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The creation of magnetism on non-magnetic semiconductor surfaces is ofimportance for the realization of spintronics devices. Especially, the couplingof electron spins within quantum nanostructures can be utilized fornanomagnetism applications. Here, we demonstrate, based on first-principlesdensity-functional theory calculations, that the adsorption of H atoms on theSi(111)-(7$\times$7) surface induces the spin polarization of surrounding Sidangling bonds (DBs) and their spin orderings. It is revealed that the Hadsorption on a rest-atom site exhibits a Jahn-Teller-like distortion thataccompanies a charge transfer from the rest atom to the nearest neighboringadatoms. This charge transfer increases the local density of states of suchthree adatoms at the Fermi level, thereby inducing a Stoner-type instability toproduce a ferrimagnetic order of adatom DBs around the adsorbed H atom.Meanwhile, the H adsorption on an adatom site cannot induce spin polarization,but, as adsorbed H atoms increase, the ferrimagnetic order of rest-atom DBsemerges through the charge transfer from rest atoms to adatoms. Our findingsprovide a microscopic mechanism of the H-induced spin orderings of Si DBs atthe atomic scale, which paves a novel way to the design of nanoscale magnetismin the representative semiconductor surface.

Hydrogen adsorption-induced nanomagnetism at the Si(111)-(7$\times$7) surface