We study the electron dynamics at a monocrystalline Pd(111) surface with stepped vicinal nanostructures modeled in a simple Kronig-Penney scheme. The unoccupied bands of the surface are resonantly excited via the resonant charge transfer (RCT) interaction of the surface with a hydrogen anion reflected at grazing angles. The interaction dynamics is simulated numerically in a quantum mechanical wave packet propagation approach. Visualization of the wave packet density shows that, when the electron is transferred to the metal, the surface and image subband states are the most likely locations of the electron as it evolves through the superlattice. The survival probability of the interacting ion exhibits strong modulations as a function of the vicinal-terrace size and shows peaks at those energies that access the image state subband dispersions. A simple square well model producing standing waves between the steps on the surface suggests the application of such ion-scattering at shallow angles to map electronic substructures in vicinal surfaces. The work also serves as the first proof-of-principle in the utility of our computational method to address, via RCT, surfaces with nanometric patterns.

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Synopsis We investigate the electron dynamics at various monocrystalline metal surfaces with stepped vicinal nanostructures. The unoccupied bands of the surface superlattice are resonantly excited via the charge transfer interaction of the surface with a H− ion which flies by at grazing angles. The ion survival exhibits modulations as a function of the vicinal-terrace size and shows peaks at energies that access the image state subbands.

We compare the electron dynamics at monocrystalline Cu(111), Au(100) and Pd(111) precursor substrates with vicinal nanosteps. The unoccupied bands of a surface superlattice are populated via the resonant charge transfer (RCT) between the surface and a H − ion that flies by at grazing angles. A quantum mechanical wave packet propagation approach is utilized to simulate the motion of the active electron where time-evolved wave packet densities are used to visualize the dynamics through the superlattice. The survived ion fraction in the reflected beam generally exhibits modulations as a function of the vicinal terrace size and shows peaks at those energies that access the image state subband dispersions. However, differences in magnitudes of the ion-survival as a function of the particular substrate selection as well as the ion-surface interaction time based on the choice of two ion-trajectories are examined. A square well model producing standing waves between the steps on the surface explains well the energies of the maxima in the ion survival probability for all the metals considered, indicating that the primary process of confinement induced subband formation is rather robust. The work may motivate measurements and applications of shallow-angle ion-scattering spectroscopy to access electronic substructures in periodically nanostructured surfaces.