Resonant inelastic X ray scattering tools to count 5f 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 M4 edge core-to-core resonant inelastic X-ray scattering (CC-RIXS)maps. The spectral intensity of different many-body finalstate multiplets directly depends on the local many-electron ground-state symmetry including the local 5 f spin configuration. By comparing U M4 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.

SCHACHERL Bianca;  TAGLIAVINI Michelangelo;  KAUFMANN Hanna;  GÖTTLICHER Jörg;  MAZZANTI Marinella;  POPA Karin;  WALTER Olaf;  PRÜSSMANN Tim;  VOLLMER Christian;  BECK Aaron;  EKANAYAKE Ruwini;  BRANSON Jacob;  NEILL Thomas;  FELLHAUER David;  REITZ Cedric;  SCHILD D.;  BRAGER Dominique;  CAHILL Christopher;  WINDORFF Cory;  SITTEL Thomas;  RAMANANTONINA Harry;  HAVERKORT Maurits;  VITOVA Tonya; 

2025-02-12

NATURE PORTFOLIO

JRC134939

2041-1723 (online),   

https://www.nature.com/articles/s41467-024-54574-7,    https://publications.jrc.ec.europa.eu/repository/handle/JRC134939,   

10.1038/s41467-024-54574-7 (online),