Effects of electronic confinement and substrate on the low-temperature growth of Pb islands on Si(1 0 0)-2 × 1 surfaces

The growth of Pb films on the Si(1 0 0)-2 × 1 surface has been investigated at low temperature using scanning tunneling microscopy. Although the orientation of the substrate is (1 0 0), flat-top Pb islands with (1 1 1) surface can be observed. The island thickness is confined within four to nine atomic layers at low coverage. Among these islands, those with a thickness of six layers are most abundant. Quantum-well states in Pb(1 1 1) islands of different thickness are acquired by scanning tunneling spectroscopy. They are found to be identical to those taken on the Pb(1 1 1) islands grown on the Si(1 1 1)7 × 7 surface. Besides Pb(1 1 1) islands, two additional types of Pb islands are formed: rectangular flat-top Pb(1 0 0) islands and rectangular three-dimensional (3D) Pb islands, and both their orientations rotate by 90° from a terrace to the adjacent one. This phenomenon implies that the structures of Pb(1 0 0) and 3D islands are influenced by the Si(1 0 0)-2 × 1 substrate.     

Cooperative growth of nano-islands on Si(1 0 0) surface

By setting up two low temperature regions on a terrace of a vicinal Si(1 0 0)-2 × 1 surface, we have studied growth of nano-islands in the two regions using a kinetic Monte Carlo simulation. At first two islands are formed and grow independently without any supply of atoms from the outside. As the growth proceeds further, two islands are connected with each other by forming a bridge region. After the connection, the growth changes dramatically showing a competitive mode in one stage and a cooperative mode in the other. Two islands grow cooperatively in a sense that a larger island ceases to grow and waits until the size of the other smaller island becomes similar to that of the larger one. When two islands become similar in size, one of the islands grows faster than the other competitively, by accumulating atoms from then smaller one. The origin of the growth mode is analyzed.     

Nucleation, coarsening and kinetic scaling of two-dimensional islands on GaSb(0 0 1)

Using a combination of molecular beam epitaxy and in situ surface X-ray diffraction, we investigate the nucleation and coarsening of monolayer high islands on GaSb(0 0 1) during deposition in real time. We find an activation energy for island nucleation of 1.55 ± 0.16 eV, indicating a stable nucleus size larger than two atoms. For intermediate temperatures where GaSb homoepitaxy is stable, the lateral coarsening of the islands after deposition is described by Ostwald ripening. The average island sizes during coarsening are isotropic, although with different size distributions in different directions. The size distributions do not change during coarsening, implying kinetic scaling.     

Fabrication of uniform Au silicide islands on the Si(1 1 1)-(7 × 7) substrate

The Au silicide islands have been fabricated by additional deposition of Au on the prepared surface at 270 °C where the Si islands of magic sizes were formed on the Si(1 1 1)-(7 × 7) dimer-adatom-stacking fault substrate. The surface structure on the Au silicide islands shows the Au/Si(1 1 1)-√3 × √3 reconstructed structure although the substrate remains 7 × 7 DAS structure. The size of the Au silicide islands depends on the size distribution of the preformed Si islands, because the initial size and shape of the Si islands play important roles in the formation of the Au silicide island. We have achieved the fabrication of the Au silicide islands of about the same size (∼5 nm) and the same shape by controlling the initial Si growth and the additional Au growth conditions.     

Strongly-driven coarsening of height-selected Pb islands on Si(1 1 1)

A theoretical model is proposed to describe the rapid coarsening observed for Pb islands on a Si(1 1 1) surface where classical kinetics breaks down. In this system, quantum size effects produce mesa-like Pb islands with chemical potentials depending strongly on their heights, in addition to the usual dependence on the step curvature. Furthermore, a dense wetting layer enables fast mass transport between islands. Incorporating these features, our theoretical model predicts evolution of the island height distribution in good agreement with experiments.     

Au island growth on a Si(1 1 1) vicinal surface

Au island nucleation and growth on a Si(1 1 1) 7 × 7 vicinal surface was studied by means of scanning tunneling microscopy. The surface was prepared to have a regular array of step bunches. Growth temperature and Au coverage were varied in the 255-430 °C substrate temperature range and from 1 to 7 monolayers, respectively. Two kinds of islands are observed on the surface: Au-Si reconstructed islands on the terraces and three-dimensional (3D) islands along the step bunches. Focusing on the latter, the dependence of island density, size and position on substrate temperature and on Au coverage is investigated. At 340 °C and above, hemispherical 3D islands nucleate systematically on the step edges.     

Nanowedge island formation on Mo(1 1 0)

The deposition of ultrathin Fe films on the Mo(1 1 0) surface at elevated temperatures results in the formation of distinctive nanowedge islands. The model of island formation presented in this work is based on both experiment and DFT calculations of Fe adatom hopping barriers. Also, a number of classical molecular dynamics simulations were carried out to illustrate fragments of the model. The islands are formed during a transition from a nanostripe morphology at around 2 ML coverage through a Bales-Zangwill type instability. Islands nucleate when the meandering step fronts are sufficiently roughened to produce a substantial overlap between adjacent steps. The islands propagate along the substrate [0 0 1] direction due to anisotropic diffusion/capture processes along the island edges. It was found that the substrate steps limit adatom diffusion and provide heterogeneous nucleation sites, resulting in a higher density of islands on a vicinal surface. As the islands can be several layers thick at their thinnest end, we propose that adatoms entering the islands undertake a so-called “vertical climb” along the sides of the island. This is facilitated by the presence of mismatch-induced dislocations that thread to the sides of the islands and produce local maxima of compressive strain. Dislocation lines also trigger initial nucleation on the surface with 2-3 ML Fe coverage. The sides of the nanowedge islands typically form along low-index crystallographic directions but can also form along dislocation lines or the substrate miscut direction.     

Mixed layer formation of copper overlayers on Ni(1 1 0) surface

Copper overlayer formation on the Ni(1 1 0) surface was studied by scanning tunneling microscopy (STM) in an ultrahigh vacuum. Atom-resolved STM images showed that initially deposited Cu is replaced with surface Ni atoms forming atom-size depressions on the Ni(1 1 0) terraces and a Ni-rich quasi-one-dimensional island along the direction. Further Cu deposition yields a mosaic structure on the islands, indicating Cu/Ni mixed layer formation. From the quantitative measurement of the Cu/Ni ratio on the substrate and the islands, impinging Cu will be replaced with surface Ni whereas expelled Ni and directly impinging Cu to the island form the mixed island. The number of Cu atoms in the islands, however, more than the directly impinging Cu, indicate significant Cu/Ni replacement at the periphery of the island.     

Temperature dependent low energy electron microscopy study of Ge growth on Si(1 1 3)

We investigated the initial Ge nucleation and Ge island growth on a Si(1 1 3) surface using low energy electron microscopy and low energy electron diffraction. The sample temperature was varied systematically between 380 °C and 590 °C. In this range, a strong temperature dependence of the island shape is observed. With increasing temperature the Ge islands are elongated in the direction. Simultaneously, the average island size increases while their density decreases. From the Arrhenius-like behaviour of the island density, a Ge adatom diffusion barrier height of about 0.53 eV is deduced.     

Growth and thermal evolution of submonolayer Pt films on Ru(0 0 0 1) studied by STM

The growth of submonolayer Pt on Ru(0 0 0 1) has been studied with scanning tunneling microscopy. We focus on the island evolution depending on Pt coverage θ_Pt, growth temperature T_G and post-growth annealing temperature T_A. Dendritic trigonal Pt islands with atomically rough borders are observed at room temperature and moderate deposition rates of about 5 × 10⁻⁴ ML/s. Two types of orientation, rotated by 180° and strongly influenced by minute amounts of oxygen are observed which is ascribed to nucleation starting at either hcp or fcc hollow sites. The preference for fcc sites changes to hcp in the presence of about one percent of oxygen. At lower growth temperatures Pt islands show a more fractal shape. Generally, atomically rough island borders smooth down at elevated growth temperatures higher than 300 K, or equivalent annealing temperatures. Dendritic Pt islands, for example, transform into compact, almost hexagonal islands, indicating similar step energies of A- and B-type of steps. Depending on the Pt coverage the thermal evolution differs somewhat: While regular islands on Ru(0 0 0 1) are formed at low coverages, vacancy islands are observed close to completion of the Pt layer.     

Sb incorporation at GaAs(0 0 1)-(2 × 4) surfaces

We examine the Sb incorporation and resulting surface reconstructions of Sb and GaSb deposited on GaAs(0 0 1). These films exhibit a mixed surface reconstruction of α2(2 × 4) and α(4 × 3). Initially, Sb reacts with Ga on the surface to form 2D islands of GaSb with an α(4 × 3) surface reconstruction. The 2D islands grow to a critical size of 30 nm², beyond which the atomic surface structure of the 2D island transforms to a α2(2 × 4) reconstruction in order to reduce the strain induced surface energy. This transformation is limited by the availability of Ga, which is necessary in higher quantities for the α2(2 × 4) reconstruction than for the α(4 × 3). The transformation results in a mixed α2(2 × 4)-α(4 × 3) surface where the surface reconstruction is coupled to the surface morphology, which may in the future provide a pathway for self-assembly of structures.     

Self-assembled InAs island formation on GaAs (1 1 0) by metalorganic vapor phase epitaxy

Formation of self-assembled InAs 3D islands on GaAs (1 1 0) substrate by metal organic vapor phase epitaxy has been investigated. Relatively uniform InAs islands with an average areal density of 10⁹ cm⁻²are formed at 400 ° C using a thin InGaAs strain reducing (SR) layer. No island formation is observed without the SR layer. Island growth on GaAs (1 1 0) is found to require a significantly lower growth temperature compared to the more conventional growth on GaAs (1 0 0) substrates. In addition, the island height is observed to depend only weakly on the growth temperature and to be almost independent of the V/III ratio and growth rate. Low-temperature photoluminescence at 1.22 eV is obtained from the overgrown islands.     

Growth mechanisms for wire-like epitaxial gold silicide islands on Si(1 1 0) surfaces

Epitaxial islands grown on various substrates are usually strained because of differences in lattice constants of the materials of the island and the substrate. Shape transition in the growth of strained islands has been proposed as a mechanism for strain relief and a way to form self-organized quantum wires. Shape transition usually leads to an elongated island growth. However, an elongated island growth may also be due to an anisotropic diffusion of material, the anisotropy being imposed by the symmetry of the substrate surface. In the present example, growth of gold silicide wire-like nanostructures on a Si(1 1 0) surface has been investigated by photoemission electron microscopy (PEEM). Growth of elongated unidirectional gold silicide islands, with an aspect ratio as large as 12:1, has been observed by PEEM following gold deposition on the Si substrate and subsequent annealing at the Au-Si eutectic temperature. Distribution of the width and the length of the gold silicide islands as a function of island area shows a feature similar to that for the shape transition. However, detailed investigations reveal that the elongated growth of gold silicide islands is rather mainly due to anisotropic diffusion of gold due to the twofold symmetry of the (1 1 0) surface of the Si substrate.     

Si nucleation on Si(1 1 1)-7 × 7: From cluster pairs to 2D islands

Nucleation of 2D islands in Si/Si(1 1 1)-7 × 7 molecular beam epitaxy is studied using scanning tunneling microscopy (STM). A detailed analysis of the population of small amorphous clusters coexisting on the surface with epitaxial 2D islands has been performed. It is shown that small clusters tend to form pairs. The pairs serve as precursors for 2D islands as confirmed by direct STM observations of the smallest 2D islands covering two adjacent half-unit cells of the 7 × 7 reconstruction. It is proved with scaling arguments that the critical nucleus for 2D island formation consists not only of the pair itself, but also includes additional adatoms not belonging to the stable clusters.     

Surface evolution and three-dimensional shape changes of SiGe/Si(0 0 1) islands during capping at various temperatures

The authors use a combination of atomic force microscopy and selective wet chemical etching of the Si capping layer to investigate both the surface and the three-dimensional SiGe/Si(0 0 1) island shape changes during capping at various temperatures. Different evolution paths are identified depending on the capping temperature. During the early stages of Si overgrowth at 450 °C, a moderate SiGe alloying occurs near the island apex. In the later stages, island burying begins through lateral growth of pyramid-like structures, which consist of pure Si. A comparison with previous overgrowth studies allows us to clarify the role of the initial island size in determining the surface evolution above buried islands. Island dissolution with material transfer to the wetting layer dominates upon capping at 580 °C. Finally, when the temperature during growth and capping is identical, the islands become flatter and wider indicating that the system starts to evolve towards an energetically preferred SiGe quantum well.     

Structural transition in cyclooctatetraene adsorbed on Ru(0 0 1) probed by thermal desorption and two-photon photoemission spectroscopy

The adsorption of 1,3,5,7-cyclooctatetraene (COT) on Ru(0 0 1) is studied by temperature-programmed desorption (TPD), work function measurements, as well as time- and angle-resolved two-photon photoemission (2PPE) spectroscopy. The TPD data show that COT films grow at 115 K in a metastable phase when the coverage is increased from the chemisorbed monolayer to the bulk-like molecular multilayer structure. The metastable states desorb at a temperature which is ≈9 K lower than the desorption temperature of the stable multilayer. At 165 ± 2 K, they undergo an irreversible and thermally activated transformation into the stable multilayer phase. This transition is accompanied by a pronounced increase in the total 2PPE yield by more than one order of magnitude as well as the appearance of image potential states. The image states have binding energies of −0.70 eV and −0.24 eV for the n = 1 and n = 2 states, respectively, and a lifetime of 20 ± 5 fs for both states. Their appearance is interpreted as an indication of island formation in the stable multilayer regime. 2PPE spectroscopy of the image potential states provides a sensitive probe of structural transitions in the adsorbate layers.     

Morphology changes due to AC induced electromigration in Gd islands on W(1 1 0)

Gd islands were grown on W(1 1 0) surface by evaporating Gd on the substrate at room temperature and subsequent annealing. STM images reveal in many cases islands which have a deep hole inside them. The appearance of the hole is associated with the application of an AC field. No such holes appear when the sample is heated by a DC current. We show that this can be explained by the combined affect of the AC field and the barrier to diffusion introduced by steps that can create a nucleus for further growth of an island which includes a hole in the middle. This may be generalized to a technique of tailoring the size, shape and distances of islands by, for example, two orthogonal AC fields with a phase delay of 90° between them.     

Kinetic Monte Carlo simulations of Pd deposition and island growth on MgO(1 0 0)

The deposition and ripening of Pd atoms on the MgO(1 0 0) surface are modeled using kinetic Monte Carlo simulations. The density of Pd islands is obtained by simulating the deposition of 0.1 ML in 3 min. Two sets of kinetic parameters are tested and compared with experiment over a 200-800 K temperature range. One model is based upon parameters obtained by fitting rate equations to experimental data and assuming the Pd monomer is the only diffusing species. The other is based upon transition rates obtained from density functional theory calculations which show that small Pd clusters are also mobile. In both models, oxygen vacancy defects on the MgO surface provide strong traps for Pd monomers and serve as nucleation sites for islands. Kinetic Monte Carlo simulations show that both models reproduce the experimentally observed island density versus temperature, despite large differences in the energetics and different diffusion mechanisms. The low temperature Pd island formation at defects is attributed to fast monomer diffusion to defects in the rate-equation-based model, whereas in the DFT-based model, small clusters form already on terraces and diffuse to defects. In the DFT-based model, the strong dimer and trimer binding energies at charged oxygen vacancy defects prevent island ripening below the experimentally observed onset temperature of 600 K.     

Interaction of Ag and O on W(1 1 0) studied by scanning tunneling microscopy

The structural changes of Ag films on W(1 1 0) upon coadsorption of oxygen have been studied by scanning tunneling microscopy. The exposure of one monolayer Ag to oxygen leads to a phase separation into an Ag bilayer and patches of O-covered W(1 1 0). The effective Ag island thickness increases linearly with oxygen exposure. For Ag submonolayer-islands the onset of the bilayer formation is delayed, the induction period increases with the available free W area. We conclude that the steps of the transport process are (1) dissociation of oxygen on W and on the Ag islands, (2) site exchange of atomic oxygen with Ag atoms predominantly at the island edges - while on W(1 1 0) the oxygen is immobile, (3) diffusion of the displaced Ag atoms to the island edges where they are incorporated into the monolayer and (4) initiation of Ag bilayer formation, once the W(1 1 0) is saturated with O. This indicates an unexpected activity of the Ag monolayer on W(1 1 0) towards oxygen dissociation. In case of a reversed deposition sequence, where submonolayer quantities of Ag are adsorbed on an oxygen-precovered W(1 1 0) surface, growth of Ag clusters is observed. The distribution of cluster size and cluster height depends critically on the spatial order within the predeposited oxygen overlayer - it is obvious that the oxygen overlayer on the W surface acts as a structured template for preferential Ag nucleation.     

STM study of successive Ge growth on “V”-stripe patterned Si (0 0 1) surfaces at different growth temperatures

The self-assembly process of Ge islands on patterned Si (0 0 1) substrates is investigated using scanning tunneling microscopy. The substrate patterns consist of one-dimensional stripes with “V”-shaped geometry and sidewalls inclined by an angle of 9° to the (0 0 1) surface. Onto these stripes, Ge is deposited in a step-wise manner at different temperatures from 520 °C to 650 °C. At low temperature, the Ge first grows nearly conformally over the patterned surface but at about 3 monolayers a strong surface roughening due to reconstruction of the surface ridges as well as side wall ripple formation occurs. At 600 °C, a similar roughening takes place, but Ge accumulates within the grooves such that at a critical thickness of 4.5 monolayers, 3D islands are formed at the bottom of the grooves. This accumulation process is enhanced at 650 °C growth, so that the island formation starts about 1 monolayers earlier. At 600 and 650 °C, all islands are all aligned at the bottom of the stripes, whereas at 550 °C Ge island form preferentially on top of ridges. The experimental observations are explained by the strong temperature dependence of Ge diffusion over the patterned surface.