Abstract
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.
Highlights
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
HHG in nonmagnetic materials is only subject to the spatial symmetry
Such a sensitive dependence of harmonic signals on density of states (DOS) found here is important, as it suggests a potentially useful application to map band states through HHG in magnetic materials. This reminds us of our earlier work on C6010, where nearly every harmonic can be uniquely assigned to a particular transition
Summary
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. In 2011, HHG in ZnO reported by Ghimire et al.[16] renewed the interest in solid state HHG, which has quickly expanded into monolayer[17] and multilayer graphene[18], MgO19,20, Si21, MoS222, Bi2Se323, SiO224,25, Ar/Kr solids[26], GaSe27–29, and metal-sapphire nanostructures[30]. To this end, little attention has been paid to magnetic systems[31,32]. Our study opens a new direction by extending high-harmonic generation to magnetic materials
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