Litcius/Paper detail

Application of multi-edge HERFD-XAS to assess the uranium valence electronic structure in potassium uranate (KUO<sub>3</sub>)

René Bes, Gregory Leinders, Kristina Kvashnina

2021Journal of Synchrotron Radiation16 citationsDOIOpen Access PDF

Abstract

is reported on the basis of a comprehensive experimental study using multi-edge HERFD-XAS and relativistic quantum chemistry calculations based on density functional theory. Very good agreement is obtained between theory and experiments, including the confirmation of previously reported Laporte forbidden f-f transitions and X-ray photoelectron spectroscopic measurements. Many spectral features are clearly identified in the probed U-f, U-p and U-d states and the contribution of the O-p states in those features could be assessed. The octahedral crystal field strength, 10Dq, was found to be 6.6 (1.5) eV and 6.9 (4) eV from experiment and calculations, respectively. Calculated electron binding energies down to U-4f states are also reported.

Topics & Concepts

Electronic structureValence (chemistry)UraniumDensity functional theoryBinding energyChemistryOctahedronPotassiumX-ray photoelectron spectroscopyCrystal structureCrystal field theoryAtomic physicsSingle crystalSpectral linePerovskite (structure)Density of statesValence electronMaterials scienceField (mathematics)Crystal (programming language)Inorganic chemistryMolecular physicsElectronCrystallographyLigand field theoryPhysical chemistryAtomic electron transitionElectron configurationQuantum chemicalTransition metalInorganic compoundChemical physicsNuclear Materials and PropertiesRadioactive element chemistry and processingRare-earth and actinide compounds