Tunable Ferromagnetism and Thermally Induced Spin Flip in Vanadium-doped Tungsten Diselenide Monolayers at Room Temperature

Abstract: The outstanding optoelectronic and valleytronic properties of transition metal dichalcogenides (TMDs) have triggered intense research efforts by the scientific community. An alternative to induce long-range ferromagnetism (FM) in TMDs is by introducing magnetic dopants to form a dilute magnetic semiconductor. Enhancing ferromagnetism in these semiconductors not only represents a key step towards modern TMD-based spintronics, but also enables exploration of new and exciting dimensionality-driven magnetic phenomena. To this end, we show tunable ferromagnetism at room temperature and a thermally induced spin flip (TISF) in monolayers of V-doped WSe2. As vanadium concentrations increase within the WSe2 monolayers the saturation magnetization increases, and it is optimal at ~4at.% vanadium; the highest doping/alloying level ever achieved for V-doped WSe2 monolayers. The TISF occurs at ~175 K and becomes more pronounced upon increasing the temperature towards room temperature. We demonstrate that TISF can be manipulated by changing the vanadium concentration within the WSe2 monolayers. We attribute TISF to the magnetic field and temperature dependent flipping of the nearest W-site magnetic moments that are antiferromagnetically coupled to the V magnetic moments in the ground state. This is fully supported by a recent spin-polarized density functional theory calculation. Our findings pave the way for the development of novel spintronic and valleytronic nanodevices based on atomically thin magnetic semiconductors and stimulate further studies in this rapidly expanding research field of 2D magnetism.