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Individual nuclear spin states can have very long lifetimes and could beuseful as qubits. Progress in this direction was achieved on MgO/Ag(001) viadetection of the hyperfine interaction (HFI) of Fe, Ti and Cu adatoms usingscanning tunneling microscopy (STM). Previously, we systematically quantifiedfrom first-principles the HFI for the whole series of 3d transition adatoms(Sc-Cu) deposited on various ultra-thin insulators, establishing the trends ofthe computed HFI with respect to the filling of the magnetic s- and d-orbitalsof the adatoms and on the bonding with the substrate. Here we explore the caseof dimers by investigating the correlation between the HFI and the magneticstate of free standing Fe dimers, single Fe adatoms and dimers deposited on abilayer of MgO(001). We find that the magnitude of the HFI can be controlled byswitching the magnetic state of the dimers. For short Fe- Fe distances, theantiferromagnetic state enhances the HFI with respect to that of theferromagnetic state. By increasing the distance between the magnetic atoms, atransition towards the opposite behavior is observed. Furthermore, wedemonstrate the ability to substantially modify the HFI by atomic control ofthe location of the adatoms on the substrate. Our results establish the limitsof applicability of the usual hyperfine hamiltonian and we propose an extensionbased on multiple scattering processes.

Interplay of magnetic states and hyperfine fields of iron dimers on MgO(001)