Resonant inelastic X-ray scattering tools to count 5 f electrons of actinides and probe bond covalency
The actinides possess a complex electronic structure, making their chemical and physical properties among the least understood in the periodic table. Advanced spectroscopic tools, able to obtain deep insights into the electronic structure and binding properties of the actinides, are highly desirable. Here, we introduce two sensitive spectroscopic tools: one determines the number of localized 5f electrons on an actinide atom, and another assesses the covalent character of actinide-ligand bonding. Both tools are based on the multiplet structure present in actinide M<sub>4</sub> edge core-to-core resonant inelastic X-ray scattering (CC-RIXS) maps. The spectral intensity of different many-body final-state multiplets directly depends on the local many-electron ground-state symmetry including the local 5 f spin configuration. By comparing U M<sub>4</sub> edge CC-RIXS data for 21 U, Np, Pu and Am compounds, we demonstrate the ability to compare the number of localized 5 f electrons and bond covalency across the actinide series.
Authors
- Jacob A. Branson (ORCID: https://orcid.org/0000-0002-3523-0303)
- Dieter Schild (ORCID: https://orcid.org/0000-0001-6034-8146)
- Thomas S. Neill (ORCID: https://orcid.org/0000-0002-4316-1328)
- Karin Popa (ORCID: https://orcid.org/0000-0003-2759-6492)
- Harry Ramanantoanina (ORCID: https://orcid.org/0000-0002-2086-6958)
- Jörg Göttlicher (ORCID: https://orcid.org/0009-0007-7230-8011)
- A. Beck (ORCID: https://orcid.org/0000-0002-9097-185X)
- Marinella Mazzanti (ORCID: https://orcid.org/0000-0002-3427-008X)
- David Fellhauer (ORCID: https://orcid.org/0000-0002-7440-0790)
- Olaf Walter (ORCID: https://orcid.org/0000-0002-2679-1715)
- Bianca Schacherl (ORCID: https://orcid.org/0000-0003-4542-0108)
- Christopher L. Cahill (ORCID: https://orcid.org/0000-0002-2015-3595)
- Tonya Vitova (ORCID: https://orcid.org/0000-0002-3117-7701)
- Cedric Yves Reitz (ORCID: https://orcid.org/0000-0001-8285-0815)
- Cory J. Windorff (ORCID: https://orcid.org/0000-0002-5208-9129)
- M. W. Haverkort (ORCID: https://orcid.org/0000-0002-7216-3146)
- Ruwini S. K. Ekanayake (ORCID: https://orcid.org/0000-0002-5255-1969)
- Thomas Sittel (ORCID: https://orcid.org/0000-0003-3523-036X)
- Dominique M. Brager (ORCID: https://orcid.org/0000-0003-0694-0805)
- C.F. Vollmer (ORCID: https://orcid.org/0000-0002-2687-0149)
- Michelangelo Tagliavini (ORCID: https://orcid.org/0009-0008-2967-0864)
- Hanna Kaufmann-Heimeshoff (ORCID: https://orcid.org/0000-0002-2977-9551)
Institutions
- New Mexico State University (US)
- Karlsruhe Institute of Technology (DE)
- Lawrence Berkeley National Laboratory (US)
- George Washington University (US)
- Heidelberg University (DE)
- University of Manchester (GB)
- Joint Research Centre (DE)
- École Polytechnique Fédérale de Lausanne (CH)
- Heidelberg Institute for Theoretical Studies (DE)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-02-10
- DOI
- https://doi.org/10.1038/s41467-024-54574-7
- Citations
- 13
- Primary Topic
- Radioactive element chemistry and processing
- Type
- article
- Field-Weighted Citation Impact
- 6.99
Funders
- U.S. Department of Energy
- George Washington University
- University of Washington
- New Mexico State University
- European Commission
- Deutsche Forschungsgemeinschaft
- Office of Science
- Basic Energy Sciences
- Chemical Sciences, Geosciences, and Biosciences Division
- Lawrence Berkeley National Laboratory