Abstract
Spectroscopic second-harmonic generation (SHG) and reflectance-anisotropy spectroscopy are used to probe a single-domain reconstructed stepped Si(001) surface off cut 6° toward [110] before and after dissociative adsorption of at the step edges. The reflectance-anisotropy spectrum and the first- and third-order Fourier components of the SHG azimuthal anisotropy exhibit broad step-induced resonant peaks near 3.1 eV that are quenched in approximate proportion to dosage, suggesting that they all share a common origin in the essential electronic resonance of the steps. Analysis with a simplified bond-hyperpolarizability model suggests that hydrogen termination redistributes oscillator strength from the chemically active nearly vertical step dangling bond into three underlying bonds, suggesting the latter may be related to the third-order Fourier component of the SHG response.
© 2010 Optical Society of America
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