Atomic-scale imaging of the surface dipole distribution of stepped surfaces

TL;DR

This study combines atomically resolved SFM and KPFM imaging with DFT calculations to reveal atomic-scale surface dipole variations on silicon vicinal surfaces, highlighting non-uniform work function related to surface dipoles.

Contribution

First simultaneous atomic-resolution SFM and KPFM imaging of a silicon vicinal surface, demonstrating intrinsic surface dipole variations explained by DFT and the Smoluchowski effect.

Findings

Surface dipole distribution varies at atomic scale.

Local contact potential difference is non-uniform.

DFT reproduces experimental images without tip modeling.

Abstract

Stepped well-ordered semiconductor surfaces are important as nanotemplates for the fabrication of one-dimensional nanostructures which are candidates of intriguing electronic properties. Therefore a detailed understanding of the underlying stepped substrates is crucial for advances in this field. Although measurements of step edges are challenging for scanning force microscopy (SFM), here we present for the first time simultaneous atomically resolved SFM and Kelvin probe force microscopy (KPFM) images of a silicon vicinal surface. We find that the local contact potential difference is not homogeneous over all silicon atoms, contrary to the common understanding of the work function. For the interpretation of the data we performed density functional theory (DFT) calculations. We explain the atomic-scale electronic features by differences in the surface dipole distribution caused by a Smoluchowski-type effect. E.g., at step edges the partial negative charge is larger at the lower-lying atoms closer to the bulk than at the atoms more protruding towards the vacuum. This is the first manifestation of such type of effect on a semiconductor surface. The DFT images accurately reproduce the experiments even without including the tip in the calculations. This underlines that the high-resolution KPFM images indeed show the intrinsic properties of the surface and not only tip-surface interactions.