Unraveling the multistage phase transformations in monolayer MoTe2−<i>x</i>

Monolayer MoTe2 exhibits a variety of derivative structural phases and associated intriguing electronic properties that enable a wealth of potential applications in future electronic and optoelectronic devices. However, a comprehensive study focusing on the complexities of the controllable phase evolution in this atomically thin film has yet to be performed. This work aims to address this issue by systematically investigating molecular beam epitaxial growth of monolayer Mo–Te compounds on bilayer graphene substrates. By utilizing scanning tunneling microscopy, we explored a series of thermally driven structural phase evolutions, including distinct T′-MoTe2, H-MoTe2, Mo6Te6 nanowires, and multistoichiometric MoTe2−x. Furthermore, we carefully investigated the critical effects of the growth parameters—annealing temperature and time and tellurium concentration—on the controllable and reversible phase transformation within monolayer MoTe2−x. The findings have significant implications for understanding the thin film synthesis and phase transformation engineering inherent to two-dimensional crystals, which can foster further development of high-performance devices.