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Spin-bearing molecules can be stabilized on surfaces and in junctions withdesirable properties such as a net spin that can be adjusted by externalstimuli. Using scanning probes, initial and final spin states can be deducedfrom topographic or spectroscopic data, but how the system transitioned betweenthese states is largely unknown. Here we address this question by manipulatingthe total spin of magnetic cobalt hydride complexes on a corrugated boronnitride surface with a hydrogen- functionalized scanning probe tip bysimultaneously tracking force and conductance. When the additional hydrogenligand is brought close to the cobalt monohydride, switching between a corre-lated S = 1 /2 Kondo state, where host electrons screen the magnetic moment,and a S = 1 state with magnetocrystalline anisotropy is observed. We show thatthe total spin changes when the system is transferred onto a new potentialenergy surface defined by the position of the hydrogen in the junction. Theseresults show how and why chemically functionalized tips are an effective toolto manipulate adatoms and molecules, and a promising new method to selectivelytune spin systems.

Potential Energy Driven Spin Manipulation via a Controllable Hydrogen Ligand