Nonlinear Optics-Driven Spin Reorientation in Ferromagnetic Materials.

Based on nonlinear optics, we propose that light irradiation could induce a nonequilibrium steady state magnetization variation. We formulize a band theory to elucidate its general microscopic mechanisms, which are rooted by the quantum geometric structure and topological nature of electronic Bloch wave functions. The existence is determined by the light polarization and specific material symmetry, based on the magnetic group theory. In general, for a magnetic system, both circularly and linearly polarized light could exert an effective magnetic field and a magnetic "velocity" (magnetization variation rate over time, serving as an effective torque) to reorient the magnetization direction. They are contributed by spin and orbital angular momenta simultaneously. Aided by group theory and first-principles calculations, we illustrate this theory using a showcase example of monolayer NiCl, showing that light irradiation effectively generates an out-of-plane effective magnetic torque, which lifts its in-plane easy magnetization. According to magnetic dynamic simulations, under light with a modest intensity, this switching could occur on the order of 0.1-1 ns time scale, demonstrating its ultrafast nature that is desirable for quantum manipulation.