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Abstract

Sulfur vacancies in MoS₂ on Au(111) have been shown to be negatively charged as reflected by a Kondo resonance. Here, we use scanning tunneling microscopy to show that these vacancies serve as anchoring sites for thiol-based molecules (CF₃−3⁢P−SH) with two distinct reaction products, one of them showing a Kondo resonance. Based on comparisons with density-functional theory (DFT) calculations, including a random structure search and computation of energies and electronic properties at a hybrid exchange-correlation functional level, we conclude that both anchored molecules are charge neutral. We propose that one of them is an anchored intact CF₂−3⁢P−SH molecule while the other one is the result of catalytically activated dehydrogenation to CF₂−3⁢P−S with subsequent anchoring. Our investigations highlight a perspective of functionalizing defects with thiol-terminated molecules that can be equipped with additional functional groups, such as charge donor or acceptor moieties, switching units, or magnetic centers.