Generating high-order optical and spin harmonics from ferromagnetic monolayers

High-order harmonic generation (HHG) in solids has entered a new phase of intensive research, with envisioned band-structure mapping on an ultrashort time scale. This partly benefits from a flurry of new HHG materials discovered, but so far has missed an important group. HHG in magnetic materials should have profound impact on future magnetic storage technology advances. Here we introduce and demonstrate HHG in ferromagnetic monolayers. We find that HHG carries spin information and sensitively depends on the relativistic spin–orbit coupling; and if they are dispersed into the crystal momentum k space, harmonics originating from real transitions can be k-resolved and carry the band structure information. Geometrically, the HHG signal is sensitive to spatial orientations of monolayers. Different from the optical counterpart, the spin HHG, though probably weak, only appears at even orders, a consequence of SU(2) symmetry. Our findings open an unexplored frontier—magneto-high-order harmonic generation. High-order harmonic generation (HHG) has been explored in different kinds of solids except magnetic materials. Here the authors theoretically predict that the HHG in ferromagnetic Fe thin films is sensitive to the spin–orbit coupling and carries band structure information.