Abstract
In order to reveal the correlation effect on the electronic properties in particular 5f electron occupation numbers of Pu/U ions in a (Pu,U) mixed oxide-PuUO4, a first principles calculation is performed by using density functional theory (DFT) plus a dynamical mean field theory (DMFT) scheme with the spin-orbit coupling (SOC) and on-site Coulomb repulsion for correlation effect due to localized Pu/U 5f orbitals. Results demonstrate that Pu/U 5f electron occupation numbers in the ground state of PuUO4 are mainly composed of 5f4/5f5 and 5f2/5f3 configurations, and exhibiting the intermediate occupation (IO) numbers with average 5f occupation numbers of about nf = 4.879 and 2.423 for Pu and U ions, respectively, irrespective of different Pu and U lattice sites in PuUO4. Pu 5f j = 5/2 and j = 7/2 components are in moderately and weakly correlated states, respectively, while U 5f j = 5/2 and j = 7/2 manifolds are both in weakly correlated states. jj and LS coupling schemes are feasible for Pu and U 5f electrons, respectively. In order to directly compare with the experimental angle-resolved photoemission spectrum (ARPES), we also estimate the momentum-resolved electronic spectrum function for this system.
Sign-in/Register to access full text options 
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
