Hypotaxy of wafer-scale single-crystal transition metal dichalcogenides

Abstract

Two-dimensional (2D) semiconductors, particularly transition metal dichalcogenides (TMDs), are promising for advanced electronics beyond silicon1,2,3. Traditionally, TMDs are epitaxially grown on crystalline substrates by chemical vapour deposition. However, this approach requires post-growth transfer to target substrates, which makes controlling thickness and scalability difficult. Here we introduce a method called hypotaxy (‘hypo’ meaning downward and ‘taxy’ meaning arrangement), which enables wafer-scale single-crystal TMD growth directly on various substrates, including amorphous and lattice-mismatched substrates, while preserving crystalline alignment with an overlying 2D template. By sulfurizing or selenizing a pre-deposited metal film under graphene, aligned TMD nuclei form, coalescing into a single-crystal film as graphene is removed. This method achieves precise MoS2 thickness control from monolayer to hundreds of layers on diverse substrates, producing 4-inch single-crystal MoS2 with high thermal conductivity (about 120？W？m？1？K？1) and mobility (around 87？cm2？V？1？s？1). Furthermore, nanopores created in graphene using oxygen plasma treatment allow MoS2 growth at a lower temperature of 400？°C, compatible with back-end-of-line processes. This hypotaxy approach extends to other TMDs, such as MoSe2, WS2 and WSe2, offering a solution to substrate limitations in conventional epitaxy and enabling wafer-scale TMDs for monolithic three-dimensional integration.