Zinc-blende GaAs Research Articles

Background-Free Near-Infrared Biphoton Emission from Single GaAs Nanowires.

The generation of photon pairs from nanoscale structures with high rates is still a challenge for the integration of quantum devices, as it suffers from parasitic signals from the substrate. In this work, we report type-0 spontaneous parametric down-conversion at 1550 nm from individual bottom-up grown zinc-blende GaAs nanowires with lengths of up to 5 μm and diameters of up to 450 nm. The nanowires were deposited on a transparent ITO substrate, and we measured a background-free coincidence rate of 0.05 Hz in a Hanbury-Brown-Twiss setup. Taking into account transmission losses, the pump fluence, and the nanowire volume, we achieved a biphoton generation of 60 GHz/Wm, which is at least 3 times higher than that of previously reported single nonlinear micro- and nanostructures. We also studied the correlations between the second-harmonic generation and the spontaneous parametric down-conversion intensities with respect to the pump polarization and in different individual nanowires.

Atomically sharp, crystal phase defined GaAs quantum dots

Crystal phase defined heterostructures, or polytype heterostructures, are atomically sharp with no intermixing, which makes them ideal contenders for a wide range of applications. Although polytype quantum dots have shown promising results as single photon sources, a high degree of control on the dimensions and the number of polytype quantum dots is necessary before any application can be developed. In this work, we show results from optical characterization of highly controlled wurtzite (wz)–zinc blende (zb) GaAs quantum dots with sharp photoluminescence signal and a strong indication of 0D density of states. One band effective mass calculations show good agreement with the measured data. Radially confined nanowires with a single wz–zb GaAs interface also show sharp photoluminescence signal and 0D density of states. This indicates the existence of quantum dot like states in triangular wells formed at the wz–zb GaAs interface. These results show the potential of polytype quantum dots for physics and optics applications.

Discrete quantum geometry and intrinsic spin Hall effect

We show that the quantum geometry of the Fermi surface can be numerically described by a 3-dimensional discrete quantum manifold. This approach not only avoids singularities in the Fermi sea, but it also enables the precise computation of the intrinsic Hall conductivity resolved in spin, as well as any other local properties of the Fermi surface. The method assures numerical accuracy when the Fermi level is arbitrarily close to singularities, and it remains robust when Kramers degeneracy is protected by symmetry. The approach is demonstrated by calculating the anomalous Hall and spin Hall conductivities of a 2-band lattice model of a Weyl semimetal and a full-band ab-initio model of zincblende GaAs.

Molecular dynamics simulation of AFM tip-based hot scratching of nanocrystalline GaAs

GaAs is a hard, brittle material and its cutting at room-temperature is rather difficult, so the work explored whether hot conditions improve its cutting performance or not. Atomic force microscope (AFM) tip-based hot machining of the (0 1 0) oriented single crystal GaAs was simulated using molecular dynamics (MD). Three representative temperatures 600 K, 900 K and 1200 K (below the melting temperature of ~1511 K) were used to cut GaAs to benchmark against the cutting performance at 300 K using indicators such as the cutting forces, kinetic coefficient of friction, cutting temperature, shear plane angle, sub-surface damage depth, shear strain in the cutting zone, and stress on the diamond tip. Hotter conditions resulted in the reduction of cutting forces by 25% however, the kinetic coefficient of friction went up by about 8%. While material removal rate was found to increase with the increase of the substrate temperature, it was accompanied by an increase of the sub-surface damage in the substrate. Simulations at 300 K showed four major types of dislocations with Burgers vector 1/2<110>, 1/6<112>, <0–11> and 1/2<1–12> underneath the cutting zone and these were found to cause ductile response in zinc-blende GaAs. Lastly, a phenomenon of chip densification was found to occur during hot cutting which referred to the fact that the amorphous cutting chips obtained from cutting at low temperature will have lower density than the chips obtained from cutting at higher temperatures.

Nanomechanical behavior of single taper-free GaAs nanowires unravelled by in-situ TEM mechanical testing and molecular dynamics simulation

Abstract Nanowire-based devices have been widely applied in optoelectronics, sensors, generators and spectroscopy. These nanowires are typically subjected to mechanical conditions during manufacture or operation. Thus, a compressive understanding of nanowire mechanical properties is increasingly required. However, only limited results have been reported owing to the challenges inherent in nanomechanical testing, particularly for quantitative tensile deformation. Herein, taper-free zinc blende GaAs nanowires with a 120 nm diameter are grown along the [111]B direction using metalorganic vapor phase epitaxy. The mechanical properties and fracture mechanisms of these single-phase GaAs nanowires are explored by in-situ uniaxial tensile deformation inside a transmission electron microscope, followed by molecular dynamics simulations. Under tensile stress, GaAs nanowires deform overally elastically until sudden brittle fracture at 3.79% strain. The fracture strength and elastic modulus are experimentally determined as 4.0 and 109.5 GPa, respectively, which are much smaller than other reported results based on compression. The tensile deformation and fracture mechanisms are further explored using molecular dynamics simulations, and the effects of different crystal structures on the GaAs nanowire mechanical behavior are discussed. These results assess the mechanical behavior of single GaAs nanowires and present critical insights into the reliable design of engineering nanodevices.

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.

Microstructural evolution in self-catalyzed GaAs nanowires during in-situ TEM study

The microstructural evolutions in self-catalyzed GaAs nanowires (NWs) were investigated by using in situ heating transmission electron microscopy (TEM). The morphological changes of the self-catalyst metal gallium (Ga) droplet, the GaAs NWs, and the atomic behavior at the interface between the self-catalyst metal gallium and GaAs NWs were carefully studied by analysis of high-resolution TEM images. The microstructural change of the Ga-droplet/GaAs-NWs started at a low temperature of ∼200 °C. Formation and destruction of atomic layers were observed at the Ga/GaAs interface and slow depletion of the Ga droplet was detected in the temperature range investigated. Above 300 °C, the evolution process dramatically changed with time: The Ga droplet depleted rapidly and fast growth of zinc-blende (ZB) GaAs structures were observed in the droplet. The Ga droplet was completely removed with time and temperature. When the temperature reached ∼600 °C, the decomposition of GaAs was detected. This process began in the wurtzite (WZ) structure and propagated to the ZB structure. The morphological and atomistic behaviors in self-catalyzed GaAs NWs were demonstrated based on thermodynamic considerations, in addition to the effect of the incident electron beam in TEM. Finally, GaAs decomposition was demonstrated in terms of congruent vaporization.

First-principle calculations of structural and optoelectronic properties of cubic CdxZn1−xSySe1−y quaternary alloys with modified Becke–Johnson (mBJ) functional

First-principle calculations in association with modified Becke–Johnson (mBJ-GGA) potentials have been performed on optoelectronic properties of CdxZn1−xSySe1−y quaternary alloys. Each semiconductor specimen within this quaternary system is a direct band gap (Γ–Γ) semiconductor. An increase in anionic (S) concentration y results in nonlinear decrease in lattice constant and increase in bulk modulus and fundamental band gap (Eg) at each cationic (Cd) concentration x. In contrast, reverse trend is observed in cationic concentration (x) dependence of each of these parameters at each anionic concentration (y). Calculated lattice constant and band gap versus concentrations (x, y) contour plots are useful in designing new quaternary alloys with targeted optoelectronic properties. An increase in calculated Eg results in decrease in each of the calculated static dielectric constant $$ \varepsilon_{1} (0) $$ , static refractive index n(0), static reflectivity R(0) and vice versa. On the other hand, an increase in calculated Eg results in the enhancement in calculated critical point energy (Ec) in each of the imaginary dielectric function $$ \varepsilon_{2} (\omega ) $$ , extinction coefficient $$ k(\omega ) $$ , optical conductivity $$ \sigma (\omega ) $$ , absorption $$ \alpha (\omega ) $$ spectra and vice versa. Calculations have also shown that zinc blende GaAs and ZnSe are suitable substrates for the growth of several CdxZn1−xSySe1−y quaternary alloys.

Lattice strain influence on conduction band nonparabolicity in GaAs and InAs: Application to intraband optical absorption in InGaAs-GaAs asymmetric step quantum wells

We use empirical sps*d5 tight-binding calculations to determine the effects of compressive biaxial lattice strain, perpendicular to the [001] crystal direction, in zinc blende GaAs and InAs. Under that approach, we have been able to compute the behavior of quantities such as the average valence band energy, the energy band gap, the conduction band effective mass, and the spin-orbit split-off energy, as functions of the biaxial strain, within a range from 0 to −7%. Expressions governing these dependencies are reported for both materials. With such information at hand it is possible to calculate the variation of the coefficient of conduction band nonparabolicity due to the presence of strain. Also, the outcome for such quantities allows to evaluate the valence band offset in GaAs/InGaAs heterointerfaces as a consequence of the strain appearing from the difference between the lattice constants of the involved materials. Taking advantage of the above mentioned results, we have performed the calculation of confined conduction band states in step-like asymmetric quantum wells of the GaAs/Inx1Ga1-x1As/Inx2Ga1-x2As/GaAs prototype, using a k→⋅p→ formalism that solves the effective mass equation arising from a bi-cuadratic (nonparabolic) dispersion law. We report the calculation of the optical absorption coefficient related with intraband transitions that involve the ground and first excited energy levels. For that purpose, the study takes into account the variation of the layer widths and compositions.

Application of k $$\cdot $$ p method on band structure of GaAs obtained through joint density-functional theory

The structural and electronic properties of zinc-blende GaAs were calculated within the framework of plane-wave density-functional theory code JDFTx by using Becke 86 in 2D and PBE exchange-correlation functionals from libXC. The standard optimized norm-conserving Vanderbilt pseudopotentials were used to calculate optimized lattice constants, band gap and spin–orbit (SO) split-off parameter. The calculated values of optimized lattice constants and direct band gap are in satisfactory agreement with other published theoretical and experimental findings. By including SO coupling, conduction bands and valence bands were studied under parabolicity to calculate effective masses. The calculated values of effective masses and SO split-off parameter are in satisfactory agreement with most recent findings. This study will be useful for more computational studies related to semiconductor spintronic devices.

Phonon thermodynamics and elastic behavior of GaAs at high temperatures and pressures

The phonons of wurtzite and zinc blende GaAs were calculated at simultaneously elevated temperature and pressure, and elastic constants were calculated as functions of pressure. Pressure caused instabilities of shorter-wavelength transverse acoustic modes in both wurtzite and zinc blende GaAs, causing them to fall to zero at 18 and 20 GPa, respectively. The Born stability criteria, which depend on elastic constants and only long wavelength phonons, therefore overestimated the pressure needed to induce instability at 0 K. At elevated temperatures, explicit anharmonicity pushes the onset of instability to higher pressures in both wurtzite and zinc blende GaAs. Phonon linewidth and densities of states data showed that the quasiharmonic approximation failed to account for temperature-induced phonon frequency shifts, and the quasiharmonic approximation became less reliable at elevated pressure. In general, the number of three-phonon processes increased with pressure, thereby increasing the temperature-driven broadening of phonon spectral lineshapes.

Calculation of Surface Properties of Cubic and Hexagonal Crystals through Molecular Statics Simulations

Surface property is an important factor that is widely considered in crystal growth and design. It is also found to play a critical role in changing the constitutive law seen in the classical elasticity theory for nanomaterials. Through molecular static simulations, this work presents the calculation of surface properties (surface energy density, surface stress and surface stiffness) of some typical cubic and hexagonal crystals: face-centered-cubic (FCC) pure metals (Cu, Ni, Pd and Ag), body-centered-cubic (BCC) pure metals (Mo and W), diamond Si, zincblende GaAs and GaN, hexagonal-close-packed (HCP) pure metals (Mg, Zr and Ti), and wurzite GaN. Sound agreements of the bulk and surface properties between this work and the literature are found. New results are first reported for the surface stiffness of BCC pure metals, surface stress and surface stiffness of HCP pure metals, Si, GaAs and GaN. Comparative studies of the surface properties are carried out to uncover trends in their behaviors. The results in this work could be helpful to the investigation of material properties and structure performances of crystals.

Improved epitaxial growth of TbAs film on III–V semiconductors

In order to achieve high epitaxial quality of rocksalt TbAs, the authors studied the molecular beam epitaxy growth of TbAs films on zincblende (001) GaAs and (001) InP:Fe wafers. Despite the opposite strain condition of TbAs on these two substrates, mixed-orientation TbAs growth was observed on both substrates. However, the nucleation time and the continuing growth of the TbAs misoriented domains were influenced by the substrate type. By suppressing the growth of misoriented domains in the TbAs film, enhanced single-crystal orientation of TbAs grown on the (001) InP:Fe substrate was observed as compared to the (001) GaAs substrate. In addition, the cube-on-cube epitaxial arrangement of (001) TbAs with a thick film of up to ∼1150 nm is maintained on the (001) InP:Fe substrate but not on the (001) GaAs substrate. The improved TbAs film growth on the InP:Fe substrate exhibited enhanced optical properties when compared to that grown on the GaAs substrate, including a threefold reduction in the scattering rate. This largely improved optical property highlights the importance of increasing the epitaxial quality of TbAs films for future optoelectronic as well as other applications.

Single-Crystalline γ-Ga2S3 Nanotubes via Epitaxial Conversion of GaAs Nanowires.

The chemical transformation of nanowire templates into nanotubes is a promising avenue toward hollow one-dimensional (1D) nanostructures. To date, high-quality single crystalline tubes of nonlayered inorganic crystals have been obtained by solid-state reactions in diffusion couples of nanowires with deposited thin film shells, but this approach presents issues in achieving single-phase tubes with a desired stoichiometry. Chemical transformations with reactants supplied from the gas- or vapor-phase can avoid these complications, allowing single-phase nanotubes to be obtained through self-termination of the reaction once the sacrificial template has been consumed. Here, we demonstrate the realization of this scenario with the transformation of zincblende GaAs nanowires into single-crystalline cubic γ-Ga2S3 nanotubes by reaction with sulfur vapor. The conversion proceeds via the formation of epitaxial GaAs-Ga2S3 core-shell structures, vacancy injection and aggregation into Kirkendall voids, elastic relaxation of the detached Ga2S3 shell, and finally complete incorporation of Ga in a crystalline chalcogenide tube. Absorption and luminescence spectroscopy on individual nanotubes show optoelectronic properties, notably a ∼3.1 eV bandgap and intense band-edge and near band-edge emission consistent with high-quality single crystals, along with transitions between gap-states due to the inherent cation-vacancy defect structure of Ga2S3. Our work establishes the transformation of nanowires via vapor-phase reactions as a viable approach for forming single-crystalline hollow 1D nanostructures with promising properties.

Crystalline GaAs Thin Film Growth on a c-Plane Sapphire Substrate

Crystalline zinc blende GaAs has been grown on a trigonal c-plane sapphire substrate by molecular beam epitaxy. The initial stage of GaAs thin film growth has been investigated extensively in this paper. When grown on c-plane sapphire, it takes (111) crystal orientation with twinning as a major problem. Direct growth of GaAs on sapphire results in three-dimensional GaAs islands, almost 50% twin volume, and a weak in-plane correlation with the substrate. Introducing a thin AlAs nucleation layer results in complete wetting of the substrate, better in-plane correlation with the substrate, and reduced twinning to 16%. Further, we investigated the effect of growth temperature, pregrowth sapphire substrate surface treatment, and in-situ annealing on the quality of the GaAs epilayer. We have been able to reduce the twin volume below 2% and an X-ray diffraction rocking curve line width to 223 arcsec. A good quality GaAs on sapphire can result in the implementation of microwave photonic functionality on a photonic chip.

Strain-Energy Release in Bent Semiconductor Nanowires Occurring by Polygonization or Nanocrack Formation.

Strain engineering of semiconductors is used to modulate carrier mobility, tune the energy bandgap, and drive growth of self-assembled nanostructures. Understanding strain-energy relaxation mechanisms including phase transformations, dislocation nucleation and migration, and fracturing is essential to both exploit this degree of freedom and avoid degradation of carrier lifetime and mobility, particularly in prestrained electronic devices and flexible electronics that undergo large changes in strain during operation. Raman spectroscopy, high-resolution transmission electron microscopy, and electron diffraction are utilized to identify strain-energy release mechanisms of bent diamond-cubic silicon (Si) and zinc-blende GaAs nanowires, which were elastically strained to >6% at room temperature and then annealed at an elevated temperature to activate relaxation mechanisms. High-temperature annealing of bent Si-nanowires leads to the nucleation, glide, and climb of dislocations, which align themselves to form grain boundaries, thereby reducing the strain energy. Herein, Si nanowires are reported to undergo polygonization, which is the formation of polygonal-shaped grains separated by grain boundaries consisting of aligned edge dislocations. Furthermore, strain is shown to drive dopant diffusion. In contrast to the behavior of Si, GaAs nanowires release strain energy by forming nanocracks in regions of tensile strain due to the weakening of As-bonds. These insights into the relaxation behavior of highly strained crystals can inform the design of nanoelectronic devices and provide guidance on mitigating degradation.

MBE-grown Zincblende MnSe1−xTex Thin Films on ZnTe

We report studies on the role of a ZnTe buffer in determining the crystalline phase of MBE-grown MnSe1−xTex alloy thin films. It was found that MBE growth of MnSe and MnTe directly onto a zincblende GaAs substrate usually result in their corresponding stable phases, which are rocksalt and hexagonal, respectively. A set of zincblende MnSe1−xTex alloy thin films with Te composition covering from 0.27 to 1 were fabricated on zincblende ZnTe buffer layers. We have addressed the lattice distortion issue due to thin film effect for these films. A combination of several structural characterizations demonstrates that a perfect lattice matched MnSe1−xTex/ZnTe heterostructure can indeed be realized. The results of this study pave the way for realizing a double-barrier MnSe1−xTex/ZnTe/MnSe1−xTex resonant tunneling diode structure with perfect lattice match as a candidate for a promising THz emitter.

Phonon thermodynamics and elastic behavior of GaN at high temperatures and pressures

The phonons of wurtzite and zinc blende GaAs were calculated at simultaneously elevated temperature and pressure, and elastic constants were calculated as functions of pressure. Pressure caused instabilities of shorter-wavelength transverse acoustic modes in both wurtzite and zinc blende GaAs, causing them to fall to zero at 18 and 20 GPa, respectively. The Born stability criteria, which depend on elastic constants and only long wavelength phonons, therefore overestimated the pressure needed to induce instability at 0 K. At elevated temperatures, explicit anharmonicity pushes the onset of instability to higher pressures in both wurtzite and zinc blende GaAs. Phonon linewidth and densities of states data showed that the quasiharmonic approximation failed to account for temperature-induced phonon frequency shifts, and the quasiharmonic approximation became less reliable at elevated pressure. In general, the number of three-phonon processes increased with pressure, thereby increasing the temperature-driven broadening of phonon spectral lineshapes.

Third harmonic generation on exciton-polaritons in bulk semiconductors subject to a magnetic field

We report on a comprehensive experimental and theoretical study of optical third harmonic generation (THG) on the exciton-polariton resonances in the zinc-blende semiconductors GaAs, CdTe, and ZnSe subject to an external magnetic field, representing a topic that had remained unexplored so far. In these crystals, crystallographic THG is allowed in the electric-dipole approximation, so that no strong magnetic-field-induced changes of the THG are expected. Therefore, it comes as a total surprise that we observe a drastic enhancement of the THG intensity by a factor of fifty for the $1s$-exciton-polariton in GaAs in magnetic fields up to 10 T. In contrast, the corresponding enhancement is moderate for CdTe and almost neglectful for ZnSe. In order to explain this strong variation, we develop a microscopic theory accounting for the optical harmonics generation on exciton-polaritons and analyze the THG mechanisms induced by the magnetic field. The calculations show that the increase of THG intensity is dominated by the magnetic field enhancement of the exciton oscillator strength which is particularly strong for GaAs in the studied range of field strengths. The much weaker increase of THG intensity in CdTe and ZnSe is explained by the considerably larger exciton binding energies, leading to a weaker modification of their oscillator strengths by the magnetic field.

Radial band bending at wurtzite–zinc-blende–GaAs interfaces

The band offset between wurtzite (wz) and zinc-blende (zb) GaAs is an important fundamental parameter in polytype heterostructure engineering. Since the interface has a type-II band alignment, it is reasonably straightforward to measure the band offset using photoluminescence (PL) e.g. on nanowires containing heterostructures between wz and zb GaAs. It has, however, been found that the transition energy in such heterostructures depends on the diameter of the nanowires which introduces uncertainties in the determined value of the band offset. In order to extract a more accurate value and to further elucidate the diameter-dependent behavior of the transition energy we have performed PL studies on a large set of GaAs nanowires. Those nanowires have different diameters and contain one wz–GaAs segment embedded in otherwise zb–GaAs. We have also studied the effect of a passivating capping layer of AlAs on the determined band offset. We find that our data is well explained by a diameter-dependent radial band bending in the nanowires. Combining modeling of the band bending with the experimental data we extract a band offset of about 125 meV and a p-type doping concentration of 1016 cm−3. Our results will improve the accuracy of future modeling of the electronic properties of wz–zb GaAs heterostructures and other engineered polytypic materials.