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Single-layer MoS₂is a direct-gap semiconductor whose band edges character is dominated by the d-orbitals of the Mo atoms. It follows that substitutional doping of the Mo atoms has a significant impact on the material’s electronic properties, namely the size of the band gap and the position of the Fermi level. Here, density functional theory is used along with the G₀W₀method to examine the effects of substituting Mo with four different transition metal dopants: Nb, Tc, Ta, and Re. Nb and Ta possess one less valence electron than Mo does and are therefore p-type dopants, while Re and Tc are n-type dopants, having one more valence electron than Mo has. Four types of substitutional structures are considered for each dopant species: isolated atoms, lines, three-atom clusters centered on a S atom (c3s), and three-atom clusters centered on a hole (c3h). The c3h structure is found to be the most stable configuration for all dopant species. However, electronic structure calculations reveal that isolated dopants are preferable for efficient n- or p-type performance. Lastly, it is shown that photoluminescence measurements can provide valuable insight into the atomic structure of the doped material. Understanding these properties of substitutionally-doped MoS₂can allow for its successful implementation into cutting-edge solid state devices.

Two-dimensional semiconductors, including transition metal dichalcogenides, are of interest in electronics and photonics but remain nonmagnetic in their intrinsic form. Previous efforts to form two-dimensional dilute magnetic semiconductors utilized extrinsic doping techniques or bulk crystal growth, detrimentally affecting uniformity, scalability, or Curie temperature. Here, we demonstrate an in situ substitutional doping of Fe atoms into MoS₂monolayers in the chemical vapor deposition growth. The iron atoms substitute molybdenum sites in MoS₂crystals, as confirmed by transmission electron microscopy and Raman signatures. We uncover an Fe-related spectral transition of Fe:MoS₂monolayers that appears at 2.28 eV above the pristine bandgap and displays pronounced ferromagnetic hysteresis. The microscopic origin is further corroborated by density functional theory calculations of dipole-allowed transitions in Fe:MoS₂. Using spatially integrating magnetization measurements and spatially resolving nitrogen-vacancy center magnetometry, we show that Fe:MoS₂monolayers remain magnetized even at ambient conditions, manifesting ferromagnetism at room temperature.