Combining theoretical chemistry and XANES multi-edge experiments to probe actinide valence states - Institut de Physique Nucléaire d'Orsay
Article Dans Une Revue Comptes Rendus. Chimie Année : 2007

Combining theoretical chemistry and XANES multi-edge experiments to probe actinide valence states

Résumé

Both structural and electronic properties of the actinide cations are of fundamental interest in order to describe the intramolecular interactions. The 5f and 6d orbitals are the first partially or totally vacant states of these elements and their properties reflect the nature of the actinideeligand bond. Because of its chemical and orbital selectivities, XANES spectroscopy is useful to probe the actinides' frontier orbitals and then understand the cation reactivity toward chelating ligands. The actinide L 3 edge contains structural information on the coordination polyhedron because of important scattering features. But very little electronic information can be extracted, due to the short core-hole lifetime, broadening the edge signal. On the other hand, the actinide M 4,5 edges provide a better resolution and allow one to achieve electronic and structural information. Furthermore, coupling simulations of the experimental spectra and quantum chemical calculations lead to quantitative information such as the determination of the actinide coordination sphere and its effective charge.

Fichier principal
Vignette du fichier
17 Fillaux CR_Chimie 2007.pdf (590.01 Ko) Télécharger le fichier
Origine Fichiers éditeurs autorisés sur une archive ouverte

Dates et versions

cea-04695780 , version 1 (12-09-2024)

Identifiants

Citer

Clara Fillaux, Jean-Claude Berthet, Steven D Conradson, Philippe Guilbaud, Dominique Guillaumont, et al.. Combining theoretical chemistry and XANES multi-edge experiments to probe actinide valence states. Comptes Rendus. Chimie, 2007, 10 (10-11), pp.859 - 871. ⟨10.1016/j.crci.2006.12.012⟩. ⟨cea-04695780⟩
50 Consultations
9 Téléchargements

Altmetric

Partager

More