The study aims to achieve an understanding of the artist’s materials and techniques used by Lucky Madlo Sibiya when he created his carved and painted wood panel artworks. A survey of the artist’s materials and techniques is of great importance, because he is represented in multiple institutional, corporate and private collections – including the University of Pretoria. His carved and painted wood panel artworks are also reaching an age (at least 20 years old, as 2019 is the twentieth anniversary of his death) when they would soon require conservation and restoration, if not stored and displayed according to sound conservation conditions and standards. For best-practice conservation and restoration, in-depth knowledge of the materiality of an artwork is needed. In order to reach an in-depth knowledge of the materiality of Sibiya’s carved and painted wood panel artworks, the survey intends to examine and document through the combination of various historical, visual and analytical techniques artworks with unrefuted provenance. The analytical techniques used are popular in heritage conservation, because they are non-invasive and non-destructive. They include provenance studies, visual examination, technical photography, X-ray Fluorescence and Fourier-transform Infrared Spectroscopy. In combination, the techniques should reveal the materials and techniques Sibiya employed. This knowledge will be used to safeguard and preserve this part of South African art heritage. / Mini Dissertation (MSocSci)--University of Pretoria, 2020. / Tangible Heritage Conservation / MSocSci (Tangible Heritage Conservation) / Unrestricted

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著者名別形の記述を修正（2022-04-21） / 京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第16850号 / 工博第3571号 / 新制||工||1540(附属図書館) / 29525 / 京都大学大学院工学研究科材料工学専攻 / (主査)教授 河合 潤, 教授 酒井 明, 教授 大塚 浩二 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM

Contrast agents are often crucial in medical imaging for disease diagnosis. Novel contrast agents, such as gold nanoparticles (AuNPs) and lanthanides, are being ex- plored for a variety of clinical applications. Preclinical testing of these contrast agents is necessary before being approved for use in humans, which requires the use of small animal imaging techniques. Small animal imaging demands the detection of these contrast agents in trace amounts at acceptable imaging time and radiation dose. Two such imaging techniques include x-ray fluorescence computed tomography (XFCT) and photon-counting CT (PCCT). XFCT combines the principles of CT with x-ray fluorescence by detecting fluorescent x-rays from contrast agents at various projections to reconstruct contrast agent maps. XFCT can image trace amounts of AuNPs but is limited to small animal imaging due to fluorescent x-ray attenuation and scatter. PCCT uses photon-counting detectors that separate the CT data into energy bins. This enables contrast agent detection by recognizing the energy dependence of x-ray attenuation in different materials, independent of AuNP depth, and can provide anatomical information that XFCT cannot. To achieve the best of both worlds, we modeled and built a table-top x-ray imaging system capable of simultaneous XFCT and PCCT imaging. We used Monte Carlo simulation software for the following work in XFCT imaging of AuNPs. We simulated XFCT induced by x-ray, electron, and proton beams scanning a small animal-sized object (phantom) containing AuNPs with Monte Carlo techniques. XFCT induced by x-rays resulted in the best image quality of AuNPs, however high-energy electron and medium-energy proton XFCT may be feasible for on-board x-ray fluorescence techniques during radiation therapy. We then simulated a scan of a phantom containing AuNPs on a table-top system to optimize the detector arrangement, size, and data acquisition strategy based on the resulting XFCT image quality and available detector equipment. To enable faster XFCT data acquisition, we separately simulated another AuNP phantom and determined the best collimator geometry for Au fluorescent x-ray detection. We also performed experiments on our table-top x-ray imaging system in the lab. Phantoms containing multiples of three lanthanide contrast agents were scanned on our tabletop x-ray imaging system using a photon-counting detector capable of sustaining high x-ray fluxes that enabled PCCT. We used a novel subtraction algorithm for reconstructing separate contrast agent maps; all lanthanides were distinct at low concentrations including gadolinium and holmium that are close in atomic number. Finally, we performed the first simultaneous XFCT and PCCT scan of a phantom and mice containing both gadolinium and gold based on the optimized parameters from our simulations. This dissertation outlines the development of our tabletop x-ray imaging system and the optimization of the complex parameters necessary to obtain XFCT and PCCT images of multiple contrast agents at biologically-relevant concentrations. / Graduate

<p>Transition metals, such as iron, manganese, and copper are essential in the development and function of biological systems. However, disrupted levels of transition metals are highly cytotoxic, and metal homeostasis is strictly maintained in cells under normal conditions. The neuropathology of several brain disorders, such as Alzheimer’s disease and Parkinson’s disease has been linked to altered metal levels. This work focused on the measurement of iron, manganese, and copper, with the aim of better elucidating their role in brain disease.</p> <p>Two experiments were carried out in C57Bl/6 mice looking at metal homeostasis: <em>1.</em> following manganese injections typically administered in manganese-enhanced MRI animal studies, and <em>2.</em> following copper deficiency in a cuprizone model of demyelination. Metal measurements were made in the brain and visceral organs using X-ray fluorescence to measure iron and copper concentrations, and neutron activation analysis to measure manganese concentrations.</p> <p>In the MEMRI study in this work, in addition to the expected manganese concentration increases in brain regions, a statistically significant decrease in iron concentration in the thalamus was found. This change in iron levels in the thalamus following manganese injections should serve as a caution that care should be taken when interpreting signal changes in brain regions.</p> <p>The cuprizone study in this thesis confirmed that copper levels are reduced following cuprizone administration. Surprisingly, manganese concentrations were significantly higher in several brain regions that have demyelination in this model, but not iron or copper. The mechanism of cuprizone toxicity was related to manganese neurotoxicity that may contribute to demyelination.</p> / Master of Science (MSc)

Previous studies have shown an association between Pb exposure and intelligence quotient (IQ). Up until now, there is a lack of technology and methodology to assess the effects of long-term Pb exposure (such as de-myelination) in brain in-vivo. So we are developing a mouse model that will allow us to assess in vivo Pb in bone and brain structure and myelination using magnetic resonance imaging (MRI). In this project, we will discuss the feasibility of an in vivo x-ray fluorescence (XRF) system for the Pb measurement in the skeleton of whole mice. A review of literature is conducted in chapter 1. Health impacts of lead, measurement of lead, pre-existing bone Pb phantoms and mouse model selection are explained thoroughly. In chapter 2, calibration and minimum detection limits (MDLs) for the XRF measurements are documented. Calibration was performed using Plaster of Paris phantoms mimicking human bone doped with Pb concentrations ranging from 0 to 100 ppm. Detection limits for the pre-existing bone Pb phantoms were found to be 1.52 μg Pb/g plaster for 1-hour measurement. For 2 strains of Pb free mice (CD-1 and C57BL/6J), which had skull and hind facing detectors respectively, MDLs of 5.66 – 7.78 μg Pb/g and 6.69 – 8.50 μg Pb/g were determined for 3-hour measurement. This detectability of MDLs by the XRF system encourages us to proceed to measure mouse-mimicking phantoms. In order to evaluate the feasibility of a 109Cd XRF system for the Pb measurement in the skeleton of whole mice, mouse-mimicking phantoms were made and measured. The effect of variations in Pb distribution across the mouse and the applicability of the normalization in mice are discussed in chapter 3. To sum up, our system can measure Pb in whole mice in vivo at the levels of Pb in bone that are anticipated in brain de-myelination studies. Our results indicate that if multiple orientations (rotated) are measured in mice, the mean bone Pb level in whole mice will be determined accurately. / Thesis / Master of Science (MSc)

Ce projet vise à développer un protocole d’analyses par fluorescence aux rayons X (XRF) afin d’appréhender le potentiel de cette méthode d’analyse géochimique à distinguer des sources de cherts du Nord-Ouest irlandais. Ces échantillons de roches ont été récoltés dans le cadre du projet Irish Lithic Landscapes dirigé par Killian Driscoll, Adrian Burke et Heather Short. Le but est donc la caractérisation des sources de matières premières utilisées par les populations préhistoriques durant la fin du Mésolithique, le Néolithique ainsi qu’au début de l’Âge du Bronze. Ces analyses pourraient ainsi compléter la base de données LIR (Lithotheque Ireland) référençant les sources de matières premières lithiques irlandaises, cette dernière pouvant ainsi être utilisée pour comparer les données géologiques et archéologiques et permettre de considérer les stratégies d’acquisition des populations anciennes et d’identifier la source de certains artéfacts en chert. La technique analytique de la fluorescence X n’étant pas sans contraintes, l’analyse statistique fut un défi. Ce projet de mémoire a mis en avant la difficulté que représentent les limites de détections propres à l’appareil XRF PANalytical Epsilon 3 ainsi que les problèmes liés à la taille des échantillonnages et à la variabilité intra-source lorsqu’elle est supérieure à celle inter-source. Bien que les résultats ne soient pas aussi concluants que souhaités, il en reste néanmoins que cette recherche est un premier pas pour des études plus poussées sur les cherts de cette région et ainsi comprendre et dépasser les problèmes rencontrés. / The aim of this project is to develop an X-ray fluorescence (XRF) analysis protocol in order to understand the potential of this geochemical analysis method to distinguish between sources of cherts in the North-West of Ireland. These rock samples were collected as part of the Irish Lithic Landscapes project led by Killian Driscoll, Adrian Burke and Heather Short, with the aim of characterizing the sources of raw materials used by prehistoric populations during the Late Mesolithic, Neolithic and early Bronze Ages. These analyses could thus complement the LIR (Lithotheque Ireland) database referencing Irish lithic raw material sources, which could then be used to compare geological and archaeological data, to consider the acquisition strategies of ancient populations and to identify the source of certain chert artifacts. As the analytical technique of X-ray fluorescence is not without its constraints, statistical analysis was a challenge. This dissertation project highlighted the difficulty represented by the detection limits specific to the PANalytical Epsilon 3 XRF instrument, as well as problems linked to sampling size and intra-source variability when it is greater than inter-source variability. Although the results are not as conclusive as desired, the fact remains that this research is a first step towards more in-depth studies of the cherts in this region, in order to understand and overcome the problems encountered.

Pyroprocessing is an electrochemical method for recovering actinides from used nuclear fuel and recycling them into fresh nuclear fuel. It is posited herein that proposed safeguards approaches on pyroprocessing for nuclear material control and accountability face several challenges due to the unproven plutonium-curium inseparability argument and the limitations of neutron counters. Thus, the Hybrid K-Edge Densitometer is currently being investigated as an assay tool for the measurement of pyroprocessing materials in order to perform effective safeguards. This work details the development of a computational model created using the Monte Carlo N-Particle code to reproduce HKED assay of samples expected from the pyroprocesses. The model incorporates detailed geometrical dimensions of the Oak Ridge National Laboratory HKED system, realistic detector pulse height spectral responses, optimum computational efficiency, and optimization capabilities. The model has been validated on experimental data representative of samples from traditional reprocessing solutions and then extended to the sample matrices and actinide concentrations of pyroprocessing. Data analysis algorithms were created in order to account for unsimulated spectral characteristics and correct inaccuracies in the simulated results. The realistic assay results obtained with the model have provided insight into the extension of the HKED technique to pyroprocessing safeguards and reduced the calibration and validation efforts in support of that design study. Application of the model has allowed for a detailed determination of the volume of the sample being actively irradiated as well as provided a basis for determining the matrix effects from the pyroprocessing salts on the HKED assay spectra.

Gold nanoparticles (GNPs) have recently attracted considerable interest for use in radiation therapy due to their unique physical and biological properties. Of interest, GNPs (and other high-atomic-number materials) have been used to enhance radiation dose in tumors by taking advantage of increased photoelectric absorption. This physical phenomenon is well-understood on a macroscopic scale. However, biological outcomes often depend on the intratumoral and even intracellular distribution of GNPs, among other factors. Therefore, there exists a need to precisely visualize and accurately quantify GNP distributions. By virtue of the photoelectric effect, x-ray fluorescence (XRF) photons (characteristic x-rays) from gold can be induced and detected, not only allowing the distribution of GNPs within biological samples to be determined but also providing a unique molecular imaging option in conjunction with bioconjugated GNPs. This work proposes the use of this imaging modality, known as XRF imaging, to develop experimental imaging techniques for detecting and quantifying sparse distributions of GNPs in preclinical settings, such as within small-animal-sized objects, tissue samples, and superficial tumors. By imaging realistic GNP distributions, computational methods can then be used to understand radiation dose enhancement on an intratumoral scale and perhaps even down to the nanoscopic, subcellular realm, elucidating observed biological outcomes (e.g., radiosensitization of tumors) from the bottom-up. Ultimately, this work will result in experimental and computational tools for developing a better understanding of GNP-mediated dose enhancement and associated radiosensitization within the scope of GNP-aided radiation therapy.

Sediment records of two Italian subalpine lakes (Lake Garda and Lake Ledro) were analyzed in order to reconstruct their ecological evolution over the past several hundred years. A multi-proxy and multi-site approach was applied in order to disentangle the effects of local anthropogenic forcings, such as nutrients, and climate impacts on the two lakes and their catchments. Biological indicators (sub-fossil pigments, diatoms and Cladocera) were used to reconstruct changes in the aquatic food web and to define the lake reference conditions, while geochemical methods, i.e. wavelength-dispersive X-ray fluorescence spectroscopy (WD-XRF), were used to provide quantitative information on the different physical or chemical processes affecting both lake and catchment systems. Sub-fossil pigments and diatoms, together with their respective inferred TP values, suggested very stable oligotrophic conditions in both lakes until the 1960s. The period following was affected by nutrient enrichment, which led to a drastic shift in the phytoplanktonic community. The response of sub-fossil pigments and diatoms to major climatic anomalies such as the Medieval Climatic Anomaly (MCA) and the Little Ice Age (LIA) were not pronounced, and the taxonomic composition remained relatively stable. On the contrary, these proxies showed an indirect response to climate variability since the beginning of the nutrient enrichment phase in the 1960s. In Lake Garda, the winter temperature regulates the water column mixing, which in its turn controls the degree of nutrient fertilization of the entire water column, and the related phytoplankton growth. In Lake Ledro a rapid reorganization of planktonic diatoms was observed only during the temperature recovery after the LIA, while recent temperature effects are masked by the prevailing nutrient effects. In Lake Garda, Cladocera remains responded in quantitative and qualitative terms to climatic changes, whereas in Lake Ledro they appeared to be mainly affected by variations in hydrological regimes, i.e. flood events. Cladocera remains corroborated the nutrient enrichment after the 1960s in both lakes as inferred by diatoms and pigments. In Lake Garda, the geochemical data showed a pronounced shift in elemental composition since the mid-1900s, when major elements and lithogenic tracers started to decrease, while some elements related to redox conditions and other (contaminant) trace elements increased. The general trends since the mid-1900s agree with the biological records. However, some differences recorded in the two different basins of Lake Garda reflected the effects of local conditions, both related to hydrology and sedimentation patterns. Lake Ledro showed higher short-term variability for most elements, even though some features were comparable to Lake Garda. The geochemical record of Lake Ledro revealed a major influence of human-induced lake-level fluctuations and catchment properties. This paleolimnological study allows us to place temporally restricted limnological surveys into a longer-term secular perspective, which is highly valuable for the definition of lake reference conditions. Because the restoration targets are usually based on the lake reference conditions, this study highlighted also the necessity to pay particular attention to the lake-specific sensitivity patterns. The multi-proxy and multi-site approach showed that the lake conditions of large and deep lakes in northern Italy, such as Lake Garda, are mainly driven by nutrient enrichment and/or climate change. In contrast, smaller lakes with larger catchment areas, such as Lake Ledro, are seemingly more impacted by conditions and processes occurring in the drainage basin.