Self-consistent density functional calculations of the crystal field levels in lanthanide and actinide dioxides

الأصل · EN

Using a recently developed method combining a nonspherical self-interaction corrected LDA+U scheme and an on-site multi-body Hamiltonian [Phys.Rev.B 83, 085106 (2011)], we calculate the crystal field parameters and crystal field (CF) excitation levels of f-element dioxides in the fluorite structure with fⁿ electronic configurations, including n=1 (PaO₂, PrO₂), n=2 (UO₂), n=3 (NpO₂), and n=4 (PuO₂). It is shown that good agreement with experimental data (within approximately 10 to 20 meV) can be obtained in all cases. The properties of the multi-electron CF ground states are analyzed.