5f Electronic Structure and Fermiology of Pu Materials

Abstract

We examine the electronic structure of δ-Pu, PuCoGa5, and PuO2 using high resolution as well as angle-resolved photoelectron spectroscopy. The fermiology of the strongly correlated metals δ-Pu and PuCoGa5 is investigated by determining the primary quasiparticle peak position with respect to the Fermi energy as well as the crystal momentum dependence of this peak for PuCoGa5. For the Mott insulator PuO2, the photoemission results are compared against the hybrid functional calculations and the prediction of significant covalency, is found to be reasonable.

Electronic structure of bulk AnO 2 (An = U, Np, Pu) and water adsorption on the (111) and (110) surfaces of UO 2 and PuO 2 from hybrid density functional theory within the periodic electrostatic embedded cluster method

“…Thus, as noted in the introduction, PuO 2 is not a Mott-Hubbard insulator, as there is a significant contribution of oxygen at the valence band edge. PuO 2 is better described as an LMCT system, in agreement with experiment [3]. The HOMO-LUMO gap for the cluster is 3.3 eV, again slightly larger than the experimental value of 2.80 eV [49].…”

“…When PuO 2 is reached the occupied 5f levels have lowered further in energy and are now located at the top of the occupied oxygen 2p band, as seen from PES [3]. PuO 2 is also an insulator; however, as the top of the valence band now has oxygen character it is no longer a Mott-Hubbard insulator but a ligand to metal charge transfer (LMCT) insulator.…”

Density Functional Theory Studies of the Electronic Structure of Solid State Actinide Oxides

“…We will return to this later. A more direct probe of the valence bands is given by the angle-resolved photoemission (ARPES) experiments 58 on a single-crystal quality thin film of PuO 2 . In that work, it was found that, unlike UO 2 , dispersion in PuO 2 is of the order of several electronvolts.…”

Electronic structure and core-level spectra of light actinide dioxides in the dynamical mean-field theory

“…Although the angular-resolved photoemission (ARPES) experiments were performed on PuO 2 , the acquired data are not able to resolve the issue yet due to the lack of orbital resolution (the measurements were done with the He II light source). 38 The analysis of ARPES data is more straightforward in UO 2 where the 5f bands are well separated and it is possible to read out their dispersion. 39 It comes out as about 0.13 eV, which is considerably smaller than our result plotted in Fig.…”