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We show that the nonlinear optical response reflects sensitively theelectronic structure of transition-metal surfaces and interfaces. $d$ and $s$electrons may contribute rather differently to the second harmonic generation(SHG) signal. This results from the different sensitivity of $d$ and $s$electrons to surface and symmetry changes. Consequently, SHG for noble metalsshows a by far larger dependence on the polarization of the incoming light thanfor transition metals like Fe, Co, Ni, in particular at lower frequencies. Thetheoretical results are compared with recent measurements. We conclude that theSHG yield is in addition to the nonlinear magneto-optical Kerr-effect asensitive fingerprint of the electronic structure at surfaces and interfaces.

physical review. b, condensed matter

Theory for the nonlinear optical response of transition metals: Polarization dependence as a fingerprint of the electronic structure at surfaces and interfaces