Highly resolved synchrotron-based investigations related to nuclear waste disposal
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Highly resolved synchrotron-based investigations related to nuclear waste disposal Melissa A. Denecke1, Manuela Borchert2, Robert G. Denning3, Wout de Nolf4, Gerald Falkenberg2, Susanne Hönig5, Martina Klinkenberg6, Kristina Kvashnina7, Stefan Neumeier6, Jens Patommel5, Tobias Petersmann8, Tim Pruessmann1, Stephan Ritter5, Christian G. Schroer5, Sandra Stephan5, Julie Villanova7, Tonya Vitova1, Gerd Wellenreuther2 1
Karlsruhe Institute of Technology, Institut für Nukleare Entsorgung, Postfach 3640, D-76021 Karlsruhe, Germany 2 Deutsches Elektronen-Synchrotron (DESY), Notkestr. 85, D-22607 Hamburg, Germany 3 University of Oxford, Magdalen College, High Street, OX1 4AU, United Kingdom 4 Department of Chemistry, University of Antwerp, Universiteitsplein 1, B-2610 Antwerp, Belgium 5 Technische Universität Dresden, Institut für Strukturphysik, D-01062 Dresden, Germany 6 Forschungszentrum Jülich, Institut für Energie- und Klimaforschung (IEK-6), Nukleare Entsorgung und Reaktorsicherheit, D-52425 Jülich, Germany 7 European Synchrotron Radiation Facility (ESRF), Grenoble, 38043, France 8 European Joint Research Center, Institute for Transuranium Elements (ITU), D-76344 Eggenstein-Leopoldshafen, Germany ABSTRACT Synchrotron-based X-ray techniques are used increasingly to characterize actinide element speciation in heterogeneous media related to nuclear waste disposal safety. Especially techniques offering added temporal, spatial and energy resolved information are advancing our understanding of f-element physics and chemistry in general and of actinide element waste disposal in particular. Examples of investigations of uranium containing systems using both highly (energy) resolved X-ray emission spectroscopy (HRXES) techniques and spatially resolved techniques with focused X-ray beams are presented in this paper: polarization dependent partial fluorescence yield X-ray absorption near edge structure (PD-PFY-XANES) spectroscopic studies of a single Cs2UO2Cl4 crystal, which experimentally reveal a splitting of the V, S and G components of the 6d valence states [1], and characterization of UO2/Mo thin films prepared on different substrates using a combination of techniques (2D and 3D micro- and nano-X-ray fluorescence, XANES and both holographic and ptychographic tomography). INTRODUCTION Advances in the brilliance and coherence of synchrotron-based X-ray techniques combined with increasing need by the scientific community for improved spatial and energy resolution are driving forces in development of new (nano) materials and improving understanding of structure/bonding relationships. Such techniques find increasing application to characterize f-element physics and chemistry in general and of actinide element waste disposal in particular. We have recently applied a high (energy) resolved X-ray emission spectroscopy (HRXES) technique, polarization dependent partial fluorescence yield X-ray absorption near edge structure (PD-PFY-XANES), to characterize empty valence state energies and occupancies
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in single crystal Cs2UO2Cl
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