Abstract
Even-order non-linear optical spectroscopy has emerged as an unusually
sensitive technique for non-invasive analysis of surfaces and buried
interfaces of centrosymmetric materials. The forefront challenges
are: to develop reliable microscopic computational methods for calculating
and interpreting measured surface non-linear spectra; to relate non-linear
surface spectra quantitatively to linear optical surface probes such
as reflectance-difference spectroscopy (RDS); and to develop convenient
methods for acquiring non-linear optical spectra over bandwidths
(several electron-volts) that encompass multiple electronic surface
resonances. We review recent advances in both calculation and measurement
of non-linear spectra, with emphasis on reconstructed and adsorbate-covered
silicon surfaces in epitaxial growth environments. Copyright © 2001
John Wiley & Sons, Ltd.
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