Dissertations / Theses on the topic 'Nuclear size (Physics)'

Epoxy resin is widely used in high voltage apparatus as insulation due to its excellent mechanical, electrical and chemical properties. Fillers are often added to epoxy resin to enhance its mechanical, thermal and chemical properties. With the new development in nanotechnology, it has been widely anticipated that the combination of nanoparticles with traditional resin systems may create nanocomposite materials with enhanced electrical, thermal and mechanical properties. The project aims to improve the overall electrical performance by adding nanoparticles into epoxy resin. In the present thesis a detailed study on dielectric permittivity, AC breakdown strength and space charge behaviour of epoxy resin/nanocomposites with nano-fillers of SiO2 and Al2O3 has been carried out. The epoxy resin/nanocomposite thin film samples were prepared and tests were carried out to measure their dielectric permittivity and tan delta value in frequency range of 1Hz- 1MHz. The space charge behaviours were also observed by using the pulse electroacoustic (PEA) technique. The influence of filler type, filler size and filler concentration on nanocomposites ac breakdown strength were also examined. In addition, traditional epoxy resin microcomposites were also prepared and tested and the results were compared with those obtained from epoxy resin/nanocomposites. The present results indicate that the presence of nano-sized fillers enhances the insulation properties of the epoxy resin and the dielectric properties are strongly influenced by the interfacial region between epoxy and nano particles. It is the key factor that affects the electrical performance of epoxy nanocomposites. The multi core model has been applied to explain the effects of such interfacial region on the electrical performance epoxy nanocomposites. A new phenomenon of space charge accumulation at higher nano size filler loading concentration has been observed at a filler loading concentration above 3wt%. This phenomenon is a result of the formation of electrical double layer surrounding the nano particles. A comparison study between epoxy nanocomposites loaded with both surface treated and non-surface treated nano particles has also been carried out. The results indicate that nano particle dispersion rate is an important factor in determine the electrical performance epoxy nanocomposites. Surface functionalisation on nano size fillers by using silane as a coupling agent could help avoiding the formation of large agglomerations resulting in better insulating performance. In addition, it has also been found that the presence of water inside epoxy nanocomposites also leads to the reduction in dielectric properties due to the formation of water layers surrounding the nano particles. Those water layers could act as a conductive path to help charge carriers travelling through the bulk of the materials.

Volcanogenic lightning has a long documented history in the scientific field, though its origins are still poorly understood. The interactions leading to electrification of ash plumes is essentially a function of the microphysics controlling and affecting ash particle collisions. This thesis presents measurements made on charged particle interactions in a fluidized bed, with large-scale applications to the phenomenon of volcanogenic lightning and charged particle dynamics in volcanic plumes. Using a fluidized bed of ash samples taken from Ecuador's Volcán Tungurahua, particles are introduced to a collisional environment, where they acquire an associated polarity. A charged copper plate is used to collect particles of a given polarity, and particle size distributions are obtained for different weight fractions of the ash. It is observed that relatively smaller particles acquire a net negative charge, while larger particles in the sample charge positively. This is a well-documented occurrence with perfectly spherical, chemically identical samples, but this work represents one of the first applications of the principle to volcanic ash. Image analysis is preformed to determine the size distribution associated with specific polarities, and the associated minimum charge on each particle is calculated based on the plate collection height and particle size. We also present results that demonstrate the relationship between particle collisions and the amount of charge exchanged. Using techniques developed to examine the collision rate within a flow, combined with the charging rates determined from this experiment, we determine a maximum charge exchange rate of 1.28±0.23 electrons transferred per collision.

The distribution of 75Se in tissue equivalent materials was investigated employing Gamma ray Emission Tomography with a rectilinear scanner utilizing NaI(Tl) and BGO detectors. The reconstructed images, using Filtered Back Projection and Iterative techniques were presented in 2D colour and 3D representations. Using a lead collimator of aperture 1.5x20 mm and 70 length, the distribution of selenium with variation of volume and concentration was examined and clearly seen. Several corrections such as background, scattering, attenuation compensation and X-ray characteristic suppression, were performed to improve the quality of the images which was evaluated in terms of the fidelity factor. The possibility of quantifying an image was considered with regard to spatial resolution and least detectable concentration. The spatial resolution was measured using two small vials containing the same concentration of selenium, the value obtained was the same as the width of the collimator aperture. The value of the least detectable concentration of selenium however, was difficult to find, due to the many ambiguous factors involved. The binding site of selenium which is based on quadrupole interaction with the surrounding electric field, was investigated employing Perturbed Angular Correlation (PAC) experiments using NaI(Tl) and BaF2 detectors. Using NaI(Tl) detectors, it was difficult to observe the perturbation, due to the poor time resolution. The BaF2 detector according to the literatures has a shorter light emission decay time constant (0.6 ns), suggested that a better time resolution than that found with the NaI(Tl) detectors could be obtained. A Perturbed Angular Correlation experiment employing BaF2 detectors and a fast-slow coincidence system was set up. The time differential PAC of selenium in solution showed an unperturbed angular correlation pattern. The main problem is the very short half life of the intermediate state of 75Se (0.3 ns), making it difficult to observe the perturbation effect. The time resolution of the system (5.4 ns) will need to be improved by an order of magnitude or more for the investigations to continue.

Denna licensiatavhandling behandlar oxidativ upplösning av UO2. Upplösning av UO2 studeras huvudsakligen då UO2-matrisen hos använt kärnbränsle förväntas fungera som en barriär mot frigörande av radionuklider i ett framtida djupförvar. Lösligheten av U(IV) är mycket låg under i djupförvaret rådande förhållanden emedan U(VI) har betydligt högre löslighet. Oxidation av UO2-matrisen kommer därför att påverka dess löslighet och därmed dess funktion som barriär. I denna avhandling studeras den relativa effektiviteten av en- och två-elektronoxidanter för upplösning av UO2. Vid låga oxidantkoncentrationer är utbytet för upplösningen för en-elektronoxidanter signifikant lägre än för två-elektronoxidanter. För en-elektronoxidanter ökar dock utbytet med ökande oxidanthalt, vilket kan förklaras av den ökade sannolikheten för två konsekutiva en-elektronoxidationer av samma reaktionssite och den ökade möjligheten till disproportionering. Radikaler och molekylära radiolysprodukters relativa inverkan på oxidativ upplösning av UO2 studeras också i denna avhandling genom mätning av mängden upplöst U(VI) i γ-bestrålade system som dominerades av olika oxidanter. Dessa studier visade att upplösningshastigheten av UO2 kan uppskattas från oxidantkoncentrationer framtagna genom simuleringar av radiolys i motsvarande homogena system och hastighetskonstanterna för ytreaktionerna. Simuleringarna visar att de molekylära oxidanterna kommer vara de viktigaste oxidanterna i alla system i denna studie vid långa bestrålningstider (>10 timmar). Vid liknande simuleringar av α-bestrålade system fanns att vid förhållanden relevanta för ett djupförvar för använt kärnbränsle, är det endast de molekylära oxidanterna (i huvudsak H2O2) som är av betydelse för upplösningen av bränslematrisen. Då använt kärnbränsle innehåller en mängd radionuklider som utsätter UO2-matrisen för kontinuerlig bestrålning, är det av vikt att undersöka hur bestrålning påverkar reaktiviteten av UO2. Bestrålningseffekten på reaktionen mellan UO2 och MnO4- studerades. Dessa försök visade att bestrålning av UO2 vid doser >40 kGy leder till att reaktiviteten ökar upp till 1.3 gånger reaktiviteten av obestrålad UO2. Den ökade reaktiviteten kvarstår efter bestrålningen och effekten kan därför möjligen tillskrivas permanenta förändringar i materialet. Vid uppskattning av reaktiviteten hos använt kärnbränsle måste hänsyn tas till denna effekt då bränslet redan efter ett par dagar i reaktor blivit utsatt för doser >40 kGy. Det har tidigare föreslagits att hastigheten för en heterogen västka/fast-fas reaktion är beroende av partikelstorleken hos det fasta materialet, vilket har studerats för UO2-partiklar i denna avhandling. Experimentellt bestämda kinetiska parametrar jämförs med de föreslagna ekvationerna för fyra storleksfraktioner av UO2-pulver och en UO2-pellet. Studien visade partikelstorleksberoendet av andra ordningens hastighetskonstant och aktiveringsenergin för oxidation av UO2 med MnO4- beskrivs relativt väl av de föreslagna ekvationerna.
The general subject of this thesis is oxidative dissolution of UO2. The dissolution of UO2 is mainly investigated because of the importance of the UO2 matrix of spent nuclear fuel as a barrier against radionuclide release in a future deep repository. U(IV) is extremely insoluble under the reducing conditions prevalent in a deep repository, whereas U(VI) is more soluble. Hence, oxidation of the UO2-matrix will affect its solubility and thereby its function as a barrier. In this thesis the relative efficiency of one- and two electron oxidants in dissolving UO2 is studied. The oxidative dissolution yield of UO2 was found to differ between one- and two-electron oxidants. At low oxidant concentrations the dissolution yields for one-electron oxidants are significantly lower than for two-electron oxidants. However, the dissolution yield for one-electron oxidants increases with increasing oxidant concentration, which could be rationalized by the increased probability for two consecutive one-electron oxidations at the same site and the increased possibility for disproportionation. Furthermore, the relative impact of radical and molecular radiolysis products on oxidative dissolution of UO2 is investigated. Experiments were performed where the amount of dissolved U(VI) was measured in γ-irradiated systems dominated by different oxidants. We have found that the UO2 dissolution rate in systems exposed to γ-irradiation can be estimated from oxidant concentrations derived from simulations of radiolysis in the corresponding homogeneous systems and rate constants for the surface reactions. These simulations show that for all systems studied in this work, the molecular oxidants will be the most important oxidants for long irradiation times (>10 hours). Similar simulations of α-irradiated systems show that in systems relevant for a deep repository for spent nuclear fuel, only the molecular oxidants (mainly H2O2) are of importance for the dissolution of the fuel matrix. The effect on UO2 reactivity by irradiation of the material is of importance when predicting the spent fuel dissolution rate since the fuel, due to its content of radionuclides, is exposed to continuous self-irradiation. The effect of irradiation on the reaction between solid UO2 and MnO4- in aqueous solutions was studied. It was found that irradiation of UO2 at doses >40 kGy increases the reactivity of the material up to ~1.3 times the reactivity of unirradiated UO2. The increased reactivity remains after the irradiation and can possibly be attributed to permanent changes in the material. This issue must be taken into account when predicting the reactivity of spent nuclear fuel since the fuel is exposed to doses >40 kGy after only a few days in the reactor. It has earlier been suggested that the rate of a heterogeneous liquid-solid reaction depends on the size of the solid particles. This was investigated for UO2 particles in this thesis. Experimental kinetic parameters are compared to the previously proposed equations for UO2 powder of four size fractions and a UO2 pellet. We have found that the particle size dependence of the second order rate constant and activation energy for oxidation of UO2 by MnO4- is described quite well by the proposed equations.
QC 20101123

The influence of lateral dimensions on the relaxation mechanism and the resulting effect on the surface topography of limited-area, linearly graded Si1-xGeX virtual substrates has been investigated for the first time. A dramatic change in the relaxation mechanism of such buffer layers has been observed for depositions on Si mesa pillars of lateral dimensions of 10μm and below. For such depositions, misfit dislocations are able to extend, unhindered, and terminate at the edges of the growth zone. In this manner, orthogonal misfit dislocation interactions are avoided, yielding a surface free of the problematic surface cross-hatch roughening. However, as the lateral dimension of the growth zone is increased to 20μm, orthogonal misfit interactions occur and relaxation is dominated by the Modified Frank-Read (MFR) multiplication mechanism. The resulting surface morphology shows a pronounced surface cross-hatch roughening. It is proposed that such cross-hatch roughening is a direct consequence of the cooperative stress fields associated with the MFR mechanism. It is postulated that the method of limited-area, linearly graded buffer layers provides a unique opportunity, by which 'ideal' virtual substrates, free of surface cross-hatch and threading dislocations, may be produced to any Ge content. In addition, a unique method by which the electrical performance of low temperature, strained layer depositions may be optimised is discussed. The method relies on the elimination, 'of as-grown lattice imperfections via a post growth thermal anneal treatment. A 25-fold increase in low temperature hole mobility of a Si0.5Ge0.5/Si0.7Ge0.3 heterostructure has been demonstrated using a 30 minute, 750°C in-situ, post growth anneal.

This thesis demonstrates the advantages and disadvantages of investigated p-type SiGe MOSFETs with high Ge content Si1#xGex p-channel grown on Si1#yGey virtual substrate (VS) (x "0'7$0'9, y "0'3$0'5) in comparison with conventional Si devices. The ways to overcome current difficulties in conventional Si technology and mixed SiGe-Si technology are shown. Current-voltage (I-V) and capacitance-voltage (C-V) DC characteristics for p-channel Si/Si1#xGex/Si1#yGey hetero-MOSFETs with high Ge content (x "0'7$0'9, y"0'3$0'5) are reported. Enhancement in the maximum drain current for the p-SiGe devices in comparison with p-Si control is 2.5-3.0 times. DC characteristic simulations of SiGe p-channel MOSFETs were used to improve the accuracy of MOSFET and heterostructure parameters extraction. Calibrated during the simulation theoretical models were used for future design. The effective mobility, the source-drain access resistance, the doping profile, the layers thickness, oxide/semiconductor interface charge and other important characteristics were extracted. The effective mobility values, extracted for p-Si0%3Ge0%7 MOSFETs, exceed the hole mobility in a conventional Si p-MOS device by a factor of 3.5 and reach the mobility of conventional Si n-MOS transistors. The peak value of me f f = 760 cm2V#1s#1 at field 0.08 MVcm#1 was obtained for p-Si/Si0%2Ge0%8/ Si0%5Ge0%5 MOSFETs. Efficiency of special n-type doped layer, also known as "punch-through" stopper, introduced into heterostructure is shown. Perfect I-V and also low frequency noise characteristics of investigated MOSFET show that the p-type Si/Si1#xGex/Si1#yGey (x "0'7 $0'9, x $y "0'3$0'4) heterostructures with "punch-through" stopper could be very impressive opportunity to conventional Si for modern semiconductor industry. For the first time, quantitative explanation of the low frequency noise reduction in metamorphic, high Ge content, SiGe p-MOSFETs compared to Si p-MOSFETs have been proposed. Quantitative analysis demonstrates the importance of both carrier number fluctuations and correlated mobility fluctuations (CMF) components to the 1/ f noise of surface channel Si p-MOSFET, but the absence of CMF for buried channel p-Si0%3Ge0%7 and p- Si0%2Ge0%8 MOSFETs. The low frequency noise was measured to be three times smaller for a 0.55 mm effective gate length p-Si0%3Ge0%7 MOSFET than the Si control, at linear regime (VDS = -50 mV) and high gate overdrive voltage (Vgt= -1.5 V). This result is very important, because we have reduction in LF noise at high gate overdrive voltages, which are typical for analogue and power electronics application. Both DC and low frequency noise characteristics show that access source and drain resistance for metamorphic p-SiGe MOSFETs (RS +RD ,1.5-2.0kW !mm) roughly 2 times lower then for conventional p-Si MOSFETs.

Denna licensiatavhandling behandlar oxidativ upplösning av UO2. Upplösning av UO2 studeras huvudsakligen då UO2-matrisen hos använt kärnbränsle förväntas fungera som en barriär mot frigörande av radionuklider i ett framtida djupförvar. Lösligheten av U(IV) är mycket låg under i djupförvaret rådande förhållanden emedan U(VI) har betydligt högre löslighet. Oxidation av UO2-matrisen kommer därför att påverka dess löslighet och därmed dess funktion som barriär. I denna avhandling studeras den relativa effektiviteten av en- och två-elektronoxidanter för upplösning av UO2. Vid låga oxidantkoncentrationer är utbytet för upplösningen för en-elektronoxidanter signifikant lägre än för två-elektronoxidanter. För en-elektronoxidanter ökar dock utbytet med ökande oxidanthalt, vilket kan förklaras av den ökade sannolikheten för två konsekutiva en-elektronoxidationer av samma reaktionssite och den ökade möjligheten till disproportionering.

Radikaler och molekylära radiolysprodukters relativa inverkan på oxidativ upplösning av UO2 studeras också i denna avhandling genom mätning av mängden upplöst U(VI) i γ-bestrålade system som dominerades av olika oxidanter. Dessa studier visade att upplösningshastigheten av UO2 kan uppskattas från oxidantkoncentrationer framtagna genom simuleringar av radiolys i motsvarande homogena system och hastighetskonstanterna för ytreaktionerna. Simuleringarna visar att de molekylära oxidanterna kommer vara de viktigaste oxidanterna i alla system i denna studie vid långa bestrålningstider (>10 timmar). Vid liknande simuleringar av α-bestrålade system fanns att vid förhållanden relevanta för ett djupförvar för använt kärnbränsle, är det endast de molekylära oxidanterna (i huvudsak H2O2) som är av betydelse för upplösningen av bränslematrisen.

Då använt kärnbränsle innehåller en mängd radionuklider som utsätter UO2-matrisen för kontinuerlig bestrålning, är det av vikt att undersöka hur bestrålning påverkar reaktiviteten av UO2. Bestrålningseffekten på reaktionen mellan UO2 och MnO4- studerades. Dessa försök visade att bestrålning av UO2 vid doser >40 kGy leder till att reaktiviteten ökar upp till 1.3 gånger reaktiviteten av obestrålad UO2. Den ökade reaktiviteten kvarstår efter bestrålningen och effekten kan därför möjligen tillskrivas permanenta förändringar i materialet. Vid uppskattning av reaktiviteten hos använt kärnbränsle måste hänsyn tas till denna effekt då bränslet redan efter ett par dagar i reaktor blivit utsatt för doser >40 kGy.

Det har tidigare föreslagits att hastigheten för en heterogen västka/fast-fas reaktion är beroende av partikelstorleken hos det fasta materialet, vilket har studerats för UO2-partiklar i denna avhandling. Experimentellt bestämda kinetiska parametrar jämförs med de föreslagna ekvationerna för fyra storleksfraktioner av UO2-pulver och en UO2-pellet. Studien visade partikelstorleksberoendet av andra ordningens hastighetskonstant och aktiveringsenergin för oxidation av UO2 med MnO4- beskrivs relativt väl av de föreslagna ekvationerna.

The general subject of this thesis is oxidative dissolution of UO₂. The dissolution of UO₂ is mainly investigated because of the importance of the UO₂ matrix of spent nuclear fuel as a barrier against radionuclide release in a future deep repository. U(IV) is extremely insoluble under the reducing conditions prevalent in a deep repository, whereas U(VI) is more soluble. Hence, oxidation of the UO₂-matrix will affect its solubility and thereby its function as a barrier. In this thesis the relative efficiency of one- and two electron oxidants in dissolving UO₂ is studied. The oxidative dissolution yield of UO₂ was found to differ between one- and two-electron oxidants. At low oxidant concentrations the dissolution yields for one-electron oxidants are significantly lower than for two-electron oxidants. However, the dissolution yield for one-electron oxidants increases with increasing oxidant concentration, which could be rationalized by the increased probability for two consecutive one-electron oxidations at the same site and the increased possibility for disproportionation.

Furthermore, the relative impact of radical and molecular radiolysis products on oxidative dissolution of UO₂ is investigated. Experiments were performed where the amount of dissolved U(VI) was measured in γ-irradiated systems dominated by different oxidants. We have found that the UO₂ dissolution rate in systems exposed to γ-irradiation can be estimated from oxidant concentrations derived from simulations of radiolysis in the corresponding homogeneous systems and rate constants for the surface reactions. These simulations show that for all systems studied in this work, the molecular oxidants will be the most important oxidants for long irradiation times (>10 hours). Similar simulations of α-irradiated systems show that in systems relevant for a deep repository for spent nuclear fuel, only the molecular oxidants (mainly H₂O₂) are of importance for the dissolution of the fuel matrix.

The effect on UO₂ reactivity by irradiation of the material is of importance when predicting the spent fuel dissolution rate since the fuel, due to its content of radionuclides, is exposed to continuous self-irradiation. The effect of irradiation on the reaction between solid UO₂ and MnO₄^- in aqueous solutions was studied. It was found that irradiation of UO2 at doses >40 kGy increases the reactivity of the material up to ~1.3 times the reactivity of unirradiated UO₂. The increased reactivity remains after the irradiation and can possibly be attributed to permanent changes in the material. This issue must be taken into account when predicting the reactivity of spent nuclear fuel since the fuel is exposed to doses >40 kGy after only a few days in the reactor.

It has earlier been suggested that the rate of a heterogeneous liquid-solid reaction depends on the size of the solid particles. This was investigated for UO₂ particles in this thesis. Experimental kinetic parameters are compared to the previously proposed equations for UO₂ powder of four size fractions and a UO₂ pellet. We have found that the particle size dependence of the second order rate constant and activation energy for oxidation of UO₂ by MnO₄^- is described quite well by the proposed equations.

Liquid chromatography is an essential technique in manufacturing biopharmaceuticals where it is used on all scales from analytical applications in R&D to full-scale production. In chromatography the target molecule, typically a protein, is separated and purified from other components and contaminants. Separation is based on different affinities of different molecules for the chromatographic medium and the physical and chemical properties of the latter determine the outcome. Controlling and designing those properties demand efficient analytical techniques. In this thesis the approach was to develop characterization methods based on nuclear magnetic resonance (NMR) spectroscopy for the assessment of various important physico-chemical properties. The rationale behind this strategy was that the versatility of NMR – with its chemical and isotopic specificity, high dynamic range, and direct proportionality between the integral intensity of the NMR signal and the concentration of spin-bearing atomic nuclei (e.g., 1H, 13C, 31P and 15N) – often renders it a very good choice for both qualitative and quantitative evaluations. These characteristics of NMR enabled us to develop two quantification methods for chromatography-media ligands, the functional groups that provide the specific interactions for the molecules being separated. Furthermore, a new method for measuring the distribution of macromolecules between the porous chromatographic beads and the surrounding liquid was established. The method, which we have named size-exclusion quantification (SEQ) NMR, utilizes the fact that it is possible to assess molecular size distribution from corresponding distribution of the molecular self-diffusion coefficient where the latter is accessible by NMR. SEQ-NMR results can also be interpreted in terms of pore-size distribution within suitable models. Finally, we studied self-diffusion of small molecules inside the pores of chromatographic beads. The results provided new insights into what affects the mass transport in such systems. The methods presented in this thesis are accurate, precise, and in many aspects better than conventional ones in terms of speed, sample consumption, and potential for automation. They are thus important tools that can assist a better understanding of the structure and function of chromatography media. In the long run, the results in this project may lead, via better chromatographic products, to better drugs and improved health.
Vätskekromatografi är en viktig teknik för tillverkning av biologiska läkemedel och används för alltifrån småskaliga analytiska applikationer till fullskalig produktion. I kromatografi separeras och renas målmolekylen (oftast ett protein), från andra komponenter och föroreningar genom att utnyttja molekylernas olika affinitet för det kromatografiska mediumet, vars fysikaliska och kemiska egenskaper har stor betydelse för hur separationen fungerar. För att kunna kontrollera och designa dessa egenskaper krävs effektiva analysmetoder. Strategin i den här avhandlingen var att utveckla metoder baserade på kärnmagnetisk resonans (NMR) spektroskopi för att karaktärisera flera viktiga fysikalisk-kemiska egenskaper. Anledningen till denna strategi är att mångsidigheten hos NMR – med dess kemiska och isotopiska specificitet, stora dynamiska omfång och direkta proportionalitet mellan NMR-signalens integralintensitet och koncentrationen av spinnbärande atomkärnor (t.ex. 1H, 13C, 31P och 15N) - ofta gör den till det bästa valet för både kvalitativa och kvantitativa tillämpningar. Dessa egenskaper hos NMR gjorde att vi kunde utveckla två kvantifieringsmetoder för kromatografimedia-ligander, dvs de funktionella grupperna som ger de specifika interaktioner som gör att molekylerna kan separeras. Dessutom har en ny metod för att mäta fördelningen av makromolekyler mellan de porösa kromatografiska pärlorna och den omgivande vätskan tagits fram. Metoden, som vi har valt att kalla size-exclusion quantification (SEQ) NMR, utnyttjar det faktum att det är möjligt att mäta molekylstorleksfördelningen genom att mäta motsvarande fördelning av självdiffusionskoefficienter, där den sistnämnda kan bestämmas med NMR. Resultaten från SEQ-NMR kan tolkas i termer av porstorleksfördelningar genom att använda lämpliga modeller. Slutligen studerade vi självdiffusion av små molekyler inuti porerna i kromatografiska pärlor. Resultaten gav nya insikter om vad som påverkar masstransporten i sådana system. De metoder som presenteras i denna avhandling är noggranna, precisa och på många sätt bättre än konventionella metoder när det gäller hastighet, låg provförbrukning och automatiseringspotential. De nya metoderna är därför viktiga verktyg som kan hjälpa till att ge en bättre förståelse av struktur och funktion hos kromatografimedia. I det långa loppet kan resultat från det här projektet kunna bidra till effektivare kromatografiska produkter, vilket i slutändan kan leda till bättre läkemedel och hälsa.

QC 20170403

La spectrométrie gamma à haute résolution offre un outil d'analyse performant pour effectuer des mesurages environnementaux. Dans le cadre de la caractérisation radiologique d'un site (naturelle ou artificielle) ainsi que pour le démantèlement d'installations nucléaires, la cartographie des radionucléides est un atout important. Le principe consiste à déplacer un spectromètre HPGe sur le site à étudier et, à partir des données nucléaires et de positionnements, d'identifier, de localiser et de quantifier les radionucléides présents dans le sol. Le développement de cet outil fait suite à une intercomparaison où un exercice orienté intervention a montré les limites des outils actuels. Une partie de ce travail s'est portée sur la représentation cartographique des données nucléaires. La connaissance des paramètres d'un spectre in situ a permis la création d'un simulateur modélisant la réponse d'un spectromètre se déplaçant au-dessus d'un sol contaminé. Ce simulateur a lui-même permis de développer les algorithmes de cartographie et de les tester dans des situations extrêmes et non réalisables. Ainsi, ce travail ouvre sur la réalisation d'un prototype viable donnant en temps réel les informations nécessaires sur l'identité et la position possible des radionucléides. La recherche réalisée sur la déconvolution des données permet de rendre en post traitement une carte de l'activité du sol par radionucléide mais également une indication sur la profondeur de la source. Le prototype nommé OSCAR (Outil Spectrométrique de Cartographie de Radionucléides) a ainsi été testé sur des sites contaminés (Suisse et Japon) et les résultats obtenus sont en accord avec des mesures de référence.

From the point of view of the electromagnetic interaction, empirical descriptions of the nucleus involve only a few parameters, one of the most important being the nuclear charge radius. This has been well measured for ground state nuclei, but it is difficult to measure for excited states, since they decay too quickly for conventional methods to be used. We study the atomic transitions in muonic ^{90}Zr and find that the nuclear charge radius of the first excited state can be inferred by measuring the gamma emissions from certain transitions. We find that with 1keV photon resolution, we can infer a difference between the charge radius of the nuclear ground state and first excited state as small as 0.13%. We will work in units where h = c = 4\pi\epsilon_0 = 1 so that e^2 = \alpha \approx 1/137 (unless otherwise specified). Mass, momentum, and energy will have units of eV, whereas distances will be given in eV^{-1}. In qualitative discussion, we will sometimes revert to discussing distances in meters due to the familiarity of typical scales (e.g. nuclear radius, Bohr radius). When working with 4-vectors in Minkowski space, we use the metric convention (+,-,-,-).
Graduate

In this thesis, I discuss two topics: The High Energy Focusing Telescope (HEFT) and the Nuclear Spectroscopic Telescope Array (NuSTAR). HEFT is the first experiment done with imaging telescopes in the hard X-ray energy band (~20-70 keV). I briefly describe the instrument and the balloon campaign. The inflight calibration of the Point Spread Function (PSF) is done with a point source observation (~50 minutes of Cyg X-1 observation). With the PSF calibrated, I attempt to measuring the size of the Crab Nebula in this energy band. Analysis for aspect reconstruction, optical axis determination and the size measurement are described in detail. The size of the Crab Nebula is energy dependent due to synchrotron burn-off. The measurement of the size at different energies can provide us with important parameters for the pulsar wind nebula (PWN) model such as the magnetization parameter. With ~60 minutes of observation of the Crab Nebula with HEFT, I measure the size of the Crab Nebula at energies of 25-58 keV. The analysis technique I used for the size measurement here can be used for measuring the size of astrophysical objects whose sizes are comparable to the width of the PSF. NuSTAR is a satellite version of the HEFT experiment although the spatial and spectral resolution of the optics are improved significantly. And thus, the fabrication technique for the HEFT optics needed to be modified. I describe the fabrication technique for the NuSTAR optics, focusing on the epoxy selection and process development and the metrology systems for characterizing the figure of the glass surfaces.

Positron emission tomography (PET) is a nuclear medicine diagnostic imaging exam of metabolic processes in the body. Radiotracers, which consist of positron emitting radioisotopes and a molecular probe, are introduced into the body, emitted radiation is detected, and tomographic images are reconstructed. The primary clinical PET application is in oncology using a glucose analogue radiotracer, which is avidly taken up by some cancers.

It is well known that PET performance and image quality degrade as body size increases, and epidemiological studies over the past two decades show that the adult US population's body size has increased dramatically and continues to increase. Larger patients have more attenuating material that increases the number of emitted photons that are scattered or absorbed within the body. Thus, for a fixed amount of injected radioactivity and acquisition duration, the number of measured true coincidence events will decrease, and the background fractions will increase. Another size-related factor, independent of attenuation, is the volume throughout which the measured coincidence counts are distributed: for a fixed acquisition duration, as the body size increases, the counts are distributed over a larger area. This is true for both a fixed amount of radioactivity, where the concentration decreases as size increases, and a fixed concentration, where the amount radioactivity increases with size.

Time-of-flight (TOF) PET is a recently commercialized technology that allows the localization, with a certain degree of error, of a positron annihilation using timing differences in the detection of coincidence photons. Both heuristic and analytical evaluations predict that TOF PET will have improved performance and image quality compared to non-TOF PET, and this improvement increases as body size increases. The goal of this dissertation is to parameterize the image quality improvement of TOF PET compared to non-TOF PET as a function of body size. Currently, no standard for comparison exists.

Previous evaluations of TOF PET's improvement have been made with either computer-simulated data or acquired data using a few discrete phantom sizes. A phantom that represents a range of attenuating dimensions, that can have a varying radioactivity distribution, and that can have radioactive inserts positioned throughout its volume would facilitate characterizing PET system performance and image quality as a function of body size. A fillable, tapered phantom, was designed, simulated, and constructed. The phantom has an oval cross-section ranging from 38.5 × 49.5 cm to 6.8 × 17.8 cm, a length of 51.1 cm, a mass of 6 kg (empty), a mass of 42 kg (water filled), and 1.25-cm acrylic walls.

For this dissertation research, PET image quality was measured using multiple, small spheres with diameters near the spatial resolution of clinical whole-body PET systems. Measurements made on a small sphere, which typically include a small number of image voxels, are susceptible to fluctuations over the few voxels, so using multiple spheres improves the statistical power of the measurements that, in turn, reduces the influence of these fluctuations. These spheres were arranged in an array and mounted throughout the tapered phantom's volume to objectively measure image quality as a function of body size. Image quality is measured by placing regions of interest on images and calculating contrast recovery, background variability, and signal to noise ratio.

Image quality as a function of body size was parameterized for TOF compared to non-TOF PET using 46 1.0-cm spheres positioned in six different body sizes in a fillable, tapered phantom. When the TOF and non-TOF PET images were reconstructed for matched contrast, the square of the ratio of the images' signal-to-noise ratios for TOF to non-TOF PET was plotted as a function, f(D), of the radioactivity distribution size, D, in cm. A linear regression was fit to the data: f(D) = 0.108D - 1.36. This was compared to the ratio of D and the localization error, σ_d, based on the system timing resolution, which is approximately 650 ps for the TOF PET system used for this research. With the image quality metrics used in this work, the ratio of TOF to non-TOF PET fits well to a linear relationship and is parallel to D/σ_d. For D < 20 cm, there is no image quality improvement, but for radioactivity distributions D > 20 cm, TOF PET improves image quality over non-TOF PET. PET imaging's clinical use has increased over the past decade, and TOF PET's image quality improvement for large patients makes TOF an important new technology because the occurrence of obesity in the US adult population continues to increase.

Dissertation

This study focuses on the analysis of atmospheric particles sampled from two different field campaigns: the field study at a cattle feeding facility in the summer from 2005 to 2008 and the Indirect and Semi-Direct Aerosol Campaign (ISDAC) in 2008. A ground site field study at a representative large cattle feeding facility in the Texas Panhandle was conducted to characterize the particle size distributions, hygroscopicity, and chemical composition of agricultural aerosols. Here, a first comprehensive dataset is reported for these physical and chemical properties of agricultural aerosols appropriate for use in a site-specific emission inventory. The emission rate and transport of the aerosols are also discussed. In addition, mixing ratios of total and gaseous ammonia were measured at the same field in 2007 and 2008. Measurements such as these provide a means to determine whether the fugitive dust emitted from a typical large feedlot represents a health concern for employees of the feeding operation and the nearby community. Detailed chemical composition of aircraft-sampled particles collected during ISDAC was studied. Filter samples were collected under a variety of conditions in and out of mixed phase and ice clouds in the Arctic. Specifically, particles were sampled from a mixed-phase cloud during a period of observed high concentrations of ice nuclei (IN), a biomass plume, and under relatively clean ambient conditions. Composition of particles was studied on a particle-by-particle basis using several microspectroscopy techniques. Based on the elemental composition analysis, more magnesium was found in Arctic cloud residues relative to ambient air. Likewise, based on the carbon speciation analysis, high IN samples contained coated inorganics, carbonate, and black or brown carbon particles. In the samples collected during a flight through a biomass burning plume, water-soluble organic carbon was the dominant overall composition. Due to their hygroscopic nature, these organics may preferably act as cloud condensation nuclei (CCN) rather than IN. Other ambient samples contained relatively higher fractions of organic and inorganic mixtures and less purely water-soluble organics than found in the biomass particles. The most likely source of inorganics would be sea salt. When present, sea salt may further enhance ice nucleation.