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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.

La caméra à pixels hybrides XPAD3 intégrée dans le micro-CT PIXSCAN II est un nouveau dispositif dans lequel le comptage de photons remplace l’intégration de charges utilisée dans les systèmes de radiographie standard. XPAD3 apporte des avantages, en particulier l’absence de bruit de courant noir et la possibilité d’imposer un seuil de discrimination sur chaque pixel. Ces particularités ont pu être exploitées au cours de ce travail de thèse en imagerie préclinique classique sur petit animal et ont permis de faire la preuve de faisabilité d’un marquage ex vivo puis intra-vital des macrophages. D’autre part les capacités de cette caméra sont intéressantes pour le développement d’une nouvelle méthode d’imagerie spectrale dite au K-edge. L’imagerie au K-edge permet de différencier des compartiments contenant un agent de contraste par rapport à l’os dans des radiographies classiques. Elle est obtenue via l’étalonnage de 3 différents seuils autour de l’énergie de liaison de la couche K de l’agent de contraste considéré. Le développement d’un nouvel d’étalonnage avec l’utilisation de pixels composites a permis d’établir la preuve de concept d’un brevet et d’obtenir les premiers résultats sur souris vivantes en divisant le temps d’acquisition par 3 avec un compromis sur la résolution spatiale. Cette nouvelle approche peut être implémentée en "2 couleurs" pour séparer deux différents types d’agents de contraste. Ceci offre une nouvelle manière de visualiser des informations biologiques pertinentes dans un contexte applicatif visant à étudier de manière dynamique (longitudinale) l’interdépendance de la vascularisation et de la réponse immunitaire au cours du développement tumoral. / The hybrid pixel camera XPAD3 integrated in the micro-CT PIXSCAN II is a new device for which photon counting replaces charge integration used in standard X-ray CT. This novel approach involves advantages, in particular the absence of dark noise and the ability to set an energy threshold on each pixel of the detected photons. This features has been exploited during this thesis work for standard small animal preclinical imaging and permitted to establish the faisability of ex vivo, and then in vivo labelling of marcrophages. On another hand, the ability of this camera is of uppermost importance for the development of K-edge imaging approaches, which exploit spectral information on the counted photons. K-edge imaging permits to identify contrast agent compartiments with regards to bones in classical radiography. K-edge imaging is obtained by selecting, for each pixel calibration, those pixel that are set at one of the three different thresholds around the K-shell’s binding energy of the selected contrast agents and then to proceed with a subtraction analysis to the images obtained above and below the K-edge energy. We develop a new way of calibrating the XPAD3 detector that permits to provide the proof of concept of a patent, and to obtain the first results on living mice by dividing the acquisition time by three with a compromise on the resolution. This novel approach can be implemented in “2 colours” in order to separate clearly two different contrast agents. This brings a new way to visualize biological information and to provide possible future approaches for the study of the inter-dependance of vascularisation and inflammation during the tumor development.

The development of a non-invasive method of visualizing gene expression in larger animals could revolutionize some aspects of gene research by opening up a wider variety of animal systems to explore; some of which may be better models of human systems. Presently, most gene expression studies employ Green Fluorescent Protein (GFP) transfected into the genome of the animal system. For larger animals, an x-ray equivalent of GFP would be desirable due to the high penetrating power of x-rays. A model gene modification system is to use the Sodium (Na) Iodide Symporter (NIS) which will cause the accumulation of iodine in cells which express the NIS. To non-invasively observe the dilute iodine accumulated by the cancer cells transfected with NIS in the head of small animals, such as a rat, two synchrotron-based imaging methods were studied: K-Edge Subtraction (KES) imaging and Fluorescence Subtraction Imaging (FSI).<p> KES needs wide monochromatic x-ray beams at two energies bracketing the K-edge of the contrast agent existing or injected in the tissues. The monochromatic beam in the synchrotron facility normally is prepared by a double crystal monochromator. The appearance of the azimuthal angle (tilt error) in the double crystal monochromator creates intensity variations across the imaging field. This misalignment was studied through another two synchrotron-based imaging methods, Diffraction Enhanced Imaging (DEI) and Multi-Image Radiography (MIR), which show this problem clearly in their processed images. The detailed analysis of the effect of the tilt error, how it affects the resulting images, and how to quantify such an error were presented in the thesis. A post processing method was implemented and the artifacts caused by the improper experimental settings were discussed.<p> With the wide monochromatic beam prepared by the double crystal monochromator, a sequence of KES experiments were done and the detection limit of KES was quantified at a projected amount of 17.5mM-cm iodine in a physical model of a rat head with a radiation dose of 2.65mGy. With the raster scan of the object relative to the monochromatic pencil beam, FSI was studied to obtain higher Signal to Noise Ratio (SNR) for local area and better detection limit compared to KES. The detection limit of FSI was measured as a projected amount of 2.5mM-cm iodine in the same physical rat head with a tolerable radiation dose of 24mGy. According to the comparison of these two imaging techniques with references to imaging time and area, radiation dose, spatial resolution, and SNR, it was concluded that these two imaging techniques can be used complementarily in imaging dilute contrast material. Due to the short imaging time and large imaging area, KES is used first to provide a global view of the object, locate the area of interest, do the preliminary diagnosis, and decide whether the further FSI is necessary. Due to its high SNR for the dilute sample, FSI can be used when the area of interest is known. The combination of these two imaging techniques will be very promising and powerful. To facilitate the comparison of KES and FSI, a quality factor was developed to evaluate the performance of the imaging system.<p> The measured detection limits in our experiments are far beyond the thyroidal iodine concentration of a rat (around 1mM). To further improve the performance of KES, a bent Laue crystal monochromator was designed to do the simultaneous iodine KES imaging which overcomes the artifacts in the iodine image caused by the temporal difference for a single set of images. The designed monochromator can provide two separated x-ray beams bracketing the K-edge of iodine at the same time with a very high spatial resolution which is only depends on the source size, a very high energy resolution which can almost compete with that of the double crystal monochromator, and an acceptable photon flux.

The development of a non-invasive method of visualizing gene expression in larger animals could revolutionize some aspects of gene research by opening up a wider variety of animal systems to explore; some of which may be better models of human systems. Presently, most gene expression studies employ Green Fluorescent Protein (GFP) transfected into the genome of the animal system. For larger animals, an x-ray equivalent of GFP would be desirable due to the high penetrating power of x-rays. A model gene modification system is to use the Sodium (Na) Iodide Symporter (NIS) which will cause the accumulation of iodine in cells which express the NIS. To non-invasively observe the dilute iodine accumulated by the cancer cells transfected with NIS in the head of small animals, such as a rat, two synchrotron-based imaging methods were studied: K-Edge Subtraction (KES) imaging and Fluorescence Subtraction Imaging (FSI).<p> KES needs wide monochromatic x-ray beams at two energies bracketing the K-edge of the contrast agent existing or injected in the tissues. The monochromatic beam in the synchrotron facility normally is prepared by a double crystal monochromator. The appearance of the azimuthal angle (tilt error) in the double crystal monochromator creates intensity variations across the imaging field. This misalignment was studied through another two synchrotron-based imaging methods, Diffraction Enhanced Imaging (DEI) and Multi-Image Radiography (MIR), which show this problem clearly in their processed images. The detailed analysis of the effect of the tilt error, how it affects the resulting images, and how to quantify such an error were presented in the thesis. A post processing method was implemented and the artifacts caused by the improper experimental settings were discussed.<p> With the wide monochromatic beam prepared by the double crystal monochromator, a sequence of KES experiments were done and the detection limit of KES was quantified at a projected amount of 17.5mM-cm iodine in a physical model of a rat head with a radiation dose of 2.65mGy. With the raster scan of the object relative to the monochromatic pencil beam, FSI was studied to obtain higher Signal to Noise Ratio (SNR) for local area and better detection limit compared to KES. The detection limit of FSI was measured as a projected amount of 2.5mM-cm iodine in the same physical rat head with a tolerable radiation dose of 24mGy. According to the comparison of these two imaging techniques with references to imaging time and area, radiation dose, spatial resolution, and SNR, it was concluded that these two imaging techniques can be used complementarily in imaging dilute contrast material. Due to the short imaging time and large imaging area, KES is used first to provide a global view of the object, locate the area of interest, do the preliminary diagnosis, and decide whether the further FSI is necessary. Due to its high SNR for the dilute sample, FSI can be used when the area of interest is known. The combination of these two imaging techniques will be very promising and powerful. To facilitate the comparison of KES and FSI, a quality factor was developed to evaluate the performance of the imaging system.<p> The measured detection limits in our experiments are far beyond the thyroidal iodine concentration of a rat (around 1mM). To further improve the performance of KES, a bent Laue crystal monochromator was designed to do the simultaneous iodine KES imaging which overcomes the artifacts in the iodine image caused by the temporal difference for a single set of images. The designed monochromator can provide two separated x-ray beams bracketing the K-edge of iodine at the same time with a very high spatial resolution which is only depends on the source size, a very high energy resolution which can almost compete with that of the double crystal monochromator, and an acceptable photon flux.

The stability of the photon beam position on synchrotron beamlines is critical for most if not all synchrotron radiation experiments. On wiggler and bend magnet beamlines, the vertical position is most critical due to the large horizontal width of the beam. The position of the beam at the experiment or optical element location is set by the position and trajectory of the electron beam source as it traverses the magnetic field of the bend magnet or the insertion device. Thus an ideal photon beam monitor would be able to simultaneously measure the photon beam’s vertical position and angle, or its position in phase space. X-ray diffraction is commonly used to prepare a monochromatic beam on x-ray beamlines usually in the form of a double crystal monochromator using perfect crystals. Diffraction from crystals couples the photon wavelength or energy to the incident angle on the crystal or lattice planes within the crystal. A monochromatic beam from such a monochromator will contain a spread of energies due to the vertical divergence of the photon beam from the source. This range of energies can easily cover the absorption edge of an element such as iodine at 33.17keV. It has been found that a system composed of a double crystal monochromator and an iodine filter that horizontally covers part of the monochromatic beam and an imaging detector can be used to independently and simultaneously measure the position and angle of the photon beam. This information can then be translated back to determine the vertical position and angle, or vertical phase space, of the electron beam source. This approach to measurement of the phase space of the source has not been done before and thus this study is the first of its kind. The goal of this thesis is to investigate the use of this combined monochromator, filter and detector as a phase space beam position monitor. The system was tested for sensitivity to position and angle under a number of synchrotron operating conditions (normal operations and special operating modes where the beam is intentionally altered in position and angle). These results were compared to other methods of beam position measurement from the literature to assess the utility of such a system as a beam diagnostic, a feedback element for electron beam control and a source of information that could be used to correct the experimental data to account for beam position and angle motion.

Spectral computed tomography (CT) has proven an important development in biomedical imaging, yet there are several limitations to this nascent technology. Near-term implementation of spectral CT imaging can be enhanced using a hybrid architecture that integrates a narrow-beam spectral 'interior' imaging chain integrated with a traditional wide-beam 'global' imaging chain. The first study demonstrates the feasibility of hybrid spectral micro-CT architecture with a first-of-its-kind system implementation and preliminary results showing improved contrast resolution and spatial resolution. The second study seeks to characterize the hybrid spectral micro-CT scan protocol for reduction of radiation exposure. In the third study, the spectral 'interior' imaging chain was optimized for K-edge imaging of high-z elemental contrast agents. In the final study, an open-source, low-cost solution for managing digital content in an academic setting was demonstrated. The results of these studies confirm the merits of a hybrid architecture and warrant further consideration in future pre-clinical and clinical spectral micro-CT and CT scanner design and protocols. / Ph. D.

Ma thèse de doctorat s’inscrit à l’interface entre la physique expérimentale et la biologie. Ce travail a été développé au sein de l’équipe imXgam du CPPM, qui a construit un prototype de micro-tomographie pour le suivi non-invasif du petit animal, équipé d’une caméra à pixels hybrides XPAD3 fonctionnant en mode comptage de rayons X. Le comptage de rayons X rendu possible par la technologie des pixels hybrides, permet de s’affranchir du bruit électronique et d’augmenter ainsi la détectabilité des tissus faiblement contrastés. Elle présente de plus la capacité d'appliquer à chaque pixel un seuil de détection en énergie permettant d’accéder à l’information spectrale des rayons X détectés et ouvre la voie au développement d’une méthode d’imagerie spectrale dite au K-edge, qui permet de différencier des agents de contraste particuliers. La caméra XPAD3 développée avec un capteur en Si présente une efficacité de détection qui limite son utilisation pour l’imagerie du vivant. Une caméra XPAD3 avec une meilleure efficacité au delà de 25 keV a été assemblée avec des capteurs en CdTe. Dans un premier temps, nous avons effectué une comparaison des caméras XPAD3/Si et XPAD3/CdTe en imagerie d’absorption standard et en imagerie au K-edge. Nous avons ensuite, en collaboration avec des biologistes de l’IBDM, assuré le suivi quantitatif et in vivo sur plusieurs mois, du développement de tumeurs hépatiques chez un modèle spécifique de souris et de l’efficacité d’un traitement ciblant les cellules tumorales. Enfin, nous avons développé un protocole d’acquisition spectrale à faible dose pour réaliser une tomographie spectrale in vivo d’un foie de souris en exploitant le K-edge du baryum. / My PhD thesis is at the interface between experimental physics and biology. This work has been developed within the imXgam team at CPPM, which has built a micro-computed tomography prototype for the non-invasive longitudinal monitoring of small animal, equipped with the XPAD3 hybrid pixel camera that operates in X-ray photon counting mode. X-ray photon counting that has been made possible by hybrid pixels, allows to free images from the electronic noise and thus to increase detectability of weakly contrasted tissues. Moreover, it provides the possibility to set an energy threshold for each pixel that allows to accessing spectral information on the detected X-rays and paving the way to the development of a spectral imaging modality also named K-edge imaging, which allows to differentiate selected contrast agents. Actually, the XPAD3 camera developed with a Si sensor presents a low detective efficiency that limits its use for biomedical imaging. A XPAD3 camera with a better efficiency above 25 keV has been assembled with high-Z CdTe sensors. Firstly, we have performed a comparison of XPAD3/Si and XPAD3/CdTe cameras for standard absorption CT and K-edge imaging. Then, in collaboration with a team of biologists from IBDM, we have carried out the quantitative and in vivo follow-up of hepatic tumour development in a specific mouse model over several months, and of the effectiveness of a treatment targeting these tumour cells. Finally, we have developed a protocol for low dose acquisition of spectral data to realize an in vivo spectral tomography of a mouse liver using the barium spectral signature.

The goal in medical x-ray imaging is to obtain the image quality requiredfor a given detection task, while ensuring that the patient dose is kept as lowas reasonably achievable. The two most common strategies for dose reductionare: optimizing incident x-ray beams and utilizing energy informationof transmitted beams with new detector techniques (spectral imaging). Inthis thesis, dose optimization schemes were investigated in two x-ray imagingsystems: digital mammography and computed tomography (CT). In digital mammography, the usefulness of anti-scatter grids was investigatedas a function of breast thickness with varying geometries and experimentalconditions. The general conclusion is that keeping the grid is optimalfor breasts thicker than 5 cm, whereas the dose can be reduced without a gridfor thinner breasts. A photon-counting silicon-strip detector developed for spectral mammographywas characterized using synchrotron radiation. Energy resolution, ΔE/Ein, was measured to vary between 0.11-0.23 in the energy range 15-40 keV, which is better than the energy resolution of 0.12-0.35 measured inthe state-of-the-art photon-counting mammography system. Pulse pileup hasshown little effect on energy resolution. In CT, the performance of a segmented silicon-strip detector developedfor spectral CT was evaluated and a theoretical comparison was made withthe state-of-the-art CT detector for some clinically relevant imaging tasks.The results indicate that the proposed photon-counting silicon CT detector issuperior to the state-of-the-art CT detector, especially for high-contrast andhigh-resolution imaging tasks. The beam quality was optimized for the proposed photon-counting spectralCT detector in two head imaging cases: non-enhanced imaging and Kedgeimaging. For non-enhanced imaging, a 120-kVp spectrum filtered by 2half value layer (HVL) copper (Z = 29) provides the best performance. Wheniodine is used in K-edge imaging, the optimal filter is 2 HVL iodine (Z = 53)and the optimal kVps are 60-75 kVp. In the case of gadolinium imaging, theradiation dose can be minimized at 120 kVp filtered by 2 HVL thulium (Z =69). / <p>QC 20160401</p>

Co-doped ZnO (ZnO:Co) thin film with room temperature ferromagnetism and spin polarized carriers is one of the advance materials and highly applicable in future development in spintronics. When ZnO:Co films deposited by a £_ growth method in a ion sputtering system, low solubility of Co (3.75%) limits further applications such that a single-guns sputtering thin film growth technique is employed in this study to outreach this limitation. A ZnO:Co bulk with 5 at% of Co was formed by a solid reaction method and used as a target. ZnO:Co films were grown in a single-gun RF sputtering system. However, all films grown at room temperature were insulator which might because sufficient oxygen content in the target and the negative charge of oxygen ion moving toward substrate making the films of full oxygen content. In this study, the post annealing in vacuum environment and the deposition of films in hydrogenation environment are conducted to try to produce various level of oxygen vacancies in the films for understanding the interplay between the oxygen vacancies and the electric transport and magnetic coupling. The present experiment contains two parts: (1) grow films with various thicknesses by controlling deposition time and then applying post annealing process, and (2) grow the films in oxygen reduced environment by introducing hydrogen during growth and taking out partial oxygen content in the plasma and the films. In the first part, the grain sizes of the films are near constant while the crystal quality is improved with the thickness of films. The worse crystal quality of grains, the better the electric transport and the stronger the magnetic coupling after post annealing processes. This indicates that the electric transport and magnetic coupling could be improved when the thin films was formed by crystals with certain disordering and contained a certain level of oxygen vacancies. In the second part, the introduced hydrogen may combine with the oxygen sputtered out from the target before deposition on substrates. It means that the films are grown in oxygen deficient conditions and result in various degrees of oxygen vacancies. Zn clusters precipitate in films when the concentration of hydrogen is over 20%, and at the meantime, they increase the conductivity and suppress the magnetic coupling in the films. These discoveries provide new perspective in understand the electric transport and ferromagnetism mechanics in DMS materials.