Spectroscopic Determination of the Electronic Structure of a Uranium Single-Ion Magnet

Abstract

Early actinide ions have large spin-orbit couplings and crystal field interactions, leading to large anisotropies. The success in using actinides as single-molecule magnets has so far been modest, underlining the need for rational strategies. Indeed, the electronic structure of actinide single-molecule magnets and its relation to their magnetic properties remains largely unexplored. A uranium(III) single-molecule magnet, [U^III {SiMe₂ NPh}₃ -tacn)(OPPh₃ )] (tacn=1,4,7-triazacyclononane), has been investigated by means of a combination of magnetic, spectroscopic and theoretical methods to elucidate the origin of its static and dynamic magnetic properties.

Keywords: ab initio calculations; crystal field splitting; electronic structure; magnetic properties; single-molecule magnets; uranium.