Wurtzite phase control for self-assisted GaAs nanowires grown by molecular beam epitaxy.

The accurate control of the crystal phase in III-V semiconductor nanowires (NWs) is an important milestone for device applications. Although cubic zinc-blende (ZB) GaAs is a well-established material in microelectronics, the controlled growth of hexagonal wurtzite (WZ) GaAs has thus far not been achieved successfully. Specifically, the prospect of growing defect-free and gold catalyst-free wurtzite GaAs would pave the way towards integration on silicon substrate and new device applications. In this article, we present a method to select and maintain the WZ crystal phase in self-assisted NWs by molecular beam epitaxy. By choosing a specific regime where the NW growth process is a self-regulated system, the main experimental parameter to select the ZB or WZ phase is the V/III flux ratio. Using an analytical growth model, we show that the V/III flux ratio can be finely tuned by changing the As flux, thus driving the system toward a stationary regime where the wetting angle of the Ga droplet can be maintained in the range of values allowing the formation of pure WZ phase. The analysis of the in situ reflection high energy electron diffraction evolution, combined with high-resolution scanning transmission electron microscopy (TEM), dark field TEM, and photoluminescence all confirm the control of an extended pure WZ segment, more than a micrometer long, obtained by molecular beam epitaxy growth of self- assisted GaAs NWs with a V/III flux ratio of 4.0. This successful controlled growth of WZ GaAs suggests potential benefits for electronics and opto-electronics applications.

Density-controlled growth of vertical InP nanowires on Si(111) substrates.

A procedure to achieve the density-controlled growth of gold-catalyzed InP nanowires (NWs) on (111) silicon substrates using the vapor-liquid-solid method by molecular beam epitaxy is reported. We develop an effective and mask-free method based on controlling the number and the size of the Au-In catalyst droplets in addition to the conditions for the NW nucleation. We show that the NW density can be tuned with values in the range of 18 µm-2 to <0.1 µm-2 by the suitable choice of the In/Au catalyst beam equivalent pressure (BEP) ratio, by the phosphorous BEP and the growth temperature. The same degree of control is transferred to InAs/InP quantum dot-nanowires, taking advantage of the ultra-low density to study by micro-photoluminescence the optical properties of a single quantum dot-nanowires emitting in the telecom band monolithically grown on silicon. Optical spectroscopy at cryogenic temperature successfully confirmed the relevance of our method to excite single InAs quantum dots on the as-grown sample, which opens the path for large-scale applications based on single quantum dot-nanowire devices integrated on silicon. .

Crystal phase engineering of self-catalyzed GaAs nanowires using a RHEED diagram.

It is well known that the crystalline structure of the III-V nanowires (NWs) is mainly controlled by the wetting contact angle of the catalyst droplet which can be tuned by the III and V flux. In this work we present a method to control the wurtzite (WZ) or zinc-blende (ZB) structure in self-catalyzed GaAs NWs grown by molecular beam epitaxy, using in situ reflection high energy electron diffraction (RHEED) diagram analysis. Since the diffraction patterns of the ZB and WZ structures differ according to the azimuth [11̄0], it is possible to follow the evolution of the intensity of specific ZB and WZ diffraction spots during NW growth as a function of the growth parameters such as the Ga flux. By analyzing the evolution of the WZ and ZB spot intensities during NW growth with specific changes of the Ga flux, it is then possible to control the crystal structure of the NWs. ZB GaAs NWs with a controlled WZ segment have thus been realized. Using a semi-empirical model for the NW growth and our in situ RHEED measurements, the critical wetting angle of the Ga catalyst droplet for the structural transition is deduced.

Growth optimization and characterization of regular arrays of GaAs/AlGaAs core/shell nanowires for tandem solar cells on silicon.

With a band gap value of 1.7 eV, Al0.2Ga0.8As is one of the ideal III-V alloys for the development of nanowire-based Tandem Solar Cells on silicon. Nevertheless, growing self-catalysed AlGaAs nanowires on silicon by solid-source molecular beam epitaxy is a very difficult task due to the oxidation of Al adatoms by the SiO2 layer present on the surface. Here we propose a nanowire structure including a p.i.n radial junction inside an Al0.2Ga0.8As shell grown on a p-GaAs core. The crystalline structure of such self-catalysed nanowires grown on an epi-ready Si(111) substrate (with a thin native SiO2 layer) was investigated by transmission electronic microscopy and photoluminescence. I(V) measurements performed on single nanowires have shown a diode-like behaviour corresponding to the radial p.i.n junction inside the Al0.2Ga0.8As shell. Moreover, a current generation under the electron beam was evidenced over the entire radial junction along the nanowires by means of electron beam induced current (EBIC) microscopy. The same structure was reproduced on patterned substrates with a SiO2 mask, producing an ordered hexagonal array. High and uniform yields from 83% to 87% of vertical nanowires were obtained on 0.9 × 0.9 cm2 patterned areas. EBIC mapping performed on these nanowires confirmed the good electrical properties of the radial junction within the nanowires.

GaAs nanowires with oxidation-proof arsenic capping for the growth of an epitaxial shell.

We propose an arsenic-capping/decapping method, allowing the growth of an epitaxial shell around the GaAs nanowire (NW) core which is exposed to an ambient atmosphere, and without the introduction of impurities. Self-catalyzed GaAs NW arrays were firstly grown on Si(111) substrates by solid-source molecular beam epitaxy. Aiming for protecting the active surface of the GaAs NW core, the arsenic-capping/decapping method has been applied. To validate the effect of this method, different core/shell NWs have been fabricated. Analyses highlight the benefit of the As capping-decapping method for further epitaxial shell growth: an epitaxial shell with a smooth surface is achieved in the case of As-capped-decapped GaAs NWs, comparable to the in situ grown GaAs/AlGaAs NWs. This As capping method opens a way for the epitaxial growth of heterogeneous material shells such as functional oxides using different reactors.

GaAs Core/SrTiO3 Shell Nanowires Grown by Molecular Beam Epitaxy.

We have studied the growth of a SrTiO3 shell on self-catalyzed GaAs nanowires grown by vapor-liquid-solid assisted molecular beam epitaxy on Si(111) substrates. To control the growth of the SrTiO3 shell, the GaAs nanowires were protected using an arsenic capping/decapping procedure in order to prevent uncontrolled oxidation and/or contamination of the nanowire facets. Reflection high energy electron diffraction, scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy were performed to determine the structural, chemical, and morphological properties of the heterostructured nanowires. Using adapted oxide growth conditions, it is shown that most of the perovskite structure SrTiO3 shell appears to be oriented with respect to the GaAs lattice. These results are promising for achieving one-dimensional epitaxial semiconductor core/functional oxide shell nanostructures.

Excitonic properties of wurtzite InP nanowires grown on silicon substrate.

In order to investigate the optical properties of wurtzite (Wz) InP nanowires grown on Si(001) by solid source molecular beam epitaxy with the vapour-liquid-solid method, the growth temperature and V/III pressure ratio have been optimized to remove any zinc-blende insertion. These pure Wz InP nanowires have been investigated by photoluminescence (PL), time-resolved PL and PL excitation. Direct observation of the second and third valence band in Wz InP nanowires using PL spectroscopy at high excitation power have been reported and, from these measurements, a crystal field splitting of 74 meV and a spin-orbit interaction energy of 145 meV were extracted. Based on the study of temperature-dependent optical properties, we have performed an investigation of the thermal escape processes of carriers and the electron-phonon coupling strength.

Wurtzite InP/InAs/InP core-shell nanowires emitting at telecommunication wavelengths on Si substrate.

Optical properties of wurtzite InP/InAs/InP core-shell nanowires grown on silicon substrates by solid source molecular beam epitaxy are studied by means of photoluminescence and microphotoluminescence. The growth conditions were optimized to obtain purely wurtzite radial quantum wells emitting in the telecom bands with a radiative lifetime in the 5-7 ns range at 14 K. Optical studies on single nanowires reveal that the polarization is mainly parallel to the growth direction. A 20-fold reduction of the photoluminescence intensity is observed between 14 and 300 K confirming the very good quality of the nanowires.

InGaAs quantum dots grown by molecular beam epitaxy for light emission on Si substrates.

The aim of this study is to achieve homogeneous, high density and dislocation free InGaAs quantum dots grown by molecular beam epitaxy for light emission on silicon substrates. This work is part of a project which aims at overcoming the severe limitation suffered by silicon regarding its optoelectronic applications, especially efficient light emission device. For this study, one of the key points is to overcome the expected type II InGaAs/Si interface by inserting the InGaAs quantum dots inside a thin silicon quantum well in SiO2 fabricated on a SOI substrate. Confinement effects of the Si/SiO2 quantum well are expected to heighten the indirect silicon bandgap and then give rise to a type I interface with the InGaAs quantum dots. Band structure and optical properties are modeled within the tight binding approximation: direct energy bandgap is demonstrated in SiO2/Si/InAs/Si/SiO2 heterostructures for very thin Si layers and absorption coefficient is calculated. Thinned SOI substrates are successfully prepared using successive etching process resulting in a 2 nm-thick Si layer on top of silica. Another key point to get light emission from InGaAs quantum dots is to avoid any dislocations or defects in the quantum dots. We investigate the quantum dot size distribution, density and structural quality at different V/III beam equivalent pressure ratios, different growth temperatures and as a function of the amount of deposited material. This study was performed for InGaAs quantum dots grown on Si(001) substrates. The capping of InGaAs quantum dots by a silicon epilayer is performed in order to get efficient photoluminescence emission from quantum dots. Scanning transmission electronic microscopy images are used to study the structural quality of the quantum dots. Dislocation free In50Ga50As QDs are successfully obtained on a (001) silicon substrate. The analysis of QDs capped with silicon by Rutherford Backscattering Spectrometry in a channeling geometry is also presented.

Temperature dependent photoluminescence properties of InAs/InP quantum dashes subjected to low energy phosphorous ion implantation and subsequent annealing.

We report on the impact of phosphorous ion-implantation-induced band gap tuning on the temperature dependent photoluminescence (PL) properties of InAs/InP quantum dashes (QDas). The high temperature range carriers' activation energy, extracted from Arrhenius plots, is found to decrease from 238 to 42 meV when the ion implantation dose increases from 10(11) cm(-2) to 5 x 10(14) cm(-2) which is consistent with the observed emission energy blueshift increase with increasing the ion implantation doses. This effect is attributed to the As/P exchange which reduces the carrier confining potential depth. For intermediate ion implantation doses the reduced carrier confining potential barrier combined with the non-uniform intermixing process, that causes an increased QDas size dispersion, result in anomalous temperature-dependent PL properties. Indeed, the temperature induced PL emission energy redshift measured between 10 K and 300 K is found to be strongly affected by the carrier redistribution within the broadened localized QDas states.

Strain, size, and composition of InAs quantum sticks embedded in InP determined via grazing incidence x-ray anomalous diffraction.

We have used x-ray anomalous diffraction to recover the model-independent Fourier transform (x-ray structure factor) of InAs quantum sticklike islands embedded in InP. The average height of the quantum sticks, as deduced from the width of the structure factor profile, is 2.54 nm. The InAs out-of-plane deformation, relative to InP, is 6.1%. Diffraction anomalous fine structure provides evidence of pure InAs quantum sticks. Finite difference method calculations reproduce well the diffraction data, and give the strain along the growth direction. The chemical mixing at interfaces is also analyzed.