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

Abstract

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 $f^n$ 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 to 20 meV) can be obtained in all cases. The properties of the multi-electron CF ground states are analyzed.

12 pages, 2 figures, 4 tables. To appear in PRB

References in corpus (6)

• Ground state properties and high pressure behavior of plutonium dioxide: Systematic density functional calculations
• Crystal field and magnetic structure of UO${}_2$
• A perturbative approach to J mixing in f-electron systems: Application to actinide dioxides
• Stability mechanism of cuboctahedral clusters in UO2: First-principles calculations
• First-Principles Theory of Multipolar Order in Neptunium Dioxide
• First-principles computational study of defect clustering in solid solutions of ThO${}_2$ with trivalent oxides

Cited by in corpus (9)

• Electronic structure and core-level spectra of light actinide dioxides in the dynamical mean-field theory
• Chemical Design of Electronic and Magnetic Energy Scales in Tetravalent Praseodymium
• On the Raman Spectrum of Plutonium dioxide: vibrational and crystal electric field modes
• U 5$f$ crystal-field ground state of UO${}_2$ probed by directional dichroism in nonresonant inelastic x-ray scattering
• Toward a first-principles theory of rare-earth ions in crystals
• Ab initio ligand field approach to determine electronic multiplet properties
• Crystal field calculations for transition metal ions by application of an opposing potential
• Theory of valence-band and core-level photoemission from plutonium dioxide
• f-electron charge densities probed using core level non-resonant inelastic x-ray scattering