Study of electronic structure in the L-edge spectroscopy of actinide materials: UO2 as an example

Literature Information

Publication Date 2019-03-18
DOI 10.1039/C9CP01021A
Impact Factor 3.676
Authors

Harry Ramanantoanina, Goutam Kuri, Matthias Martin, Johannes Bertsch


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Abstract

While the electronic structure calculation for actinide materials, using ligand-field phenomenology in conjunction with density functional theory (LFDFT) treating configurations with single or two open-shells 5f and 6d electrons, is well established and currently practiced, the consideration of the three open-shells electron configurations for LFDFT treatment is a challenging task addressed in the present work. Herein, we report the first-principles method, developed for the first time on the basis of LFDFT, to evaluate the uranium L3-edge X-ray absorption near-edge structure (XANES), which requires non-equivalent active electrons within the 2p, 5f and 6d orbitals of the uranium ion. The theoretical results, when compared with the experimental XANES data measured from uranium dioxide fresh fuel pellets and rector-exposed spent fuel materials, show good agreement with the experimental findings elucidating the local oxidation in the spent fuel materials. This report is relevant for the commonly used L-edge spectroscopy of actinide isotopes and important for understanding the structural, optical and electronic properties of actinide-based materials.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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