Abstract
The generation of Second-Harmonic (SH) radiation from simple metals has 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 convergence on the magnitude and some of the dispersion characteristics of SH generation in free-electron metals like aluminum. However, the sensitivity of the SH-generation process to crystal symmetry, surface morphology, and surface electronic states indicates that nonlinear optical properties are influenced by processes which cannot be explained using a model based on an isotropic electron gas. Here, we review some recent experimental work indicating where deviation from jellium-based models occurs and attempts to understand these.
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