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By employing a mixed SnO$_2$+Sn source, we demonstrate suboxide molecular beam epitaxy growth of phase-pure single crystalline metastable SnO(001) thin films at a growth rate of ~1.0nm/min without the need for additional oxygen. These films grow epitaxially across a wide substrate temperature range from 150 to 450{\deg}C. Hence, we present an alternative pathway to overcome the limitations of high Sn or SnO$_2$ cell temperatures and narrow growth windows encountered in previous MBE growth of metastable SnO. In-situ laser reflectometry and line-of-sight quadrupole mass spectrometry were used to investigate the rate of SnO desorption as a function of substrate temperature. While SnO ad-molecules desorption at Ts = 450{\deg}C was growth-rate limiting,the SnO films did not desorb at this temperature after growth in vacuum. The SnO (001) thin films are transparent and unintentionally p-type doped, with hole concentrations and mobilities in the range of 0.9 to 6.0x10$^{18}$cm$^{-3}$ and 2.0 to 5.5 cm$^2$/V.s, respectively. These p-type SnO films obtained at low temperatures are promising for back-end-of-line (BEOL) compatible applications and for integration with n-type oxides in p-n heterojunction and field-effect transistors, Comment: 18 pages, 10 figures

Core-shell GaAs-based nanowires monolithically integrated on Si constitute a promising class of nanostructures that could enable light emitters for fast inter- and intrachip optical connections. We introduce and fabricate a novel coaxial GaAs/(In,Ga)As dot-in-a-well nanowire heterostructure to reach spontaneous emission in the Si transparent region, which is crucial for applications in Si photonics. Specifically, we achieve room temperature emission at 1.27 $\mu$m in the telecommunication O band. The presence of quantum dots in the heterostructure is evidenced by a structural analysis based on scanning transmission electron microscopy. The spontaneous emission of these nanowire structures is investigated by cathodoluminescence and photoluminescence spectroscopy. Thermal redistribution of charge carriers to larger quantum dots explains the long wavelength emission achieved at room temperature. Finally, in order to demonstrate the feasibility of the presented nanowire heterostructures as electrically driven light emitters monolithically integrated on Si, a light emitting diode is fabricated exhibiting room-temperature electroluminescence at 1.26 $\mu$m., Comment: This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in ACS Applied Nano Materials (2019), copyright (C) American Chemical Society after peer review. To access the final edited and published work see this https://doi.org/10.1021/acsanm.9b01866, the supporting information is available (free of charge) under the same link

International audience; Dilute bismuth (Bi) III-V alloys have recently attracted great attention, due to their properties of band-gap reduction and spin-orbit splitting. The incorporation of Bi into antimonide based III-V semiconductors is very attractive for the development of new optoelectronic devices working in the mid-infrared range (2-5 µm). However, due to its large size, Bi does not readily incorporate into III-V alloys and the epitaxy of III-V dilute bismides is thus very challenging. This book chapter presents the most recent developments in the epitaxy and characterization of GaSbBi alloys and heterostructures.

To determine the band alignment at the GaSb1-xBix/GaSb interface, a set of GaSb1-xBix/GaSb quantum wells (QWs) of various widths (7, 11, and 15 nm) and contents (Bi ≤ 12%) were grown by molecular beam epitaxy and investigated by photoreflectance (PR) spectroscopy. In PR spectra, the optical transitions related to both the ground and the excited states in the QW were clearly observed. It is a direct experimental evidence that the GaSb1-xBix/GaSb QW is a type-I QW with a deep quantum confinement in both the conduction and valence bands. From the comparison of PR data with calculations of energies of QW transitions performed for the varying valence band offset (VBO), the best agreement between experimental data and theoretical calculations has been found for the VBO ∼50 ± 5%. A very similar VBO was obtained from ab initio calculations. These calculations show that the incorporation of Bi atoms into a GaSb host modifies both the conduction and valence band: the conduction-band position changes linearly at a rate of ∼15–16 meV per % Bi and the valence band position changes at a rate of ∼15–16 meV per % Bi. The calculated shifts of valence and conduction bands give the variation of VBO between GaSb1-xBix and GaSb in the range of ∼48%–52%, which is in good agreement with conclusions derived from PR measurements. In addition, it has been found that the electron effective mass reduces linearly with the increase in Bi concentration (x): m e f f G a S b B i = m e f f G a S b − 0.2 x, where m e f f G a S b is the electron effective mass of GaSb. Moreover, a strong photoluminescence (PL) was observed and a negligible Stokes shift (less than a few meV) between the PL peak and the fundamental transition in the PR spectrum was detected for all QWs at low temperatures. It means that the investigated QWs are very homogeneous, and the carrier localization for this alloy is very weak in contrast to other dilute bismides.

Epitaxial GaP/Si heterostructures grown by molecular beam epitaxy (MBE) and migration-enhanced epitaxy (MEE) have been studied, primarily using aberration-corrected scanning transmission electron microscopy (AC-STEM). Atomically-resolved structure images, which are sensitive to atomic-column intensity revealed the detailed geometry of antiphase boundaries that were both parallel and also inclined to the growth direction. The polar/non-polar GaP/Si interfaces were neither atomically flat laterally nor abrupt vertically. Measurements of intensity profiles using both bright-field and dark-field AC-STEM images, as well as chemically-sensitive g002 dark-field imaging, indicated substantial interfacial intermixing, which increased significantly from ∼1.3 nm (MEE growth at 440 °C) to ∼2.1 nm (MBE growth at 600 °C). The finite interface width will impact theoretical predictions of charge imbalance and strong electric fields across the heterointerface.

We present a novel two-step growth approach for the Ga-assisted growth of GaAs nanowires (NWs) by molecular beam epitaxy on Si. In the first step only Ga is deposited for the controlled formation of Ga droplets and in the second step NWs are grown from these droplets at lower Ga flux. This variation of the Ga flux leads to a decoupling of the formation of Ga droplets and the formation of NWs. Thus, the total density of crystal objects can be varied by only changing the parameters of the first step. Also, the NW length distribution of such an ensemble is more homogeneous. Annealing of the droplets can improve the homogeneity even further. The resulting GaAs NW ensembles are ideally suited for the subsequent growth of shell structures. Finally, our new approach enabled us to explore the nucleation of different crystalline objects and analyze the impact of the droplet size on the vertical yield of NWs in detail.

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In this chapter, we go over epitaxial growth of bismide thin films, multiple quantum wells, and nanostructures (nanowires) using molecular beam epitaxy (MBE) and their surface morphology, structural, and optical properties are investigated along with device applications. We describe how the Bi content in GaAs1−xBix epilayers grown on (100), (411)A, and (411)B GaAs substrates can be controlled by the growth conditions. Nonstandard growth conditions such as two-substrate-temperature technique (TST) are required for GaAs1−xBix because of the strong tendency of Bi atom segregation under usual growth conditions. We have reported a GaAs0.96Bi0.04/GaAs multiple quantum well LED grown by TST technique with a room temperature photoluminescence and electroluminescence at 1.23 μm emission wavelength. The TST procedure proves as a very efficient method to reduce Bi segregation and thus improves the quality of the GaAsBi layer at GaAs interfaces.

We analyze the microstructure of a series of Ga(Sb, Bi)/GaSb quantum wells (QW) with varying Bi content and QW thicknesses using transmission electron microscopy. The structures are grown on GaSb(001) substrates by low-temperature molecular beam epitaxy. Although Ga(Sb, Bi) is regarded as a highly-mismatched alloy, the material is of remarkable quality and no extended defects or nanoclusters are detected in the pseudomorphic layers. Regardless their different Bi content (ranging from 4% to 11%) all QW samples seem to be homogeneous in composition and no composition fluctuations are detected. The QW/barriers are nevertheless affected by thickness fluctuations, where the thickness slightly varies from QW to QW but also laterally. Despite the samples exhibit well-defined QW/barrier interfaces, we note that the Ga(Sb, Bi)-on-GaSb interface is rougher than the GaSb-on-Ga(Sb, Bi) one. The morphological smoothing effect at the GaSb-on-Ga(Sb, Bi) interface is attributed to the well-known surfactant behavior of Bi in connection with Bi surface segregation, as evidenced from experimental Bi distribution profiles.

International audience; Using transmission electron microscopy, we present an in-depth microstructural analysis of a series of Ga(Sb,Bi) epilayers and Ga(Sb,Bi)/GaSb quantum wells grown on GaSb(001) substrates by molecular beam epitaxy. Despite the dilute bismide compound Ga(Sb,Bi) is regarded as a highly-mismatched alloy, we find that the material is of remarkable structural perfection, even up to 11%–14% Bi, the maximum Bi concentration incorporated into GaSb so far. No extended defects, nanoclusters, or composition modulations are detectable in the pseudomorphic layers. In addition, the quantum wells exhibit regular and homogeneous morphologies including smooth and stable interfaces with a chemical width on the same order as in other high-quality III–V heterointerfaces. These results may give reasons for the recent successful realization of mid-infrared lasers with room temperature operation based on the very same quantum well structures.

The realization of semiconductor structures with stable excitons at room temperature is crucial for the development of excitonics and polaritonics. Quantum confinement has commonly been employed for enhancing excitonic effects in semiconductor heterostructures. Dielectric confinement, which gives rises to much stronger enhancement, has proven to be more difficult to achieve because of the rapid nonradiative surface/interface recombination in hybrid dielectric-semiconductor structures. Here, we demonstrate intense excitonic emission from bare GaN nanowires with diameters down to 6 nm. The large dielectric mismatch between the nanowires and vacuum greatly enhances the Coulomb interaction, with the thinnest nanowires showing the strongest dielectric confinement and the highest radiative efficiency at room temperature. In situ monitoring of the fabrication of these structures allows one to accurately control the degree of dielectric enhancement. These ultrathin nanowires may constitute the basis for the fabrication of advanced low-dimensional structures with an unprecedented degree of confinement.

Twin boundaries and boundaries between zincblende (ZB) and wurtzite (WZ) segments of GaAs-related nanowires (NWs) form intrinsic heterointerfaces with essential consequences for the application of such nanomaterials in optoelectronic devices. We show that for GaAs and GaAs/(Al, Ga)As core/shell NWs, crystal twinning along the NW axis can be imaged with a spatial resolution of 10 nm using secondary electrons in a scanning electron microscope (SEM). Changes of the crystal structure from the ZB to the WZ phase have been investigated by electron backscatter diffraction. In addition to these methods, we employ spectrally and spatially resolved cathodoluminescence measurements in the same SEM to study the correlation between the structural and optical properties in single NWs. Two GaAs/AlAs/GaAs core/shell/shell NWs differing significantly in the crystal structure along their axis have been investigated combining these three techniques in order to demonstrate the strength of the employed methodology. Our experiments show that based on commonly available SEM methods, an overview of the structural properties along an entire NW and their impact on the spectral and spatial luminescence distribution can be efficiently obtained providing a quick feedback for the optimization of growth conditions.

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We discuss observations of InN nanowires (NWs) by plan-view high-resolution transmission electron microscopy (TEM). The main difficulties arise from suitable methods available for plan-view specimen preparation. We explore different approaches and find that the best results are obtained using a refined preparation method based on the conventional procedure for plan-view TEM of thin films, specifically modified for the NW morphology. The fundamental aspects of such a preparation are the initial mechanical stabilization of the NWs and the minimization of the ion-milling process after dimpling the samples until perforation. The combined analysis by plan-view and cross-sectional TEM of the NWs allows determination of the degree of strain relaxation and reveals the formation of an unintentional shell layer (2–3-nm thick) around the InN NWs. The shell layer is composed of bcc In2O3 nanocrystals with a preferred orientation with respect to the wurtzite InN: In2O3 [111] || InN [0001] and In2O3 || InN< $$ 11\bar 20 $$ >.

Single GaN nanowires formed spontaneously on a given substrate represent nanoscopic single crystals free of any extended defects. However, due to the high area density of thus formed GaN nanowire ensembles, individual nanowires coalesce with others in their immediate vicinity. This coalescence process may introduce strain and structural defects, foiling the idea of defect-free material due to the nanowire geometry. To investigate the consequences of this process, a quantitative measure of the coalescence of nanowire ensembles is required. We derive objective criteria to determine the coalescence degree of GaN nanowire ensembles. These criteria are based on the area-perimeter relationship of the cross-sectional shapes observed, and in particular on their circularity. Employing these criteria, we distinguish single nanowires from coalesced aggregates in an ensemble, determine the diameter distribution of both, and finally analyze the coalescence degree of nanowire ensembles with increasing fill factor.

We explore the Bi-surfactant-directed self-assembly and structure of InAs quantum dots grown on GaAs(110) by molecular beam epitaxy. The addition of a Bi flux during InAs deposition changes the InAs growth mode from two-dimensional (2D) Frank-van der Merwe to Stranski-Krastanov, resulting in the formation of three-dimensional (3D) InAs islands on the surface. Furthermore, exposing static InAs 2D layers to Bi induces a rearrangement of the strained layer into 3D islands. We explore the effect of varying the InAs thickness and Bi flux for these two growth approaches, observing a critical thickness for 3D island formation in both cases. Characterization of (110) InAs quantum dots with high-resolution transmission electron microscopy reveals that larger islands grown by the Stranski-Krastanov mode are plastically relaxed, while small islands grown by the on-demand approach are coherent. Strain relaxation along the [1-10] direction is achieved by 90 degree pure-edge dislocations with dislocation lines running along [001]. In contrast, strain relief along [001] is by 60 degree misfit dislocations. This behaviour is consistent with observations of planar (In,Ga)As/GaAs(110) layers. These results illustrate how surfactant Bi can provoke and control quantum dot formation where it normally does not occur.

Complex morphology is observed in the GaAs:Bi cap layer of Ga(As,Bi) films grown on GaAs(001) substrates by low-temperature (LT) molecular beam epitaxy (MBE). The microstructure is dominated by the presence of V-shaped domains in the LT-GaAs cap layer and by the (unintentional) inhomogeneous incorporation of Bi from the underlying Ga(As,Bi) layer growth. Aberration-corrected scanning transmission electron microscopy techniques enabled two types of domain to be identified: (i) twinned domains and (ii) Bi-rich atomically ordered domains with triple periodicity. The observed microstructure is discussed in the context of LT-MBE growth in combination with the presence of a small amount of Bi, which seemingly alters adatom diffusivity. Surface processes and (surface) kinetic factors play a key role in the resultant morphology and explain the appearance of both types of domains.Complex morphology is observed in the GaAs:Bi cap layer of Ga(As,Bi) films grown on GaAs(001) substrates by low-temperature (LT) molecular beam epitaxy (MBE). The microstructure is dominated by the presence of V-shaped domains in the LT-GaAs cap layer and by the (unintentional) inhomogeneous incorporation of Bi from the underlying Ga(As,Bi) layer growth. Aberration-corrected scanning transmission electron microscopy techniques enabled two types of domain to be identified: (i) twinned domains and (ii) Bi-rich atomically ordered domains with triple periodicity. The observed microstructure is discussed in the context of LT-MBE growth in combination with the presence of a small amount of Bi, which seemingly alters adatom diffusivity. Surface processes and (surface) kinetic factors play a key role in the resultant morphology and explain the appearance of both types of domains.

Bi-containing III-V semiconductors constitute an exciting class of metastable compounds with wide-ranging potential optoelectronic and electronic applications. However, the growth of III-V-Bi alloys requires group-III-rich growth conditions, which pose severe challenges for planar growth. In this work, we exploit the naturally-Ga-rich environment present inside the metallic droplet of a self-catalyzed GaAs nanowire (NW) to synthesize metastable GaAs/GaAs1−x Bi x axial NW heterostructures with high Bi contents. The axial GaAs1−x Bi x segments are realized with molecular beam epitaxy by first enriching only the vapor–liquid–solid (VLS) Ga droplets with Bi, followed by exposing the resulting Ga-Bi droplets to As2 at temperatures ranging from 270 °C to 380 °C to precipitate GaAs1−x Bi x only under the NW droplets. Microstructural and elemental characterization reveals the presence of single crystal zincblende GaAs1−x Bi x axial NW segments with Bi contents up to (10 ± 2)%. This work illustrates how the unique local growth environment present during the VLS NW growth can be exploited to synthesize heterostructures with metastable compounds.

We study the temperature dependence of the photoluminescence (PL) from InAs quantum dot chains (QDC) grown by MBE on [011]- and [01 1 ¯ ]-oriented UV nanoimprint lithography processed groove patterns. We observe an increase of PL intensity from the [01 1 ¯ ]-oriented QDCs within the temperature range from 20–70 K, which is attributed to thermally activated carrier transport from small quantum dots accumulated on the sidewalls of the [01 1 ¯ ]-oriented grooves to the quantum dots at the bottom of the groove. We utilize a rate equation model to quantitatively analyze the carrier transfer mechanism. Furthermore, we show that the defect related carrier loss mechanism, which accounts for weak PL quenching at low temperatures, is similar for QDCs and self-assembled quantum dots (SAQD) that were used as a reference. The carrier loss mechanism that causes the rapid quenching of SAQD PL at high temperatures is identified as exciton escape, while for the QDCs it is either single carrier escape or escape of uncorrelated electron–hole pairs. This result reveals a significant difference in the carrier dynamics of site-controlled QDCs and SAQDs.

We report a GaAs0.96Bi0.04/GaAs multiple quantum well (MQW) light emitting diode (LED) grown by molecular beam epitaxy using a two-substrate-temperature (TST) technique. In particular, the QWs and the barriers in the intrinsic region were grown at the different temperatures of [Formula: see text] = 350 °C and [Formula: see text] respectively. Investigations of the microstructure using transmission electron microscopy (TEM) reveal homogeneous MQWs free of extended defects. Furthermore, the local determination of the Bi distribution profile across the MQWs region using TEM techniques confirm the uniform Bi distribution, while revealing a slightly chemically graded GaAs-on-GaAsBi interface due to Bi surface segregation. Despite this small broadening, we found that Bi segregation is significantly reduced (up to 18% reduction) compared to previous reports on Bi segregation in GaAsBi/GaAs MQWs. Hence, the TST procedure proves as a very efficient method to reduce Bi segregation and thus increase the quality of the layers and interfaces. These improvements positively reflect in the optical properties. Room temperature photoluminescence and electroluminescence (EL) at 1.23 μm emission wavelength are successfully demonstrated using TST MQWs containing less Bi content than in previous reports. Finally, LED fabricated using the present TST technique show current-voltage (I-V) curves with a forward voltage of 3.3 V at an injection current of 130 mA under 1.0 kA cm-2 current excitation. These results not only demonstrate that TST technique provides optical device quality GaAsBi/GaAs MQWs but highlight the relevance of TST-based growth techniques on the fabrication of future heterostructure devices based on dilute bismides.

In this work, we report on the spontaneous formation of ordered arrays of nanometer-sized Bi-rich structures due to lateral composition modulations in Ga(As,Bi)/GaAs quantum wells grown by molecular beam epitaxy. The overall microstructure and chemical distribution is investigated using transmission electron microscopy. The information is complemented by synchrotron x-ray grazing incidence diffraction, which provides insight into the in-plane arrangement. Due to the vertical inheritance of the lateral modulation, the Bi-rich nanostructures eventually shape into a three-dimensional assembly. Whereas the Bi-rich nanostructures are created via two-dimensional phase separation at the growing surface, our results suggest that the process is assisted by Bi segregation which is demonstrated to be strong and more complex than expected, implying both lateral and vertical (surface segregation) mass transport. As demonstrated here, the inherent thermodynamic miscibility gap of Ga(As,Bi) alloys can be exploited to create highly uniform Bi-rich units embedded in a quantum confinement structure.

A novel route based on the structural transition from amorphously deposited material to epitaxial films via thermally induced crystallization is probed for wire formation at side-walls of shallow ridges on patterned GaAs(1 1 3)A substrates. Growth is elaborated on the plane GaAs(0 0 1) and then applied to the patterned GaAs(1 1 3)A substrates. Amorphous layers of InAs and GaAs are deposited by migration-enhanced epitaxy at a growth temperature of T g =100 °C. Annealing at temperatures between 450 and 550 'C transforms these films into crystalline state. The reported technique facilitates the growth of (In,Ga)As-QWs with high In content and very low interface roughness. Despite strong non-equilibrium conditions during low-temperature deposition, efficient photoluminescence emission is obtained, which is further enhanced by post-growth rapid thermal annealing, concomitant with a controllable spectral blue-shift. The characterization of patterned GaAs(1 1 3)A overgrown with (In,Ga)As attest to the formation of wire-like structures.

We have determined the interface profiles of GaAs/Al0.25Ga0.75As and GaAs/AlAs terahertz quantum-cascade laser structures using transmission electron microscopy (TEM). The experimental composition profiles are directly extracted from the analysis of the diffracted intensity distribution of g002 dark-field TEM images. Simulated composition profiles, which have been obtained using a Fourier-transform-based model, are in remarkably good agreement with the experimental results so that the determined interface parameter can be used for designing terahertz quantum-cascade lasers. Due to the interface grading, these actual profiles reveal a significantly lower aluminum content of the Al0.25Ga0.75As and AlAs barriers than the nominal values.

A comparative study of the influence of Sb and N ion concentration on the properties of GaInNAs (GINA) quantum wells (QWs) is presented. We find that for perfect two-dimensional (2D) QW there is no direct perceptible improvement in structural quality due to the introduction of Sb. Moreover, contrast variations in the QW suggest an inhomogeneous Sb incorporation. A different behaviour of the integrated photoluminescence (PL) intensity with temperature is observed when comparing the 2D samples grown with/without Sb. Regarding the GINA QWs exhibiting a three-dimensional (3D) morphology, we observe a significant improvement in structural quality for the samples grown with added Sb, as well as for those Sb-free samples but grown under a low N- ions density. Nevertheless, 2D and 3D samples show clear common properties: the GINA:Sb QWs exhibit an improved PL efficiency, but only at high temperatures. On the contrary, the Sb-free samples grown under a low N- ions concentration exhibit a brighter PL at all temperatures considered.

We report on the structural and optical properties of GaSbBi single layers and GaSbBi/GaSb quantum well heterostructures grown by molecular beam epitaxy on GaSb substrates. Excellent crystal quality and room-temperature photoluminescence are achieved in both cases. We demonstrate laser operation from laser diodes with an active zone composed of three GaSb0.885Bi0.115/GaSb quantum wells. These devices exhibit continuous-wave lasing at 2.5 μm at 80 K, and lasing under pulsed operation at room-temperature near 2.7 μm.

Hardness of epitaxial GaAs1−xNx films on GaAs(001) with different film thicknesses, varying from 80 to 700 nm, and nitrogen compositions x between zero (pure GaAs) and 0.031, were studied by means of nano-indentation. As a result, a disproportionate and monotonic increase by 17% in hardness was proved in the dilute range from GaAs to GaAs0.969N0.031. We are tracing this observation to solid solution strengthening, an extrinsic effect based on dislocation pinning due to interstitial nitrogen. On the other hand, intrinsic effects related to different electronegativities of As and N (i.e., altered bonding conditions) could be ruled out. Furthermore, in tensilely strained GaAs1−xNx layers, the appearance of cracks acts as the main strain relieving mechanism. A correlation between cracking and hardness reduction is investigated and discussed as a further relaxation pathway.

The emission energies and their intensity distributions of excitonic radiative recombination in a non-uniform GaAs-based quantum well (QW) system are investigated by spatially resolved cathodoluminescence (CL) spectroscopy. By measuring the spectrally discriminated CL intensities originating from the different QWs as a function of excitation position, we are able to map out how the compositional distribution of the alloy barriers affects the CL intensities of the respective QW exciton bands. Surprisingly intense high-energy emission is observed due to the presence of an unintentionally introduced interface layer formed in the barrier heterostructure, when it is in resonance with the excited subband transition of a neighboring QW.

We used spatially resolved photoluminescence (PL) and resonant Raman spectroscopy to study the electronic structure of single GaAs nanowires (NWs) consisting of zinc-blende (ZB) and wurtzite (WZ) segments. For narrow ZB segments and stacking faults the energy range of the observed PL peak positions is found to deviate from that of the maxima in resonance Raman profiles. These different energy ranges reflect the fact that the PL recombination is dominated by spatially indirect transitions whereas the resonance enhancement of Raman scattering is caused by direct transitions. Our results provide evidence for the type II band alignment between ZB and WZ GaAs and a coherent picture of all near-band-gap transition energies in GaAs NWs.

InAs/InAs1−xSbx type II superlattices designed for mid-wavelength infrared photo-detection have been studied using several electron microscopy methods, with specific attention directed towards interface chemical diffusion caused by Sb segregation. Reciprocal-space image analysis using the geometric phase method showed asymmetric interfacial strain profiles at the InAs-on-InAsSb interface. Measurement of local Sb compositional profiles across the superlattices using electron energy-loss spectroscopy and 002 dark-field imaging confirmed asymmetric Sb distribution, with the InAs-on-InAsSb interface being chemically graded. In contrast, the InAsSb-on-InAs interface showed a small intrinsic interface width. Careful evaluation of the experimental Sb composition profiles using a combined segregation and sigmoidal model reached quantitative agreement. Segregation dominated over the sigmoidal growth at the InAs-on-InAsSb interface, and the segregation probability of 0.81 ± 0.01 obtained from the two microscopy tec...

Near-infrared detection is reported for a double-barrier quantum-well infrared photodetector based on a 30-A GaAs1−yNy (y≈0.01) quantum well. The growth procedure using plasma-assisted molecular-beam epitaxy is described. The as-grown sample exhibits a detection wavelength of 1.64 μm at 25 K. The detection peak strengthens and redshifts to 1.67 μm following rapid thermal annealing at 850 °C for 30 s. The detection peak position is consistent with the calculated band structure based on the band-anticrossing model for nitrogen incorporation into GaAs.

We experimentally demonstrate a sigmoidal variation of the composition profile across semiconductor heterointerfaces. The wide range of material systems (III-arsenides, III-antimonides, III-V quaternary compounds, III-nitrides) exhibiting such a profile suggests a universal behavior. We show that sigmoidal profiles emerge from a simple model of cooperative growth mediated by two-dimensional island formation, wherein cooperative effects are described by a specific functional dependence of the sticking coefficient on the surface coverage. Experimental results confirm that, except in the very early stages, island growth prevails over nucleation as the mechanism governing the interface development and ultimately determines the sigmoidal shape of the chemical profile in these two-dimensional grown layers. In agreement with our experimental findings, the model also predicts a minimum value of the interfacial width, with the minimum attainable value depending on the chemical identity of the species.

The influence of the substrate temperature, III/V flux ratio, and mask geometry on the selective area growth of GaN nanocolumns is investigated. For a given set of growth conditions, the mask design (diameter and pitch of the nanoholes) is found to be crucial to achieve selective growth within the nanoholes. The local III/V flux ratio within these nanoholes is a key factor that can be tuned, either by modifying the growth conditions or the mask geometry. On the other hand, some specific growth conditions may lead to selective growth but not be suitable for subsequent vertical growth. With optimized conditions, ordered GaN nanocolumns can be grown with a wide variety of diameters. In this work, ordered GaN nanocolumns with diameter as small as 50 nm are shown.

This work reports on the growth by molecular beam epitaxy and characterization of InN/InGaN multiple quantum wells (MQWs) emitting at 1.5 μm. X-ray diffraction (XRD) spectra show satellite peaks up to the second order. Estimated values of well (3 nm) and barrier (9 nm) thicknesses were derived from transmission electron microscopy and the fit between experimental data and simulated XRD spectra. Transmission electron microscopy and XRD simulations also confirmed that the InGaN barriers are relaxed with respect to the GaN template, while the InN MQWs grew under biaxial compression on the InGaN barriers. Low temperature (14 K) photoluminescence measurements reveal an emission from the InN MQWs at 1.5 μm. Measurements as a function of temperature indicate the existence of localized states, probably due to InN quantum wells’ thickness fluctuations as observed by transmission electron microscopy.

Using spatially resolved cathodoluminescence spectroscopy, we investigate the spatial luminescence distribution in a fully strained (In,Ga)N layer, in particular, its correlation with the distribution of threading dislocations (TDs). Regarding the impact of TDs on the luminescence properties, we can clearly distinguish between pure edge-type TDs and TDs with screw component. At the positions of both types of TDs, we establish nonradiative recombination sinks. The radius for carrier capture is at least four times larger for TDs with screw component as for pure edge-type TDs. The large capture radius of the former is due to a spiral-like growth mode resulting in an increase in the In content in the center of the spiral domains in comparison to their periphery.

International audience; The unique properties of the noncommon-atom InAs/GaSb short-period-superlattices (SPSL) strongly depend on the interface structure. These interfaces are characterized using transmission electron microscopy (TEM). The compositional sharpness is obtained from the comparison of the experimental contrast in g002 two-beam dark-field TEM images with simulated intensity profiles, which are calculated assuming that the element distribution profiles are described by sigmoidal functions. The interfacial intermixing, defined by the chemical width, is obtained for SPSL with different periods and layer thicknesses, even in the extreme case of nominally less than 3 ML thick InAs layers. Nominal 1 ML InSb layers intentionally inserted are also identified.

Indium incorporation into wurtzite (0001)-oriented InxAlyGa1−x−yN layers grown by plasma-assisted molecular beam epitaxy was studied as a function of the growth temperature (565–635 °C) and the AlN mole fraction (0.01

Transmission electron microscopy (TEM) techniques are applied to characterize the interfaces of epitaxial III-V semiconductor heterostructures with high spatial resolution and to analyze compositional variations at interfaces. As expected, realistic interfaces of compound semiconductors are not chemically sharp but there is a transition region at the interface. The functional dependence of the smooth change in composition is sigmoidal and can be described using an analytical expression, thus enabling a quantitative characterization of the interface width. The model gives a very good description of the distribution profiles and applies to several material systems, including the interfaces of As-based alloys and those of the non-common-atom InAs/GaSb short-period superlattices. The analysis of (Ga,In)(N,As)/GaAs quantum wells reveals that there is a connection between the interface properties in this material system and the miscibility gap of the alloy. (C) 2008 Elsevier B.V. All rights reserved.

Raman measurements in high quality InN nanocolumns display a coupled LO phonon-plasmon mode together with uncoupled phonons. The coupled mode is attributed to the spontaneous accumulation of electrons on the lateral surfaces of the nanocolumns. For increasing growth temperature, the electron density decreases as the growth rate increases. The present results indicate that electron accumulation layers do not only form on polar surfaces of InN but also occur on nonpolar ones. According to recent calculations, we attribute the electron surface accumulation to the temperature dependent In-rich surface reconstruction on the nanocolumn sidewalls.

The ability to characterize a structure into the finest details in a quantitative manner is a key issue to understanding and controlling nanoscale phase separation in novel nanomaterials. In this work, we consider the detectability of lateral composition modulation (LCM), a type of nanoscale phase separation in GaAs(1-x)Bix epilayers, by x-ray diffraction (XRD). We show that the satellite peaks due to LCM are hardly detectable in reasonable time with a lab x-ray diffractometer for GaAs(1-x)Bix samples with an average x up to 25% and relative modulation up to 50%. This is in contrast to LCM reported in other III-V combinations, where the intensity of the satellite peak is relatively high and can be easily detected. Our theoretical considerations are complemented experimentally using highly brilliant synchrotron radiation. The results are in good agreement with the predictions. This work provides a guideline for the systematic characterization of LCM in zincblende III-V semiconductor epilayers and points to the critical role of quantitative characterization of nanoscale phase separation.

Tellurium (Te)-doping of self-catalyzed GaAs nanowires (NWs) grown by molecular beam epitaxy is reported. The effect of Te-doping on the morphological and crystal structure of the NWs is investigated by scanning electron microscopy and high-resolution transmission electron microscopy. The study reveals that the lateral growth rate increases and axial growth rate decreases with increasing Te doping level. The changes in the NW morphology can be reverted to some extent by changing the growth temperature. At high doping levels, formation of twinning superlattice is observed alongside with the {111}-facetted sidewalls. Finally, the incorporation of Te is confirmed by Raman spectroscopy.

In this work we show dilute nitride (InGaAsN and GaAsN) based laser diodes and detectors grown by Molecular Beam Epitaxy as good candidates to be used in optical fiber sensors applications. The maturity of GaAs technology allow us to develop laser devices less expensive and complex than the present InP based diodes which exhibit limited performances. Laser emission up to 1.23 μm is achieved for these devices. In addition, a new generation of (In)GaAsN quantum well intersubband detectors is also presented. This structures can be tailored to operate in a very short interval of wavelengths (namely 0.4 to 1 μm) centered in the range between 1.3 and 2 μm with a responsivity around 3 mA/W. The excellent selectivity of these detectors make them suitable to be matched with the emission wavelength of the source, thus avoiding the interference of external light sources. Both devices can be tuned to work in the range of interest for optical fibers, giving rise to a number of potential applications including Er-doped optical amplifiers, and optical fiber sensors.

We report the observation of atomic ordering of triple-period (TP)-A and -B type in low temperature (LT) grown GaAsBi alloy using transmission electron microscopy (TEM). In addition to previous reports, where only TP-A ordering was identified in III-V alloys, here, we confirm by electron diffraction, high-resolution (HR) TEM, and HR Z-contrast scanning TEM that two ordering variants coexists for LT-GaAsBi. We find that the TP-A ordering variant dominates over the TP-B variant. TP-A domains extend over 50–100 nm (projected lateral width) and are of higher perfection compared to TP-B domains. HR Z-contrast scanning TEM on different domains reveals a variation in the Bi occupancy in the {111} planes with triple period sequence. Since the formation of ordered phases has been directly linked to the occurrence of specific surface reconstructions, our results suggest a correlation between the TP-A and B type domains and the multiple stability of n × 3 and 3 × n reconstructions on the (001) surface of GaAsBi under low temperature growth.

An efficient model is proposed to evaluate the impact of interface grading on the properties of semiconductor heterostructures. In the plane-wave approximation, the interface grading is taken into account by simply multiplying the Fourier components of the potential by a Gaussian function, which results only in a very small increase of the computation time. We show that the interface grading may affect the transition energies, the field strength for resonant coupling of subbands, and even the miniband formation in complex systems such as quantum-cascade lasers. This model provides a convenient tool for the incorporation of interface grading into the design of heterostructures.

We report the formation and phase transformation of Bi-containing clusters in GaAs(1-x)Bi(x) epilayers upon annealing. The GaAs(1-x)Bi(x) layers were grown by molecular beam epitaxy under low (220 °C) and high (315 °C) temperatures and subsequently annealed using different temperatures and annealing times. Bi-containing clusters were identified only in the annealed samples that were grown at low temperature, revealing a relatively homogeneous size distribution. Depending on the annealing temperature and duration, the clusters show different sizes ranging from 5 to 20 nm, as well as different crystallographic phase, being coherently strained zincblende GaAs(1-x)Bi(x) (zb Bi-rich Ga(As, Bi)) clusters or rhombohedral pure Bi (rh-Bi) clusters. We found that: (1) the formation of the zb Bi-rich Ga(As, Bi) clusters is driven by the intrinsic tendency of the alloy to phase separately and is mediated by the native point defects present in the low temperature grown epilayers; (2) the phase transformation from zb Bi-rich Ga(As, Bi) to rh-Bi nucleates in zincblende {111} planes and grows until total consumption of Bi in the GaAs matrix. We propose a model accounting for the formation and phase transformation of Bi-containing clusters in this system. Furthermore, our study reveals the possibility to realize self-organized zb Bi-rich Ga(As, Bi) clusters that can exhibit QD-like features.