Relativistic configuration-interaction calculations of U I hyperfine constants

TL;DR

This paper presents a relativistic configuration-interaction method for calculating hyperfine constants in neutral uranium, achieving high accuracy with a more efficient approach that includes valence electrons in the starting potential.

Contribution

The study introduces an improved RCI method using a starting potential with valence electrons, enabling accurate hyperfine constant calculations for complex atoms like uranium.

Findings

Achieved within 5% accuracy for 5 low-energy levels

Recommended a new nuclear magnetic moment of 0.43(2)

Method can be extended to other atoms and properties

Abstract

Neutral uranium (U I) is a very difficult atom for theoretical calculations due to a large number of valence electrons, six, strong valence-valence and valence-core correlations, high density of states, and relativistic effects. Configuration-interaction many-body perturbation theory (CI-MBPT) can treat efficiently valence-core correlations and relativistic effects, but because the formalism was developed for Dirac-Hartree-Fock (DHF) starting potential that does not contain valence electrons, quite large CI space is needed to compensate for +6 charge of such a potential. Much more efficient is relativistic configuration-interaction (RCI) approach which uses relatively accurate starting DHF potential that includes some valence electrons to make the valence electron Hamiltonian diagonally dominated for some states. Here we report calculations of U I hyperfine constants of several low-energy states using the RCI method with the starting potential that includes four f valence electrons. With this starting potential, it is possible to use the single-configuration approximation or small basis sets to obtain quite accurate results for hyperfine structure constants. In fact, by scaling nuclear magnetic moment, the agreement for 5 levels was within 5\%, and a new magnetic moment can be recommended 0.43(2). The method can be further developed to include more extensive data sets to improve accuracy and can be applied to other atoms and for calculations of other properties, for example, relevant to fundamental symmetry tests.