Non-magnetic ground state of PuO${}_2$

Abstract

The correlated band theory implemented as a combination of the local density approximation with the exact diagonalization of the Anderson impurity model is applied to PuO${}_2$. We obtain an insulating electronic structure consistent with the experimental photoemission spectra. The calculations yield the band gap of 1.8 eV and a non-magnetic singlet ground state that is characterized by a non-integer filling of the plutonium $f$ shell ($n_f\approx 4.5$). Due to sizeable hybridization of the $f$ shell with the $p$ states of oxygen, the ground state is more complex than the four-electron Russell--Saunders ${}^5{\mathrm{I}}_4$ manifold split by the crystal field. The inclusion of hybridization improves the agreement between the theory and experiment for the magnetic susceptibility.

Main article with 3 figures, and supplementary information with 4 figures

References in corpus (4)

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• A perturbative approach to J mixing in f-electron systems: Application to actinide dioxides
• Electronic structure and spectral properties of Am, Cm and Bk: Charge density self-consistent LDA+HIA calculations in FP-LAPW basis
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Cited by in corpus (3)

• Electronic structure and core-level spectra of light actinide dioxides in the dynamical mean-field theory
• On the Raman Spectrum of Plutonium dioxide: vibrational and crystal electric field modes
• Theory of valence-band and core-level photoemission from plutonium dioxide