The accurate control of the crystal phase in III-V semiconductor nanowires (NWs) is an important milestone for device applications. In this work, we present a method to select and maintain the wurtzite (WZ) crystal phase in self-assisted NWs. By choosing a specific regime where the NW growth process is a self-regulated system, the main experimental parameter to select the zinc-blende (ZB) or WZ phase is the V/III flux ratio. The latter can be monitored by changing the As flux, and drives the system toward a stationary regime when the wetting angle of the Ga droplet falls in a target interval, typically in the 90° - 125° range for the WZ phase growth. The analysis of the in situ RHEED evolution, high-resolution scanning transmission electron microscopy (HRSTEM), dark field transmission electron microscopy (DF-TEM), and photoluminescence (PL) data all confirm the control of an extended few micrometers long pure WZ segment obtained by MBE growth of self-assisted GaAs NWs with a V/III flux ratio of 4.0.
Phase-Controlled Epitaxy and Anisotropic Antiferromagnetism of Polar Wurtzite MnTe
Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）；Centre of Excellence ENSEMBLE3 Sp. z o.o.（ENSEMBLE3卓越中心有限公司）；International Research Centre Magtop, Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所磁顶国际研究中心）；Center for Science and Innovation in Spintronics, Tohoku University（东北大学自旋电子学科学与创新中心）；Laboratory for Nanoelectronics and Spintronics, Research Institute of Electrical Communication, Tohoku University（东北大学电气通信研究所纳米电子与自旋电子学实验室）
Nearly 30% increase of the ferromagnetic phase transition temperature has been achieved in strained MnAs nanocrystals embedded in a wurtzite GaAs matrix. Wurtzite GaAs exerts tensile stress on hexagonal MnAs nanocrystals, preventing a hexagonal to orthorhombic structural phase transition, which in the bulk MnAs is combined with the magnetic one. This effect results in a remarkable shift of the magneto-structural phase transition temperature from 313 K in the bulk MnAs to above 400 K in the tensely strained MnAs nanocrystals. This finding is corroborated by the state of the art transmission ele…
Moire based strain analysis in wurtzite GaAs -- rock-salt (Pb,Sn)Te core-shell nanowires grown by molecular beam epitaxy
Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）；Faculty of Physics, University of Warsaw（华沙大学物理学院）；Ensemble3 Centre of Excellence（Ensemble3卓越中心）；International Research Center MagTop, Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所国际研究中心MagTop）
Structural and magnetic properties of (In,Ga)As-(Ga,Mn)As core-shell nanowires grown by molecular beam epitaxy on GaAs(111)B substrate with gold catalyst have been investigated.(In,Ga)As core nanowires were grown at high temperature (500 °C) whereas (Ga,Mn)As shells were deposited on the {1-100} side facets of the cores at much lower temperature (220 °C). High resolution transmission electron microscopy images and high spectral resolution Raman scattering data show that both the cores and the shells of the nanowires have wurtzite crystalline structure. Scanning and transmission electron micros…
Electronic structures of wurtzite GaAs nanowires in the [0001] direction were studied using first-principles calculations. It was found that the band gap of GaAs nanowires experience a direct-to-indirect transition when the diameter of the nanowires is smaller than ~28 Å. For those thin GaAs nanowires with an indirect band gap, it was found that the gap can be tuned to be direct if a moderate external uniaxial strain is applied. Both tensile and compressive strain can trigger the indirect-to-direct gap transition. The critical strains for the gap-transition are determined by the energy crossov…
Metastable wurtzite crystal phases of semiconductors comprise enormous potential for high-performance electro-optical devices, owed to their extended tunable direct band gap range. However, synthesizing these materials in good quality and beyond nanowire size constraints has remained elusive. In this work, the epitaxy of wurtzite InP microdisks and related geometries on insulator for optical applications is explored. This is achieved by an elaborate combination of selective area growth of fins and a zipper-induced epitaxial lateral overgrowth, which enables co-integration of diversely shaped c…
We studied and optimized the molecular beam epitaxy of GaSb layers on vicinal (001) Si substrates using a GaAs nucleation layer. An in-depth analysis of the different growth stages under optimized conditions revealed the formation of a high density of small GaAs islands forming a quasi-two-dimensional layer. GaSb then nucleated atop this layer as three-dimensional islands before turning to two-dimensional growth within a few nanometers. Moreover, reflexion high-energy electron diffraction revealed a fast relaxation of GaAs on Si and of GaSb on GaAs. The GaSb layer quality was better than that …
In this paper some specific issues related to point defects in GaAs nanowires are addressed with the help of density functional theory calculations. These issues mainly arise from the growth of nanowires under conditions different from those used for thin films or bulk GaAs, such as the co-existence of zincblende and wurtzite polytypes, the use of gold particles as catalyst, and the arsenic-limited growth regime. Hence, we carry out density-functional calculations for As vacancies, Ga_As antisites, and Au impurities in ZB and WZ GaAs crystals. Our results show that As vacancies can diffuse wit…
Comprehensive investigations on ZnSe/GaAs and GaAs/ZnSe interfaces were carried out by photoluminescence (PL) and transmission electron microscopy (TEM), as a part of realizing high quality ZnSe-GaAs (100) hetero-valent structures (HS). The nature of ZnSe/GaAs interface under different surface terminations of GaAs was examined. The ZnSe/Ga-terminated GaAs was found to have a superior optical and microstructural quality, with a chemical interface consisting of a mixture of both the GaAs and ZnSe atomic constituents. For GaAs/ZnSe interface studies, a low-temperature migration enhanced epitaxy (…
The structural and optical properties of 3 different kinds of GaAs nanowires with 100% zinc-blende structure and with an average of 30% and 70% wurtzite are presented. A variety of shorter and longer segments of zinc-blende or wurtzite crystal phases are observed by transmission electron microscopy in the nanowires. Sharp photoluminescence lines are observed with emission energies tuned from 1.515 eV down to 1.43 eV when the percentage of wurtzite is increased. The downward shift of the emission peaks can be understood by carrier confinement at the interfaces, in quantum wells and in random sh…
Self-organized pattern formation by the process of reverse epitaxial growth has been investigated on GaAs (001) surfaces during 1 keV Ar+ bombardment at target temperature of 450 degC for a wide range of incident angles. Highly ordered ripple formation driven by diffusion instability is evidenced at near normal incidence angles. Concurrent sample rotation shows that the ripple morphology and its orientation do not depend on the incident beam direction; rather they are determined by the symmetry of the crystal face.
GaAs nanowires (NWs) grown by molecular-beam epitaxy may contain segments of both the zincblende (ZB) and wurtzite (WZ) phases. Depending on the growth conditions, we find that optical emission of such NWs occurs either predominantly above or below the band gap energy of ZB GaAs [E(g,ZB)]. This result is consistent with the assumption that the band gap energy of wurtzite GaAs [E(g,WZ)] is larger than E(g,ZB) and that GaAs NWs with alternating ZB and WZ segments along the wire axis establish a type II band alignment, where electrons captured within the ZB segments recombine with holes of the ne…
InGaAs/GaAsBi/InGaAs quantum wells (QWs) were grown on GaAs substrates by gas source molecular beam epitaxy for realizing the type II band-edge line-up. Both type I and type II transitions were observed in the Bi containing W QWs and the photoluminescence intensity was enhanced in the sample with a high Bi content, which is mainly due to the improvement of carrier confinement. Blue-shift of type II transitions at high excitation power density was observed and ascribed to the band-bending effect. The calculated transition energies based on 8 band k.p model fit well with the experiment results. …
Incorporation of Bi into GaAs-(Ga,Al)As-Ga(As,Bi) core-shell nanowires grown by molecular beam epitaxy is studied with transmission electron microscopy. Nanowires are grown on GaAs(111)B substrates with Au-droplet assisted mode. Bi-doped shells are grown at low temperature (300 °C) with a close to stoichiometric Ga/As flux ratio. At low Bi fluxes, the Ga(As,Bi) shells are smooth, with Bi completely incorporated into the shells. Higher Bi fluxes (Bi/As flux ratio ~ 4%) led to partial segregation of Bi as droplets on the nanowires sidewalls, preferentially located at the nanowire segments with w…
The addition of boron to GaAs nanowires grown by self-catalyzed molecular beam epitaxy was found to have a strong effect on the nanowire morphology, with axial growth greatly reduced as the nominal boron concentration was increased. Transmission electron microscopy measurements show that the Ga catalyst droplet was unintentionally consumed during growth. Concurrent radial growth, a rough surface morphology and tapering of nanowires grown under boron flux suggest that this droplet consumption is due to reduced Ga adatom diffusion on the nanowire sidewalls in the presence of boron. Modelling of …
We demonstrate nearly-spherical, strain-free, self-assembled Ge quantum dots (QDs) fully encapsulated by AlAs, grown on (100) GaAs by molecular beam epitaxy (MBE). The QDs were formed without a wetting layer using a high temperature, in-situ anneal. Subsequent AlAs overgrowth was free from threading dislocations and anti-phase domains. The straddling band alignment for Ge in AlAs promises strong and tunable confinement for both electrons and holes. The reflection high-energy electron diffraction (RHEED) pattern changed from 2x3 to 2x5 with anneal, which can be explained by surface reconstructi…
Mn-doped GaAs nanowires were grown in the self-catalytic growth mode on oxidized Si(100) surface by molecular beam epitaxy and characterized by scanning and transmission electron microscopy, Raman scattering, photoluminescence, cathodoluminescence, and electron transport measurements. The transmission electron microscopy studies evidenced the substantial accumulation of Mn inside the catalyzing Ga droplets at the top of the nanowires. Optical and transport measurements revealed that the limit of Mn content for self-catalysed growth of GaAs nanowires corresponds to the doping level, i.e., is mu…
Thin crystalline layers of TaAs Weyl semimetal (9 and 18 nm thick) are grown by molecular beam epitaxy on GaAs(001) substrates. The (001) planes of the tetragonal TaAs lattice are parallel to the GaAs(001) substrate, but the corresponding in-plane crystallographic directions of the substrate and the layer are rotated by 45°. In spite of a substantial lattice mismatch (about 19%) between GaAs(001) substrate and TaAs epilayer no misfit dislocations are observed at the GaAs(001)/TaAs(001) interface. Only stacking fault defects in TaAs are detected with transmission electron microscopy. Thorough X…
The lattice mismatch between interesting 2D materials and commonly available 3D substrates is one of the obstacles in the epitaxial growth of monolithic 2D/3D heterostructures, but a number of 2D materials have not yet been considered for epitaxy. Here we present the first molecular beam epitaxy growth of NiTe$_{2}$ 2D transition metal dichalcogenide. Importantly, the growth is realized on a nearly lattice matched GaAs(111)B substrate. Structural properties of the grown layers are investigated by electron diffraction, X-ray diffraction, and scanning tunnelling microscopy. Surface coverage and …
Using ab initio methods based on the density functional theory, we investigate the segregation and formation energies for various dopants (Si, Be, Zn, Sn), commonly used to obtain p- or ntype conductivity in GaAs and InAs nanowires. The distribution of Au and O atoms, which may be unintentionally incorporated during the wire growth, is also studied. The calculations performed for nanowires of zinc blende and wurtzite structure show that the distribution of most of the impurities depends on the crystal structure of the wires. For example, it is shown that the same growth conditions can lead to …
Hexagonal group IV materials like silicon and germanium are expected to display remarkable optoelectronic properties for future development of photonic technologies. However, the fabrication of hexagonal group IV semiconductors within the vapour-liquid-solid method has been obtained using gold as a catalyst thus far. In this letter, we show the synthesis of hexagonal Ge on self-assisted GaAs nanowires using molecular beam epitaxy. With an accurate tuning of the Ga and As molecular beam flux we selected the crystal phase, cubic or hexagonal, of the GaAs NWs during the growth. A 500 nm-long hexa…
Polarization dependent Raman scattering experiments realized on single GaAs nanowires with different percentages of zinc-blende and wurtzite structure are presented. The selection rules for the special case of nanowires are found and discussed. In the case of zinc-blende, the transversal optical mode E1(TO) at 267 cm-1 exhibits the highest intensity when the incident and analyzed polarization are parallel to the nanowire axis. This is a consequence of the nanowire geometry and dielectric mismatch with the environment, and in quite good agreement with the Raman selection rules. We also find a c…
(Ga,Mn)As in wurtzite crystal structure, is coherently grown by molecular beam epitaxy on the {1100} side facets of wurtizte (Ga,In)As nanowires and further encapsulated by (Ga,Al)As and low temperature GaAs. For the first time a true long-range ferromagnetic magnetic order is observed in non-planar (Ga,Mn)As, which is attributed to a more effective hole confinement in the shell containing Mn by a proper selection/choice of both the core and outer shell materials.
Self-selective growth of GaAs1-xBix on GaAs zinc blende/wurtzite nanowire heterostructures
Lund University（隆德大学）；NanoLund, Lund University（隆德大学纳米隆德）；Centre for Analysis and Synthesis, Lund University（隆德大学分析与合成中心）；MAX IV Laboratory, Lund University（隆德大学MAX IV实验室）；Niels Bohr Institute, University of Copenhagen（哥本哈根大学尼尔斯玻尔研究所）
We demonstrate selective area epitaxy of GaAs films using patterned graphene masks on a Ge (001) substrate. The GaAs selectively grows on exposed regions of the Ge substrate, for graphene spacings as large as 10 microns. The selectivity is highly dependent on the growth temperature and annealing time, which we explain in terms of temperature dependent sticking coefficients and surface diffusion. The high nucleation selectivity over several microns sets constraints on experimental realizations of remote epitaxy.
We employ first-principles techniques tailored to properly describe semiconductors (modified Becke-Johnson potential added to the exchange-correlation functional), to obtain the electronic band structures of both the zinc-blende and wurtzite phases of GaAs, GaSb, InAs, and InSb. We extract the spin-orbit fields for the relevant valence and conduction bands at zone center, by fitting the spin-splittings resulting from the lack of space inversion symmetry of these bulk crystal structures, to known functional forms---third-order polynomials. We also determine the orientations of the spin-orbit ve…
Mn doped GaAs thin films were grown using molecular beam epitaxy at high and low substrate temperatures. The elemental concentration depth profiles in the thin films were determined by using Auger electron spectroscopy combined with ion etching. The Mn concentration is higher near the surface and then decreases with depth for films grown at high substrate temperatures. The Mn concentration profile is much more uniform when films are grown using a low substrate temperature. What was unexpectedly found are high levels of oxygen in the low substrate temperature grown thin films.
We report on some surprising optical properties of diluted nitride InGaAs_(1-y)N_y /GaAs (y<<1) pyramidal site-controlled quantum dots, grown by metalorganic vapor phase epitaxy on patterned GaAs (111)B substrates. Microphotoluminescence characterizations showed antibinding exciton/ biexciton behavior, a spread of exciton lifetimes in an otherwise very uniform sample, with unexpected long neutral exciton lifetimes (up to 7 ns) and a nearly zero fine structure splitting on a majority of dots.
We investigate the full and half-shells of Pb(1-x)Sn(x)Te topological crystalline insulator deposited by molecular beam epitaxy on the sidewalls of wurtzite GaAs nanowires (NWs). Due to the distinct orientation of the IV-VI shell with respect to the III-V core the lattice mismatch along the nanowire axis is less than 4%. The Pb(1-x)Sn(x)Te solid solution is chosen due to the topological crystalline insulator properties for some critical concentrations of Sn (x >= 0.4). The IV-VI shells are grown with different compositions spanning from binary SnTe, through Pb(1-x)Sn(x)Te with decreasing x val…
An efficient electrical spin injection into an InGaAs/GaAs quantum well light emitting diode is demonstrated thanks to a CoFeB/MgO spin injector. The textured MgO tunnel barrier is fabricated by two different techniques: sputtering and molecular beam epitaxy (MBE). The maximal spin injection efficiency is comparable for both methods. Additionally, the effect of annealing is also investigated for the two types of samples. Both samples show the same trend: an increase of the electroluminescence circular polarization (Pc) with the increase of annealing temperature, followed by a saturation of Pc …
The high cost of substrates for III-V growth can be cost limiting for technologies that require large semiconductor areas. Thus, being able to separate device layers and reuse the original substrate is highly desirable, but existing techniques to lift off a film from a substrate have substantial drawbacks. This work discusses some of the complexities with the growth of a water-soluble, alkali-halide salt thin film between a III-V substrate and overlayer. Much of the difficulty stems from the growth of GaAs on an actively decomposing NaCl surface at elevated temperatures. Interestingly, the pre…
We demonstrate the epitaxial growth of EuO on GaAs by reactive molecular beam epitaxy. Thin films are grown in an adsorption-controlled regime with the aid of an MgO diffusion barrier. Despite the large lattice mismatch, it is shown that EuO grows well on MgO(001) with excellent magnetic properties. Epitaxy on GaAs is cube-on-cube and longitudinal magneto-optic Kerr effect measurements demonstrate a large Kerr rotation of 0.57°, a significant remanent magnetization, and a Curie temperature of 69 K.
We studied the size distribution and its scaling behavior of self-assembled InAlAs/AlGaAs quantum dots (QDs) grown on GaAs with the Stranski-Krastanov (SK) mode by molecular beam epitaxy (MBE), at both 480°C and 510°C, as a function of InAlAs coverage. A scaling function of the volume was found for the first time in ternary alloy QDs. The function was similar to that of InAs/GaAs QDs, which agreed with the scaling function for the two-dimensional submonolayer homoepitaxy simulation with a critical island size of i = 1. However, a character of i = 0 was also found as a tail in the large volume.
We have deposited Co films on the GaAs(001) surface by using an e-beam evaporation method. The thicknesses of the Co films are measured by using x-ray reflectivity and Rutherford backscattering. The magnetic properties of the films have been measured using superconducting quantum interference device. The magnetization of the films was found to decrease with increasing film thickness. The slight degradation of magnetic properties is attributed to increasing roughness on the Co surface or the Co/GaAs interface during the Co deposition.
Unraveling the nature of quasi van der Waals Epitaxy of magnetic topological insulators Cr: (BixSb1-x)2Te3 on a GaAs (111) substrate through coherently strained interface
We present in this work a simple Quantum Well (QW) structure consisting of GaAs wells with AlGaAs barriers as a probe for measuring the performance of arsine purifiers within a MetalOrganic Vapour Phase Epitaxy system. Comparisons between two different commercially available purifiers are based on the analysis of low temperature photoluminescence emission spectra from thick QWs, grown on GaAs substrates misoriented slightly from (100). Neutral excitons emitted from these structures show extremely narrow linewidths, comparable to those which can be obtained by Molecular Beam Epitaxy in an ultra…
While the properties of wurtzite GaAs have been extensively studied during the past decade, little is known about the influence of the crystal polytype on ternary (In,Ga)As quantum well structures. We address this question with a unique combination of correlated, spatially-resolved measurement techniques on core-shell nanowires that contain extended segments of both the zincblende and wurtzite polytypes. Cathodoluminescence hyperspectral imaging reveals a blueshift of the quantum well emission energy by $75\pm15$ meV in the wurtzite polytype segment. Nanoprobe x-ray diffraction and atom probe …
N-type doping of GaAs nanowires has proven to be difficult because the amphoteric character of silicon impurities is enhanced by the nanowire growth mechanism and growth conditions. The controllable growth of n-type GaAs nanowires with carrier density as high as 1020 electron/cm3 by self-assisted molecular beam epitaxy using Te donors is demonstrated here. Carrier density and electron mobility of highly doped nanowires are extracted through a combination of transport measurement and Kelvin probe force microscopy analysis in single-wire field-effect devices. Low-temperature photoluminescence is…
The discovery of topological insulators (TIs) and their unique electronic properties has motivated research into a variety of applications, including quantum computing. It has been proposed that TI surface states will be energetically discretized in a quantum dot nanoparticle. These discretized states could then be used as basis states for a qubit that is more resistant to decoherence. In this work, prototypical TI Bi2Se3 nanoparticles are grown on GaAs (001) using the droplet epitaxy technique, and we demonstrate the control of nanoparticle height, area, and density by changing the duration o…
We present self-assembly of InAs/InAlAs quantum dots by droplet epitaxy technique on vicinal GaAs(111)A substrates. The small miscut angle, while maintaining the symmetries imposed to the quantum dot from the surface, allows fast growth rate thanks to the presence of preferential nucleation sites at the step edges. A 100 nm InAlAs metamorphic layer with In content > 50% is already almost fully relaxed with a very flat surface. The quantum dots emit at the 1.3 μm telecom O-band with the fine structure splitting as low as 16 μeV, thus making them suitable as photon sources in quantum communicati…
We fabricated GaAs/AlGaAs quantum dots by droplet epitaxy method, and obtained the geometries of the dots from scanning transmission electron microscopy data. Post-thermal annealing is essential for the optical activation of quantum dots grown by droplet epitaxy. We investigated the emission energy shifts of the dots and underlying superlattice by post-thermal annealing with photoluminescence and cathodoluminescence measurements, and specified the emissions from the dots by selectively etching the structure down to a lower layer of quantum dots. We studied the influences of the degree of annea…
We report epitaxial growth of vanadium diselenide (VSe$_2$) thin films in the octahedrally-coordinated (1T) structure on GaAs(111)B substrates by molecular beam epitaxy. Film thickness from a single monolayer (ML) up to 30 ML is demonstrated. Structural and chemical studies using by x-ray diffraction, transmission electron microscopy, scanning tunneling microscopy and x-ray photoelectron spectroscopy indicate high quality thin films. Further studies show that monolayer VSe$_2$ films on GaAs are not air-stable and are susceptible to oxidation within a matter of hours, which indicates that a pro…
Mn concentration depth profiles in Mn-doped GaAs thin films grown at substrate temperatures of 580 and 250 °C using various Mn cell temperatures have been investigated with dynamic secondary ion mass spectrometry and Auger electron spectroscopy. When the samples are grown at a low substrate temperature of 250 °C, the Mn distributes uniformly. For the samples grown at a high substrate temperature of 580 °C, the concentration depth profiles are easily fitted with a temperature-dependent Fermi function only if the Mn concentration is above the solubility limit. However, when the Mn concentration …
