ABSTRACT
One-dimensional wires are known to be inherently unstable at finite temperature. Here, we show that long-range order of atomic Au double chains adsorbed on a Si(553) surface is not only stabilized by interaction with the substrate, but spontaneous self-healing of structural defects is actually enforced by the adsorption of atomic species such as Au or H. This is true even for random adsorbate distribution. Combining atomistic models within density functional theory with low energy electron diffraction and high-resolution electron energy loss spectroscopy, we demonstrate that this apparently counterintuitive behavior is mainly caused by adsorption-induced band filling of modified surface bands, i.e., by the strong electronic correlation throughout the whole terrace. Although adsorption preferably occurs at the step edge, it enhances the dimerization and the stiffness of the Au dimers. Thus, the intertwinement of quasi-1D properties with delocalized 2D effects enforces the atomic wire order.
ABSTRACT
The plasmonic signals of quasi-1D electron systems are a clear and direct measure of their metallic behavior. Due to the finite size of such systems in reality, plasmonic signals from a gold-induced superstructure on Si(5 5 3) can be studied with infrared spectroscopy. The infrared spectroscopic features have turned out to be extremely sensitive to adsorbates. Even without geometrical changes of the surface superstructure, the effects of doping, of the adsorbate induced electronic surface scattering, and of the electronic polarizability changes on top of the substrate surface give rise to measurable changes of the plasmonic signal. Especially strong changes of the plasmonic signal have been observed for gold, oxygen, and hydrogen exposure. The plasmonic resonance gradually disappears under these exposures, indicating the transion to an insulating behavior, which is in accordance with published results obtained from other experimental methods. For C70 and, as shown here for the first time, TAPP-Br, the plasmonic signal almost retains its original intensity even up to coverages of many monolayers. For C70, the changes of the spectral shape, e.g. of electronic damping and of the resonance position, were also found to be marginal. On the other hand, TAPP-Br adsorption shifts the plasmonic resonance to higher frequencies and strongly increases the electronic damping. Given the dispersion relation for plasmonic resonances of 1D electron systems, the findings for TAPP-Br indicate a push-back effect and therefore stronger confinement of the free charge carriers in the quasi-one-dimensonal channel due to the coverage by the flat TAPP-Br molecules. On the gold-doped Si(5 5 3)-Au surface TAPP-Br acts as counter dopant and increases the plasmonic signal.
