The main purpose of this Thesis is the experimental characterization of the electronic and geometric structures of objects called clusters. A cluster consists of a finite group of bound atoms or molecules. Due to its finite size, it may present completely different properties than those of the isolated atom and the bulk. The clusters studied in this work are constituted by rare-gas atoms, organic molecules, and metal atoms. Intense cluster beams were created using either an adiabatic expansion source or a gas-aggregation source, and investigated by means of synchrotron radiation based photoelectron spectroscopy. The reports presented in this Thesis may be divided into three parts. The first one deals with results concerning homogeneous molecular clusters (benzene- and methyl-related clusters) highlighting how molecular properties, such as dipole moment and polarizability, influence the cluster structure. The second part focuses on studies of solvation processes in clusters. In particular, the adsorption of polar molecules on rare-gas clusters is studied. It is shown that the doping method, i.e. the technique used to expose clusters to molecules, and the fraction of polar molecules are important factors in determining the location of the molecules in the clusters. Finally, a summary of investigations performed on metal clusters is presented. The applicability of solid state models to analyse the cluster spectra is considered, and the differences between the atomic, cluster and solid electronic structures are discussed.

This thesis concerns the development and characterisation of X-ray imaging systems based on single photon processing. “Colour” X-ray imaging opens up new perspectives within the fields of medical X-ray diagnosis and also in industrial X-ray quality control. The difference in absorption for different “colours” can be used to discern materials in the object. For instance, this information might be used to identify diseases such as brittle-bone disease. The “colour” of the X-rays can be identified if the detector system can process each X-ray photon individually. Such a detector system is called a “single photon processing” system or, less precise, a “photon counting system”. With modern technology it is possible to construct photon counting detector systems that can resolve details to a level of approximately 50 µm. However with such small pixels a problem will occur. In a semiconductor detector each absorbed X-ray photon creates a cloud of charge which contributes to the image. For high photon energies the size of the charge cloud is comparable to 50 µm and might be distributed between several pixels in the image. Charge sharing is a key problem since, not only is the resolution degenerated, but it also destroys the “colour” information in the image. This thesis presents characterisation and simulations to provide a detailed understanding of the physical processes concerning charge sharing in detectors from the MEDIPIX collaboration. Charge summing schemes utilising pixel to pixel communications are proposed. Charge sharing can also be suppressed by introducing 3D-detector structures. In the next generation of the MEDIPIX system, Medipix3, charge summing will be implemented. This system, equipped with a 3D-silicon detector, or a thin planar high-Z detector of good quality, has the potential to become a commercial product for medical imaging. This would be beneficial to the public health within the entire European Union. / Denna avhandling berör utveckling och karaktärisering av fotonräknande röntgensystem. ”Färgröntgen” öppnar nya perspektiv för medicinsk röntgendiagnostik och även för materialröntgen inom industrin. Skillnaden i absorption av olika ”färger” kan användas för att särskilja olika material i ett objekt. Färginformationen kan till exempel användas i sjukvården för att identifiera benskörhet. Färgen på röntgenfotonen kan identifieras om detektorsystemet kan detektera varje foton individuellt. Sådana detektorsystem kallas ”fotonräknande” system. Med modern teknik är det möjligt att konstruera fotonräknande detektorsystem som kan urskilja detaljer ner till en upplösning på circa 50 µm. Med så små pixlar kommer ett problem att uppstå. I en halvledardetektor ger varje absorberad foton upphov till ett laddningsmoln som bidrar till den erhållna bilden. För höga fotonenergier är storleken på laddningsmolnet jämförbar med 50 µm och molnet kan därför fördelas över flera pixlar i bilden. Laddningsdelning är ett centralt problem delvis på grund av att bildens upplösning försämras, men framför allt för att färginformationen i bilden förstörs. Denna avhandling presenterar karaktärisering och simulering för att ge en mer detaljerad förståelse för fysikaliska processer som bidrar till laddningsdelning i detektorer från MEDIPIX-projekter. Designstrategier för summering av laddning genom kommunikation från pixel till pixel föreslås. Laddningsdelning kan också begränsas genom att introducera detektorkonstruktioner i 3D-struktur. I nästa generation av MEDIPIX-systemet, Medipix3, kommer summering av laddning att vara implementerat. Detta system, utrustat med en 3D-detektor i kisel, eller en tunn plan detektor av högabsorberande material med god kvalitet, har potentialen att kunna kommersialiseras för medicinska röntgensystem. Detta skulle bidra till bättre folkhälsa inom hela Europeiska Unionen.

Die Entwicklung und Erprobung von metallischen Implantatwerkstoffen mit biologischen Beschichtungen für den Einsatz im menschlichen Knochen verlangt, neben der Untersuchung grundlegender zellbiologischer Wechselwirkungen, eine ganzheitliche Betrachtung ihrer Wirkungsweise im lebenden Organismus. Die vorwiegend angewandte Methode zur Quantifizierung des Potentials von Biofunktionalisierungen metallischer Implantate ist dabei die histologische Auswertung. Diese stützt sich aber auf Informationen aus nur wenigen und eher zufälligen Schnittlagen im Probenvolumen, was mit einer hohen Anzahl an Tierexperimenten ausgeglichen wird. Mit der Mikrocomputertomographie steht neben der klassischen Histologie eine zerstörungsfreie Methode zur Verfügung, welche eine detaillierte dreidimensionale Darstellung des neugebildeten Knochengewebes ermöglicht. Die Abbildungsqualität des mineralischen Knochengewebes um Titanimplantate, als Grundlage für eine Vergleichbarkeit von Tomographie und Histologie, wurde anhand von drei Mikrofokus-Computertomographen und einem Synchrotron-Computertomographen am HASYLAB untersucht. Die tomographische Untersuchung von Hartgewebe einschließlich metallischer Implantate zeigte mit Hilfe von Synchrotronstrahlung die beste qualitative Übereinstimmung zur histologischen Bildgebung. Für die Quantifizierung der Knochenneubildung wurden interaktive Analysemodelle erarbeitet, welche eine vereinheitlichte Auswertung von histologischen und tomographischen Informationen erlaubt. Auf Grundlage der entwickelten Analyseprozeduren war es erstmals möglich, die statistische Belastbarkeit der Ergebnisse aus der histologischen und tomographischen Analyse zu untersuchen. Dabei konnte gezeigt werden, dass hinsichtlich der Herausstellung von Unterschieden bei der Osseointegration modifizierter Titanimplantate mit beiden Methoden ähnliche Ergebnistrends gefunden werden. Eine Signifikanz (p < 0,01) der Unterschiede bei der Knochenneubildung konnte jedoch ausschließlich mit der mikrotomographischen Analyse herausgestellt werden. Die Ergebnisse bei der Darstellung und Analyse des mineralischen Gewebes durch die Nutzung der Synchrotrontomographie gehen weit über die Grenzen der histologischen Untersuchungen hinaus. Durch den dreidimensionalen Charakter der Informationen ergeben sich dabei neue Bewertungsmodelle zur Beurteilung der Osseointegration von biofunktionalisierten Implantaten. Die mikrotomographische Analyse führt gegenüber der histologischen Auswertung durch die geringe Irrtumswahrscheinlichkeit der Ergebnisse bei deutlich verminderter Probenanzahl zu einer erheblichen Verringerung von Tierversuchen.

Seit mit den Synchrotronstrahlungsquellen dritter Generation hochbrillante Röntgenquellen zur Verfügung stehen, haben sich Vollfeldmikroskopie und Rastersondenmikroskopie mit harter Röntgenstrahlung als besonders nützliche Untersuchungsmethoden etabliert. Insbesondere bei der vergrößernden Mikroskopie mit harter Röntgenstrahlung werden Röntgenkameras mit hoher Anforderung bezüglich der Ortsauflösung benötigt. Im Rahmen dieser Diplomarbeit wurde ein zweidimensionaler Röntgendetektor für die Mikroskopie mit harter Röntgenstrahlung entworfen, gebaut und im Experiment getestet und charakterisiert. Hauptaugenmerk war dabei ein möglichst hohes Ortsauflösungsvermögen des Detektors verbunden mit einem großen effektiven dynamischen Bereich. Als vielversprechendes Konzept erwies sich dabei die Verwendung eines einkristallinen Szintillators, der mittels einer Mikroskopoptik auf einen CCD-Chip abgebildet wird. Im Experiment stellte sich heraus, dass der im Zuge dieser Diplomarbeit konzipierte Flächendetektor sämtliche an ihn gestellten Anforderungen hervorragend erfüllt. Obwohl ursprünglich für die vergrößernde Tomographie mit harter Röntgenstrahlung entwickelt, findet die Röntgenkamera darüber hinaus beim Justieren nanofokussierender refraktiver Röntgenlinsen in Rastersondenmikroskopen Verwendung. / With the advent of highly-brilliant third generation synchrotron radiation sources, hard x-ray full-field microscopy and hard x-ray scanning microscopy were developed and have been shown to be excellent methods for scientific investigations. Especially for magnified hard x-ray full-field microscopy, there is the need for two-dimensional x-ray detectors with highest demands on spatial resolution and effective dynamic range. In the course of this diploma thesis, such an area x-ray detector with high spatial resolution and large dynamic range was designed and built and then tested and characterized in experiment. The high-resolution x-ray camera consists of a visible light microscope which images the sensitive layer of a single-crystal scintillator on the CCD chip of a CCD camera. A test experiment gave evidence that the x-ray camera actually fulfills all the requirements with regard to spatial resolution, sensitivity and effective dynamic range. Originally, the detector was developed for magnified hard x-ray tomography, but in addition, it is applied for alignment purposes of nanofocusing refractive x-ray lenses in a hard x-ray scanning microscope.

La mesure de l’émittance transverse du faisceau est fondamentale pour tous les accélérateurs, et en particulier pour les collisionneurs, son évaluation precise étant essentielle pour maximiser la luminosité et ainsi la performance des faisceaux de collision.Le rayonnement synchrotron (SR) est un outil polyvalent pour le diagnostic non-destructif de faisceau, exploité au CERN pour mesurer la taille des faisceaux de protons des deux machines du complexe dont l’énergie est la plus élevée, le SPS et le LHC où l’intensité du faisceau ne permet plus les techniques invasives.Le travail de thèse documenté dans ce rapport s’est concentré sur la conception, le développement, la caractérisation et l’optimisation des moniteurs de taille de faisceau basés sur le SR. Cette étude est fondée sur un ensemble de calculs théoriques, de simulation numériques et d’expériences conduite au sein des laboratoires et accélérateurs du CERN. Un outil de simulation puissant a été développé, combinant des logiciels classiques de simulation de SR et de propagation optique, permettant ainsi la caractérisation complète d’un moniteur SR de la source jusqu’au détecteur.La source SR a pu être entièrement caractérisée par cette technique, puis les résultats validés par observation directe et par la calibration à basse énergie basée sur les mesures effectuées avec les wire-scanners (WS), qui sont la référence en terme de mesure de taille de faisceau, ou telles que la comparaison directe avec la taille des faisceaux obtenue par déconvolution de la luminosité instantanée du LHC.Avec l’augmentation de l’énergie dans le LHC (7TeV), le faisceau verra sa taille diminuer jusqu’à atteindre la limite de la technique d’imagerie du SR. Ainsi, plusieurs solutions ont été investiguées afin d’améliorer la performance du système: la sélection d’une des deux polarisations du SR, la réduction des effets liés à la profondeur de champ par l’utilisation de fentes optiques et l’utilisation d’une longueur d’onde réduite à 250 nm.En parallèle à l’effort de réduction de la diffraction optique, le miroir d’extraction du SR qui s’était avéré être la source principale des aberrations du système a été entièrement reconçu. En effet, la détérioration du miroir a été causée par son couplage EM avec les champs du faisceau, ce qui a conduit à une surchauffe du coating et à sa dégradation. Une nouvelle géométrie de miroir et de son support permettant une douce transition en termes de couplage d’impédance longitudinale dans le beam pipe a été définie et caractérisée par la technique dite du “streched wire”. Egalement, comme méthode alternative à l’imagerie directe, un nouveau moniteur basé sur la technique d’interférométrie à deux fentes du SR, non limité par la diffraction, a également été développé. Le principe de cette méthode est basé sur la relation directe entre la visibilité des franges d’interférence et la taille de faisceau.Comme l’emittance du faisceau est la donnée d’intérêt pour la performance du LHC, il est aussi important de caractériser avec précision l’optique du LHC à la source du SR. Dans ce but, la méthode “K-modulation” a été utilisée pour la première fois au LHC en IR4. Les β ont été mesurés à l’emplacement de tous les quadrupoles et ont été évalués via deux algorithmes de propagation différents au BSRT et au WS. / Measuring the beam transverse emittance is fundamental in every accelerator, in particular for colliders, where its precise determination is essential to maximize the luminosity and thus the performance of the colliding beams.
 Synchrotron Radiation (SR) is a versatile tool for non-destructive beam diagnostics, since its characteristics are closely related to those of the source beam. At CERN, being the only available diagnostics at high beam intensity and energy, SR monitors are exploited as the proton beam size monitor of the two higher energy machines, the Super Proton Synchrotron (SPS) and the Large Hadron Collider (LHC). The thesis work documented in this report focused on the design, development, characterization and optimization of these beam size monitors. Such studies were based on a comprehensive set of theoretical calculations, numerical simulations and experiments.A powerful simulation tool has been developed combining conventional softwares for SR simulation and optics design, thus allowing the description of an SR monitor from its source up to the detector. 
The simulations were confirmed by direct observations, and a detailed performance studies of the operational SR imaging monitor in the LHC, where different techniques for experimentally validating the system were applied, such as cross-calibrations with the wire scanners at low intensity (that are considered as a reference) and direct comparison with beam sizes de-convoluted from the LHC luminosity measurements.In 2015, the beam sizes to be measured with the further increase of the LHC beam energy to 7 TeV will decrease down to ∼190 μm. In these conditions, the SR imaging technique was found at its limits of applicability since the error on the beam size determination is proportional to the ratio of the system resolution and the measured beam size. Therefore, various solutions were probed to improve the system’s performance such as the choice of one light polarization, the reduction of depth of field effect and the reduction of the imaging wavelength down to 250 nm.In parallel to reducing the diffraction contribution to the resolution broadening, the extraction mirror, found as the main sources of aberrations in the system was redesigned. Its failure was caused by the EM coupling with the beam’s fields that led to overheating and deterioration of the coating. A new system’s geometry featuring a smoother transition in the beam pipe was qualified in terms of longitudinal coupling impedance via the stretched wire technique. A comparison with the older system was carried out and resulted in a reduction of the total power dissipated in the extraction system by at least a factor of four.A new, non-diffraction limited, SR-based monitor based on double slit interferometry was designed as well as an alternative method to the direct imaging. Its principle is based on the direct relation between the interferogram fringes visibility and the beam size.Since the beam emittance is the physical quantity of interest in the performance analysis of the LHC, determining the optical functions at the SR monitors is as relevant as measuring the beam size. The “K-modulation” method for the optical function determination was applied for the first time in the LHC IR4, where most of the profile monitors sit. The βs at the quadrupoles were measured and via two different propagation algorithms the βs at the BSRT and the WS were obtained reducing significantly the uncertainty at the monitors location.

No description available.

This thesis introduce my work on transverse and longitudinal non linear dynamics of an electron beam in ThomX, a novel X-ray source based on Compton backscattering. In this work I implemented in simulation code theoretical models to calculate transverse and longitudinal non linear dynamics under Compton back scattering. The processes studied include collective effect such as longitudinal space charge, resistive wall and coherent synchrotron radiation, intra beam scattering. I also implemented a longitudinal feedback algorithm and studied the effect of the feedback's delay in the simulation to explore its effects on beam dynamics. This code allows to perform a full 6D simulation of the beam dynamics in a ring under Compton back scattering taking into account the feedback stabilisation for the 400 000 turns (~ 20 ms) of one injection cycle. One important feature is that this simulation code can be run on a computer farm. Using this code I investigated the electrons dynamics in ThomX and the flux of scattered Compton photons. I analysed the relative contribution of each physical phenomena to the overall beam dynamics and how to mitigate their disruptive effect. As part of my work on longitudinal phase feedback I also measured and analysed properties of the ELETTRA RF cavity to be used on ThomX.

This thesis work reports in depth analyses of measured µ-XRD and µ-XAS data from standard UO2, chromia (Cr2O3) doped UO2 and MOX fuels, and interpretation of the results considering the role of chromium as a dopant as well as several fission product elements. The lattice parameters of UO2 in fresh and irradiated samples and elastic strain energy densities in the irradiated UO2 samples have been measured and quantified. The µ-XRD patterns have further allowed the evaluation of the crystalline domain size and sub-grain formation at different locations of the irradiated fuel pellets. Attempts have been made to determine lattice parameter and next neighbor atomic environment in chromia-precipitates found in fresh chromia-doped fuel pellets. The local structure around Cr in as-fabricated chromia-doped UO2 matrix and the influence of irradiation on the state of chromium in irradiated fuel matrix have been addressed. Finally, for a comparative understanding of fission gases behavior and irradiation induced re-solution phenomenon in standard and chromia-doped UO2, the last part of the present work tries to clarify the fission gas Kr atomic environment in these irradiated fuels. The work performed on Kr, by micro-beam XAS, comprises the determination of Kr next neighbor distances, an estimation of gas atom densities in the aggregates, and apparent internal pressures in the gas bubbles.

19 Dec 2004. / Published through the Information Bridge: DOE Scientific and Technical Information. "IS-T 1936" Jongik Park. 12/19/2004. Report is also available in paper and microfiche from NTIS.

Bimetallic Rh-V system was studied by means of surface science experimental methods. Properties of ultra-thin Rh-V layers supported by γ-Al2O3 were compared with model systems prepared by vacuum V deposition on Rh(111), Rh(110) and polycrystalline rhodium. Formation of ordered V- Rh(111)-(2×2), V-Rh(110)-(2×1) and V-Rh(110)-(1×2) subsurface alloys and their electronic and atomic structure were investigated and models of the surface reconstructions were proposed. Influence of the subsurface alloy formation on interaction with CO and O2 molecules as well as the influence of the molecule adsorption on this alloy was investigated. The bond between CO molecules and Rh-V alloy surface was weakened due to pronounced changes in surface valence band structure. Oxygen which adsorbed on the alloy surface reacted with the subsurface vanadium at elevated temperature and blocked the interaction of the metal substrate with CO molecules.