Optical second harmonic generation (SHG) in reflection from Cr/Fe(100)
and Au/Fe(100) shows a longitudinal nonlinear Kerr rotation that may
be tuned at will between 0 degrees and 90 degrees, where the linear Ke
rr angle is always less than 0.1 degrees. The result is in perfect agr
eement with a simple phenomenological model assuming interface contrib
utions only, and with spin dependent bandstructure calculations.