cm²-Scale Synthesis of MoTe₂ Thin Films with Large Grains and Layer Control

Owing to the small energy differences between its polymorphs, MoTe₂ can access a full spectrum of electronic states from the 2H semiconducting state to the 1T' semimetallic state and from the T_d Weyl semimetallic state to the superconducting state in the 1T' and T_d phase at low temperature. Thus, it is a model system for phase transformation studies as well as quantum phenomena such as the quantum spin Hall effect and topological superconductivity. Careful studies of MoTe₂ and its potential applications require large-area MoTe₂ thin films with high crystallinity and thickness control. Here, we present cm²-scale synthesis of 2H-MoTe₂ thin films with layer control and large grains that span several microns. Layer control is achieved by controlling the initial thickness of the precursor MoO thin films, which are deposited on sapphire substrates by atomic layer deposition and subsequently tellurized. Despite the van der Waals epitaxy, the precursor-substrate interface is found to critically determine the uniformity in thickness and grain size of the resulting MoTe₂ films: MoTe₂ grown on sapphire show uniform films while MoTe₂ grown on amorphous SiO₂ substrates form islands. This synthesis strategy decouples the layer control from the variabilities of growth conditions for robust growth results and is applicable to growing other transition-metal dichalcogenides with layer control.