Recent advances in computational modelling of mononuclear actinide single molecule magnets†

Abstract

Significant progress has been made in lanthanide-based single mononuclear SMMs in the past two decades, raising their magnetic memories to liquid nitrogen temperature. On the other hand, a handful of actinide-based mononuclear SMMs, primarily based on uranium, have been reported. Among the advantages of actinides over lanthanides are their more significant spin–orbit coupling and stronger metal–ligand covalency, which make them better candidates for providing mononuclear SMMs with high energy barriers. However, the lack of design criteria based on theoretical studies and their more challenging experimental preparation has led to limited results that are still distant from their promising potential. Recently, there has been an increasing interest in their ab initio modelling to understand their electronic structure and magnetic properties. This has led to setting up the first steps regarding their chemical design, thus opening new possibilities for improvement in the near future. In this review, we focus on these recent works and rationalise how far the field has come forward, exploring the potential of designing an advanced generation of actinide mononuclear SMMs.