Millimeter-scale single-crystalline semiconducting MoTe 2 via solid-to-solid phase transformation

Among the Mo- and W-based two-dimensional (2D) transition metal dichalcogenides (TMDCs), MoTe is particularly interesting for phase-engineering applications, because it has the smallest free energy difference between the semiconducting 2H phase and metallic 1T' phase. In this work, we reveal that, under the proper circumstance, Mo and Te atoms can rearrange themselves to transform from a polycrystalline 1T' phase into a single-crystalline 2H phase in a large scale. We manifest the mechanisms of the solid-to-solid transformation by conducting the density functional theory calculations, transmission electron microscopy, energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy and Raman spectroscopy. The phase transformation can be well described by the time-temperature-transformation diagram. By optimizing the kinetic rates of nucleation and crystal growth, we have synthesized single-crystalline 2H-MoTe domain with diameter of 2.34 mm, centimeter-scale 2H-MoTe thin film with domain size up to several hundred micrometers, and the seamless 1T'-2H MoTe coplanar homojunction. The 1T'-2H MoTe homojunction provides an elegant solution for ohmic contact of 2D semiconductors. The controlled solid-to-solid phase transformation in 2D limit provides a new route to realize wafer-scale single-crystalline 2D semiconductor and coplanar heterostructure for 2D circuitry.