Predicting the electronic structure and magnetic properties of UO2+, UO2(CO)5+ and UO2(Ar)5+ using wavefunction based methods

The electronic structure and magnetic properties of UO2+, and two complexes, UO2(CO)5+ and UO2(Ar)5+ in D5h symmetry are studied with a combination of relativistic theoretical methods: ab-initio wavefunction calculations, density functional theory (DFT), and crystal-field (CF) models with parameters extracted from the ab-initio calculations. The model Hamiltonian techniques are employed to describe theoretically the state interaction and the “competition” between Crystal field (CF) and spin-orbit coupling (SO), this is important besides for a correct description of the sign of the g-factors using also a symmetry criteria.

This work aims to highlight the utility of concerted theoretical approaches for the investigation of f-element complexes, namely a combination of crystal-field (CF) based models with ab-initio wavefunction calculations. 36