Matching Items (15)

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Effect of Defects on Calculation of Electron Energy Loss Spectra of Ceria and Titania

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Climate change is one of the biggest challenges facing today's society.Since the late 19th century, the global average temperature has been rising. In order to minimize the temperature increase of the earth, it is necessary to develop alternative energy technologies

Climate change is one of the biggest challenges facing today's society.Since the late 19th century, the global average temperature has been rising. In order to minimize the temperature increase of the earth, it is necessary to develop alternative energy technologies that do not depend on fossil fuels. Solar fuels are one potential energy source for the future. Solar fuel technologies use catalysts to convert low energy molecules into fuels via artificial photosynthesis. TiO2, or titania, is an important model photocatalyst for studying these reactions. It is also important to use remaining fossil fuel resources efficiently and with the lowest possible greenhouse gas emissions. Fuel cells are electrochemical devices that aim to accomplish this goal and CeO2, or ceria, is an important material used in these devices. One way to observe the atomic structure of a material is with a transmission electron microscope (TEM). A traditional transmission electron microscope employs a beam of fast electrons to form atomic resolution images of a material. While imaging gives information about the positions of the atoms in the material, spectroscopy gives information about the composition and bonding of the material. A type of spectroscopy that can be performed inside the transmission electron microscope is electron energy loss spectroscopy (EELS), which provides a fundamental understanding of the electronic structure of a material. The energy loss spectrum also contains information on the chemical bonding in the material, and theoretical calculations that model the spectra are essential to correctly interpreting this bonding information. FEFF is a software that performs EELS calculations. Calculations of the oxygen K edges of TiO2 and CeO2 were made using FEFF in order to understand the changes that occur in the spectrum when oxygen vacancies are introduced as well as the changes near a grain boundary.

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2013-12

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社交網站對於國際經濟的影響

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隨著全球一體化,社交網絡在國際平台上擁有了相當出色的表現,影響全球人民的生活,特別有助於國際經濟發展,因此引起了各國的關注。雖然如此,它們具體的效果是難以去評估的。本文在前人研究的基礎上探討社交網絡的經營模式以及它對於國際經濟的影響。在微觀層面可以看到社交網的存在對市場有著直接的影響。在宏觀層面上,社交網站通過其網站設計推銷其他公司產品,提高廣告商的知名度,刺激消費。這兩方面,本文討論社交網的影響為何跟傳統公司有差別。

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2013-12

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A Study of an Inclusion Observed Under Transmission Electron Microscopy in Synechocystis sp. PCC 6803

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Transmission electron microscopy has been used to identify poly-3-hydroxybutyrate (PHB) granules in cyanobacteria for over 40 years. Electron-transparent (sometimes containing a slightly electron-dense area in the inclusions) or slightly electron-dense spherical inclusions found in transmission electron micrographs of cyanobacteria are

Transmission electron microscopy has been used to identify poly-3-hydroxybutyrate (PHB) granules in cyanobacteria for over 40 years. Electron-transparent (sometimes containing a slightly electron-dense area in the inclusions) or slightly electron-dense spherical inclusions found in transmission electron micrographs of cyanobacteria are often assumed to be PHB granules. The aim of this study was to test this assumption in Synechocystis sp. PCC 6803, and to determine whether all inclusions of this kind are indeed PHB granules. Based on the results gathered, it is concluded that not all of the slightly electron-dense spherical inclusions are PHB granules in Synechocystis sp. PCC 6803. This result is potentially applicable to other cyanobacteria.

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2013-05

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Combined photo- and thermionic electron emission from low work function diamond films

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In this dissertation, combined photo-induced and thermionic electron emission from low work function diamond films is studied through low energy electron spectroscopy analysis and other associated techniques. Nitrogen-doped, hydrogen-terminated diamond films prepared by the microwave plasma chemical vapor deposition method

In this dissertation, combined photo-induced and thermionic electron emission from low work function diamond films is studied through low energy electron spectroscopy analysis and other associated techniques. Nitrogen-doped, hydrogen-terminated diamond films prepared by the microwave plasma chemical vapor deposition method have been the most focused material. The theme of this research is represented by four interrelated issues. (1) An in-depth study describes combined photo-induced and thermionic emission from nitrogen-doped diamond films on molybdenum substrates, which were illuminated with visible light photons, and the electron emission spectra were recorded as a function of temperature. The diamond films displayed significant emissivity with a low work function of ~ 1.5 eV. The results indicate that these diamond emitters can be applied in combined solar and thermal energy conversion. (2) The nitrogen-doped diamond was further investigated to understand the physical mechanism and material-related properties that enable the combined electron emission. Through analysis of the spectroscopy, optical absorbance and photoelectron microscopy results from sample sets prepared with different configurations, it was deduced that the photo-induced electron generation involves both the ultra-nanocrystalline diamond and the interface between the diamond film and metal substrate. (3) Based on results from the first two studies, possible photon-enhanced thermionic emission was examined from nitrogen-doped diamond films deposited on silicon substrates, which could provide the basis for a novel approach for concentrated solar energy conversion. A significant increase of emission intensity was observed at elevated temperatures, which was analyzed using computer-based modeling and a combination of different emission mechanisms. (4) In addition, the electronic structure of vanadium-oxide-terminated diamond surfaces was studied through in-situ photoemission spectroscopy. Thin layers of vanadium were deposited on oxygen-terminated diamond surfaces which led to oxide formation. After thermal annealing, a negative electron affinity was found on boron-doped diamond, while a positive electron affinity was found on nitrogen-doped diamond. A model based on the barrier at the diamond-oxide interface was employed to analyze the results. Based on results of this dissertation, applications of diamond-based energy conversion devices for combined solar- and thermal energy conversion are proposed.

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2013

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Synthesis and in situ environmental transmission electron microscopy investigations of ceria-based oxides for solid oxide fuel cell anodes

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The behavior of a solid oxide fuel cell (SOFC) cermet (ceramic-metal composite) anode under reaction conditions depends significantly on the structure, morphology and atomic scale interactions between the metal and the ceramic components. In situ environmental transmission electron microscope (ETEM)

The behavior of a solid oxide fuel cell (SOFC) cermet (ceramic-metal composite) anode under reaction conditions depends significantly on the structure, morphology and atomic scale interactions between the metal and the ceramic components. In situ environmental transmission electron microscope (ETEM) is an important tool which not only allows us to perform the basic nanoscale characterization of the anode materials, but also to observe in real-time, the dynamic changes in the anode material under near-reaction conditions. The earlier part of this dissertation is focused on the synthesis and characterization of Pr- and Gd-doped cerium oxide anode materials. A novel spray drying set-up was designed and constructed for preparing nanoparticles of these mixed-oxides and nickel oxide for anode fabrication. X-ray powder diffraction was used to investigate the crystal structure and lattice parameters of the synthesized materials. Particle size distribution, morphology and chemical composition were investigated using transmission electron microscope (TEM). The nanoparticles were found to possess pit-like defects of average size 2 nm after subjecting the spray-dried material to heat treatment at 700 °C for 2 h in air. A novel electron energy-loss spectroscopy (EELS) quantification technique for determining the Pr and Gd concentrations in the mixed oxides was developed. Nano-scale compositional heterogeneity was observed in these materials. The later part of the dissertation focuses mainly on in situ investigations of the anode materials under a H2 environment in the ETEM. Nano-scale changes in the stand-alone ceramic components of the cermet anode were first investigated. Particle size and composition of the individual nanoparticles of Pr-doped ceria (PDC) were found to affect their reducibility in H2 gas. Upon reduction, amorphization of the nanoparticles was observed and was linked to the presence of pit-like defects in the spray-dried material. Investigation of metal-ceramic interactions in the Ni-loaded PDC nanoparticles indicated a localized reduction of Ce in the vicinity of the Ni/PDC interface at 420 °C. Formation of a reduction zone around the interface was attributed to H spillover which was observed directly in the ETEM. Preliminary results on the fabrication of model SOFCs and in situ behavior of Ni/Gd-doped ceria anodes have been presented.

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2011

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Fluctuation electron microscopy of amorphous and polycrystalline materials

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Fluctuation Electron Microscopy (FEM) has become an effective materials' structure characterization technique, capable of probing medium-range order (MRO) that may be present in amorphous materials. Although its sensitivity to MRO has been exercised in numerous studies, FEM is not yet

Fluctuation Electron Microscopy (FEM) has become an effective materials' structure characterization technique, capable of probing medium-range order (MRO) that may be present in amorphous materials. Although its sensitivity to MRO has been exercised in numerous studies, FEM is not yet a quantitative technique. The holdup has been the discrepancy between the computed kinematical variance and the experimental variance, which previously was attributed to source incoherence. Although high-brightness, high coherence, electron guns are now routinely available in modern electron microscopes, they have not eliminated this discrepancy between theory and experiment. The main objective of this thesis was to explore, and to reveal, the reasons behind this conundrum.

The study was started with an analysis of the speckle statistics of tilted dark-field TEM images obtained from an amorphous carbon sample, which confirmed that the structural ordering is sensitively detected by FEM. This analysis also revealed the inconsistency between predictions of the source incoherence model and the experimentally observed variance.

FEM of amorphous carbon, amorphous silicon and ultra nanocrystalline diamond samples was carried out in an attempt to explore the conundrum. Electron probe and sample parameters were varied to observe the scattering intensity variance behavior. Results were compared to models of probe incoherence, diffuse scattering, atom displacement damage, energy loss events and multiple scattering. Models of displacement decoherence matched the experimental results best.

Decoherence was also explored by an interferometric diffraction method using bilayer amorphous samples, and results are consistent with strong displacement decoherence in addition to temporal decoherence arising from the electron source energy spread and energy loss events in thick samples.

It is clear that decoherence plays an important role in the long-standing discrepancy between experimental FEM and its theoretical predictions.

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2015

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Investigation into a laser welded interconnection method for Interdigitated Back Contact (IBC) solar cell modules

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Interconnection methods for IBC photovoltaic (PV) module integration have widely been explored yet a concrete and cost-effective solution has yet to be found. Traditional methods of tabbing and stringing which are still being used today impart increased stress on the

Interconnection methods for IBC photovoltaic (PV) module integration have widely been explored yet a concrete and cost-effective solution has yet to be found. Traditional methods of tabbing and stringing which are still being used today impart increased stress on the cells, not to mention the high temperatures induced during the soldering process as well. In this work and effective and economical interconnection method is demonstrated, by laser welding an embossed aluminum (Al) electrode layer to screen-printed silver (Ag) on the solar cell. Contact resistivity below 1mΩ.cm2 is measured with the proposed design. Cross-sectional analysis of interfaces is conducted via Scanning Electron Microscopy (SEM) and Energy Dispersive X-ray Spectroscopy (EDXS) methods. Typical laser weld phenomenon observed involves Al ejection at the entrance of the weld, followed by Al and Ag fusing together mid-way through the weld spot, as revealed by cross-sectional depth analysis. The effects of voltage and lamp intensity are also tested on the welding process. With the range of voltages tested, 240V seems to show the least process variability and the most uniform contact between Al and Ag layers, upon using an Ethylene-Vinyl Acetate (EVA) encapsulant. Two lamp intensities were also explored with a Polyolefin (POE) encapsulant with Al and Ag layers seen welded together as well. Smaller effect sizes at lamp 2 intensity showed better contact. A process variability analysis was conducted to understand the effects of the two different lamps on welds being formed. Lamp 2 showed a bi-modal size distribution with a higher peak intensity, with more pulses coupling into the sample, as compared to lamp 1.

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2019

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Electron Microscopy Characterization of GaN-on-GaN Vertical Power Devices

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Wide bandgap semiconductors are of much current interest due to their superior electrical properties. This dissertation describes electron microscopy characterization of GaN-on-GaN structures for high-power vertical device applications. Unintentionally-doped (UID) GaN layers grown homoepitaxially via metal-organic chemical vapor deposition on

Wide bandgap semiconductors are of much current interest due to their superior electrical properties. This dissertation describes electron microscopy characterization of GaN-on-GaN structures for high-power vertical device applications. Unintentionally-doped (UID) GaN layers grown homoepitaxially via metal-organic chemical vapor deposition on freestanding GaN substrates, were subjected to dry etching, and layers of UID-GaN/p-GaN were over-grown. The as-grown and regrown heterostructures were examined in cross-section using transmission electron microscopy (TEM). Two different etching treatments, fast-etch-only and multiple etches with decreasing power, were employed. The fast-etch-only devices showed GaN-on-GaN interface at etched location, and low device breakdown voltages were measured (~ 45-95V). In comparison, no interfaces were visible after multiple etching steps, and the corresponding breakdown voltages were much higher (~1200-1270V). These results emphasized importance of optimizing surface etching techniques for avoiding degraded device performance.
The morphology of GaN-on-GaN devices after reverse-bias electrical stressing to breakdown was investigated. All failed devices had irreversible structural damage, showing large surface craters (~15-35 microns deep) with lengthy surface cracks. Cross-sectional TEM of failed devices showed high densities of threading dislocations (TDs) around the cracks and near crater surfaces. Progressive ion-milling across damaged devices revealed high densities of TDs and the presence of voids beneath cracks: these features were not observed in unstressed devices. The morphology of GaN substrates grown by hydride vapor-phase epitaxy (HVPE) and by ammonothermal methods were correlated with reverse-bias results. HVPE substrates showed arrays of surface features when observed by X-ray topography (XRT). All fabricated devices that overlapped with these features had typical reverse-bias voltages less than 100V at a leakage current limit of 10-6 A. In contrast, devices not overlapping with such features reached voltages greater than 300V. After etching, HVPE substrate surfaces showed defect clusters and macro-pits, whereas XRT images of ammonothermal substrate revealed no visible features. However, some devices fabricated on ammonothermal substrate failed at low voltages. Devices on HVPE and ammonothermal substrates with low breakdown voltages showed crater-like surface damage and revealed TDs (~25µm deep) and voids; such features were not observed in devices reaching higher voltages. These results should assist in developing protocols to fabricate reliable high-voltage devices.

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2021

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Atomic scale characterizations of two-dimensional anisotropic materials and their heterostructures

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There has been a surge in two-dimensional (2D) materials field since the discovery of graphene in 2004. Recently, a new class of layered atomically thin materials that exhibit in-plane structural anisotropy, such as black phosphorous, transition metal trichalcogenides and rhenium

There has been a surge in two-dimensional (2D) materials field since the discovery of graphene in 2004. Recently, a new class of layered atomically thin materials that exhibit in-plane structural anisotropy, such as black phosphorous, transition metal trichalcogenides and rhenium dichalcogenides (ReS2), have attracted great attention. The reduced symmetry in these novel 2D materials gives rise to highly anisotropic physical properties that enable unique applications in next-gen electronics and optoelectronics. For example, higher carrier mobility along one preferential crystal direction for anisotropic field effect transistors and anisotropic photon absorption for polarization-sensitive photodetectors.

This dissertation endeavors to address two key challenges towards practical application of anisotropic materials. One is the scalable production of high quality 2D anisotropic thin films, and the other is the controllability over anisotropy present in synthesized crystals. The investigation is focused primarily on rhenium disulfide because of its chemical similarity to conventional 2D transition metal dichalcogenides and yet anisotropic nature. Carefully designed vapor phase deposition has been demonstrated effective for batch synthesis of high quality ReS2 monolayer. Heteroepitaxial growth proves to be a feasible route for controlling anisotropic directions. Scanning/transmission electron microscopy and angle-resolved Raman spectroscopy have been extensively applied to reveal the structure-property relationship in synthesized 2D anisotropic layers and their heterostructures.

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2018

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Excursions in Electron Energy-Loss Spectroscopy

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Recent improvements in energy resolution for electron energy-loss spectroscopy in the scanning transmission electron microscope (STEM-EELS) allow novel effects in the low-loss region of the electron energy-loss spectrum to be observed. This dissertation explores what new information can be obtained

Recent improvements in energy resolution for electron energy-loss spectroscopy in the scanning transmission electron microscope (STEM-EELS) allow novel effects in the low-loss region of the electron energy-loss spectrum to be observed. This dissertation explores what new information can be obtained with the combination of meV EELS energy resolution and atomic spatial resolution in the STEM. To set up this up, I review nanoparticle shape effects in the electrostatic approximation and compare the “classical” and “quantum” approaches to EELS simulation. Past the electrostatic approximation, the imaging of waveguide-type modes is modeled in ribbons and cylinders (in “classical" and “quantum" approaches, respectively), showing how the spatial variations of such modes can now be imaged using EELS. Then, returning to the electrostatic approximation, I present microscopic applications of low-loss STEM-EELS. I develop a “classical” model coupling the surface plasmons of a sharp metallic nanoparticle to the dipolar vibrations of an adsorbate molecule, which allows expected molecular signal enhancements to be quantified and the resultant Fano-type asymmetric spectral line shapes to be explained, and I present “quantum” modelling for the charged nitrogen-vacancy (NV-) and neutral silicon-vacancy (SiV0) color centers in diamond, including cross-sections and spectral maps from density functional theory. These results are summarized before concluding.

Many of these results have been previously published in Physical Review B. The main results of Ch. 2 and Ch. 4 were packaged as “Enhanced vibrational electron energy-loss spectroscopy of adsorbate molecules” (99, 104110), and much of Ch. 5 appeared as “Prospects for detecting individual defect centers using spatially resolved electron energy loss spectroscopy” (100, 134103). The results from Ch. 3 are being prepared for a forthcoming article in the Journal of Chemical Physics.

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2020