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We compare step morphologies on surfaces of Al-rich metallic alloys, both quasicrystalline and crystalline. We present evidence that the large-scale step structure observed on Al-rich quasicrystals after quenching to room temperature reflects equilibrium structure at an elevated temperature. These steps are relatively rough, i.e., have high diffusivity, compared to those on crystalline surfaces. For the fivefold quasicrystal surface, step diffusivity increases as step height decreases, but this trend is not obeyed in a broader comparison between quasicrystals and crystals. On a shorter scale, the steps on Al-rich alloys tend to exhibit local facets (short linear segments), with different facet lengths, a feature which could develop during quenching to room temperature. Facets are shortest and most difficult to identify for the fivefold quasicrystal surface.

Epitaxial thin film growth by vapor deposition or molecular beam epitaxy under ultra‐high vacuum conditions generally occurs in two stages: (i) nucleation and growth of well‐separated islands on the substrate; (ii) subsequent formation of a thicker continuous film with possible kinetic roughening. For homoepitaxial growth, two‐dimensional (2D) monolayer islands are formed during submonolayer deposition. Typically, the presence of a step‐edge barrier inhibits downward transport and leads to the formation of mounds (multilayer stacks of 2D islands) during multilayer growth. For heteroepitaxial growth, islands formed in the initial stages of deposition sometimes have a 2D monolayer structure. However, they may instead exhibit bilayer or 3D multilayer structure due to, e.g., a high film surface energy, strain, or quantum size effects. Various growth modes are possible for thicker films. Atomistic modeling provides the most detailed picture of film growth. For coherent (defect‐free) epitaxial films, lattice‐gas modeling analyzed by kinetic Monte Carlo simulation (KMC) is particularly successful in describing film growth on the appropriate time and length scales. For large islands or complex systems, another effective and instructive approach is laterally coarse‐grained step‐dynamics modeling which tracks only the evolution of step edges in each layer. However, fully coarse‐grained 3D continuum modeling for the evolution of a film height function does not yet have predictive capability. Examples are provided for: Ag homoepitaxy on (100), (111) and (110) surfaces; Ag heteroepitaxy on lattice‐matched substrates including NiAl(110), NiAl(100), and Fe(100); and Ag heteroepitaxy on 5‐fold icosohedral Al‐Pd‐Mn and 2‐fold decagonal Al‐Cu‐Co quasicrystalline surfaces.

We analyze the formation of two-dimensional Ag islands following deposition of about 0.1 ML of Ag on Ag(100) over a temperature regime ranging from classical nucleation and growth behavior to almost immobile adatoms, from 300 to 125 K. Particular emphasis is placed on the post-deposition dynamics at the lower end of the temperature range, where the saturation island density is not reached at the end of the deposition, and nucleation and aggregation processes continue with adatoms from the remaining adatom gas. Our analysis combines VT scanning tunneling microscopy experiments with kinetic Monte Carlo simulation of appropriate atomistic models. The only adjustable parameters in the model are the terrace diffusion barrier and prefactor, which can be determined from island density behavior near room temperature. Other processes such as rapid edge diffusion, and ``easy'' nucleation and aggregation of diagonally adjacent adatoms, are treated as instantaneous. The model excellently reproduces all aspects of behavior at low temperatures, demonstrating that nucleation and growth processes can be described in one consistent scheme, down to the regime of almost immobile adatoms.

Scanning-tunneling microscopy studies combined with atomistic modeling for Ag/Ag(100) homoepitaxy reveal complex growth behavior at 300 K: initial smooth growth up to \ensuremath{\sim}25 ML, where three-dimensional (3D) mounds develop from 2D islands; then an extended regime of mound steepening for \ensuremath{\sim}1000 ML producing unexpected rough growth; and finally an asymptotic regime with cooperative mound ordering and coalescence dynamics quite distinct from that in systems with up-down symmetry. The steepening regime is compressed upon lowering temperature, so while initial growth is rougher, asymptotic growth is actually smoother.

A realistic atomistic lattice-gas model is developed which describes the key features of film morphologies observed for multilayer homoepitaxial growth on Ag(100) in the temperature range 175-300 K corresponding to “mound formation”. The model accounts for irreversible formation of islands in each layer mediated by terrace diffusion, growth coalescence of islands within each layer, a non-uniform step edge barrier inhibiting downward transport, and restricted rounding of kinks by adatoms at island edges (at lower temperatures).

We develop and analyze 1+1- and 2+1-dimensional (d) models for multilayer homoepitaxial growth of metal films at low temperatures (T), where intralayer terrace diffusion is inoperative. This work is motivated by recent variable-temperature scanning tunneling microscopy studies of Ag/Ag(100) homoepitaxy down to 50 K. Adsorption sites are bridge sites in our 1+1d models, and fourfold hollow sites in our 2+1d models for fcc(100) or bcc(100) surfaces. For growth at 0 K, we introduce a 'restricted downward funneling' model, wherein deposited atoms can be trapped on the sides of steep nanoprotrusions rather than always funneling down to lower adsorption sites. This leads to the formation of overhangs and internal defects (or voids), and associated 'rough' growth. Upon increasing T, we propose that a series of interlayer diffusion processes become operative, with activation barriers below that for terrace diffusion. This leads to 'smooth' growth of the film for higher T (but still within the regime where terrace diffusion is absent), similar to that observed in models incorporating 'complete downward funneling.'

Scanning tunneling microscopy is used to analyze the nanoscale morphology of 25 ML films of Ag deposited on Ag(100) at temperatures (T) between 55 and 300 K. A transition from self-affine growth to ''mound formation'' occurs as T increases above about 140 K. The roughness decreases with increasing T up until 140 K in the self-affine growth regime, and then increases until about 210 K before decreasing again in the mounding regime. We analyze mounding behavior via a lattice-gas model incorporating: downward funneling of depositing atoms from step edges to lower fourfold hollow adsorption sites; terrace diffusion of adatoms with a barrier of 0.40 eV leading to irreversible island formation in each layer; efficient transport of adatoms along island edges to kink sites; and downward thermal transport of adatoms inhibited by a step-edge barrier of 0.06--0.07 eV along close-packed step edges (but with no barrier along kinked or open steps). This model reasonably recovers the T-dependence of not just the roughness, but also of the mound slopes and lateral dimensions above 190 K. To accurately describe lateral dimensions, an appropriate treatment of the intralayer merging of growing islands is shown to be critical. To describe behavior below 190 K, onemore » must account for inhibited rounding of kinks by adatoms at island edges, as this controls island shapes, and thus the extent of open steps and of easy downward transport. Elsewhere, we describe the low-T regime of self-affine growth (with no terrace diffusion) accounting for a breakdown of the simple downward funneling picture.« less

Ag(100) homoepitaxy constitutes one of the simplest systems in which to study thin-film growth. Yet we find that the roughness variation with temperature is extraordinarily complex. Specifically, as the deposition temperature is reduced from 300 to 50 K, the roughness of 25 monolayer films first increases, then decreases, then increases again. A transition from mound formation to self-affine (semifractal) growth occurs at {approx}135 K. The underlying mechanisms are postulated. An atomistic model incorporating these mechanisms reproduces the experimental data quantitatively. (c) 2000 The American Physical Society.

We model the growth of Ag films deposited on Ag(100) below 140K. Our recent Variable-Temperature Scanning Tunneling Microscopy (VTSTM) studies reveal “smooth growth” from 120-140K, consistent with earlier diffraction studies. However, we also find rougher growth for lower temperatures. This unexpected behavior is modeled by describing the deposition dynamics using a “restricted downward funneling” model, wherein deposited atoms get caught on the sides of steep nanoprotrusions (which are prevalent below 120K), rather than always funneling down to lower four-fold hollow adsorption sites. At OK, where no thermal diffusion processes are operative, this leads to the formation of overhangs and internal defects (or voids). Above 40K, low barrier interlayer diffusion processes become operative, producing the observed smooth growth by 120K. We also discuss how the apparent film morphology mapped out by the STM tip “smears” features of the actual film morphology (which are small at low temperature), and also can lead to underestimation of the roughness.