Optically Driven Magnetic Phase Transition of Monolayer RuCl3

Strong light-matter interactions within nanoscale structures offer the possibility of optically controlling material properties. Motivated by the recent discovery of intrinsic long-range magnetic order in two-dimensional materials, which allow for the creation of novel magnetic devices of unprecedented small size, we predict that light can couple with magnetism and efficiently tune magnetic orders of monolayer ruthenium trichloride (RuCl3). First-principles calculations show that both free carriers and optically excited electron–hole pairs can switch monolayer RuCl3 from a proximate spin-liquid phase to a stable ferromagnetic phase. Specifically, a moderate electron–hole pair density (on the order of 1 × 1013 cm–2) can significantly stabilize the ferromagnetic phase by 10 meV/f.u. in comparison to the competing zigzag phase, so that the predicted ferromagnetism can be driven by optical pumping experiments. Analysis shows that this magnetic phase transition is driven by a combined effect of doping-induced lattice strain and itinerant ferromagnetism. According to Ising-model calculations, we find that the Curie temperature of the ferromagnetic phase can be increased significantly by raising carrier or electron–hole pair density. This enhanced optomagnetic effect opens new opportunities to manipulate two-dimensional magnetism through noncontact, optical approaches.