Orbital-Selective Electronic Reconstruction in PuFeO 3 : Spin–Orbit-Driven Hybridization and Correlation Effects from First-Principles Dynamical Modeling

Intermediate configurations in the plutonium and iron perovskite compound PuFeO 3 are investigated using a combined density functional theory plus dynamical mean-field theory (DFT + DMFT) approach. Our findings reveal orbital-selective metal–insulator transitions driven by spin–orbit split Pu-5f states. Itinerant 5f 5/2 electrons exhibit correlated metallic behavior, while localized 5f 7/2 states display Mott-insulating characteristics. We report an average 5f occupancy of 4.649, suggesting intermediate valence states. Quantum mechanical analysis highlights the Pu-5f/Fe-3d hybridization, confirmed by the orbital-resolved self-energy and spectral function calculations. This study provides new insights into the electronic structure and bonding mechanisms of Pu-based perovskites, advancing the understanding of strongly correlated actinide materials.