Imaging the Single‐Electron Ln–Ln Bonding Orbital in a Dimetallofullerene Molecular Magnet

Abstract Chemically robust single‐molecule magnets (SMMs) with sufficiently high blocking temperatures T_B are among the key building blocks for the realization of molecular spintronic or quantum computing devices. Such device applications require access to the magnetic system of a SMM molecule by means of electronic transport, which primarily depends on the interaction of magnetic orbitals with the electronic states of the metallic electrodes. Scanning tunneling microscopy in combination with ab initio calculations allows to directly address the unoccupied component of the single‐electron molecular orbital that mediates the ferromagnetic exchange coupling between two 4f ions within a lanthanide endohedral dimetallofullerene deposited on a graphene surface. The single‐electron metal–metal bond provides a direct access to the molecule's magnetic system in the transport experiments, paving the way for investigation and controlled manipulation of the spin system of individual dimetallofullerene SMMs, essential for molecular spintronics.