Quantum Engineering of Spin and Anisotropy in Magnetic Molecular Junctions

Abstract: Single molecule magnets and single spin centers can be individually addressed when coupled to contacts forming an electrical junction. In order to control and engineer the magnetism of quantum devices, it is necessary to quantify how the structural and chemical environment of the junction affects the spin center. Metrics such as coordination number or symmetry provide a simple method to quantify the local environment, but neglect the many-body interactions of an impurity spin when coupled to contacts. Here, we utilize a highly corrugated hexagonal boron nitride (h-BN) monolayer to mediate the coupling between a cobalt spin in CoHx (x=1,2) complexes and the metal contact. While the hydrogen atoms control the total effective spin, the corrugation is found to smoothly tune the Kondo exchange interaction between the spin and the underlying metal. Using scanning tunneling microscopy and spectroscopy together with numerical simulations, we quantitatively demonstrate how the Kondo exchange interaction mimics chemical tailoring and changes the magnetic anisotropy.