The Intricate Love Affairs between MoS₂ and Metallic Substrates

Mechanical exfoliation yields high‐quality 2D materials but is challenging to scale up due to the small lateral size and low yield of the exfoliated crystals. Gold‐mediated exfoliation of macroscale monolayer MoS 2 and related crystals addresses this problem. However, it remains unclear whether this method can be extended to other metals. Herein, mechanical exfoliation of MoS 2 on a range of metallic substrates is studied. It is found that Au outperforms all the other metals in their ability to exfoliate macroscale monolayer MoS 2 . This is rationalized by gold's ability to resist oxidation, which is compromised on other metals and leads to a weakened binding with MoS 2 . An anomalously high monolayer yield found for Ag suggests that the large interfacial strain in the metal–MoS 2 heterostructures measured by Raman spectroscopy also is a critical factor facilitating the exfoliation, while the relative differences in the metal–MoS 2 binding play only a minor role. These results provide a new incentive for investigations of 2D material‐substrate combinations applicable where high‐quality 2D crystals of macroscopic dimensions are of importance.