Large-Area, Two-Dimensional MoS₂ Exfoliated on Gold: Direct Experimental Access to the Metal-Semiconductor Interface

Two-dimensional semiconductors such as MoS₂ are promising for future electrical devices. The interface to metals is a crucial and critical aspect for these devices because undesirably high resistances due to Fermi level pinning are present, resulting in unwanted energy losses. To date, experimental information on such junctions has been obtained mainly indirectly by evaluating transistor characteristics. The fact that the metal-semiconductor interface is typically embedded, further complicates the investigation of the underlying physical mechanisms at the interface. Here, we present a method to provide access to a realistic metal-semiconductor interface by large-area exfoliation of single-layer MoS₂ on clean polycrystalline gold surfaces. This approach allows us to measure the relative charge neutrality level at the MoS₂-gold interface and its spatial variation almost directly using Kelvin probe force microscopy even under ambient conditions. By bringing together hitherto unconnected findings about the MoS₂-gold interface, we can explain the anomalous Raman signature of MoS₂ in contact to metals [ACS Nano. 7, 2013, 11350] which has been the subject of intense recent discussions. In detail, we identify the unusual Raman mode as the A_1g mode with a reduced Raman shift (397 cm^-1) due to the weakening of the Mo-S bond. Combined with our X-ray photoelectron spectroscopy data and the measured charge neutrality level, this is in good agreement with a previously predicted mechanism for Fermi level pinning at the MoS₂-gold interface [Nano Lett. 14, 2014, 1714]. As a consequence, the strength of the MoS₂-gold contact can be determined from the intensity ratio between the reduced A_1g mode and the unperturbed A_1g mode.