Tuning the Magnetic and Electronic Properties of Monolayer VI3 by 3d Transition Metal Doping: A First-Principles Study

Abstract Two-dimensional (2D) materials with robust magnetism have drawn immense attention for their promising applications in spintronics. Recently, intrinsic ferromagnetic vanadium triiodide (VI3) has been synthesized experimentally. To enhance its spintronic property, we modified VI3 by interstitial doping with 3d transition metals (TM) and used first-principles calculations to investigate the geometric structure, formation energy, electronic property, and magnetism of pristine VI3 and 3d TM-doped VI3 monolayer. Among eight transition metal (Sc-, Ti-, V-, Cr-, Mn-, Fe-, Co-, and Ni-) doped VI3 materials, four of them (Ti-, V-, Mn-, and Ni-doped VI3) show robust magnetism with full spin polarization near the Fermi energy. Our research demonstrates that Ti-doped VI3 results in half-metallic semiconductor properties (HMS), while V-doped VI3 and Ni-doped VI3 result in half-semiconductor properties (HSC). Surprisingly, Mn-doped VI3 exhibits an unusual bipolar magnetic semiconductor property (BMS). This unique combination of strong ferromagnetism and 100% spin polarization with a half-metallic, half-semiconductor, or bipolar semiconductor property renders 3d TM-doped VI3 as potential candidates for next generation semiconductor spintronic applications. These spin-polarized materials will be extremely useful for spin-current generation and other spintronic applications.