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This thesis investigates the unique properties of 2D devices such as twisted semiconducting bilayers and a-RuCl₃ heterostructures employing scanning tunneling microscopy (STM) and spectroscopy (STS) probes. The research presented here sheds light on the vast opportunities that 2D materials provide in condensed matter systems as well as future device applications. Among 2D materials, transition metal dichalcogenide (TMD) heterobilayers provide a promising platform to study many quantum phenomena such as excitonic states due to their tunability of band gap. In addition, TMDs are excellent candidates to achieve localized states and carrier confinement, crucial for single photon emitters used in quantum computation and information. We begin this thesis with a brief overview of STM/STS and utilizing these techniques on 2D materials in the first and second chapters.The third chapter of this work investigates the twisted bilayer of WSe₂ and MoSe₂ in the H-stacking configuration using STM/STS which was previously challenging to measure. The spectroscopic results obtained from the heterobilayer indicate that a combination of structural rippling and electronic coupling generates unexpectedly large \moire potentials, in the range of several hundred meV. Our analysis reveals that the \moire structure and internal strain, rather than interlayer coupling, are the main factors of the moire potential. Large moire potentials lead to deeply trapped carriers such as electron-hole pairs, so-called excitons. Our findings open new routes toward investigating excitonic states in twisted TMDs. In the next chapter, we investigate the ultralocalized states of twisted WSe₂/MoSe₂ nanobubbles. Mechanical and electrical nanostructurings are expected to modify the band properties of transition metal dichalcogenides at the nanoscale. To visualize this effect, we use STM and near-field photoluminescence to examine the electronic and optical properties of nanobubbles in the semiconducting heterostructures. Our findings reveal a significant change in the local bandgap at the nanobubble, with a continuous evolution towards the edge of the bubble. Moreover, at the edge of the nanobubble, we show the formation of in gap bound states. A continuous redshift of the interlayer exciton on entering the bubble is also detected by the nano-PL. Using self-consistent Schrodinger-Poisson simulations, we further show that strong doping in the bubble region leading to band bending is responsible for achieving ultralocalized states. Overall, this work demonstrates the potential of 2D TMDs for developing well-controlled optical emitters for quantum technologies and photonics. We next turn to the effect of the electric field in band gap tuning of WSe₂/WS₂ heterobilayer. The tunability of band gap is a crucial element in device engineering to achieve quantum emitters. The electrostatic gate generates doping and an electric field giving access to continuous tunability, higher doping level, and integration capability to nanoelectronic devices. We employ scanning tunneling microscopy (STM) and spectroscopy (STS) to probe the band properties of twisted heterobilayer with high energy and spatial resolution. We observe continuous band gap tuning up to several hundreds of meV change by sweeping the back gate. We introduced a capacitance model to take into account the finite tip size leading to an enhanced electric field. The result of our calculation captures well the band gap change observed by STS measurements. Our study offers a new route toward creating highly tunable semiconductors for carrier confinement in quantum technology. In the next chapters, we focus on a-RuCl₃ heterointerfaces. We first explore the nanobubble of graphene/a-RuCl3 to create sharp p-n junctions. The ability to create sharp lateral p-n junctions is a critical requirement for the observation of numerous quantum phenomena. To accomplish this, we used a charge-transfer based heterostructure consisting of graphene and a-RuCl₃ to create nanoscale lateral p-n junctions in the vicinity of nanobubbles. Our approach relied on a combination of scanning tunneling microscopy (STM) and spectroscopy (STS), as well as scattering-type scanning near-field optical microscopy (s-SNOM), which allowed us to examine both the electronic and optical responses of these nanobubble p-n junctions. Our results showed a massive doping variation across the nanobubble with a band offset of 0.6 eV. Further, we observe the formation of an abrupt junction along nanobubble boundaries with an exceptionally sharp lateral width (<3 nm). This is one order of magnitude smaller length scale than previous lithographic methods. Our work paves the way toward device engineering via interfacial charge transfer in graphene and other low-density 2D materials. In chapter 7, we describe the use of low-temperature scanning tunneling microscopy (STM) measurements to observe the \moire pattern in graphene/a-RuCl3 heterostructure to validate the InterMatch method. This method is effective in predicting the charge transfer, strain, and stability of an interface. The InterMatch method was applied to moire patterns of graphene/a-RuCl3 to predict the stable interface structure. STM topographs show three regions with distinct moire wavelengths due to atomic reconstructions. Using the InterMatch method, we perform a comprehensive mapping of the space of superlattice configurations and we identify the energetically favorable superlattices that occur in a small range of twist angles. This range is consistent with the STM results. Moreover, the spectra on these regions exhibit strong resonances with the spacing between resonances following the expectation from Landau levels on a Dirac spectrum due to strain and doping. The results of our scanning tunneling microscopy (STM) measurements confirm that the InterMatch method is effective in predicting the charge transfer and stability of interfaces between materials. We next investigate WSe₂/a-RuCl₃ heterostructure through a multi-faceted approach. Our exploration encompassed diverse techniques such as STM, and optical measurements. We detect a significant charge transfer between the two layers by STM measurements, leading to a shift in the Fermi level towards the valence band of WSe₂. Our findings are supported by optical measurements and DFT calculations, which confirm the p-doped WSe₂ observed through STM. The results of this work highlight a-RuCl₃ potential for contact engineering of TMDs and unlocking their functionalities for the next generation optoelectronic devices. In the last chapter of this thesis, I provide a brief conclusion as well as a few future directions and insights for investigating 2D materials.

京都大学 / 新制・課程博士 / 博士(工学) / 甲第23482号 / 工博第4894号 / 新制||工||1765(附属図書館) / 京都大学大学院工学研究科社会基盤工学専攻 / (主査)教授 森 信人, 准教授 原田 英治, 准教授 志村 智也 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM

<p> A review of the conducting paper analogue for plotting two-dimensional electric and magnetic fields is given. An improved capacitively-coupled conducting paper analogue is described that will map either single or multiple, uniformly-distributed-source Poissonian fields. A DEW map construction technique is detailed that uses a thin tape dielectric and silver-painted source electrodes. Equipotentials on the conducting paper surface correspond to lines of constant magnetic vector potential or flux lines. Differential voltages are analogous to flux density. The equipotential distribution is plotted using a null technique with a unique point on the map surface held at virtual ground potential. The time-varying equations governing the capacitively- coupled analogue are derived. As a result of these equations, an analogue for the skin effect phenomenon in conductors has been demonstrated.</p> / Thesis / Master of Engineering (ME)

<p>Petroleum products, such as base oils and jet fuels, play an essential role in modern society since they are necessary as lubricants for engines and as fuels for airplanes. The ability to accurately characterize these petroleum products is crucial for the successful generation of these compound mixtures with desirable properties. Unfortunately, analysis of petroleum products remains challenging due to the fact that they often contain thousands of different hydrocarbons. The petroleum industry relies heavily on powerful analytical techniques to evaluate the chemical compositions of petroleum products in order to improve their crude oil refinery procedures. Tandem mass spectrometry is the only analytical technique that has the potential to provide both elemental composition and structural information for individual analytes in complex mixtures. When coupled to chromatography, different tandem mass spectrometry methods facilitate the analysis of individual hydrocarbons in complex mixtures and therefore provide more detailed compositional information for petroleum products than other analytical methods. Fundamental studies that explore the physical and chemical properties of hydrocarbons also facilitate the development of new mass spectrometric ionization techniques for these analytes. The research discussed in this dissertation can be divided into three parts: the development and validation of new quantitation methodology for compounds representing twelve different hydrocarbon types in jet fuels (Chapters 3), the comparison of (+)APCI MS and GCxGC/(+)EI TOF MS for the analysis of saturated and aromatic hydrocarbons in group III heavy base oils (Chapter 4), and experimental measurement of proton affinities of alkanes (Chapter 5).</p>

京都大学 / 新制・課程博士 / 博士(エネルギー科学) / 甲第23586号 / エネ博第432号 / 新制||エネ||82(附属図書館) / 京都大学大学院エネルギー科学研究科エネルギー応用科学専攻 / (主査)教授 松田 一成, 教授 宮内 雄平 / 学位規則第4条第1項該当 / Doctor of Energy Science / Kyoto University / DFAM

Thesis advisor: Kevin S. Bedell / We present several results based upon non-trivial extensions of Landau-Fermi liquid theory. First proposed in the mid-20th century, the Fermi liquid approach assumes an adiabatic “switching-on” of the interaction, which allows one to describe the collective excitations of the many-body system in terms of weakly-interacting quasiparticles and quasiholes. At its core, Landau-Fermi liquid theory is often considered a perturbative approach to study the equilibrium thermodynamics and out-of-equilibrium response of weakly-correlated itinerant fermions, and therefore non-trivial extensions and consequences are usually overlooked in the contemporary literature. Instead, more emphasis is often placed on the breakdown of Fermi liquid theory, either due to strong correlations, quantum critical fluctuations, or dimensional constraints. After a brief introduction to the theory of a Fermi liquid, I will first apply the Landau quasiparticle paradigm to the theory of itinerant Majorana-like fermions. Defined as fermionic particles which are their own anti-particle, traditional Majorana zero modes found in topological materials lack a coherent number operator, and therefore do not support a Fermi liquid-like ground state. To remedy this, we will apply a combinatorical approach to build a statistical theory of self-conjugate particles, explicitly showing that, under this definition, a filled Fermi surface exists at zero temperature. Landau-Fermi liquid theory is then used to describe the interacting phase of these Majorana particles, from which we find unique signatures of zero sound in addition to exotic, non-analytic contributions to the specific heat. The latter is then exploited as a “smoking-gun” signature for Majorana-like excitations in the candidate Kitaev material Ag3LiIr2O6, where experimental measurements show good agreement with a sharply-defined, “Majorana-Fermi surface” predicted in the underlying combinatorial treatment. I will then depart from Fermi liquid theory proper to tackle the necessary conditions for the applicability of Luttinger’s theorem. In a nutshell, Luttinger’s theorem is a powerful theorem which states that the volume of phase space contained in the Fermi surface is invariant with respect to interaction strength. In this way, whereas Fermi liquid only describes fermionic excitations near the Fermi surface, Luttinger’s theorem describes the fermionic degrees of freedom throughout the entire Fermi sphere. We will show that Luttinger’s theorem remains valid only for certain frequency and momentum-dependencies of the self-energy, which correlate to the exis- tence of a generalized Fermi surface. In addition, we will show that the existence of a power-law Green’s function (a unique feature of “un-particle” systems and a proposed characteristic of the pseudo-gap phase of the cuprate superconductors) forces Luttinger’s theorem and Fermi liquid theory to be mutually exclusive for any non-trivial power of the Feynman propagator. Finally, we will return to Landau-Fermi liquid theory, and close with novel out-of-equilibrium behavior and stability in unconventional Fermi liquids. First, we will consider a perfectly two- dimensional Fermi liquid. Due to the reduction in dimension, the traditional mode expansion in terms of Legendre polynomials is modified to an expansion in terms of Chebyshev polynomials. The resulting orthogonality conditions greatly modifies the stability and collective modes in the 2D system. Second, we will look at a Fermi liquid in the presence of a non-trivial gauge field. The existence of a gauge field will effectively shift the Fermi surface in momentum space, resulting in, once again, a modified stability condition for the underlying Fermi liquid. Supplemented with a modernized version of Mermin’s condition for the propagation of zero sound, we outline the full effects a spin symmetric or anti-symmetric gauge would have on a Fermi liquid ground state. / Thesis (PhD) — Boston College, 2021. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.

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This thesis presents a numerical formulation which incorporates the effects of joints, cracks, and fractures into a mathematical mode used to in an existing finite element code. Two separate crack definitions were incorporated, one involving a discrete crack model, and the other a continuum approach defining a new material with regularly spaced joints. Several examples are also presented demonstrating the use of this capability.