Transmission electron microscopic evaluation of InGaAs/InAlAs in-plane superlattices grown on slightly misoriented (110)InP substrates by molecular beam epitaxy

InGaAs/InAlAs in-plane superlattices (IPSLs) consisting of InAs/GaAs and InAs/AlAs monolayer superlattices grown on slightly misoriented (110)InP substrates by molecular beam epitaxy have been structurally evaluated by transmission electron microscopy. We used (110)InP 3° tilted toward the [00 ] direction. The ISPLs were fabricated by an alternative growth of half monolayers of AlAs and GaAs and one monolayer of InAs while maintaining regular arrays of one monolayer steps on the growth surface. In electron diffraction patterns from the ( 10) cross-section, two types of superstructure spots double-positioned in the 001 direction are observed, consistent with the existence of the IPSLs. Dark-field imaging from the superstructure spots reveal a periodic diffraction contrast with an average lateral periodicity of about 4 nm, i.e., one terrace width. However, meandering of the vertical interface and partial disordering in the IPSLs are often observed. From high resolution ( 10) cross-sectional TEM images, the presence of IPSLs was also confirmed with an atomic scale resolution, although their vertical interface are meandering. In electron diffraction patterns from the (110) plan-view, extra-spots similar to those observed in the ( 10) cross-section were seen. Dark-field images from the superstructure spots indicated that the IPSLs were formed almost exactly along the 110 direction, suggesting that the steps on the growth surface are very straight along the 110 direction.     

InGaAs/InAlAs in-plane superlattices grown on slightly misoriented (110) InP substrates by molecular beam epitaxy

InGaAs/InAlAs in-plane superlattices (IPSLs) composed of InAs/GaAs and InAs/AlAs monolayer superlattices were grown using molecular beam epitaxy. The substrates were misoriented (110) InP tilting 3° toward the [00 ] direction. We grew half monolayers of AlAs and GaAs and single monolayers of InAs alternately, keeping regular arrays of single monolayer steps. The structures were evaluated by transmission electron microscopy (TEM). In a transmission electron diffraction pattern from the ( 10) cross-section, we observed two types of superstructure spot pairs double-positioned in the [001] direction, indicating the formation of the intended IPSL structures. In a cross-sectional TEM dark-field image, we observed the InGaAs/InAlAs superlattice structures formed almost in the [001] direction. The mean period of the superlattices was approximately 4 nm, which was comparable to the terrace width expected from the substrate tilt angle. However, IPSL structures were not completely formed, i.e., the lateral interfaces meandered along the growth direction, and partial disorderings were often observed. The photoluminescence spectrum from the IPSL had a peak corresponding to the InGaAs (2 nm thick)/InAlAs (2 nm thick) superlattice in addition to a peak corresponding to the In_0.5Al_0.25Ga_0.25As alloy.     

Surface diffusion kinetics of GaAs and AlAs metalorganic vapor-phase epitaxy

We have investigated the surface kinetics during metalorganic vapor-phase epitaxy (MOVPE), using high-vacuum scanning tunneling microscopy (STM) observation of two-dimensional (2D) nuclei and denuded zones. Using Monte Carlo simulations based on the solid-on-solid model, from 2D nucleus densities we estimated the surface diffusion coefficients of GaAs and AlAs to be 2 × 10⁻⁶ and 1.5 × 10⁻⁷ cm²/s at 530°C, and the energy barriers for migration to be 0.62 and 0.8 eV, respectively. The 2D nucleus size in the [110] direction was about two times larger than that in the [ 10] direction. The size anisotropy is caused primarily by a difference in the lateral sticking probability (P_s) between steps along the [ 10] direction (A steps) and steps along the [110] direction (B steps). The P_s ratio was estimated to be more than 3:1. Denuded zone widths on upper terraces were 2 ± 0.5 times wider than those on lower terraces. This showed that P_s at descending steps was 10 to 3 × 10² times larger than P_s at ascending steps.     

As-rich reconstruction stability observed by high temperature scanning tunnelling microscopy

Atomic resolution scanning tunnelling microscopy (STM) has been used to study in-situ the As-terminated reconstructions formed on GaAs(0 0 1) surfaces in the presence of an As₄ flux. The reconstructions c(4×4), (2×4) and (3×1) are long established for GaAs(0 0 1) between 400 and 600 °C for varying Ga and As flux, however the stoichiometry of incommensurate transient reconstructions is still uncertain. By performing high temperature STM on an initial (2×4) surface between 250 and 450 °C in the absence of an As flux, small domains with varying reconstruction are observed in a similar manner to the InAs/GaAs(0 0 1) wetting layer. The local storage of excess Ga in Ga-rich domains could provide insight into sub ML homo- and hetero-epitaxial growth.     

Facets formation of pyramidal Si nanocrystals selectively grown on Si(0 0 1) windows in ultrathin SiO2 films

We have used in situ scanning tunneling microscopy (STM) to study the facet formation in the selective growth of pyramidal Si nanocrystals on Si(0 0 1) windows in ultrathin 0.3-nm-thick SiO₂ films. Broad (0 0 1) surfaces developed as the top of the crystals, and {1, 1, (2n+1)} (n=1–6) facets formed the sidewalls. As growth continued, the slope angle of sidewall facets increased, and {1, 1, 9} and {1, 1, (2m+1)} (0 <m < 4) facets often came to coexist on the sidewalls. On well-oriented Si(0 0 1) surfaces, layer-by-layer growth in the [0 0 1] direction was dominant. On vicinal Si(0 0 1) surfaces, lateral step growth took place in the initial stage, and the layer-by-layer growth was suppressed until after a large (0 0 1) surface had formed as the top of the crystal.     

A scanning tunnelling microscopy study of the deposition of Si on GaAs(001); Implications for Si δ-doping

Atomic resolution scanning tunnelling microscopy (STM) has been used to study the adsorption of Si on GaAs(001) surfaces, grown in situ by molecular beam epitaxy (MBE), with a view to understanding the incorporation of Si in δ-doped GaAs structures. Under the low-temperature deposition conditions chosen, the clean GaAs surface is characterized by a well-defined c(4×4) reflection high-energy electron diffraction (RHEED) pattern, a structure involving termination with two layers of As. Filled states STM images of this surface indicate that the basic structural unit, when complete, consists of rectangular blocks of six As atoms with the As-As bond in the surface layer aligned along the [110] direction. Deposition of <0.05 ML of Si at 400°C onto this surface shows significant disruption of the underlying structure. A series of dimer rows are formed on the surface which, with increasing coverage, form anisotropic "needle-like" islands which show no tendency to coalesce even at relatively high coverages (0.5 ML). The formation of these islands accompanies the splitting of the 1/2 order rods in the RHEED pattern along [110]. As the Si is known to occupy only Ga sites, the Si atoms displace the top layer As atoms of the c(4×4) structure, with the displaced As atoms forming dimers in a new top layer. The results are consistent with a recently proposed site exchange model and subsequent island formation for surfactant mediated epitaxial growth.     

Anisotropic lateral growth in GaAs MOCVD layers on (001) substrates

For metalorganic chemical vapor deposition, a fast lateral growth rate is observed for the first time on (001) GaAs having round mesas. The lateral growth rate is greater than the vertical growth rate by a factor of 3–5. The lateral growth rates have anisotropy with respect to the crystallographic directions on the (001) surfaces. The fastest growth direction is the [110] and the slowest one is the [ 10]. The [110] and [ 10] growth rates were found to be strongly dependent on growth conditions, though the vertical one is independent. The [110] growth rate decreases with decreasing As pressure, while the [ 10] remains constant. As growth temperature increases, both the [110] and the [ 10] growth rates decrease. A simple model for the lateral growth mechanism is proposed from the consideration of atomic arrangements and the number of dangling bonds at [110] and [ 10] step sites. According to the model, the lateral growth rate is proportional to the number of bonds available for binding Ga atoms at step sites. The model can explain well the anisotropy in the lateral growth rate and its dependence on the growth conditions.     

Growth of InAs on GaAs(1 0 0) by low-pressure metalorganic chemical vapor deposition employing in situ generated arsine radicals

InAs was grown by low-pressure metalorganic chemical vapor deposition on vicinal GaAs(1 0 0) substrates misoriented by 2° toward [0 0 1]. We observed InAs crystal growth, at substrate temperatures down to 300°C, employing in situ plasma-generated arsine radicals as the arsenic source. The in situ generated arsine was produced by placing solid arsenic downstream of a microwave driven hydrogen plasma. Trimethylindium (TMIn) feedstock carried by hydrogen gas was used as the indium source. The Arrhenius plot of InAs growth rate vs. reciprocal substrate temperature displayed an activation energy of 46.1 kcal/mol in the temperature range of 300–350°C. This measured activation energy value is very close to the energy necessary to remove the first methyl radical from the TMIn molecule, which has never been reported in prior InAs growth to the best of authors’ knowledge. The film growth mechanism is discussed. The crystallinity, infrared spectrum, electrical properties and impurity levels of grown InAs are also presented.     

Stranski-Krastanov formation of InAs quantum dots monitored during growth by reflectance anisotropy spectroscopy and spectroscopic ellipsometry

In this study the successful application of reflectance anisotropy spectroscopy (RAS) and spectroscopic ellipsometry (SE) for the in-situ investigation of InAs quantum dot growth on GaAs (001) in Stranski-Krastanov growth mode is reported. Both techniques provide the precise determination of the growth mode transition from two-dimensional InAs layer to three-dimensional island growth. In order to optimize the growth conditions, spectral and time-resolved measurements were performed for different growth parameters (temperatures, growth rates and V/III ratios). For high temperature deposition large additional anisotropies, caused by clusters elongated in the [110] direction were found. Decreasing the deposition rate (0.5 to 0.125 ML/s) also results in the formation of large clusters, as decreases in reflectivity due to larger stray light losses prove. Finally, increasing the AsH₃ partial pressure leads to an earlier onset of island formation and an enhanced tendency for cluster formation.     

Initial growth behavior of GaAs on ZnSe in MOVPE

We have used atomic force microscopy to investigate the initial stages of the growth of GaAs on ZnSe by metalorganic vapor phase epitaxy. Underlying ZnSe with an atomically flat surface is achieved by growth at 450°C and post-growth annealing at the same temperature. The growth modes of GaAs on the ZnSe surface strongly depend on growth temperatures. The growth carried out at 450°C is 2-dimensional, while that at 550°C is highly 3-dimensional (3D), where the 3D islands are elongated in the [110] direction. The growth behavior, unlike homoepitaxy, is well interpreted in terms of low sticking coefficient and anisotropic lateral growth rate in the heterovalent heteroepitaxy.     

Surface diffusion length of Ga adatoms in molecular-beam epitaxy on GaAs(100)-(110) facet structures

By the molecular-beam epitaxial (MBE) growth of GaAs on [001]-mesa stripes patterned on GaAs(100) substrates, (110) facets were formed on the mesa edges defining (100)-(110) facet structures. The surface diffusion length of Ga adatoms along the [010] direction on the mesa stripes was obtained for a variety of growth conditions by in-situ scanning microprobe reflection high-energy electron diffraction (μ-RHEED). Using these values and the corresponding growth rate on the GaAs(110) facets, the diffusion length on the (110) plane was estimated. We found that the Ga diffusion length on the (110) plane is longer than that on the (100) and (111)B planes. The long diffusion length on the (110) plane is discussed in terms of the particular surface reconstruction on this plane.     

Role of step orientation and step-step interaction in the in-situ creation of laterally confined semiconductor nanostructures via growth: A simulated annealing study on a parallel computing platform

We report a systematic simulated annealing study of the energetics of bi-layer height steps with edges running parallel (A type), perpendicular (B type) and at 45° (C type) to surface As dangling orbitals on As(2×4) reconstructed GaAs(001) vicinal surfaces. Employing semi-empirical interatomic potentials having two- and three-body interaction terms, we calculate the step energy and the step-step interaction energy as a function of the step separation. The step-step interaction energies are attractive for B type steps and repulsive for A and C types, in all cases decreasing in magnitude with increasing step separation. The results affirm a connection between the orientation of dangling orbitals at the step edge and the corresponding step-step elastic interaction induced nature and directionality of the surface stress. Such surface stress could be a driving force for the directional migration of atoms observed in the case of MBE growth on patterned non-planar GaAs substrates that has led to the realization of quantum wire and quantum box structures.     

Atomic force microscope observation of the initial stage of InAs growth on GaAs substrates

The initial stage of InAs growth on GaAs(001) substrates has been investigated by atomic force microscopy. Three-dimensional (3D) islands of a uniformly small size and high density were observed at the initial stage not only for low substrate temperature (T_s) but also for low V/III ratio. This is explained by a simple model based on the difference in the growth rate between strained and relaxed InAs surfaces. The 3D islands are found to agglomerate after the growth is interrupted under As pressure. We suppress the agglomeration and obtain an atomically flat InAs surface.     

Growth of embedded ErAs nanorods on (4 1 1)A and (4 1 1)B GaAs by molecular beam epitaxy

The low solubility of Er in GaAs results in the formation of ErAs nanostructures when GaAs is grown with 5–6 at% Er/Ga ratio by molecular beam epitaxy on GaAs surfaces. For growth on the (4 1 1)A GaAs surface, cross-sectional scanning transmission electron microscopy images show the presence of ErAs nanorods embedded in a GaAs matrix extending along the [2 1 1] direction with a spacing of roughly 7 nm and a diameter of roughly 2 nm. Growth on the GaAs (4 1 1)B surface resulted in only nanoparticle formation. Variation of the polarized optical absorption with in-plane polarization angle is consistent with coupling to surface plasmon resonances of the semimetallic nanostructures.     

X-ray analysis of Self-Organized InAs/InGaAs Quantum Dot Structure

We report on an X-ray study of an InAs/InGaAs/GaAs multi quantum dot stack grown by metalorganic chemical vapor deposition using grazing incidence reflectometry, high-resolution X-ray diffraction, reciprocal space mapping and pole figure analysis. No direct signal from the quantum dots is found by the high-resolution techniques. All rocking curves on different symmetric and asymmetric Bragg reflections can be simulated within the framework of dynamical theory assuming a perfect tretragonally distorted InAs/InGaAs/GaAs multiquantum well system. A pole figure analysis in the vicinity of the (113) and (022) reflections, however, reveals a signal from the quantum dots. There is a considerable indium enrichment in the quantum dots as compared to the wetting layer indicating a strong In-diffusion during their formation. Moreover, a strongly anisotropic diffuse scattering distribution with respect to the [110] and [1-10] directions is found.     

Formation of Ge-diffusion-suppressed GaAs layers and InAs quantum dots on Ge/Si substrates

Crystal growth of GaAs layers and InAs quantum dots (QDs) on the GaAs layers was investigated on Ge/Si substrates using ultrahigh vacuum chemical vapor deposition. Ga-rich GaAs with anti-site Ga atoms grown at a low V/III ratio was found to suppress the diffusion of Ge into GaAs. S-K mode QD formation was observed on GaAs layers grown on Ge/Si substrates with Ga-rich GaAs initial layers, and improved photoluminescence from 1.3 μm-emitting InAs QDs was demonstrated.     

Atomic Processes during Crystal Growth Studied by Reflection High-Energy Electron Diffraction

After a short retrospect on the development of the electron diffraction techniques it is shown that the atomic-scale morphology of the crystal surface and growth processes on it can be studied in detail during molecular beam epitaxy (MBE) by reflection high-energy electron diffraction (RHEED). This is demonstrated for the evolution of the terrace-step-structure of the singular GaAs (001) surface during growth and after growth interruption and for the attachment of Si atoms at misorientation steps on vicinal GaAs (001) surfaces.     

Structural analysis of AlGaAs quantum wires on vicinal (110)GaAs by transmission electron microscopy and energy dispersive X-ray spectroscopy

Giant step structures consisting of coherently aligned multi-atomic steps were naturally formed during the molecular beam epitaxy growth of Al_0.5Ga_0.5As/GaAs superlattices (SLs) on vicinal (110)GaAs surfaces misoriented 6° toward (111)A. The growth of AlAs/Al_xGa_1−xAs/AlAs quantum wells (QWs) on the giant step structures realized Al_x0Ga_1−x0As (x₀<x) quantum wires (QWRs). We studied the giant step structures and the QWRs by transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDX). TEM observations revealed that the QWRs were formed at the step edges. The cross sections of the QWRs were as small as 10 nm×20 nm and the lateral distances between them were about 0.15 μm. We clarified the roles of the SLs to form the coherent giant step structures. From EDX analysis, it was estimated that the AlAs composition in the Al_0.5Ga_0.5As layers varied from 0.5 (terrace) to 0.41 (step edge). In the AlAs/Al_xGa_1−xAs/AlAs QWs, the AlAs compositional modulation and the confinement by the AlAs barriers led to the embedded Al_x0Ga_1−x0As regions. These results supported the existence of the Al_x0Ga_1−x0As QWRs on the giant step structures.     

MOVPE growth of GaAs on Ge substrates by inserting a thin low temperature buffer layer

High quality GaAs layers have been grown by low pressure MOVPE on Ge(001) and Ge(001) 9° off oriented in [110] direction by using a thin low temperature (LT) GaAs layer. Investigations of the initial growth step were performed at different V/III ratios and temperatures. To show the good buffer layer quality solar cell structures were grown on off oriented n‐Ge(001) and n‐GaAs(001) substrates. The surface morphology was studied by atomic force microscopy which showed the step‐flow growth mode on 1.2 µm thick GaAs/Ge structures. The crystalline qualities of this structures and the smooth surface morphology were investigated by double crystal X‐ray diffraction (XRD) and atomic force microscopy (AFM). (© 2006 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

90° double reflection high-energy electron diffraction experiments on vicinal surfaces of GaAs

Reflection high-energy electron diffraction (RHEED) experiments recording the intensity of the specular beam in two azimuths have been carried out simultaneously. The critical temperature for the transition from 2D nucleation to step-flow growth was simultaneously estimated in the [ 10] and [110] directions by observing the disappearance of RHEED intensity oscillations on GaAs(001) substrates 2° misoriented towards GaAs(111)A. It was found that the oscillations disappear at a lower substrate temperature in the [110] azimuth. The difference in the transition temperatures was 25°C.