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

摘要

Using a recently developed method combining a nonspherical self-interaction corrected LDA + U scheme and an on-site multibody Hamiltonian [Phys. Rev. B 83,085106 (2011)], we calculate the crystal field parameters and crystal field (CF) excitation levels of /-element dioxides in the fluorite structure with f~n electronic configurations, including n = 1 (PaO_2, PrO_2, n = 2 (UO_2), n = 3 (NpO_2), and n = 4 (PUO_2). It is shown that good agreement with experimental data (within approximately 10-20 meV) can be obtained in all cases. The properties of the multielectron CF ground states are analyzed.