Invited Paper AC+AS+MI+SA+SS-MoA1
Nonmagnetic Ground State of PuO2
Monday, November 10, 2014, 2:00 pm, Room 301
The correlated band theory implemented as a combination of the local density approximation with the dynamical mean-field theory is applied to PuO2. We obtain an insulating electronic structure consistent with the experimental photoemission spectra, and a nonmagnetic ground state that is characterized by a noninteger filling of the plutonium f shell (nf ≈ 4.4). Due to a sizable hybridization of the f shell with the p states of oxygen, the ground state is more complex than the four-electron Russell–Saunders 5I4 manifold split by the crystal field. The dynamical mean-field theory, which in the present case can be schematically viewed as an extension of the crystal-field model with hybridization terms, improves the agreement between the theory and experiment for the magnetic susceptibility [1]. Encouraged by the good accuracy achieved for PuO2 , we apply the theory to several other tetravalent actinide oxides. [1] A. B. Shick, J. Kolorenč, L. Havela, T. Gouder, and R. Caciuffo, Phys. Rev. B 89, 041109 (2014).