Atomic properties of actinide ions with particle-hole configurations

TL;DR

This paper introduces a hybrid relativistic method combining configuration interaction and coupled-cluster approaches to accurately calculate atomic properties of actinide ions with particle-hole configurations, addressing experimental puzzles.

Contribution

The study presents the first high-precision calculations of actinide ions Th$^{4+}$ and U$^{6+}$ using a novel hybrid computational method.

Findings

Excellent agreement with experimental data for La$^{3+}$

First precision calculations for Th$^{4+}$ and U$^{6+}$ ions

Effective treatment of electronic correlations in complex ions

Abstract

We study the effects of higher-order electronic correlations in the systems with particle-hole excited states using a relativistic hybrid method that combines configuration interaction and linearized coupled-cluster approaches. We find the configuration interaction part of the calculation sufficiently complete for eight electrons while maintaining good quality of the effective coupled-cluster potential for the core. Excellent agreement with experiment was demonstrated for a test case of La$^{3+}$. We apply our method for homologue actinide ions Th$^{4+}$ and U$^{6+}$ which are of experimental interest due to a puzzle associated with the resonant excitation Stark ionization spectroscopy (RESIS) method. These ions are also of interest to actinide chemistry and this is the first precision calculation of their atomic properties.