Two dimensional transition metal dichalcogenides grown by chemical vapor deposition

Abstract

An atomically thin film of semiconducting transition metal dichalcogenides (TMDCs) is emerging as a class of key materials in chemistry and physics due to their remarkable chemical and electronic properties. The TMDCs are layered materials with weak out-of-plane van der Waals (vdW) interaction and strong in-plane covalent bonding enabling scalable exfoliation into two-dimensional (2D) layers of atomic thickness. The growth techniques to prepare these 2D TMDC materials in high yield and large scale with high crystallinity have attracted intensive attention recently because of the new properties and potentials in nano-elctronic, optoelectronic, spintronic and valleytronic applications.

In this thesis, I develop methods for the chemical synthesis of 2D TMDCs films. The relevant growth mechanism and material characteristics of these films are also investigated. Molybdenum disulfide (MoS2) is synthesized by using molybdenum trioxide (MoO3) and sulfur (S) powder as the precursor. The films are formed on substrate pre-treated with reduced graphene oxide as the catalyst. However, this method cannot be extended to other TMDC materials such as molybdenum diselenide (MoSe2) and tungsten diselenide (WSe2) because reduced graphene oxide (rGO) reacts with selenium to form alloy materials rather than TMDC films. At the same time, the conversion of MoO3 to MoSe2 or that of tungsten trioxide (WO3) to WSe2 without the assistance of hydrogen in the chemical reaction is not thermodynamically feasible because the oxygen in the metal oxide cannot be replaced by selenium due to lower reactivity of the latter. On the other hand, I demonstrate that MoSe2 film can be synthesized directly by using MoSe2 and Se powder. Furthermore, the method of sulfurization or selenization of pre-deposited metal film can be promising due to precise thickness/size controls. Finally, some perspectives on the engineering challenges and fabrication methods of this family of materials will be given.