The generation of Second-Harmonic (SK) radiation from simple metals ha
s been the subject of numerous investigations for almost three decades
. The use of clean metal surfaces in the experiments and increasingly
sophisticated jellium-based theoretical models has led to a convergenc
e on the magnitude and some of the dispersion characteristics of SH ge
neration in free-electron metals like aluminum. However, the sensitivi
ty of the SH-generation process to crystal symmetry, surface morpholog
y, and surface electronic states indicates that nonlinear optical prop
erties are influenced by processes which cannot be explained using a m
odel based on an isotropic electron gas. Here, we review some recent e
xperimental work indicating where deviation from jellium-based models
occurs and attempts to understand these.