Extracting maximum information from polarized surface vibrational spectra: application to etched, H-terminated Si(110) surfaces.
A general method to maximize the information extracted from polarized surface absorption spectra is developed and applied to the study of etched Si(110) surfaces. In essence, this technique transforms spectra from the experimental reference frame, which is defined by the direction of the surface electric field during irradiation by s- and p-polarized light, into a more appropriate Cartesian reference frame defined by the surface normal and the plane of incidence. If the Cartesian reference frame is aligned with high symmetry directions of the system, significant spectral simplification can result. This analysis relies on the well-known boundary conditions on interfacial electric fields and is independent of any adsorbate screening or the effective dielectric constant of the adsorbate layer. The validity of this analysis is demonstrated on the spectra of NH4F-etched, H-terminated Si(110). The transition dipole moments of the symmetric and antisymmetric Si[Single Bond]H stretch modes associated with flat terraces are polarized along the [110] and [001] directions, respectively. Two additional modes with transition dipoles polarized along the [001] and [110] directions are assigned to defect species associated with microfaceting and other surface roughness. Data taken in two different experimental geometries are shown to be in excellent quantitative agreement, confirming the validity of the technique. Additionally, the measured adsorbate layer dielectric constant is in good agreement with previously reported values for hydrogen-terminated silicon surfaces.
Clark
Ian T
IT
Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, USA.
Aldinger
Brandon S
BS
Gupta
Ankush
A
Hines
Melissa A
MA