Theory of valence-band and core-level photoemission from plutonium dioxide

TL;DR

This paper applies a combined local-density approximation and dynamical mean-field theory to PuO2, successfully reproducing its insulating electronic structure and explaining core-level spectra through hybridization effects.

Contribution

It introduces a detailed theoretical approach to model PuO2's electronic structure, capturing its insulating behavior and spectral features.

Findings

PuO2 has an insulating electronic structure consistent with experiments.

The ground state is nonmagnetic with noninteger 5f shell filling.

Satellite features in spectra are due to 5f and oxygen 2p hybridization.

Abstract

The correlated-band theory implemented as a combination of the local-density approximation with the dynamical mean-field theory is applied to PuO2. An insulating electronic structure, consistent with the experimental valence-band photoemission spectra, is obtained. The calculations yield a nonmagnetic ground state that is characterized by a noninteger filling of the plutonium 5f shell. The noninteger filling as well as the satellites appearing in the 4f core-level photoemission spectra originate in a sizable hybridization of the 5f shell with the 2p states of oxygen.