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Uranium and plutonium's 5f electrons are tenuously poised between stronglybonding with ligand spd-states and residing close to the nucleus. The unusualproperties of these elements and their compounds (eg. the six differentallotropes of elemental plutonium) are widely believed to depend on the relatedattributes of f-orbital occupancy and delocalization, for which a quantitativemeasure is lacking. By employing resonant x-ray emission spectroscopy (RXES)and x-ray absorption near-edge structure (XANES) spectroscopy and makingcomparisons to specific heat measurements, we demonstrate the presence ofmulticonfigurational f-orbital states in the actinide elements U and Pu, and ina wide range of uranium and plutonium intermetallic compounds. These resultsprovide a robust experimental basis for a new framework for understanding thestrongly-correlated behavior of actinide materials.

Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics