Intermediate configurations in a plutonium and iron perovskite compound:
A multi-level study
Abstract
Microscopic properties of a Pu-Fe mixed oxide (MOX) are investigated by
means of single-particle approximations and a many-body theory.
Calculation results demonstrate that Pu 5 fj
=5/2, 5 fj =7/2
components display conducting and insulating states, respectively. While
for Fe 3 d electrons, eg and t
2 g components both exhibit the
conducting state. Intermediate and weak correlations emerge for Pu 5
fj =5/2, 5
fj =7/2 regimes, respectively,
while Fe 3 d eg and t 2
g states both exhibit the strong correlation. Fe
3 d/Pu 5 f quasiparticle weights suggest that PuFeO
3 has an orbital-dependent localization. jj and
intermediate angular momentum coupling mechanisms are feasible for 5
f (Pu) and 3 d (Fe) states, respectively. 5
fn configuration coupling produces an
intermediate configuration (thus Pu having a mixed oxidation state),
inducing quasiparticle multiplets. The quasiparticle band structure
agrees with the spectra features inferred from the density of state. The
relative lattice volume has no proportional or opposite trend with
evolution of Pu 5 f&Fe 3 d occupancies. Duality of the
electron localization, electron/valence/configuration fluctuation and
intermediate configuration/valence/occupancy show that multi-scale
features of the correlated materials could be modulated by means of
various working conditions.