The advent of highly-coherent x-ray light sources, such as those now available world-wide in modern third-generation synchrotrons and increasingly available in free-electron lasers, is driving the need for improved analytical and experimental techniques which exploit the coherency of the generated light. As the light illuminating a sample approaches full coherence, a simple Fourier transform describes the diffraction pattern generated by the scattered light in the far field; because the Fourier transform of an object is unique, coherent scattering can directly probe local structure in the scattering object instead of bulk properties. In this dissertation, we exploit the coherence of Advanced Light Source beamline 12.0.2 to build three types of novel coherent scattering microscopes. First, we extend the techniques of coherent diffractive imaging and Fourier transform holography, which uses iterative computational methods to invert oversampled coherent speckle patterns, into reflection geometry. This proof-of-principle experiment demonstrates a method by which reflection Bragg peaks, such as those from the orbitally-ordered phase of complex metal oxides, might eventually be imaged. Second, we apply a similar imaging method to the x-ray beam itself to directly image the mutual coherence function with only a single diffraction pattern. This technique supersedes the double-slit experiments commonly seen in the scattering literature to measure the mutual intensity function by using a set of apertures which effectively contains all possible double slit geometries. Third, we show how to evaluate the speckle patterns taken from a labyrinthine domain pattern for "hidden" rotational symmetries. For this measurement, we modify the iterative algorithms used to invert speckle patterns to generate a large number of domain configurations with the same incoherent scattering profile as the candidate pattern and then use these simulations as the basis for a statistical inference of the degree of ordering in the domain configuration. We propose extending this measurement to position-resolved speckle patterns, creating a symmetry-sensitive microscope. The three new techniques described herein may be employed at current and future light sources.

No description available.

xxv, 207 p. ; ill. (some col.) A print copy of this title is available from the UO Libraries, under the call number: SCIENCE QD172.T6 T87 2008 / A growing interest in the physics of complex systems such as in the transition-metal oxide family has exploded recently, especially in the last 20 years or so. One notable effect is the change in electrical resistivity of a system by orders of magnitude in an applied magnetic field, coined the "colossal magnetoresistance effect". In efforts to understand these types of effects, there has been an unveiling of a rich variety of phenomena in the field of strongly correlated electron physics that has come to dominate the current scientific times. Most notable is the competition of myriad types of order: magnetic, lattice, charge and orbital all self-organize to display a fascinating array of phases on a variety of length scales. Furthermore, it has become apparent that new probes are needed to grasp some of this physics that transcends current condensed matter theory, where much of the behavior of these types of systems has remained unexplored. We have developed a new technique to gain more information about the system than with conventional x-ray diffraction. By scattering highly coherent, low energy x-rays, we can measure manganite speckle: a "fingerprint' of the microscopic structure in the bulk. The coherence of the x-rays can further be used to elucidate new insight into the dynamics of these phases. We describe here a number of novel effects near the orbital order phase transition in a half-doped manganite. We observe a small fluctuating component in the scattered signal that is correlated with three effects: both a rapidly decreasing total signal and orbital domain size, as well as an abrupt onset of a broad background intensity that we attribute to the thermal production of correlated polarons. Our results suggest that the transition is characterized by a competition between a pinned orbital domain topology that remains static, and mobile domain boundaries that exhibit slow, spatiotemporal fluctuations. This study opens up a new chapter to the study of manganite physics as coherent x-ray scattering offers a new direction to understand the strange and exotic behavior demonstrated in the multifaceted manganites. / Adviser: Stephen Kevan

The field of X-ray imaging and X-ray diffraction have been combined in a new technique called Tomographic Energy Dispersive Diffraction Imaging (TEDDI). This diffraction imaging technique allows 3D sample images to be obtained, non-destructively, where each imaged point contains the atomic structural information associated with its diffraction pattern. The main drawback of the TEDDI technique is the long collection times needed to produce the images. In order to overcome this obstacle the rapid TEDDI (rTEDDI) system has been developed at the University of Manchester's Material Science Centre. The research and development of rTEDDI has been the focus of this PhD thesis. A proof of concept for the rTEDDI imaging technique was obtained using thin samples on station 7.6 SRS Daresbury. In this case a first generation array collimator was used in conjunction with an energy resolving Si pixelated detector. Structural information such as lattice parameters, crystal system and phase identiffcation were obtained for metal, polymer and deer antler bone samples. The use of high Z semiconductor detector material was investigated in order to increase the potential of TEDDI for larger and more dense samples. To enable penetration of larger samples high energy X-rays needed to be utilized. In order to detect these higher energies with a good efficiency the detector media was changed from Si to CdZnTe (CZT).The second generation rTEDDI, using CZT as the detection media, was intended to be used under high flux/high energy synchrotron radiation conditions. Testing of the system under these conditions on station 16.3 SRS Daresbury showed an inability to produce diffraction imaging. An in depth investigation into detector and collimator array performance showed a two fold cause. The ERD2004 detector was unable to handle the high countrates experienced during high flux/high energy synchrotron radiation conditions. The MK1.2 collimator array was found to become partially transparent to X-ray energies around the absorption edge of W resulting in the swamping of the diffraction signal under high flux/high energy synchrotron radiation conditions. A new detector Application Specific Integrated Circuit (ASIC) design, developed by the detector division and the Rutherford Appleton Laboratory, and Data Aquisition (DAQ) system, developed by Aspect Systems, as well as a number of new collimator array designs were developed and tested. Testing of the new collimator array structures have shown positive results and the new HEXITECdetector which was designed to be able to handle high countrates, have shown an unprecedented inter pixel uniformity and energy resolution which have been attributed to the ASIC performance and the use of better quality CZT material.

Diffraction Enhanced Imaging (DEI) is an X-ray imaging technique providing specific information about the molecular structure of a tissue by means of coherently scattered photons. A Controlled Drift Detector (CDD) is a novel 2D silicon imager developed to be used in X-ray imaging techniques. In this work a final (complete and detailed) analysis of DEI data taken with the CDD in the ELETTRA synchrotron light source facility in Trieste (Italy) in 2005, is presented and the applicability of both this new technique and the novel detector are discussed.

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L’imagerie basée sur la diffraction des rayons X est une technique non-invasive puissante pour l’identification et caractérisation de matériaux différents. Comparée aux techniques traditionnelles utilisant la transmission des rayons X, elle permet d’extraire des informations beaucoup plus caractéristiques pour le matériau inspecté, comme les positions des pics de Bragg pour des matériaux cristallins et le facteur de forme moléculaire pour les matériaux amorphes. Le potentiel de cette méthode a été reconnu par de nombreuses équipes de recherche et de nombreuses applications comme l’inspection de bagage, le contrôle non-destructif, la détection de drogue et la caractérisation de tissus biologiques ont été proposées. La méthode par dispersion d’énergie (EDXRD) est particulièrement adaptée à ce type d’application car elle permet l’utilisation d’un tube à rayons X conventionnel, l’acquisition du spectre entier en une fois et des architectures parallélisées pour l’inspection d’un objet entier en un temps raisonnable. L’objectif de ce travail est d’optimiser toute la chaîne de caractérisation. L’optimisation comprend deux aspects : l’optimisation du système d’acquisition et du traitement des données. La dernière concerne particulièrement la correction des spectres de diffraction dégradés par le processus d’acquisition. Des méthodes de reconstruction sont proposées et validées sur des spectres simulés et expérimentaux. L’optimisation du système est réalisée en utilisant des facteurs de mérite comme l’efficacité quantique de détection (DQE), le rapport contraste sur bruit (CNR) et les courbes de caractéristiques opérationnelles de réception (ROC).La première application choisie, c’est l’imagerie du sein basée sur la diffraction qui a pour but de distinguer des tissus cancéreux des tissus sains. Deux configurations de collimation sans multiplexage combinant EDXRD et ADXRD sont proposées suite au processus d’optimisation. Une étude de simulation du système entier et d’un fantôme de sein a été réalisée afin de déterminer la dose requise pour la détection d’un petit carcinome de 4 mm. La deuxième application concerne la détection de matériaux illicites pendant le contrôle de sécurité. L’intérêt possible d’un système de collimation multiplexé a été étudié. / X-ray diffraction imaging is a powerful noninvasive technique to identify or characterize different materials. Compared to traditional techniques using X-ray transmission, it allows to extract more material characteristic information, such as the Bragg peak positions for crystalline materials as well as the molecular form factor for amorphous materials. The potential of this technique has been recognized by many researchers and numerous applications such as luggage inspection, nondestructive testing, drug detection and biological tissue characterization have been proposed.The method of energy dispersive X-ray diffraction (EDXRD) is particularly suited for this type of applications as it allows the use of a conventional X-ray tube, the acquisition of the whole spectrum at the same time and parallelized architectures to inspect an entire object in a reasonable time. The purpose of the present work is to optimize the whole material characterization chain. Optimization comprises two aspects: optimization of the acquisition system and of data processing. The last one concerns especially the correction of diffraction pattern degraded by acquisition process. Reconstruction methods are proposed and validated on simulated and experimental spectra. System optimization is realized using figures of merit such as detective quantum efficiency (DQE), contrast to noise ratio (CNR) and receiver operating characteristic (ROC) curves.The first chosen application is XRD based breast imaging which aims to distinguish cancerous tissues from healthy tissues. Two non-multiplexed collimation configurations combining EDXRD and ADXRD are proposed after optimization procedure. A simulation study of the whole system and a breast phantom was realized to determine the required dose to detect a 4 mm carcinoma nodule. The second application concerns detection of illicit materials during security check. The possible benefit of a multiplexed collimation system was examined.