Ultra-High optical quality WS2 Atomic-Layers via a Growth-Etch MOCVD Approach

Metal organic chemical vapor deposition (MOCVD) is one of the main methodologies used for thin film fabrication in the semiconductor industry today and is considered one of the most promising routes to achieve large-scale and high-quality 2D transition metal dichalcogenides (TMDCs). However, MOCVD suffers from some serious drawbacks, such as small domain size (low crystallinity) and carbon contamination, resulting in poor optical quality, which may inhibit its implementation for the large-scale fabrication of atomic-thin semiconductors. Here we present a Growth-Etch MOCVD (GE-MOCVD) methodology, in which a small amount of water vapor is introduced during the growth, while the precursors are delivered in pulses. The evolution of the growth as a function of the amount of water vapor, the number and type of cycles and the gas composition is described. We show a domain size increase of more than four orders of magnitude relative to the conventional process. The improved crystal quality of WS2 (and WSe2) domains was demonstrated by means of Raman spectroscopy, photoluminescence (PL) spectroscopy and HRTEM studies. Moreover, time-resolved PL studies show a very long fluorescence lifetimes, comparable to those observed in mechanically exfoliated flakes. Thus, this unprecedented MOCVD-derived TMDC with ultra-high optical quality may open new opportunities to integrate such large-scale growth methodology into novel and existing technologies.