Single-molecule magnets beyond a single lanthanide ion: the art of coupling

The promising future of storing and processing quantized information at the molecular level has been attracting the study of Single-Molecule Magnets (SMMs) for almost three decades. Although some recent breakthroughs are mainly about the SMMs containing only one lanthanide ion, we believe SMMs can tell a much deeper story than the single-ion anisotropy. Here in this Perspective, we will try to draw a unified picture of SMMs as a delicately coupled spin system between multiple spin centres. The hierarchical couplings will be presented step-by-step, from the intra-atomic hyperfine coupling, to the direct and indirect intra-molecular couplings with neighbouring spin centres, and all the way to the inter-molecular and spin–phonon couplings. Along with the discussions on their distinctive impacts on the energy level structures and thus magnetic behaviours, a promising big picture for further studies is proposed, encouraging the multifaceted developments of molecular magnetism and beyond.