LAUSR

Two-dimensional (2D) alloys represent a versatile platform that extends the properties of atomically thin transition-metal dichalcogenides. Here, using molecular beam epitaxy (MBE), we investigate the growth of 2D vanadium-molybdenum diselenide alloys, VxMo1-xSe2, on highly oriented pyrolytic graphite, and unveil their structural, chemical and electronic integrities via measurements by scanning tunneling microscopy/spectroscopy (STM/STS), synchrotron X-ray photoemission (XPS), and X-ray absorption spectroscopy (XAS). Essentially, we found a critical value of x = ~0.44, below which phase separation occurs, and above which a homogeneous metallic phase is favored. Another observation is an effective increase in the density of mirror twin boundaries of constituting MoSe2 in the low V concentration regime (x ≤ 0.05). Density functional theory calculations support our experimental results on the thermal stability of 2D VxMo1-xSe2 alloys, and suggest an H phase of the homogeneous alloys with alternating parallel V and Mo strips randomly in-plane stacked. Element-specific XAS of the 2D alloys, which clearly indicates quenched atomic multiplets similar to the case of 2H-VSe2, provides strong evidence for the H phase of the 2D alloys. This work provides a comprehensive understanding of the thermal stability, chemical state and electronic structure of 2D VxMo1-xSe2 alloys, useful for the future design of 2D electronic devices.