life, stable function under extreme circumstances, is always pursued. Under the pressure from these ever-growing demands, the corresponding Li-ion battery production is faced with a lot of new challenges. Regarding the battery production, the present Li-ion battery manufacturing heavily relies on the use of certain repo-toxic solvent, N-methyl-2-pyrrolidone (NMP), which arouses safety concerns to human health. In the pursuit of a higher energy density, silicon anode, bearing ten times the gravimetric capacity of commercially-dominating graphite anode, is intensively studied as the anode material for next-generation Li-ion batteries. However, its degradation mechanism is not completely revealed yet, which makes the methods of effective optimizations hard to be developed. In terms of the cost control, Na-ion batteries have been revisited and have received extra attention in the past decade owing to the abundance in raw materials and the high compatibility with state-of-art Li-ion industry while blank space in understanding primary electrochemical properties, such as impedance signals, has not been totally filled. This will also cause the misunderstandings in such interpretation and, thereby, postpone the pace of relevant advancement. Targeting these proposed issues, this thesis provides a series of feasible solutions via careful investigation and rational analysis with the aid of various advanced (non)electrochemical techniques, which offers a few unique perspectives in studying Li- and Na-ion batteries, and further facilitates the following research and development in the corresponding communities.
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Title: Improving Niobium Superconducting Radio-Frequency Cavities by Studying Tantalum
Creator: Helfrich, Halle
Date: 2023
Description: Niobium superconducting radio-frequency (SRF) cavities are widely used accelerating structures. Improvements in both quality factor, Q0, and...
Show moreNiobium superconducting radio-frequency (SRF) cavities are widely used accelerating structures. Improvements in both quality factor, Q0, and maximum accelerating gradient, Eacc, have been made to SRF cavities by introducing new processing techniques. These breakthroughs include processes such as nitrogen doping(N-Doping) and infusion, electrochemical polishing (EP) and High Pressure Rinsing (HPR). [1] There is still abundant opportunity to improve the cavities or, rather, the material they’re primarily composed of: niobium. A focus here is the role the native oxide of Nb plays in SRF cavity performance. The values of interest in a given cavity are its quality factor Q0, maximum accelerating gradient Eacc and surface resistance Rs . This work characterizes Nb and Ta foils prepared under identical conditions using X-ray photoelectron spectroscopy (XPS) to compare surface oxides and better understand RF loss mechanisms in Nb SRF cavities and qubits. It is well established that Ta qubits experience much longer coherence times than Nb qubits, which is probably due to the larger RF losses in Nb oxide. By studying Tantalum, an element similar to Niobium, the mechanisms of the losses that originate in the oxide and suboxide layers present on the surface of Nb cavities might finally be unlocked. We find noticeable differences in the oxides of Nb and Ta formed by air exposure of clean foils. In particular, Ta does not display the TaO2 suboxide in XPS, while Nb commonly shows NbO2. This suggests that suboxides are an additional contributor of RF losses. We also suggest that thin Ta film coatings of Nb SRF cavities may be a way of increasing Q0. It is in the interest of the accelerator community to fully understand the surface impurities present in Nb SRF cavities so that strategies for mitigating the effects can be proposed.
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