Abstract
Optical second harmonic generation (SHG) and sum frequency generation (SFG) provide a unique opportunity for studying surface and interface properties. After introducing the phenomenological theory of SHG at metal surfaces, we discuss recent microscopic evaluations of the nonlinear surface polarizability components. As before, we focus on the nonlinear response at simple metal surfaces. In these systems, the isotropic perpendicular component of the surface polarization is particularly important since it is determined by the gradients of the normal component of the electric field. A striking result of the TDLDA calculations is that, as in the linear case, the main spectral features are the threshold excitation and multipole surface plasmon. These excitations play an important role in SHG from Al and adsorbed alkali metal layers. The remarkable surface sensitivity of the perpendicular polarization can be seen if the metal is charged. We also discuss surfaces at which the inversion symmetry is broken in the parallel direction, for example, the (111) face of fcc crystals and stepped metal surfaces. The anisotropic component of the surface polarization in these systems can be as large as the main isotropic component.
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Liebsch, A. (1997). Nonlinear Optics. In: Electronic Excitations at Metal Surfaces. Physics of Solids and Liquids. Springer, Boston, MA. https://doi.org/10.1007/978-1-4757-5107-9_5
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DOI: https://doi.org/10.1007/978-1-4757-5107-9_5
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