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Physical vapor deposition and defect engineering of europium doped lutetium oxideGillard, Scott James 10 July 2017 (has links)
Lutetium oxide doped with europium (Lu2O3:Eu3+) has been established as a promising scintillator material with properties that are advantageous when compared to other scintillators such as cesium iodide doped with thallium (CsI:Tl). Due to high X-ray attenuation characteristics, Lu2O3:Eu3+ is an attractive material for use in high resolution digital X-ray imaging systems. However, challenges still remain especially in the area of light output for Lu2O3:Eu3+. Processing by physical vapor deposition (PVD) and manipulation of oxygen defect structure was explored in order to better understand the effect on the scintillation phenomena.
PVD results were obtained using high temperature radio frequency sputtering (RF) and pulsed laser deposition (PLD) systems. Characterization of light output by radial noise power spectrum density measurements revealed that high temperature RF films were superior to those obtained using PLD. Optimization of sputtered films based on light output over a range of process parameters, namely temperature, power, pressure, and substrate orientation was investigated. Parameterization of deposition conditions revealed that: 75 watts, 10.00 mtorr, and 800°C were optimum conditions for Lu2O3:Eu3+ films.
Manipulation of anionic defect structure in similar material systems has been shown to improve scintillation response. Similar methods for Lu2O3:Eu3+ were explored for hot pressed samples of Lu2O3:Eu3+; via controlled atmosphere annealing, and use of extrinsic co-doping with calcium. The controlled atmosphere experiments established the importance of oxygen defect structure within Lu2O3:Eu3+ and showed that fully oxidized samples were preferred for light output. The second method utilized co-doping by the addition of calcium which induced oxygen vacancies and by Frenkel equilibrium changed the oxygen interstitial population within the Lu2O3:Eu3+ structure. The addition of calcium was investigated and revealed that scintillation was improved with a maximum response occurring at 340ppm of calcium. PVD optimization and co-doping experimental results provided a template for the use of calcium co-doped Lu2O3:Eu3+ targets for deposition of films. Preliminary deposition results were promising and revealed that small additions (around 550 ppm) of calcium resulted in better activator efficiency. Calcium co-doped films have a predicted increase in the light yield greater than 14% when compared to analogous un-doped Lu2O3:Eu3+ films at 60keV.
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Defects in ceriaGidby, Marcus January 2009 (has links)
<p>The solid oxide fuel cell (SOFC) technology has been under research since thelate 1950s, and most of the research has been on designs utilizing yttria stabilized zirconia (YSZ) as the electrolyte of choice. However, the SOFC technology has the major drawback of requiring high operation temperatures (up to 1000 degrees Celcius), so research of alternative materials have come into interest that would possibly require a lower working temperature without any significant loss of conductivity.One such material of interest for the electrolyte is compounds of ceriumdioxide (ceria). Ceria is well known for its ability to release oxygen by formingoxygen vacancies under oxygen-poor conditions, which increases its oxygen ionconductivity, and works at a lower temperature than the YSZ compounds whenproperly doped. Conversely, ceria is also able to absorb oxygen under oxygen-rich conditions, and those two abilities make it a very good material to use in catalytic converters for reduction of carbon monoxide and nitrogen oxide emission. The ability for the oxygen ions to easily relocate inbetween the different lattice sites is likely the key property of oxygen ion transportation in ceria. Also, in oxygen-rich conditions, the absorbed oxygen atom is assumed to join the structure at either the roomy octrahedral sites, or the vacant tetrahedral sites. Following that, the oxygen atom may relocate to other vacant locations, given it can overcome a possible potential barrier.</p><p>This thesis studies how those interstitial oxygen vacancies (defects) affect theenergy profile of ceria-based supercells by first principles calculations. The system is modeled within the density functional theory (DFT) with aid of (extended) local density approximation (LDA+U) using the software VASP. Furthermore, it is studied how those vacancies affect neighbouring oxygen atoms, and wether or not it is energetically benificial for the neighbouring atoms to readjust their positions closer or further away from the vacancy. The purpose of this thesis is to analyze wether or not it is theoretically possible that interstitial oxygen vacancies may cause neighbouring oxygen atoms to naturally relocate to the octahedral site in ceria, and how this affects the overall energy profile of the material.</p>
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Defects in ceriaGidby, Marcus January 2009 (has links)
The solid oxide fuel cell (SOFC) technology has been under research since thelate 1950s, and most of the research has been on designs utilizing yttria stabilized zirconia (YSZ) as the electrolyte of choice. However, the SOFC technology has the major drawback of requiring high operation temperatures (up to 1000 degrees Celcius), so research of alternative materials have come into interest that would possibly require a lower working temperature without any significant loss of conductivity.One such material of interest for the electrolyte is compounds of ceriumdioxide (ceria). Ceria is well known for its ability to release oxygen by formingoxygen vacancies under oxygen-poor conditions, which increases its oxygen ionconductivity, and works at a lower temperature than the YSZ compounds whenproperly doped. Conversely, ceria is also able to absorb oxygen under oxygen-rich conditions, and those two abilities make it a very good material to use in catalytic converters for reduction of carbon monoxide and nitrogen oxide emission. The ability for the oxygen ions to easily relocate inbetween the different lattice sites is likely the key property of oxygen ion transportation in ceria. Also, in oxygen-rich conditions, the absorbed oxygen atom is assumed to join the structure at either the roomy octrahedral sites, or the vacant tetrahedral sites. Following that, the oxygen atom may relocate to other vacant locations, given it can overcome a possible potential barrier. This thesis studies how those interstitial oxygen vacancies (defects) affect theenergy profile of ceria-based supercells by first principles calculations. The system is modeled within the density functional theory (DFT) with aid of (extended) local density approximation (LDA+U) using the software VASP. Furthermore, it is studied how those vacancies affect neighbouring oxygen atoms, and wether or not it is energetically benificial for the neighbouring atoms to readjust their positions closer or further away from the vacancy. The purpose of this thesis is to analyze wether or not it is theoretically possible that interstitial oxygen vacancies may cause neighbouring oxygen atoms to naturally relocate to the octahedral site in ceria, and how this affects the overall energy profile of the material.
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