Relativistic configuration-interaction perturbation-theory calculations of energy levels and -factors in neutral plutonium
Phys. Rev. A 114, 042812 – Published 15 October, 2026
DOI: https://doi.org/10.1103/7zmt-rxc4
Abstract
Neutral plutonium (Pu I) is an exceptionally complex atomic system owing to its eight valence electrons, strong valence-valence and valence-core correlations, and pronounced relativistic effects. The resulting high density of states and small energy separations among levels with the same total angular momentum lead to strong configuration mixing, making reliable predictions of level energies and Landé -factors particularly challenging. Configuration-interaction many-body perturbation theory (CIMBPT) can, in principle, treat these effects, but in practice often requires very large configuration spaces when the conventional Dirac-Hartree-Fock (DHF) starting potential is constructed for a closed-shell core. In this work, we employ a relativistic configuration-interaction perturbation-theory (CIPT) approach based on a DHF starting potential that explicitly includes six electrons. This choice provides a more suitable starting Hamiltonian for Pu I than the conventional approximation used in CIMBPT, which for Pu I corresponds to removing all eight valence electrons () in constructing the self-consistent potential. It improves single-configuration energies and enables a more efficient treatment of configuration mixing at substantially reduced computational cost. Benchmark comparisons with available experimental data demonstrate good overall agreement for both energies and Landé -factors. The present results indicate that CIPT provides an efficient and practical framework for describing the low-energy electronic structure of complex actinides and can be extended to other heavy atoms relevant to precision spectroscopy and symmetry-violation studies.