Two-Dimensional Lateral Epitaxy of 2H (MoSe₂)-1T′ (ReSe₂) Phases

Two-dimensional (2D) transition metal dichalcogenide (TMDC) heterostructures have been proposed as potential candidates for a variety of applications like quantum computing, neuromorphic computing, solar cells, and flexible field effective transistors. The 2D TMDC heterostructures at the present stage face difficulties being implemented in these applications because of lack of large and sharp heterostructure interfaces. Herein, we address this problem via a CVD technique to grow thermodynamically stable heterostructure of 2H/1T′ MoSe₂-ReSe₂ using conventional transition metal phase diagrams as a reference. We demonstrate how the thermodynamics of mixing in the MoReSe₂ system during CVD growth dictates the formation of atomically sharp interfaces between MoSe₂ and ReSe₂, which can be confirmed by high-resolution scanning transmission electron microscopy imaging, revealing zigzag selenium-terminated interface between the epitaxial 2H and 1T′ lattices. Our work provides useful insights for understanding the stability of 2D heterostructures and interfaces between chemically, structurally, and electronically different phases.