Atomic and electronic properties in plutonium trichloride: A multi-scale view

Abstract

The atomic and electronic properties of the plutonium trichloride (PuCl₃) system are investigated in terms of a multi-scale simulation by using single-particle approximations, a many-body approach, and an ab initio molecular dynamics (AIMD) simulation. The impurity Green’s functions indicate that j = 5/2 and j = 7/2 manifolds of Pu electrons exhibit the conducting regimes. The mostly localized (n_5f ∼ 5.015) 5f-derived spectra feature, spin–orbit coupling, many-body transition of 5fⁿ (n = 4 ∼ 6) atomic configurations are responsible for the quasiparticle multiplets near the Fermi level. The coexistence of the lower Hubbard band, the upper Hubbard band, the atomic multiplet peaks and broad Hubbard bands, suggests that PuCl₃ could be identified as a Racah material. Generally, the AIMD simulation is qualitatively in accord with the many-body calculations in this work.