Atmospheric-pressure chemical vapor deposition (CVD) is used to grow monolayer MoS 2 two-dimensional crystals at elevated temperatures on silicon substrates with a 300 nm oxide layer. Our CVD reaction is hydrogen free, with the sulfur precursor placed in a furnace separate from the MoO 3 precursor to individually control their heating profiles and provide greater flexibility in the growth recipe. We intentionally establish a sharp gradient of MoO 3 precursor concentration on the growth substrate to explore its sensitivity to the resultant MoS 2 domain growth within a relatively uniform temperature range. We find that the shape of MoS 2 domains is highly dependent upon the spatial location on the silicon substrate, with variation from triangular to hexagonal geometries. The shape change of domains is attributed to local changes in the Mo:S ratio of precursors (1:>2, 1:2, and 1:<2) and its influence on the kinetic growth dynamics of edges. These results improve our understanding of the factors that influence the growth of MoS 2 domains and their shape evolution.

Defects in graphene alter its electrical, chemical, magnetic and mechanical properties. The intentional creation of defects in graphene offers a means for engineering its properties. Techniques such as ion irradiation intentionally induce atomic defects in graphene, for example, divacancies, but these defects are randomly scattered over large distances. Control of defect formation with nanoscale precision remains a significant challenge. Here we show control over both the location and average complexity of defect formation in graphene by tailoring its exposure to a focussed electron beam. Divacancies and larger disordered structures are produced within a 10×10 nm 2 region of graphene and imaged after creation using an aberrationcorrected transmission electron microscope. some of the created defects were stable, whereas others relaxed to simpler structures through bond rotations and surface adatom incorporation. These results are important for the utilization of atomic defects in graphene-based research.

A simple method is presented for synthesizing large single crystal graphene domains on melted copper using atmospheric pressure chemical vapor deposition (CVD). This is achieved by performing the reaction above the melting point of copper (1090 °C) and using a molybdenum or tungsten support to prevent balling of the copper from dewetting. By controlling the amount of hydrogen during growth, individual single crystal domains of monolayer graphene greater than 200 μm are produced within a continuous film. Stopping growth before a complete film is formed reveals individual hexagonal domains of graphene that are epitaxially aligned in their orientation. Angular resolved photoemission spectroscopy is used to show that the graphene grown on copper exhibits a linear dispersion relationship and no sign of doping. HRTEM and electron diffraction reveal a uniform high quality crystalline atomic structure of monolayer graphene.

Focused electron beam irradiation has been used to create mono and divacancies in graphene within a defined area, which then act as trap sites for mobile Fe atoms initially resident on the graphene surface. Aberration-corrected transmission electron microscopy at 80 kV has been used to study the real time dynamics of Fe atoms filling the vacancy sites in graphene with atomic resolution. We find that the incorporation of a dopant atom results in pronounced displacements of the surrounding carbon atoms of up to 0.5 Å, which is in good agreement with density functional theory calculations. Once incorporated into the graphene lattice, Fe atoms can transition to adjacent lattice positions and reversibly switch their bonding between four and three nearest neighbors. The C atoms adjacent to the Fe atoms are found to be more susceptible to Stone-Wales type bond rotations with these bond rotations associated with changes in the dopant bonding configuration. These results demonstrate the use of controlled electron beam irradiation to incorporate dopants into the graphene lattice with nanoscale spatial control.

We show that controlling the introduction time and the amount of sulphur (S) vapour relative to the WO3 precursor during the chemical vapour deposition (CVD) growth of WS2 is critical to achieving large crystal domains on the surface of silicon wafers with a 300 nm oxide layer. We use a two furnace system that enables the S precursor to be separately heated from the WO3 precursor and growth substrate. Accurate control of the S introduction time enabled the formation of triangular WS2 domains with edges up to 370 μm which are visible to the naked eye. The WS2 domains exhibit room-temperature photoluminescence with a peak value around ∼635 nm and a full-width at half-maximum (FWHM) of ∼12 nm. Selected area electron diffraction from different regions of the triangular WS2 domains showed that they are single crystal structures.