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Alloying enables engineering of the electronic structure of semiconductors for optoelectronic applications. Due to their similar lattice parameters, the two-dimensional semiconducting transition metal dichalcogenides of the MoWSeS group (MX 2  where M = Mo or W and X = S or Se) can be grown as high-quality materials with low defect concentrations. Here we investigate the atomic and electronic structure of Mo (1− x ) W x S 2  alloys using a combination of high-resolution experimental techniques and simulations. Analysis of the Mo and W atomic positions in these alloys, grown by chemical vapour transport, shows that they are randomly distributed, consistent with Monte Carlo simulations that use interaction energies determined from first-principles calculations. Electronic structure parameters are directly determined from angle resolved photoemission spectroscopy measurements. These show that the spin–orbit splitting at the valence band edge increases linearly with W content from MoS 2  to WS 2 , in agreement with linear-scaling density functional theory predictions. The spin–orbit splitting at the conduction band edge is predicted to reduce to zero at intermediate compositions. Despite this, polarisation-resolved photoluminescence spectra on monolayer Mo 0.5 W 0.5 S 2  show significant circular dichroism, indicating that spin-valley locking is retained. These results demonstrate that alloying is an important tool for controlling the electronic structure of MX 2  for spintronic and valleytronic applications.

Atomic and electronic structure of two-dimensional Mo(1− x )W x S2 alloys

Atomic and electronic structure of two-dimensional Mo₍₁₋ _x )W _x S₂ alloys