Electronic theory for the nonlinear magneto-optical response of transition metals at surfaces and interfaces: Dependence of the Kerr rotation on the polarization and magnetic easy axis.

We extend our previous study of the polarization dependence of the nonlinear optical response to the case of magnetic surfaces and buried magnetic interfaces. We calculate for the longitudinal and polar configuration the nonlinear magneto-optical Kerr rotation angle. In particular, we show which tensor elements of the susceptibilities are involved in the enhancement of the Kerr rotation in nonlinear optics for different configurations and we demonstrate by a detailed analysis how the direction of the magnetization and thus the easy axis at surfaces and buried interfaces can be determined from the polarization dependence of the nonlinear magneto-optical response, since the nonlinear Kerr rotation is sensitive to the electromagnetic field components instead of merely the intensities. We also prove from the microscopic treatment of spin-orbit coupling that there is an intrinsic phase difference of 90 between tensor elements which are even or odd under magnetization reversal in contrast to linear magneto-optics. Finally, we compare our results with several experiments on Co/Cu films and on Co/Au and Fe/Cr multilayers. We conclude that the nonlinear magneto-optical Kerr-effect determines uniquely the magnetic structure and in particular the magnetic easy axis in films and