Lanthanide-based single molecule magnets through the prism of ab-initio calculations

In the beginning of the century, the emergence of lanthanide-based systems exhibiting slow relaxation of their magnetization opened a new chapter in the field of molecular magnetism. These so called Single-Molecule Magnets (SMMs) may find in a near future many important applications such as high-density data storage, molecular spintronic or quantum computing. Over the recent years, quantum chemical approaches, going from multiconfigurational wavefunction-based methodologies to (periodic) density functional theory have shown to be powerful tools to gain deep insight into electronic and magnetic features of such lanthanide-based SMMs. This presentation will focus on recent applications of such state-of-the-art computational protocols in the understanding of Ln-based SMMs behaviors.