Abstract
Two-dimensional (2D) ferromagnetic (FM) semiconductors play imperative roles in the development of spintronic devices. However, the Curie temperature (Tc) of most 2D FM semiconductors are fairly low for practical applications. Herein, using the first-principles calculations, it revealed that the magnetic coupling strength within CrI3 can be modulated via the construction of CrI3/VSe2 van der Waals heterostructure. The system remains semiconducting with the band gap of 0.22 eV (GGA level). Its Tc can be boosted to ∼210 K via p-type doping, well above the liquid nitrogen temperature, which makes it a step closer to practical application. The greatly promoted FM coupling is originated from the additional super-exchange paths as well as the enhanced in-plane Cr-I-Cr super-exchange interaction. It is found that the interlayer magnetic coupling is tunable upon the stacking alignment, which is feasible to manipulate the magnetic orders using external mechanical motion.
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