p-Type transition-metal doping of large-area MoS₂ thin films grown by chemical vapor deposition

Two-dimensional transition metal dichalcogenides (e.g. MoS₂) have recently emerged as a promising material system for electronic and optoelectronic applications. A major challenge for these materials, however, is to realize bipolar electrical transport properties (i.e. both p-type and n-type conduction), which is critical for enhancing device performance and functionalities. Here, we demonstrate the transition metal zinc as a p-type dopant in the otherwise n-type MoS₂, through systematic characterizations of large area Zn-doped MoS₂ thin films grown by a one-step chemical vapor deposition (CVD) approach. Raman characterization and X-ray photoelectron spectroscopy studies identified millimeter-scale, monolayer films with 1-2% Zn as dopants. Zinc doping suppresses n-type conductivity in MoS₂ and shifts its Fermi level downwards. The stability and p-type nature of Zn dopants were further confirmed by density-functional-theory calculations of formation energies and electronic band structures. The electrical transport properties of Zn-MoS₂ films can be influenced by stoichiometry, and p-type gate transfer characteristics were realized by thermal treatment under a sulfur atmosphere. Our work highlights transition-metal doping followed by sulfur vacancy elimination in CVD grown films as a promising route for achieving large area p-type transition metal dichalcogenide films that are essential for practical applications in electronics and optoelectronics.