Second-harmonic generation and effect of adsorbates for free-electron metal and semiconductor surfaces |
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Authors: | Frank Rebentrost |
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Institution: | Max-Planck-Institut für Quantenoptik 85748, Garching near Munich, Germany |
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Abstract: | We discuss aspects of a developing microscopic theory of SHG from simple metal and semiconductor surfaces. For semiconductors calculations of the dynamical nonlinear susceptibility on the basis of realistic tight-binding parametrizations of the electronic Hamiltonian provide a practical scheme. In the resulting spectra the effect of the dangling bonds on SHG is clearly seen together with a strong decrease upon saturation with H atoms. In the metal case the adsorbate induced changes of the static nonlinear electron density can be calculated self-consistently by applying density functional theory to the jellium model. The second-order dipole moment determines the effect of adsorbates on the SHG intensity in the adiabatic limit. Quite general a correlation with the nature of the adsorbate expressed by its electronegativity and the characteristic charge transfer, adsorption dipole and polarizabilities in first and second order is found. |
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