Surface localized phonon modes at the Si(553)-Au nanowire system

Abstract

The vibrational properties of the Si(553)-Au surface are studied by Raman spectroscopy and ab initio calculations. A multitude of surface localized phonon modes with wave number below 200 ${\mathrm{cm}}^{\ensuremath{-}1}$ is experimentally observed, along with two modes at about 400 ${\mathrm{cm}}^{\ensuremath{-}1}$. Atomistic models within density functional theory allow to assign the low-energy spectral features to vibrations within the Au chain, while the Raman signatures at higher energies are mostly localized at the Si step edge. The Raman activity of nominally silent modes associated with a large charge transfer between Au chain and Si step edge states is explained by scattering at charge density fluctuations. Temperature-dependent measurements reveal specific mode shifts that are discussed in terms of a recently proposed order-disorder phase transition. The presence of model-specific displacement patterns allows us to identify the structural models compatible with the measured spectra at low and at room temperature.