The current paper presents a state-of-the-art review in the field of interaction of atomic and molecular clusters with solids. We do not attempt to overview the entire broad field, but rather concentrate on the impact phenomena: how the physics of the cluster-surface interaction depends on the kinetic energy and what effects are induced under different energetic regimes. The review starts with an introduction to the field and a short history of cluster beam development. Then fundamental physical aspects of cluster formation and the most common methods for the production of cluster beams are overviewed. For cluster-surface interactions, one of the important scenarios is the low-energy regime where the kinetic energy per atom of the accelerated cluster stays well below the binding (cohesive) energy of the cluster constituents. This case is often called This is the peer-reviewed author's version of a work that was accepted for publication in Surface Science Reports. Changes resulting from the publishing process, such as editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version
The diversity of nanoparticle shapes generated by condensation from gaseous matter reflects the fundamental competition between thermodynamic equilibration and the persistence of metastable configurations during growth. In the kinetically limited regime, intermediate geometries that are favoured only in early formation stages can be imprinted in the finally observed ensemble of differently structured specimens. Here we demonstrate that single-shot wide-angle scattering of femtosecond soft X-ray free-electron laser pulses allows three-dimensional characterization of the resulting metastable nanoparticle structures. For individual free silver particles, which can be considered frozen in space for the duration of photon exposure, both shape and orientation are uncovered from measured scattering images. We identify regular shapes, including species with fivefold symmetry and surprisingly large aspect ratio up to particle radii of the order of 100 nm. Our approach includes scattering effects beyond Born’s approximation and is remarkably efficient—opening up new routes in ultrafast nanophysics and free-electron laser science.
Gold atom chains on vicinal Si(111) surfaces exhibit an unusual doublet of half-filled bands, whose origin has remained uncertain. The splitting is identified by angle-resolved photoemission as a spin splitting induced by the spin-orbit interaction (Rashba effect), in agreement with a theoretical prediction by Sánchez-Portal, Riikonen, and Martin. This interaction leads to a characteristic pattern of avoided band crossings at a superlattice zone boundary. Two out of four crossings are avoided, with a minigap E_{G}=85 meV and a k offset of 0.05 A;{-1}.
We propose a new structural model for the Si(111)-(5×2)-Au reconstruction. The model incorporates a new experimental value of 0.6 monolayer for the coverage of gold atoms, equivalent to six gold atoms per 5×2 cell. Five main theoretical results, obtained from first-principles total-energy calculations, support the model. (1) In the presence of silicon adatoms the periodicity of the gold rows spontaneously doubles, in agreement with experiment. (2) The dependence of the surface energy on the adatom coverage indicates that a uniformly covered phase is unstable and will phase-separate into empty and covered regions, as observed experimentally. (3) Theoretical scanning tunneling microscopy images are in excellent agreement with experiment. (4) The calculated band structure is consistent with angle-resolved photoemission spectra; analysis of their correspondence allows the straightforward assignment of observed surface states to specific atoms. (5) The calculated activation barrier for diffusion of silicon adatoms along the row direction is in excellent agreement with the experimentally measured barrier.
The energetic position of the Au(111) Shockley surface state is compared before and after adsorbing different rare gas monolayers (Ar, Kr, and Xe). We used ultraviolet photoelectron spectroscopy (UPS) and scanning tunneling spectroscopy (STS) in combination to get more complete information by using the advantages of both methods. For determining the energetic position and the effective mass of the surface state in UPS an analytic mathematical method is used, which takes the finite angular resolution of the analyzer into account. We performed STS scans for the pure Au(111) surface as well as covered with a monolayer Kr and Xe. For an accurate analysis it is possible to use an extended Kronig-Penney model to take into account the influence of the 23ϫ ͱ 3 reconstruction. We found that the first monolayer of a rare gas induces shifts of around 50-150 meV increasing with the gas atomic number, whereas a second monolayer has only a small influence of about 3-18 meV. Using an image potential model it is possible to characterize these shifts qualitatively. For a semiquantitative analysis the phase accumulation model is applied. Within this model we can describe the experimental data roughly with a Coulomb potential changing in dependence of the electron affinity and the dielectric constant of the rare gas.
A reversible structural transition is observed on Si(553)-Au by scanning tunneling microscopy, triggered by electrons injected from the tip into the surface. The periodicity of atomic chains near the step edges changes from the 1×3 ground state to a 1×2 excited state with increasing tunneling current. The threshold current for this transition is reduced at lower temperatures. In conjunction with first-principles density-functional calculations it is shown that the 1×2 phase is created by temporary doping of the atom chains. Random telegraph fluctuations between two levels of the tunneling current provide direct access to the dynamics of the phase transition, revealing lifetimes in the millisecond range.
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