Electronic structure of light actinide dioxides

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We achieve a consistent and comprehensive description of the electronic structure of thee actinide oxides – Mott insulators where the forbidden gap appears as a consequence of strong correlations among electrons. The density-functional theory (DFT) predicts in these oxides either a non-magnetic metal or a magnetically ordered insulator. In reality, they are paramagnetic insulators at room temperature, and PuO2 is even entirely non-magnetic. We show how the improved description provided by the dynamical mean-field theory (DMFT) yields opening of the gap in the paramagnetic phase and quenching of the magnetic moments from the partially filled 5f shells in PuO2. We verify our calculations against experimental photoemission from valence bands as well as from core levels. In the paper, we also discuss details of technical developments that made these calculations possible.

Electronic structure of actinide dioxides and angle-resolved photoemission.
Description
Band structure and simulated angle-resolved photoemission. Computed band structure in three actinide dioxides – UO2, NpO2, PuO2. In the lower row, the effect of a limited resolution is included to simulate experimental angle-resolved photoemission spectra (ARPES).