Basal plane oxygen exchange of epitaxial MoS2 without edge oxidation

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The intentional formation of defects in transition-metal dichalcogenides, such as MoS2, is an attractive way to modify the electronic and chemical properties of this class of 2D materials. However, the mechanisms and methods available for selective doping or modification of the basal plane must be improved. Here we investigate the process of O defect formation in epitaxial single-layer MoS2 on Au(1 1 1) using scanning tunneling microscopy (STM) and ambient pressure x-ray photoelectron spectroscopy (AP-XPS) during oxidation with O2 and H2O gas from low vacuum to the mbar range. Both oxidants result in exchange of S in the upper part of the basal plane with O, in line with air exposure experiments. Temperature-dependent measurements show that this is an activated process with an experimentally estimated reaction barrier of ∼0.79 ± 0.20 eV. We surprisingly find that the morphology of the MoS2 flakes and their edges remain intact in O2, even for relatively high degrees of basal plane O exchange, in contrast to the oxidation behavior of exfoliated single-layer MoS2. From analysis of atom-resolved STM images of the MoS2 edges, we can attribute this unusual stability to a passivating effect of excess edge sulfur species adsorbed under the sulfiding conditions of the MoS2 synthesis in H2S gas. We thus demonstrate that control over pre-sulfidation of the edges, temperature and pressure during oxidation can be used in a fast process to form strongly O doped single-layer MoS2 with no degradation of the initial shape and edge structure of the epitaxial MoS2 sheet.

OriginalsprogEngelsk
Artikelnummer045013
Tidsskrift2D materials
Vol/bind6
Nummer4
ISSN2053-1583
DOI
StatusUdgivet - okt. 2019

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