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Alloying enables engineering of the electronic structure of semiconductorsfor optoelectronic applications. Due to their similar lattice parameters, thetwo-dimensional semiconducting transition metal dichalcogenides of the MoWSeSgroup (MX2 where M= Mo or W and X=S or Se) can be grown as high-qualitymaterials with low defect concentrations. Here we investigate the atomic andelectronic structure of Mo(1-x)WxS2 alloys using a combination ofhigh-resolution experimental techniques and simulations. Analysis of the Mo andW atomic positions in these alloys, grown by chemical vapour transport, showsthat they are randomly distributed, consistent with Monte Carlo simulationsthat use interaction energies determined from first-principles calculations.Electronic structure parameters are directly determined from angle resolvedphotoemission spectroscopy measurements. These show that the spin-orbitsplitting at the valence band edge increases linearly with W content from MoS2to WS2, in agreement with linear-scaling density functional theory (LS-DFT)predictions. The spin-orbit splitting at the conduction band edge is predictedto reduce to zero at intermediate compositions. Despite this,polarisation-resolved photoluminescence spectra on monolayer Mo0.5W0.5S2 showsignificant circular dichroism, indicating that spin-valley locking isretained. These results demonstrate that alloying is an important tool forcontrolling the electronic structure of MX2 for spintronic and valleytronicapplications.

Atomic and electronic structure of two-dimensional Mo(1-x)WxS2 alloys