Towards quantitative understanding of formation and stability of Ge hut islands on Si(001)

We analyze Ge hut island formation on Si(001), using first-principles calculations of energies, stresses, and their strain dependence of Ge/Si(105) and Ge/Si(001) surfaces combined with continuum modeling. We give a quantitative assessment on strain stabilization of Ge(105) facets, estimate the critical size for hut nucleation or formation, and evaluate the magnitude of surface stress discontinuity at the island's edge and its effect on island stability.     

Mechanism and kinetics of early growth stages of a GaN film

The growth of GaN islands on the substrate surface covered with an AlN buffer layer is theoretically investigated at the stages of nucleation and Ostwald ripening in the temperature range 480–1000°C. The following inferences are made from analyzing the results obtained. (1) At temperatures T>650°C, the growth of islands is controlled by the chemical reaction of formation of GaN molecules around the periphery of the island surface. Islands nucleated at these temperatures are characterized by a large spread in their sizes. (2) At temperatures T<600°C, the island growth is governed by the surface diffusion of nitrogen atoms. Islands nucleated at these temperatures are virtually identical in size. (3) In the temperature range 600–650°C, the mechanism of island growth gradually changes over from the mechanism associated with the surface diffusion of nitrogen atoms with a large mean free path to the mechanism determined by the diffusion of gallium atoms with a smaller mean free path. The supersaturation, flux, and size distribution functions of GaN nuclei are calculated at different substrate temperatures. The phase diagrams describing the evolution in the phase composition of GaN islands with variations in temperature are constructed.     

Growth of Cu Films on Si(111)-7×7 Surfaces at Low Temperature: A Scanning Tunnelling Microscopy Study

Morphologies of Cu(111) films on Si(111)-7×7 surfaces prepared at lowtemperature are investigated by scanning tunnelling microscopy (STM) andreflection high-energy electron diffraction (RHEED). At the initial growth stage, Cu films are flat due to the formation of silicide at the interface that decreases the mismatch between Cu films and the Si substrate. Different from the usual multilayer growth of Cu/Cu(111), on the silicide layer a layer-by-layer growth is observed. The two dimensional (2D) growth is explained by the enhanced high island density at low deposition temperature. Increasing deposition rateproduces films with different morphologies, which is the result of Ostwald ripening.     

Shape, facet evolution and photoluminescence of Ge islands capped with Si at different temperatures

We investigate the embedding of Ge islands in a Si matrix by means of atomic force microscopy and photoluminescence (PL) spectroscopy. The Ge islands were grown between 360°C and 840°C and subsequently capped with Si at different temperatures. For the highest Ge growth temperature (840°C), we show that the surface flattens at high Si capping temperatures while new facets can be identified at the island base for intermediate capping temperatures (650–450°C). At low capping temperatures (300–350°C), the island morphology is preserved. In contrast to the observed island shape changes, the decreasing Si capping temperature causes only a small redshift of the island related PL signal for islands grown on high temperatures. This redshift increases for Ge islands grown at lower temperatures due to an increased Ge content in the islands. By applying low-temperature capping (300°C) on the different island types, we show that the emission wavelength can be extended up to 2.06 μm for hut clusters grown at 400°C. Further decreasing of the island growth temperature to 360°C leads to a PL blueshift, which is explained by charge carrier confinement in Ge quantum dots.     

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.     

高速率沉积磁控溅射技术制备Ge点的退火生长研究

采用磁控溅射技术在Si衬底上以350?C沉积14 nm的非晶Ge薄膜,通过退火改变系统生长热能,实现了低维Ge/Si点的生长.利用原子力显微镜(AFM)和拉曼(Raman)光谱所获得的形貌和声子振动信息,对Ge点的形成机理和演变规律进行了研究.实验结果表明:在675?C退火30 min后,非晶Ge薄膜转变为密度高达8.5×109cm-2的Ge点.通过Ostwald熟化理论、表面扩散模型和对激活能的计算,很好地解释了退火过程中,Ge原子在Si表面迁移、最终形成纳米点的行为.研究结果表明用高速沉积磁控溅射配合热退火制备Ge/Si纳米点的方法,可为自组织量子点生长实验提供一定的理论支撑.     

Ge nanocrystals in magnetron sputtered SiO2

Structural and optical properties of Ge nanocrystals in SiO₂ films created by magnetron sputtering and heat treatment have been investigated. The formation of nanocrystals is found to be influenced by the temperature of heat treatment and the Ge concentration in the films. After heat treatment at 1000 °C nanocrystals are present throughout the film, with the exception of a region close to the surface that does not contain nanocrystals. This effect is assigned to oxidation of Ge in this part of the film. The size distribution of the nanocrystals is analyzed by transmission electron microscopy for a range of deposition and heat-treatment parameters. By analyzing the transmission electron microscopy images, it is possible to estimate the fraction of nanoclusters that are crystalline for a given set of growth parameters. This analysis shows that all the nanoclusters are created in the crystalline state. Raman spectroscopy is employed to probe the Ge–Ge bonds. In combination with transmission electron microscopy, this information can be used to distinguish between growth modes such as nucleation or Ostwald ripening. The photoluminescence spectra exhibit a strong broad line at 625 nm, the presence of which is demonstrated to correlate to the presence of Ge nanocrystals. PACS 61.46.+w; 78.55.-m; 78.67.-n     

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.     

Novel SiGe island coarsening kinetics: ostwald ripening and elastic interactions

Real-time light scattering measurements of coherent island coarsening during SiGe/Si heteroepitaxy reveal unusual kinetics. In particular, the mean island volume increases superlinearly with time, while the areal density of islands decreases at a faster-than-linear rate. Neither observation is consistent with standard considerations of Ostwald ripening. Modification of the standard theory to incorporate the effect of elastic interactions in the growing island array reproduces the observed behavior.     

Effect of strain on the appearance of subcritical nuclei of ge nanohuts on Si(001)

Real-time scanning tunneling microscopy observations of nucleation and heteroepitaxial growth of Ge nanocrystals (from germane) on Si(001) indicate that in the absence of Si-Ge intermixing the formation of full hut cluster islands is preceded by the nucleation of "subcritical" nuclei consisting of two adjacent truncated tetrahedral pyramids, which, upon unification, form a tiny square-based pyramidal "critical nucleus" It is suggested that such a precursor aids in surpassing the nucleation barrier and that the recently reported gradual faceting of prepyramids is characteristic of only Ge(Si) alloys.     

Simulation study on nanocluster growth deposited on a substrate

We present a model equation that describes nucleation and growth of hemispherical nanoclusters or islands deposited on a substrate for the small surface coverage case. The model is formulated in terms of a set of rate equations for the island sizes, combined with the time-dependent behavior of supersaturation and island nucleation rate. As an example to demonstrate the usefulness of the model, we study effects of the deposition rate of adatoms on the nanocluster growth. Large-scale computer simulation results show that the broadness of island size distribution is a decreasing function of the deposition rate for small rates, and bimodal distributions are obtained for large rates.     

Metastability of ultradense arrays of quantum dots

We present a linear stability analysis of ultradense arrays of coherently strained islands against Ostwald ripening. Surprisingly, short-range elastic interactions are found to overcome the destabilizing contribution of surface energy, leading to a metastable array of quantum dots. Simulations of Ostwald ripening kinetics directly verify the existence of this metastable regime and confirm the nature of the most unstable mode for subcritical island coverage.     

Surface processes in electrocrystallization

A short review of the theories of crystal growth of perfect and imperfect planeS is given. Experimental evidence of two-dimensional nucleation mechanism of growth of perfect crystal planes is provided for the first time and some crystallographic parameters of this process are determined. A quantitative verification of Frank's theory is given by investigating the growth phenomena on nearly perfect planes. The effect of screw dislocations on crystal growth is studied and some phenomena concerning the influence of surface active impurities on crystal growth and dissolution are reported.

The theory of heterogeneous phase formation is briefly discussed and an experimental verification of the basic relation following this theory is given. The effect of the crystallographic structure upon nucleation is closely studied. A method permitting the determination of the activity distribution curve of nucleation sites on the basis of their critical supersaturation is also given.     

Scaling of submonolayer island growth with reversible adatom exchange in surfactant-mediated epitaxy

Surfactant-mediated epitaxial growth is studied with a realistic model, which includes three main kinetic processes: diffusion of adatoms on the surfactant terrace, exchange of adatoms with their underneath surfactant atoms, and reexchange in which an exchanged adatom resurfaces to the top of the surfactant layer. The scaling behavior of nucleus density and island size distributions in the initial stage of growth is investigated by using kinetic Monte Carlo simulations. The results show that the temperature dependence of nucleus density and island size distributions governed by the reexchanging-controlled nucleation at high temperatures exhibits similar scaling behavior to that obtained by the standard diffusion-mediated nucleation at low temperatures. However, at intermediate temperatures, the exchanging-controlled nucleation leads to an increase of nucleus density with temperature, while the island size distribution scales to a monotonically decreasing function, showing nonstandard scaling behavior.     

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.     

Mechanisms and kinetics of the initial stages of growth of films grown by chemical vapor deposition

The initial stages of growth of films and coatings by chemical vapor deposition are investigated. A system of equations is derived which describes the evolution of an island film at the stage of Ostwald ripening under conditions characteristic of vapor deposition. Solving this system of equations yields the dependence of all of the main characteristics of island films (the size distribution function of the islands, the dependence of the mean radius and density of the islands) as functions of time and the spatial coordinate. Suggestions are given for the preparation of films with prescribed properties. Zh. Tekh. Fiz. 68, 111–117 (July 1998)     

Ge quantum dots on a large band gap semiconductor: the first growth stages on 4H–SiC(0 0 0 1)

The Ge growth on SiC(0 0 0 1) follows a Stranski–Krastanov mode for Si-rich (3×3) and reconstructed surfaces. For Ge deposit in particular temperature conditions, a new (4×4) superstructure takes place and the reflection high energy electron diffraction (RHEED) specular spot intensity presents one oscillation proving a wetting layer formation. An island nucleation is then ascertained by the oscillation vanishing and by the appearance of a k-modulated RHEED pattern. On the other hand, on a C-rich surface, a direct Ge island nucleation is observed from the first growth stage. Indeed, for 1 ML Ge, the RHEED diagram consists in spots and rings, and the atomic force microscopy analysis indicates a high density (8×10¹⁰ cm⁻²) of small islands (30 nm, h3 nm). The RHEED spot analysis shows a preferential epitaxial relationship with the substrate Ge(1 1 1)//SiC(0 0 0 1). The Ge–C bonding being energetically unfavourable, Ge tends to form islands immediately rather than wetting the graphite-terminated surface. The Ge growth mode on C-rich surface is thus of Volmer–Weber type.     

Ostwald ripening of beta-carotene nanoparticles

Ostwald ripening, the interfacial-energy-driven dissolution and reprecipitation of solutes, becomes an increasingly significant problem for nanoparticle formulations. We present the first quantitative study of Ostwald ripening for nanoparticle dispersions. The Lifshitz-Slyozov-Wagner (LSW) theory of particle growth driven by diffusion is applied to study beta-carotene nanoparticles with sizes of O(100 nm) formed by our block-copolymer protected Flash Nanoprecipitation process. A numerical implementation of the LSW theory that accounts for the original particle size distribution is presented. The predicted particle sizes from the numerical simulation are compared with the experimental results measured by dynamical light scattering. The results show quantitative agreement with no adjustable parameters. The addition of antisolvent results in the reduction of the ripening rate by dramatically decreasing bulk solubility.     

A kinetic Monte Carlo investigation of island nucleation and growth in thin-film epitaxy in the presence of substrate-mediated interactions

Island nucleation and growth during thin-film epitaxy is typically described using mean-field rate equations, which can be solved to predict the density of stable islands as a function of the deposition rate and the diffusivity of an isolated adatom. Recent theoretical and experimental studies indicate that medium- and long-range interactions between adatoms may change the simple picture that nucleation theory provides, because the presence of these interactions invalidates some of its assumptions. In this work, we investigate the ramifications of medium-range, substrate-mediated interactions for aspects of island nucleation and growth. The interactions are quantified for Ag on a strained Ag (111) substrate using density-functional-theory calculations. We discuss our incorporation of these interactions into a kinetic Monte Carlo model to study thin-film epitaxy. The simulated thin-film growth is compared to predictions by standard nucleation theory. We discuss features of island nucleation and growth that are actuated by the presence of medium-range interactions. Received: 30 April 2001 / Accepted: 23 July 2001 / Published online: 3 April 2002     

EFFECTS OF ISLAND-EDGE EXCHANGE BARRIER ON 2D PATTERN FORMATION IN SURFACTANT-MEDIATED EPITAXY

The nucleation and growth of two-dimensional islands in a surfactant-mediated epitaxy system have been studied by computer simulation. To improve the recent results published in the literature, we use a configuration-dependent energy barrier for the exchange process at the island edge in our model. The simulations produce fractal islands at high temperatures or low deposition fluxes, and a transition to regular compact islands occurs at lower temperatures or higher fluxes, in good agreement with the recent experimental results. The barrier for the island-edge exchange has quite a strong effect on the island density as a function of temperature and flux. A small change of the island-edge exchange barrier induces a large variation of the island density in the low-temperature or high-flux region. The flux-dependent island density shows a clear scaling-law behaviour in the intermediate-flux region. The scaling exponent increases evidently as the island-edge exchange barrier increases.