Diffusion and magnetization of metal adatoms on single-layer molybdenum disulfide at elevated temperatures

The present work models temperature-dependent ( 500 - 1300 K ) diffusion dynamics of Ag, Au, and Cu adatoms on MoS2 as well as electronic and magnetic properties of adatom (Ag, Au, and Cu)/MoS2 systems. Modeling is done by means of ab initio molecular dynamics (AIMD) simulations that account for van der Waals corrections and electronic spin degrees of freedom in the framework of density functional theory. It is found that Ag and Au adatoms exhibit super-diffusive motion on MoS2 at all temperatures, while Cu adatoms follow a random walk pattern of uncorrelated surface jumps. The observed behavior is consistent with AIMD-calculated effective migration barriers E a ( E a Ag = 190 ± 50 meV , E a Au = 67 ± 7 meV , and E a Cu = 300 ± 100 meV ) and can be understood on the basis of the considerably flatter potential energy landscapes encountered by Ag and Au adatoms on the MoS2 surface (corrugation of the order of tens of meV), as compared to Cu adatoms (corrugation > 100 meV ). Moreover, evaluation of the electronic and magnetic properties of AIMD configurations suggest that Ag, Au, and Cu monomer adsorption induces semimetallic features in at least one spin channel of the adatom/MoS2 electronic structure at elevated temperatures. The overall results presented herein may provide insights into fabricating 2D-material-based heterostructure devices beyond graphene.