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The unique optical and electronic properties of two-dimensional transitionmetal dichalcogenides (2D TMDs) make them promising materials for applicationsin (opto-)electronics, catalysis and more. Specifically, alloys of 2D TMDs havebroad potential applications owing to their composition-controlled properties.Several important challenges remain regarding controllable and scalablefabrication of these alloys, such as achieving control over their atomicordering (i.e. clustering or random mixing of the transition metal atoms withinthe 2D layers). In this work, atomic layer deposition (ALD) is used tosynthesize the TMD alloy Mo$_{1-x}$W$_{x}$S$_{2}$ with excellent compositioncontrol along the complete composition range 0 $\leq$ x $\leq$ 1. Importantly,this composition control allows us to control the atomic ordering of the alloyfrom well-mixed to clustered while keeping the alloy composition fixed, as isconfirmed directly through atomic-resolution HAADF-STEM imaging. The controlover atomic ordering leads to tuning of the bandgap, as is demonstrated usingoptical transmission spectroscopy. The relation between this tuning of theelectronic structure and the atomic ordering of the alloy was further confirmedthrough ab-initio calculations. Furthermore, as the atomic ordering modulatesfrom clustered to well-mixed, the typical MoS$_{2}$ and WS$_{2}$ A$_{1g}$vibrational modes converge. Our results demonstrate that atomic ordering is animportant parameter that can be tuned experimentally to finely tune thefundamental properties of 2D TMD alloys for specific applications.

Controlling transition metal atomic ordering in two-dimensional Mo$_{1-x}$W$_{x}$S$_{2}$ alloys