Historical developments, trends, pitfalls and strategies in improving f-element single molecule magnets are described.

Single-molecule magnets display magnetic bistability of molecular origin, which may one day be exploited in magnetic data storage devices. Recently it was realised that increasing the magnetic moment of polynuclear molecules does not automatically lead to a substantial increase in magnetic bistability. Attention has thus increasingly focussed on ions with large magnetic anisotropies, especially lanthanides. In spite of large effective energy barriers towards relaxation of the magnetic moment, this has so far not led to a big increase in magnetic bistability. Here we present a comprehensive study of a mononuclear, tetrahedrally coordinated cobalt(II) single-molecule magnet, which has a very high effective energy barrier and displays pronounced magnetic bistability. The combined experimental-theoretical approach enables an in-depth understanding of the origin of these favourable properties, which are shown to arise from a strong ligand field in combination with axial distortion. Our findings allow formulation of clear design principles for improved materials.

Cobalt unfettered by its ligand field: Applied magnetic fields induce a field in any compound with unpaired electrons. However, for the induced field to persist once the applied field is gone, the electrons must be configured to manifest orbital angular momentum. Generally, the influence of ligands severely restricts that property in transition metal complexes. Bunting et al. now show that a cobalt ion is just barely affected by two linearly coordinated carbon ligands and, as such, exhibits maximal orbital angular momentum. Although its magnetic properties mainly pertain at very low temperature, its structure offers a more general design principle. Science , this issue p. eaat7319