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Scanning tunneling microscopy shows that copper deposited at room temperature onto a freshly exfoliated MoS2 surface forms Cu(111) clusters with periodic preferred heights of 5, 8, and 11 atomic layers. These height intervals correlate with Fermi nesting regions along the necks of the bulk Cu Fermi surface, indicating a connection between physical and electronic structures. Density functional theory calculations of freestanding Cu(111) films support this as well, predicting a lower density of states at the Fermi level for these preferred heights. This is consistent with other noble metals deposited on MoS2 that exhibit electronic growth, in which the metal films self-assemble as nanostructures minimizing quantum electronic energies. Here, we have discovered that it is critical for the metal deposition to begin on a clean MoS2 surface. If copper is deposited onto an already Cu coated surface, even if the original film displays electronic growth, the resulting Cu film lacks quantization. Instead, the preferred heights of the Cu clusters simply increase linearly with the amount of Cu deposited upon the surface. We believe this is due to different bonding conditions during the initial stages of growth. Newly deposited copper would bond strongly to the already present copper clusters, rather than the weak bonding, which exists to the van der Waals terminated surface of MoS2. The stronger bonding with previously deposited clusters hinders additional Cu atoms from reaching their lowest quantum energy state. The interface characteristics of the van der Waals surface enable surface engineering of self-assembled structures to achieve different applications. 

Near surface defects can significantly impact the quality of metallic interconnects and other interfaces necessary to create device structures incorporating two-dimensional materials. Furthermore, the impact of such defects can strongly depend on their organization. In this study, we present scanning tunneling microscopy images and tunneling spectroscopy of point and linear defects near the surface of natural MoS2. The point defects share similar structural and electronic characteristics and occur with comparable frequency as subsurface sulfur vacancies observed previously on natural MoS2. The linear defects observed here occur less frequently than the point defects but share the same depth profile and electronic structure. These data indicate that the linear defects are actually a one-dimensional organization of subsurface sulfur vacancies. Our density functional calculations agree with this assessment in that, for sufficient local defect concentrations, it is energetically more favorable for the defects to be organized in a linear fashion rather than as clusters or even isolated single point defects. Given these measurements were taken from naturally formed MoS2, this organization likely occurs during crystal formation. Considering the impact of one-dimensional organization on the local properties of layered materials, and the potential for them to be introduced purposefully during crystal formation, research into the formation mechanism and properties of these defects could enable new paths for defect engineering in MoS2-based systems.