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The reversible control of a single spin of an atom or a molecule is of greatinterest in Kondo physics and a potential application in spin basedelectronics.Here we demonstrate that the Kondo resonance of manganesephthalocyanine molecules on an Au(111) substrate have been reversibly switchedoff and on via a robust route through attachment and detachment of singlehydrogen atom to the magnetic core of the molecule. As further revealed bydensity functional theory calculations, even though the total number ofelectrons of the Mn ion remains almost the same in the process, gaining onesingle hydrogen atom leads to redistribution of charges within 3d orbitals witha reduction of the molecular spin state from S = 3/2 to S = 1 that directlycontributes to the Kondo resonance disappearance. This process is reversed by alocal voltage pulse or thermal annealing to desorb the hydrogen atom.

Reversible Single Spin Control of Individual Magnetic Molecule by Hydrogen Atom Adsorption