Synthesis of ultrahigh-quality monolayer molybdenum disulfide through in-situ defect healing with thiol molecules

TL;DR

This paper introduces a novel CVD method using thiol as a liquid precursor to synthesize ultrahigh-quality monolayer MoS2 with minimal sulfur vacancies and exceptional optical properties, advancing 2D material production.

Contribution

It demonstrates a new thiol-based CVD process that significantly reduces defects in monolayer MoS2 compared to traditional methods.

Findings

Lowest sulfur vacancy concentration among reported CVD MoS2

Ultrahigh optical quality of synthesized MoS2

Thiol molecules repair sulfur vacancies during growth

Abstract

Monolayer transition metal dichalcogenides (TMDCs) are two-dimensional (2D) materials with many potential applications. Chemical vapour deposition (CVD) is a promising method to synthesize these materials. However, CVD-grown materials generally have poorer quality than mechanically exfoliated ones and contain more defects due to the difficulties in controlling precursors' distribution and concentration during growth where solid precursors are used. Here, we propose to use thiol as a liquid precursor for CVD growth of high quality and uniform 2D MoS2. Atomic-resolved structure characterizations indicate that the concentration of sulfur vacancies in the MoS2 grown from thiol is the lowest among all reported CVD samples. Low temperature spectroscopic characterization further reveals the ultrahigh optical quality of the grown MoS2. Density functional theory simulations indicate that thiol molecules could interact with sulfur vacancies in MoS2 and repair these defects during the growth of MoS2, resulting in high quality MoS2. This work provides a facile and controllable method for the growth of high-quality 2D materials with ultralow sulfur vacancies and high optical quality, which will benefit their optoelectronic applications.