Two-dimensional (2D) transition-metal dichalcogenides (TMDCs) are considered highly promising platforms for next-generation optoelectronic devices. Owing to its atomically thin structure, device performance is strongly impacted by a minute amount of defects. Although defects are usually considered to be disturbing, defect engineering has become an important strategy to control and design new properties of 2D materials. Here, we produce single S vacancies in a monolayer of MoS2 on Au(111). Using a combination of scanning tunneling and atomic force microscopy, we show that these defects are negatively charged and give rise to a Kondo resonance, revealing the presence of an unpaired electron spin exchange coupled to the metal substrate. The strength of the exchange coupling depends on the density of states at the Fermi level, which is modulated by the moiré structure of the MoS2 lattice and the Au(111) substrate. In the absence of direct hybridization of MoS2 with the metal substrate, the S vacancy remains charge neutral. Our results suggest that defect engineering may be used to induce and tune magnetic properties of otherwise nonmagnetic materials.
