Using an electronic tight-binding theory we calculate the nonlinear magneto-optical response from an x-Cu/1Fe/Cu(001) film as a function of frequency and Cu overlayer thickness (x=3. . .25). We find very strong spinpolarized quantum well oscillations in the nonlinear magneto-optical Kerr effect (NOLIMOKE). These are enhanced by the large density of Fe d states close to the Fermi level acting as intermediate states for frequency doubling.In good agreement with experiment we find two oscillation periods of 6-7 and 11 monolayers the latter being more pronounced.
Typeset using REVT E X 1The magnetism of low-dimensional metallic structures such as surfaces, thin films, and multilayer sandwiches has recently become an exciting new field of research and applications [1]. In particular, thin magnetic films and multilayers exhibit a rich variety of properties not previously found in bulk magnetism such as enhanced or reduced moments [2], oscillatory exchange coupling through nonmagnetic spacers [3][4][5], giant magnetoresistance [6,7], and the reorientation of the magnetic easy axis upon thickness and temperature variation [8][9][10][11]. Especially the observation of spin-polarized quantum well states (QWS) [12][13][14][15] in Cu/Co (001) has attracted a great deal of attention. It has become clear that quantum well states are indeed responsible for the important oscillatory behavior of the exchange coupling of ferromagnetic thin films via nonmagnetic spacers [16,17]. Presently mainly photoemission (PE) and inverse photoemission (IPE) [12][13][14][15] have been used to identify QWS effects. Very recently a possible connection between thickness dependent changes in NOLIMOKE and QWS [18] has been proposed.It is the goal of this Letter to show that also nonlinear optics, in particular NOLIMOKE, is a new sensitive tool for studying QWS. We find very interesting structure in the NO-LIMOKE signal due to particular transitions in k-space. This is very remarkable since it indicates that NOLIMOKE is able to detect very sensitively k-dependent structures. This new effect seems to be of general interest for the physics of nonlinear optics and its relationship to the underlying electronic structure. Note, this is not the case for linear optics, since there the contribution of the Drude term of the dielectric function creates a strong background of transitions from all k-directions. Nonlinear optics, in contrast to linear op-