Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics

Abstract

Uranium and plutonium's 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (eg. the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization, for which a quantitative measure is lacking. By employing resonant x-ray emission spectroscopy (RXES) and x-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu, and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework for understanding the strongly-correlated behavior of actinide materials.

arXiv comment30 pages, concatenated article and supporting information, 10 figures

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Cited by in corpus (19)

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• Mixed valency and site-preference chemistry for Cerium and its compounds: A predictive DFT study
• Resonant x-ray spectroscopy of uranium intermetallics at the U $M_{4,5}$ edges
• Suppression of ferromagnetism in the LaVxCr1-xGe3 system
• Chemical Design of Electronic and Magnetic Energy Scales in Tetravalent Praseodymium
• Probing 5f-state configurations in URu2Si2 with U L3-edge resonant x-ray emission spectroscopy
• Synchrotron Radiation Techniques and their Application to Actinide Materials
• Nature of the 5$f$ electronic structure of plutonium
• Plutonium-Based Heavy-Fermion Systems
• Isochronal annealing effects on local structure, crystalline fraction, and undamaged region size of radiation damage in Ga-stabilized $\delta$-Pu
• Phase stabilization by electronic entropy in plutonium
• Fermi surface topology and de Hass-van Alphen orbits in PuIn${}_3$ and PuSn${}_3$ compounds
• Quasiparticle multiplets and 5f electronic correlation in prototypical plutonium borides
• Hybridization effect on the X-ray absorption spectra for actinide materials: Application to PuB${}_4$
• Dualism of the 4f electrons and high-temperature antiferromagnetism of the heavy-fermion compound YbCoC${}_2$
• Electronically driven collapse of the bulk modulus in $\delta$-plutonium
• Valence instability across magnetostructural transition in USb${}_2$
• Thermal Equation of State of U${}_6$Fe from Experiments and Calculations
• UCd${}_{11}$: A strongly localized 5$f^3$ material