Toward Controlled Growth of Two-Dimensional Transition Metal Dichalcogenides: Chemical Vapor Deposition Approaches

Abstract

Recently, atomically thin two-dimensional (2D) transition metal dichalcogenides (TMDCs) materials have drawn significant attention due to their unique optical and electrical properties1, 2. This offers unique opportunities for the next-generation electronic and optoelectronic devices3. Specifically, recent innovations in the big-data-driven prediction of new 2D materials, integration of new device architectures, interfacial engineering of contacts between semiconductor/metals and semiconductor/dielectrics as well as encapsulation in hexagonal boron nitride4, 5 have further propelled the electrical mobility to be on a par with or even beyond the silicon (Si) counterpart. These strategies hold tantalizing prospects on extending the Moore's law. Yet, there is still room for improvement before 2D TMDCs become truly technologically relevant. The challenge lies in the full validation of the intrinsic charge transport that is associated with the specific nature and ordered arrangement of atoms in the atomically thin crystal lattice. This requires, the controlled stitch of both metals and chalcogenides in an atom-by-atom fashion. To this end, a variety of synthetic approaches have been developed, this includes but not limited to chemical vapor deposition (CVD) 6, 7, mechanical exfoliation8 and solution-based exfoliation9. Among which, CVD shows better controllability over thicknesses, geometric shapes, sizes, and qualities through manipulation of the growth factors, e.g., growth temperature, pressure, precursor ratio, and gas carrier. These complex growth environments will significantly confound the scalability, crystallinity, defect density, and reproducibility of the CVD approach. Therefore, an impetus exists to gain fundamental insights into the universal growth mechanism that is currently lacking and therefore curbs the realization o the controlled epitaxy of high-mobility three-atom-thick semiconducting TMDCs films with wafer-scale-homogeneity. In this thesis, a mechanistic study toward revealing the epitaxy growth mechanism is established to include 1) epitaxy growth of multilayer, 2) epitaxy growth of heterostructures, and 3) epitaxy growth of high quality (exceedingly low defect density) of 2D TMDCs materials through a controlled CVD strategy.