Optical second- and third-harmonic generation on epitaxial films of the ferromagnetic semiconductor europium oxide reveal selective coupling to the magnetic and crystallographic properties of the compound. Second-harmonic generation couples linearly to the order parameter parametrizing the long-range ferromagnetic order. In contrast, third-harmonic generation couples to the crystallographic lattice and to the short-range spin-spin correlations manifesting macroscopically as a magnetostrictive effect. These results demonstrate the potential of nonlinear optics for acquiring unique information about the crystallographic, electronic, and magnetic properties of spintronics compounds.
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