Simultaneous monitoring of different surface processes on different streaks of the reflection high energy electron diffraction pattern

The recently discovered additional phase shift of reflection high energy electron diffraction (RHEED) intensity oscillations at heterointerfaces significantly deepens the analysis of surface dynamics using RHEED. The evolution of the phase shift is different for the {01} and (00) streaks of the same RHEED pattern because the two streaks show a different sensitivity on surface morphology: whereas diffraction into {01} streaks requires good lateral periodicity of the surface, no lateral periodicity is required for diffraction into the (00) streak. Therefore, the signal on the (00) streak should be most sensitive towards steps running along the electron beam, while the {01} beams sample mostly terraces. We demonstrate the potential and sensitivity of this effect using GaAs-AlAs(100) interfaces and discuss its compatibility with current models of RHEED oscillations. The effects is then applied to characterize the incorporation dynamics of segregating and non-segregating dopants.     

Surface reconstruction of sulfur-terminated GaAs(001) observed during annealing process by scanning tunneling microscopy

The surface reconstruction of in-situ prepared sulfur-terminated (S-terminated) and sulfur-protected (S-protected) GaAs(001) is studied by scanning tunneling microscopy (STM) at high temperatures of up to 260°C. We demonstrate a new reordering process from the (4×6) Ga-stabilized surface to the (2×6) S-stabilized surface and a novel method of air protection using a S passivation layer. Moreover, the in-situ observation of the annealing process of this S-protection layer is performed by high-temperature STM, avoiding the adsorption from environments and verifying that the (2×6) structure still becomes dominant on the S-terminated GaAs(001) surface without the effects of As atoms.     

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.     

Epitaxial Growth of Silver Bromide on Mica from the Melt

It is shown that it is possible to grow silver bromide crystals with definite crystallographic orientation by solidification of liquid silver bromide between mica and quartz plates by cooling the mica side. The orientation is (111). The maximum dimensions were 15mm × 15 mm × 1 mm. The surface is investigated by electron reflection (RHEED). The crystals have a smooth surface and can be used for optical application without surface reconstruction.     

GaSb薄膜生长的RHEED研究

采用分子束外延技术,在GaAs衬底上生长GaSb薄膜时,利用反射式高能电子衍射仪(RHEED)对衬底表面清洁状况、外延层厚度等进行在线监控.通过RHEED讨论低温缓冲层对GaSb薄膜表面结构和生长机制的作用,可以估算衬底温度,并能计算出薄膜的生长速率.实验测量GaSb的生长周期为1.96s,每秒沉积0.51单分子层.低温缓冲层提高了在GaAs衬底上外延GaSb薄膜的生长质量.     

Arsenic-free GaAs substrate preparation and direct growth of GaAs/AlGaAs multiple quantum well without buffer layer

High-temperature treatment of GaAs substrate without As flux in a preparation chamber was investigated as a substrate surface cleaning method for molecular beam epitaxial (MBE) growth. Oxide gases such as CO and CO₂ were almost completely desorbed at a temperature above which Ga and As started to evaporate from the substrate. During the cleaning at a temperature as high as 575°C for 30 min, about 100 nm thick GaAs was evaporated from the substrate, but its surface maintained mirror-like smoothness and showed streak pattern with surface reconstruction pattern in the reflection high energy electron diffraction (RHEED) observation. Direct growth of GaAs/Al GaAs quantum well (QW) structures was tried on such surfaces without introducing any buffer layers. The QW structure showed photoluminescence with both intensity and full width at half maximum comparable with those for the QW grown on the substrate cleaned by the conventional method with introducing a GaAs buffer layer.     

Structural and photoluminescence characteristics of molecular beam epitaxy-grown vertically aligned In0.33Ga0.67As/GaAs quantum dots

In this paper, we present the results of structural and photoluminescence (PL) studies on vertically aligned, 20-period In_0.33Ga_0.67As/GaAs quantum dot stacks, grown by molecular beam epitaxy (MBE). Two different In_0.33Ga_0.67As/GaAs quantum dot stacks were compared. In one case, the In_0.33Ga_0.67As layer thickness was chosen to be just above its transition thickness, and in the other case, the In_0.33Ga_0.67As layer thickness was chosen to be 30% larger than its transition thickness. The 2D–3D growth mode transition time was determined using reflection high-energy electron diffraction (RHEED). Structural studies were done on these samples using high-resolution X-ray diffraction (HRXRD) and cross-sectional transmission electron microscopy (XTEM). A careful analysis showed that the satellite peaks recorded in X-ray rocking curve show two types of periodicities in one sample. We attribute this additional periodicity to the presence of an aligned vertical stack of quantum dots. We also show that the additional periodicity is not significant in a sample in which the quantum dots are not prominently formed. By analyzing the X-ray rocking curve in conjunction with RHEED and PL, we have estimated the structural parameters of the quantum dot stack. These parameters agree well with those obtained from XTEM measurements.     

Surface diffusion lenght during MOMBE and CBE growth measured by μ-RHEED

The growth rates of layers grown on a mesa-etched (001) GaAs surface were measured by in-situ scanning microprobe reflection high-energy electron diffraction (μ-RHEED) from the period of the RHEED intensity oscillation in real time. The diffusion lenght of the surface adatoms of column III elements was determined from the gradient of the variation of the growth rates in the cases of MBE, MOMBE using trimethylgallium (TMGa) and CBE using TMGa or triethylgallium (TEGa) and arsine (AsH₃). The obtained values of the diffusion lengths were of the order of a micrometer in every case of the source-material combination. In the case of metalorganic materials as Ga source, it was found that the diffusion length was larger than that of Ga atom from metal Ga source. Since the substrate temperature of the present experiment is high enough to decompose TMGa and TEGa on the surface, Ga adatoms are considered to be responsible to the surface diffusion. Therefore, it is considered that the derivatives of the metalorganic molecules such as methyl radicals affect the diffusion of Ga adatoms.     

Surface and interfacial structure of epitaxial SrTiO3 thin films on (0 0 1) Si grown by molecular beam epitaxy

Effects of relaxation of interfacial misfit strain and non-stoichiometry on surface morphology and surface and interfacial structures of epitaxial SrTiO₃ (STO) thin films on (0 0 1) Si during initial growth by molecular beam epitaxy (MBE) were investigated. In situ reflection high-energy electron diffraction (RHEED) in combination with X-ray diffraction (XRD), atomic force microscopy (AFM), X-ray photoelectron spectrometry (XPS) and transmission electron microscopy (TEM) techniques were employed. Relaxation of the interfacial misfit strain between STO and Si as measured by in situ RHEED indicates initial growth is not pseudomorphic, and the interfacial misfit strain is relaxed during and immediately after the first monolayer (ML) deposition. The interfacial strain up to 15 ML results from thermal mismatch strain rather than lattice mismatch strain. Stoichiometry of STO affects not only surface morphology but interfacial structure. We have identified a nanoscale Sr₄Ti₃O₁₀ second phase at the STO/Si interface in a Sr-rich film.     

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.     

RHEED studies of the growth of Si(001) by gas source MBE from disilane

The growth of Si(001) from a gas source molecular beam epitaxy system (Si-GSMBE) using disilane (Si₂H₆) was investigated using reflection high-energy electron diffraction (RHEED). The surface reconstructions occurring between 100 and 775°C were studied as a function of both substrate temperature and surface coverage. We report the first observation of (2x2) and c(4x4) reconstructions during growth at substrate temperatures near 645°C using Si₂H₆. All growth was found to be initiated by the formation of three-dimensional (3D) islands which coalesced at substrate temperatures above 600°C. The surface reconstruction was found to change from a disordered to an ordered (2x1)+(1x2) structure at 775°C via intermediate (2x2) and c(4x4) phases. Thereafter, growth was found to proceed in a 2D layer-by-layer fashion, as evidenced by the observation of RHEED intensity oscillations. This technique has been used, for the first time, to calibrate growth rates during Si-GSMBE. The intensity oscillations were measured as a function of both substrate temperature and incident beam flux. Strong and damped oscillations were observed between 610 and 680°C, in the two-dimensional growth regime. At higher temperatures, growth by step propagation dominated while at lower temperatures, growth became increasingly three-dimensional and consequently oscillations were weak or absent. Similarly, there was a minimum flux limit ( <0.16 SCCM), below which no oscillations were recorded.     

Structure and chemical composition of LiB3O5 surfaces

The electronic and structural properties of LiB₃O₅ (LBO) surfaces have been studied by X‐ray photoemission spectroscopy (XPS) and reflectance high‐energy electron diffraction (RHEED). The as‐grown (110) crystal face and mechanically polished (001) surfaces have been investigated comparatively. Electronic structure of LBO has been determined on as‐grown (110) crystal face previously cleaned by chemical etching with RHEED control. The correlation of valence band structure and measured binding energies with earlier reported results has been discussed. Core‐level spectroscopy reveals strong enriching of mechanically polished LBO surface with carbon, when nanodiamond powder is used as an abrasive. So high carbon level as C:B = 0.7 has been observed at the surface while the ratio Li:B:O remains according to LBO chemical composition. The association of LBO Kikuchi‐lines with strong background has been shown by RHEED analysis of the surface. Thus, the polished LBO surface constitutes a high structure quality LBO with the inclusions of some amorphous carbon compound. (© 2003 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Nucleation and ripening of seeded InAs/GaAs quantum dots

We have investigated the nucleation and ripening of pairs of InAs/GaAs quantum dot layers separated by thin (2–20 nm) GaAs spacer layers. Reflection high energy electron diffraction (RHEED) measurements show that the 2D–3D transition in the second layer can occur for less than 1 monolayer deposition of InAs. Immediately after the islanding transition in the second layer chevrons were observed with included angles as low as 20° and this angle was seen to increase continuously to 45±2° as more material was deposited. Atomic force microscopy showed the dot density in both layers to be the same. It is proposed that surface morphology can radically alter processes that determine the nucleation and ripening of the 3D islands.     

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.     

Growth of EuTe islands on SnTe by molecular beam epitaxy

Semiconductor magnetic quantum dots are very promising structures, with novel properties that find multiple applications in spintronic devices. EuTe is a wide gap semiconductor with NaCl structure, and strong magnetic moments S=7/2 at the half filled 4f⁷ electronic levels. On the other hand, SnTe is a narrow gap semiconductor with the same crystal structure and 4% lattice mismatch with EuTe. In this work, we investigate the molecular beam epitaxial growth of EuTe on SnTe after the critical thickness for island formation is surpassed, as a previous step to the growth of organized magnetic quantum dots. The topology and strain state of EuTe islands were studied as a function of growth temperature and EuTe nominal layer thickness. Reflection high energy electron diffraction (RHEED) was used in-situ to monitor surface morphology and strain state. RHEED results were complemented and enriched with atomic force microscopy and grazing incidence X-ray diffraction measurements made at the XRD2 beamline of the Brazilian Synchrotron. EuTe islands of increasing height and diameter are obtained when the EuTe nominal thickness increases, with higher aspect ratio for the islands grown at lower temperatures. As the islands grow, a relaxation toward the EuTe bulk lattice parameter was observed. The relaxation process was partially reverted by the growth of the SnTe cap layer, vital to protect the EuTe islands from oxidation. A simple model is outlined to describe the distortions caused by the EuTe islands on the SnTe buffer and cap layers. The SnTe cap layers formed interesting plateau structures with easily controlled wall height, that could find applications as a template for future nanostructures growth.     

The characterization of the growth of sub-monolayer coverages (1/200th to 1 monolayer) of Si and Be on GaAs(001): A reflectance anisotropy spectroscopy and reflection high-energy electron diffraction study

The techniques of reflectance anisotropy spectroscopy (RAS) and reflection high-energy electron diffraction (RHEED) have been employed, for the first time in concert, to characterize the growth of sub-monolayer coverages of both Si and Be deposited onto the GaAs(001)-c(4×4) surface. The RHEED observations enabled the RAS spectra collected for a series of Si and Be coverages, in the range 0.005 to 1.000 monolayer (ML), to be interpreted in terms of changes in the sample surface structure. For the case of Si/GaAs(001) the following series of surface reconstructions were observed with increasing Si coverage: c(4×4), c(4×4)/(1×2), (1×2), (1×2)/(3×1) and, (3×1). During the deposition of Be/GaAs(001), c(4×4), c(4×4)/(1×2), c(4×4)/(1×3), (1×2)/(1×3), (1×3), and (1×2) reconstructions were noted to evolve. The fact that unique, but highly reproducible, RAS signatures were obtained for each of these surface phases demonstrates the applicability of a combined RHEED/RAS system for monitoring sub-monolayer heteroepitaxial growth with a surface sensitivity of the order of 1/200th of a monolayer.     

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.     

Molecular beam epitaxial growth and thermodynamic analysis of InGaAs and InAlAs lattice matched to InP

Reflection high-energy electron diffraction (RHEED) intensity oscillations have been used to detect the onset of metal droplet formation on the surface of InAs, InGaAs and InAlAs during molecular beam epitaxy. The growth conditions which produce such droplets are shown to be in good agreement with predictions based on thermodynamic arguments.     

Thermodynamic analysis of GaAs growth by molecular beam epitaxy at the surface structure transition from 3 × 1 to 4 × 2

The molecular beam epitaxy (MBE) growth of GaAs layers on a single crystal is studied in relation with the stability domain of the GaAs compound in the Ga-As binary system. The growth parameters, i.e. The Ga and As impinging atomic flows, are compared to the necessary flows as calculated by thermodynamics. In order to take into account in the real growth situation, which is not strictly at equilibrium, the flow balance at the surface of the crystal between the impinging flows and the growth and evaporated flows is written for quasi-equilibrium growth conditions, including condensation and evaporation coefficients that split the “so-called” sticking coefficient in parts related to the condensation or the evaporation phenomenon for each gaseous species. A comparison between the quasi-equilibrium simulation of the growth and the experiment is made with the assumption that the surface structure transition from gallium-stabilized to arsenic-stabilized surface corresponds to the growth of a GaAs crystal at its solidus boundary rich in gallium. The surface structure transitions are observed by reflection high energy electron diffraction (RHEED) and the impinging atomic flows are carefully calibrated and also controlled by RHEED oscillations as observed after gallium or arsenic excess as deposited on the surface. The results show that the growth is effectively performed close to equilibrium conditions as evidenced by the values of the condensations and evaporation coefficients. The evaporation coefficient of gallium is 0.4, showing that this component is the supersaturated one at the surface, and this value agrees with theoretical predictions for an evaporation process (during growth) controlled by the surface diffusion process of monoatomic species between steps.     

Simultaneous reflection high-energy electron diffraction oscillations and mass spectroscopy investigations during molecular beam epitaxy growth of (001) GaAs - smooth surfaces or stoichiometric films?

Film composition and surface morphology of molecular beam epitaxy (MBE)-grown GaAs(001) surfaces were investigated in situ as a function of flux ratio J_Ga/J_As4. The flux of As₄ molecules desorbing from the sample surface was measured with a quadrupole mass spectrometer (QMS) simultaneously with the observation of reflection high energy electron diffraction (RHEED) intensity oscillations. The incorporation ratio, given by the number of incorporated Ga atoms per As atom, was calculated independent of both the QMS data and the decreasing growth rate for growth conditions with As deficiency, as obtained from the RHEED oscillation frequency. Stoichiometric growth was found up to a flux ratio J_Ga/J_As4 ≈ 0.9. At flux ratios of 1.1 to 1.2, a minimum of the damping of the RHEED oscillation amplitude indicates a very smooth growth front profile, but Ga excess appears to be incorporated mainly in As sites without disturbing the crystal lattice. This assumption was confirmed by photoluminescence (PL) spectroscopy of films grown at a flux ratio J_Ga/J_As4 of 1.2. An additional PL peak was observed, which indicates the incorporation of Ga atoms on As sites.