Moiré Tuning of Spin Excitations: Individual Fe Atoms on MoS_{2}/Au(111)

Magnetic adatoms on properly designed surfaces constitute exquisite systems for addressing, controlling, and manipulating single quantum spins. Here, we show that monolayers of MoS_{2} on a Au(111) surface provide a versatile platform for controllably tuning the coupling between adatom spins and substrate electrons. Even for equivalent adsorption sites with respect to the atomic MoS_{2} lattice, we observe that Fe adatoms exhibit behaviors ranging from pure spin excitations, characteristic of negligible exchange and dominant single-ion anisotropy, to a fully developed Kondo resonance, indicating strong exchange and negligible single-ion anisotropy. This tunability emerges from a moiré structure of MoS_{2} on Au(111) in conjunction with pronounced many-body renormalizations. We also find striking spectral variations in the immediate vicinity of the Fe atoms, which we explain by quantum interference reflecting the formation of Fe-S hybrid states despite the nominally inert nature of the substrate. Our work establishes monolayer MoS_{2} as a tuning layer for adjusting the quantum spin properties over an extraordinarily broad parameter range. The considerable variability can be exploited for quantum spin manipulations.