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Fundamentals of Actinide Chemistry by Cutting Edge X-ray Methods and Models

Kvashnina, K.

Abstract

Understanding the mechanisms of different chemical reactions with actinides at the atomic level is a key step towards safe disposal of nuclear wastes and towards the identification of physical-chemical processes of radionuclides in the environment. This contribution will provide an overview of the recently performed studies on Uranium, Thorium, Plutonium and Cerium contained materials at the Rossendorf Beamline (ROBL) of the European Synchrotron (ESRF) in Grenoble (France). This innovative, recently upgraded, world-wide unique experimental station, funded and operated by HZDR in Dresden (Germany) was used to study actinide systems by several experimental methods: X-ray absorption spectroscopy in high energy resolution fluorescence detection (HERFD) mode, Resonant inelastic X-ray scattering (RIXS) at the An L3 and M4,5 edge and X-ray diffraction (XRD). We will show how the detail information about local and electronic structure of actinide materials can be obtained, including information on the electron-electron interactions, hybridization between molecular orbitals, the occupation and the degree of the f-electron localization. The experimental spectral features have been analysed using a number of theoretical methods based on density functional theory and atomic multiplet theory. It might be of interest for fundamental research in chemistry and physics of actinide systems as well as for the applied science.

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Permalink: https://www.hzdr.de/publications/Publ-28658