D.F. Reyes

Bismuth incorporation and the role of ordering in GaAsBi/GaAs structures

The structure and composition of single GaAsBi/GaAs epilayers grown by molecular beam epitaxy were investigated by optical and transmission electron microscopy techniques. Firstly, the GaAsBi layers exhibit two distinct regions and a varying Bi composition profile in the growth direction. In the lower (25 nm) region, the Bi content decays exponentially from an initial maximum value, while the upper region comprises an almost constant Bi content until the end of the layer. Secondly, despite the relatively low Bi content, CuPtB-type ordering was observed both in electron diffraction patterns and in fast Fourier transform reconstructions from high-resolution transmission electron microscopy images. The estimation of the long-range ordering parameter and the development of ordering maps by using geometrical phase algorithms indicate a direct connection between the solubility of Bi and the amount of ordering. The occurrence of both phase separation and atomic ordering has a significant effect on the optical properties of these layers.PACS78.55.Cr III-V semiconductors; 68.55.Nq composition and phase identification; 68.55.Ln defects and impurities: doping, implantation, distribution, concentration, etc; 64.75.St phase separation and segregation in

Formation of Tetragonal InBi Clusters in InAsBi/InAs(100) Heterostructures Grown by Molecular Beam Epitaxy

This work analyses the Bi incorporation in InAs1-xBix/InAs(100) epilayers grown by MBE through advanced transmission electron microscopy techniques. Samples grown from 350–400 °C resulted in Bi contents <3.3% exhibiting compositional variation in the growth direction. In contrast, roughly spherical clusters appeared in the sample grown at lower temperatures. The clusters are made up of the binary InBi with a tetragonal PbO phase surrounded by a matrix of InAs0.95Bi0.05 indicating the Bi solubility limit in InAs. These InBi crystals underwent a cubic distortion and are tilted 55° with regard to the InAsBi matrix. The crystallographic relationships are analysed in detail.

Photoluminescence Enhancement of InAs(Bi) Quantum Dots by Bi Clustering

The distribution of bismuth in InAs1-xBix/GaAs quantum dots is analyzed by atomic-column resolution electron microscopy and imaging simulation techniques. A random Bi distribution is measured in the case of <0.03 ML/s Bi flux during the InAs growth with no significant variations in the shape or size of quantum dots, resulting in a low redshift and the degradation of the photoluminescence. However, for a 0.06 ML/s Bi flux the lateral indium segregation into the quantum dots is enhanced and Bi is incorporated inside them. As a result, a strong redshift and an increase of the peak intensity are found in this sample.

Impact of N on the atomic-scale Sb distribution in quaternary GaAsSbN-capped InAs quantum dots

The use of GaAsSbN capping layers on InAs/GaAs quantum dots (QDs) has recently been proposed for micro- and optoelectronic applications for their ability to independently tailor electron and hole confinement potentials. However, there is a lack of knowledge about the structural and compositional changes associated with the process of simultaneous Sb and N incorporation. In the present work, we have characterized using transmission electron microscopy techniques the effects of adding N in the GaAsSb/InAs/GaAs QD system. Firstly, strain maps of the regions away from the InAs QDs had revealed a huge reduction of the strain fields with the N incorporation but a higher inhomogeneity, which points to a composition modulation enhancement with the presence of Sb-rich and Sb-poor regions in the range of a few nanometers. On the other hand, the average strain in the QDs and surroundings is also similar in both cases. It could be explained by the accumulation of Sb above the QDs, compensating the tensile strain induced by the N incorporation together with an In-Ga intermixing inhibition. Indeed, compositional maps of column resolution from aberration-corrected Z-contrast images confirmed that the addition of N enhances the preferential deposition of Sb above the InAs QD, giving rise to an undulation of the growth front. As an outcome, the strong redshift in the photoluminescence spectrum of the GaAsSbN sample cannot be attributed only to the N-related reduction of the conduction band offset but also to an enhancement of the effect of Sb on the QD band structure.

Bismuth concentration inhomogeneity in GaAsBi bulk and quantum well structures

The optical and structural properties of GaAsBi bulk and quantum well (QW) samples grown under various conditions were studied by photoluminescence (PL), high resolution x-ray diffraction (HR-XRD) and transmission electron microscopy (TEM). At 10 K, the 90 nm bulk sample shows two PL peaks at 1.18 and 1.3 eV. The temperature and power dependent PL data suggest that both PL peaks originate from the GaAsBi layer which consists of two regions with different Bi concentrations. The TEM images verify that the Bi concentration decreases monotonically across the layer, showing a high Bi concentration (~0.053) close to the bottom interface which then reduces to ~0.02 for thicknesses >25 nm. Besides, the high Bi content region cannot be detected by HR-XRD due to a broad and weak diffraction intensity. For multiple QW samples, a similar Bi profile was also observed in which the first well has a significantly higher Bi content compared to the other wells. The energy separation between the PL peaks is 0.12 eV and is consistent with the energy difference observed for the bulk sample. However, two PL peaks were not observed in the other GaAsBi bulk sample which was grown under different conditions, showing the importance of growth optimizations.

Capping layer growth rate and the optical and structural properties of GaAsSbN-capped InAs/GaAs quantum dots

Changing the growth rate during the heteroepitaxial capping of InAs/GaAs quantum dots (QDs) with a 5 nm-thick GaAsSbN capping layer (CL) strongly modifies the QD structural and optical properties. A size and shape transition from taller pyramids to flatter lens-shaped QDs is observed when the CL growth rate is decreased from 1.5 to 0.5 ML/s. This indicates that the QD dissolution processes taking place during capping can be controlled to some extent by the GaAsSbN CL growth rate, with high growth rates allowing a complete preservation of the QDs. However, the dissolution processes are shown to have a leveling effect on the QD height, giving rise to a narrower size distribution for lower growth rates. Contrary to what could be expected, these effects are opposite to the strong blue-shift and improvement of the photoluminescence (PL) observed for higher growth rates. Nevertheless, the PL results can be understood in terms of the strong impact of the growth rate on the Sb and N incorporation into the CL, whi...

Effect of annealing in the Sb and In distribution of type II GaAsSb-capped InAs quantum dots

Type II emission optoelectronic devices using GaAsSb strain reduction layers (SRL) over InAs quantum dots (QDs) have aroused great interest. Recent studies have demonstrated an extraordinary increase in photoluminescence (PL) intensity maintaining type II emission after a rapid thermal anneal (RTA), but with an undesirable blueshift. In this work, we have characterized the effect of RTA on InAs/GaAs QDs embedded in a SRL of GaAsSb by transmission electron microscopy (TEM) and finite element simulations. We find that annealing alters both the distribution of Sb in the SRL as well as the exchange of cations (In and Ga) between the QDs and the SRL. First, annealing causes modifications in the capping layer, reducing its thickness but maintaining the maximum Sb content and improving its homogeneity. In addition, the formation of Sb-rich clusters with loop dislocations is noticed, which seems not to be an impediment for an increased PL intensity. Second, RTA produces flatter QDs with larger base diameter and induces a more homogeneous QD height distribution. The Sb is accumulated over the QDs and the RTA enlarges the Sb-rich region, but the Sb contents are very similar. This fact leaves the type II alignment without major changes. Atomic-scale strain analysis of the nanostructures reveal a strong intermixing of In/Ga between the QDs and the capping layer, which is the main responsible mechanism of the PL blueshift. The improvement of the crystalline quality of the capping layer together with higher homogeneity QD sizes could be the origin of the enhancement of the PL emission.

Quantitative analysis of the interplay between InAs quantum dots and wetting layer during the GaAs capping process

A procedure to quantitatively analyse the relationship between the wetting layer (WL) and the quantum dots (QDs) as a whole in a statistical way is proposed. As we will show in the manuscript, it allows determining, not only the proportion of deposited InAs held in the WL, but also the average In content inside the QDs. First, the amount of InAs deposited is measured for calibration in three different WL structures without QDs by two methodologies: strain mappings in high-resolution transmission electron microscopy images and compositional mappings with ChemiSTEM x-ray energy spectrometry. The area under the average profiles obtained by both methodologies emerges as the best parameter to quantify the amount of InAs in the WL, in agreement with high-resolution x-ray diffraction results. Second, the effect of three different GaAs capping layer (CL) growth rates on the decomposition of the QDs is evaluated. The CL growth rate has a strong influence on the QD volume as well as the WL characteristics. Slower CL growth rates produce an In enrichment of the WL if compared to faster ones, together with a diminution of the QD height. In addition, assuming that the QD density does not change with the different CL growth rates, an estimation of the average In content inside the QDs is given. The high Ga/In intermixing during the decomposition of buried QDs does not only trigger a reduction of the QD height, but above all, a higher impoverishment of the In content inside the QDs, therefore modifying the two most important parameters that determine the optical properties of these structures.

Correcting sample drift using Fourier harmonics

During image acquisition of crystalline materials by high-resolution scanning transmission electron microscopy, the sample drift could lead to distortions and shears that hinder their quantitative analysis and characterization. In order to measure and correct this effect, several authors have proposed different methodologies making use of series of images. In this work, we introduce a methodology to determine the drift angle via Fourier analysis by using a single image based on the measurements between the angles of the second Fourier harmonics in different quadrants. Two different approaches, that are independent of the angle of acquisition of the image, are evaluated. In addition, our results demonstrate that the determination of the drift angle is more accurate by using the measurements of non-consecutive quadrants when the angle of acquisition is an odd multiple of 45°.

Evaluation of the In desorption during the capping process of diluted nitride In(Ga)As quantum dots

Diluted nitride self-assembled In(Ga)AsN quantum dots (QDs) grown on GaAs substrates are potential candidates to emit in the windows of maximum transmittance for optical fibres (1.3-1.55 μm). In this paper, we analyse the effect of nitrogen addition on the indium desorption occurring during the capping process of InxGa1−xAs QDs (x = l and 0.7). The samples have been grown by molecular beam epitaxy and studied through transmission electron microscopy (TEM) and photoluminescence techniques. The composition distribution inside the dots was determined by statistical moire analysis and measured by energy dispersive X-ray spectroscopy. First, the addition of nitrogen in In(Ga)As QDs gave rise to a strong redshift in the emission peak, together with a large loss of intensity and monochromaticity. Moreover, these samples showed changes in the QDs morphology as well as an increase in the density of defects. The statistical compositional analysis displayed a normal distribution in InAs QDs with an average In content of 0.7. Nevertheless, the addition of Ga and/or N leads to a bimodal distribution of the Indium content with two separated QD populations. We suggest that the nitrogen incorporation enhances the indium fixation inside the QDs where the indium/gallium ratio plays an important role in this process. The strong redshift observed in the PL should be explained not only by the N incorporation but also by the higher In content inside the QDs