Electron-mediated ferromagnetism and small spin-orbit interaction in a molecular-beam-epitaxy grown n-type $GaAs/Al_{0.3}Ga_{0.7}As$ heterostructure with Mn $δ$-doping
A. Bove, F. Altomare, N. B. Kundtz, Albert M. Chang, Y. J. Cho, X. Liu, J. Furdyna
备注：
4 pages with 4 figures, to be submitted to Physical Review Letters, revised version changed some content
We report the first evidence of electron-mediated ferromagnetism in a molecular-beam-epitaxy (MBE) grown $GaAs/Al_{0.3}Ga_{0.7}As$ heterostructure with Mn $δ$-doping. The interaction between the magnetic dopants (Mn) and the Two-Dimensional Electron Gas (2DEG) realizes magnetic ordering when the temperature is below the Curie temperature ($T_{C} \sim 1.7K$) and the 2DEG is brought in close proximity to the Mn layer by gating. The Anomalous Hall Effect (AHE) contribution to the total Hall resistance is shown to be about three to four orders of magnitude smaller than in the case of hole-mediated ferromagnetism indicating the presence of small spin-orbit interaction.
GaMnAs/GaAs films were grown via molecular beam epitaxy using both low and high substrate temperatures. The films were investigated using Hall effect and photoluminescence (PL) measurements from 8 to 300 K. The carrier concentrations in the samples grown at a low substrate temperature are greater than those in the samples grown at a high substrate temperature. The PL spectra show a GaAs exciton peak, a peak involving a carbon acceptor, a substitutional Mn acceptor-related peak and an optical phonon-related peak.
We introduce a high-temperature droplet epitaxy procedure, based on the control of the arsenization dynamics of nanoscale droplets of liquid Ga on GaAs(111)A surfaces. The use of high temperatures for the self-assembly of droplet epitaxy quantum dots solves major issues related to material defects, introduced during the droplet epitaxy fabrication process, which limited its use for single and entangled photon sources for quantum photonics applications. We identify the region in the parameter space which allows quantum dots to self-assemble with the desired emission wavelength and highly symmet…
GaAs nanowires are grown by molecular beam epitaxy using a self-catalyzed, Ga-assisted growth technique. Position control is achieved by nano-patterning a SiO2 layer with arrays of holes with a hole diameter of 85 nm and a hole pitch varying between 200 nm and 2 \mum. Gallium droplets form preferentially at the etched holes acting as catalyst for the nanowire growth. The nanowires have hexagonal cross-sections with {110} side facets and crystallize predominantly in zincblende. The interdistance dependence of the nanowire growth rate indicates a change of the III/V ratio towards As-rich conditi…
Among very low disorder systems of condensed matter, the high mobility two-dimensional electron gas confined in gallium arsenide/aluminum gallium arsenide heterostructures holds a privileged position as platform for the discovery of new electronic states driven by strong Coulomb interactions. Molecular beam epitaxy (MBE), an ultra-high vacuum thin-film deposition technique, produces the highest quality 2DEGs and has played a central role in a number of discoveries that have at their root the interplay of reduced dimensionality, strong electron-electron interactions, and disorder. This review a…
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 the growth and characterization of a new Diluted Magnetic Semiconductor (DMS) heterostructure that presents a Two-Dimensional Electron Gas (2DEG) with a carrier density $n \sim 1.08 \times 10^{12} cm^{-2}$ and a mobility $μ\sim 600 cm^{2} / (Vs)$ at T $\sim$ 4.2K. As far as we know this is the highest mobility value reported in the literature for GaMnAs systems. A novel technique was developed to make Ohmic contact to the buried 2DEG without destroying the magnetic properties of our crystal.
We report optical orientation experiments in individual, strain free GaAs quantum dots in AlGaAs grown by droplet epitaxy. Circularly polarized optical excitation yields strong circular polarization of the resulting photoluminescence at 4K. Optical injection of spin polarized electrons into a dot gives rise to dynamical nuclear polarization that considerably changes the exciton Zeeman splitting (Overhauser shift). We show that the created nuclear polarization is bistable and present a direct measurement of the build-up time of the nuclear polarization in a single GaAs dot in the order of one s…
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.
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 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 …
Two-dimensional materials (2D) arranged in hybrid van der Waals (vdW) heterostructures provide a route toward the assembly of 2D and conventional III-V semiconductors. Here, we report the structural and electronic properties of single layer WSe2 grown by molecular beam epitaxy on Se-terminated GaAs(111)B. Reflection high-energy electron diffraction images exhibit sharp streaky features indicative of a high-quality WSe2 layer produced via vdW epitaxy. This is confirmed by in-plane x-ray diffraction. The single layer of WSe2 and the absence of interdiffusion at the interface are confirmed by hig…
We investigate the optical emission and decay dynamics of excitons confined in large strain-free GaAs quantum dots grown by droplet epitaxy. From time-resolved measurements combined with a theoretical model we show that droplet-epitaxy quantum dots have a quantum efficiency of about 75% and an oscillator strength between 8 and 10. The quantum dots are found to be fully described by a model for strongly-confined excitons, in contrast to the theoretical prediction that excitons in large quantum dots exhibit the so-called giant oscillator strength. We attribute these findings to localized ground-…
Molecular beam epitaxy is employed to manufacture self-assembled InAs/GaAs quantum dot Schottky resonant tunneling diodes. By virtue of a thin AlAs insertion barrier, the thermal current is effectively reduced and electron resonant tunneling through quantum dots under both forward and reverse biased conditions is observed at relatively high temperature of 77K. The ground states of quantum dots are found to be at ~0.19eV below the conduction band of GaAs matrix. The theoretical computations are in conformity with experimental data.
We present an extensive density functional theory study of the electronic, magnetic and transport properties of GaAs and AlAs digital ferromagnetic heterostructures. These can be obtained by $δ$-doping with Mn the GaAs layers of a GaAs/AlAs superlattice. Our analysis spans a range of Mn concentrations and considers the presence of compensating defects such as As antisites. In the defect-free case all the heterostructures studied present an half-metallic electronic structure. In contrast when As antisites are present the half-metallic state is destroyed and the heterostructures behave as dirty …
We present measurements of low frequency charge noise and conductance drift in modulation doped GaAs/AlGaAs heterostructures grown by molecular beam epitaxy in which the silicon doping density has been varied from $2.4\times 10^{18} cm^{-3}$ (critically doped) to $6.0\times 10^{18} cm^{-3}$ (overdoped). Quantum point contacts were used to detect charge fluctuations. A clear reduction of both short time scale telegraphic noise and long time scale conductance drift with decreased doping density was observed. These measurements indicate that the {\it neutral} doping region plays a significant rol…
Magneto-photoluminescence measurements of individual zinc-blende GaAs/AlAs core/shell nanowires are reported. At low temperature a strong emission line at 1.507 eV is observed under low power (nW) excitation. Measurements performed in high magnetic field allowed us to detect in this emission several lines associated with excitons bound to defect pairs. Such lines were observed before in epitaxial GaAs of very high quality, as reported by Kunzel and Ploog. This demonstrates that the optical quality of our GaAs/AlAs core/shell nanowires is comparable to the best GaAs layers grown by molecular be…
We report the successful synthesis of ZnO:Cu thin films doped with holes, resulting in room temperature ferromagnetism. Hole doping is achieved by As-diffusion from the GaAs substrate into ZnO films, assisted by thermal annealing. The As-diffusion is probed with the help of x-ray absorption spectra collected at the As K-edge which show enhanced signature of diffusion in the annealed samples. Introduction of holes, due to the As doping, in ZnO films is further evidenced by the Cu L3,2-edge spectra. XMCD and magnetic measurements show that the ferromagnetic interaction between doped Cu ions is e…
We demonstrate charge tuning in strain free GaAs/AlGaAs quantum dots (QDs) grown by droplet epitaxy on a GaAs(111)A substrate. Application of a bias voltage allows the controlled charging of the QDs from $-3|e|$ to $+2|e|$. The resulting changes in QD emission energy and exciton fine-structure are recorded in micro-photoluminescence experiments at T=4K. We uncover the existence of excited valence and conduction states, in addition to the s-shell-like ground state. We record a second series of emission lines about 25meV above the charged exciton emission coming from excited charged excitons. Fo…
We report transport mobility measurements for clean, two-dimensional (2D) electron systems confined to GaAs quantum wells (QWs), grown via molecular beam epitaxy, in two families of structures, a standard, symmetrically-doped GaAs set of QWs with Al$_{0.32}$Ga$_{0.68}$As barriers, and one with additional AlAs cladding surrounding the QWs. Our results indicate that the mobility in narrow QWs with no cladding is consistent with existing theoretical calculations where interface roughness effects are softened by the penetration of the electron wave function into the adjacent low barriers. In contr…
We report quantum dots fabricated on very shallow 2-dimensional electron gases, only 30 nm below the surface, in undoped GaAs/AlGaAs heterostructures grown by molecular beam epitaxy. Due to the absence of dopants, an improvement of more than one order of magnitude in mobility (at 2E11 /cm^2) with respect to doped heterostructures with similar depths is observed. These undoped wafers can easily be gated with surface metallic gates patterned by e-beam lithography, as demonstrated here from single-level transport through a quantum dot showing large charging energies (up to 1.75 meV) and excited s…
We demonstrate a method of making a very shallow, gateable, undoped 2-dimensional electron gas. We have developed a method of making very low resistivity contacts to these structures and systematically studied the evolution of the mobility as a function of the depth of the 2DEG (from 300nm to 30nm). We demonstrate a way of extracting quantitative information about the background impurity concentration in GaAs and AlGaAs, the interface roughness and the charge in the surface states from the data. This information is very useful from the perspective of molecular beam epitaxy (MBE) growth. It is …
We report on the transport properties of a high mobility two-dimensional hole system (2DHS) confined in GaAs/AlGaAs quantum wells grown molecular-beam epitaxy on the (100) surface of GaAs. The quantum wells are modulation-doped with carbon utilizing a novel resistive filament source. At T=0.3K and carrier density p=1x10^11cm^-2, a mobility of 10^6cm^2/Vs is achieved. At fixed carrier density p=10^11cm^-2, the mobility is found to be a non-monotonic function of the quantum well width. The mobility peaks at 10^6cm^2/Vs for a 15nm well and is reduced for both smaller and larger well widths for th…
Recent experiments [1] suggest that the ferromagnetism (FM) in GaAs: Mn is determined by the impurity band rather than holes in the valence band. We discuss here the physical mechanism of FM mediated by the carriers in impurity band, where the Mn d-level play a crucial role. The theory is based on the first principle approach.
We report on photocurrent and photoconductance processes in a freely suspended p-doped single GaAs nanowire. The nanowires are grown by molecular beam epitaxy (MBE), and they are electrically contacted by a focused ion beam (FIB) deposition technique. The observed photocurrent is generated at the Schottky contacts between the nanowire and metal source-drain electrodes, while the observed photoconductance signal can be explained by a photogating effect induced by optically generated charge carriers located at the surface of the nanowire. Both optoelectronic effects are sensitive to the polariza…
We exploit ferromagnetic imprinting to create complex laterally defined regions of nuclear spin polarization in lithographically patterned MnAs/GaAs epilayers grown by molecular beam epitaxy (MBE). A time-resolved Kerr rotation microscope with approximately 1 micron spatial resolution uses electron spin precession to directly image the GaAs nuclear polarization. These measurements indicate that the polarization varies from a maximum under magnetic mesas to zero several microns from the mesa perimeter, resulting in large (10**4 T/m) effective field gradients. The results reveal a flexible schem…
Resonant transport is demonstrated in a hybrid superconductor-semiconductor heterostructure junction grown by molecular beam epitaxy on GaAs. This heterostructure realizes the model system introduced by de Gennes and Saint-James in 1963 [P. G. de Gennes and D. Saint-James, Phys. Lett. {\bf 4}, 151 (1963)]. At low temperatures a single marked resonance peak is shown superimposed to the characteristic Andreev-dominated subgap conductance. The observed magnetotransport properties are successfully analyzed within the random matrix theory of quantum transport, and ballistic effects are included by …
We demonstrate first measurements of successful spin generation in crystalline Co$_2$FeSi/MgO/GaAs hybrid structures grown by molecular-beam epitaxy (MBE), with different MgO interlayer thicknesses. Using non-local spin valve and non-local Hanle measurement configurations, we determine spin lifetimes of ${τ\approx 100}$~ns and spin diffusion lengths of ${λ\approx 5.6}$~$μ$m for different MgO layer thicknesses proving the high quality of the GaAs transport channel. For an optimized MgO layer thickness, the bias dependence of the spin valve signals indicates the verification of the half-metallic…
We present an experimental investigation of the magnetic, electrical and structural properties of Ga0.94Mn0.06As1-yPy layers grown by molecular beam epitaxy on GaAs substrates for y less than or equal to 0.3. X-ray diffraction measurements reveal that the layers are under tensile strain which gives rise to a magnetic easy axis perpendicular to the plane of the layers. The strength of the magnetic anisotropy and the coercive field increase as the phosphorous concentration is increased. The resistivity of all samples shows metallic behaviour with the resistivity increasing as y increases. These …
Breaking the time-reversal symmetry of a topological insulator (TI) by ferromagnetism can induce exotic magnetoelectric phenomena such as quantized anomalous Hall (QAH) effect. Experimental observation of QAH effect in a magnetically doped TI requires ferromagnetism not relying on the charge carriers. We have realized the ferromagnetism independent of both polarity and density of carriers in Cr-doped BixSb2-xTe3 thin films grown by molecular beam epitaxy. Meanwhile, the anomalous Hall effect is found significantly enhanced with decreasing carrier density, with the anomalous Hall angle reaching…
A source of single photons and quantum entangled photon pairs is a key element in quantum information networks. Here, we demonstrate the electrically driven generation of quantum entangled pairs using a naturally symmetric GaAs quantum dot grown by droplet epitaxy. Coincidence histograms obtained at a temperature of 10 K reveal the generation of quantum entangled pairs that have a fidelity to the Bell pairs of 0.71 +- 0.015, much beyond the classical limit. The quantum nature of the emitted pairs is conserved at temperatures of up to ~65 K, and is essentially limited by the charge carrier conf…
Three different elements, Silicon, Selenium, and Tellurium, are ion-implanted in Gallium arsenide to form a conducting layer that serves as a back-gate to a molecular beam epitaxy (MBE) overgrown two-dimensional electron gas (2DEG). While the heavy ion Tellurium creates too many damages in the gallium arsenide to form a conducting layer, both Silicon and Selenium show promising results combined with MBE-grown high-quality 2DEGs. Similar 2DEG mobility compared to non-implanted reference samples is achieved for both Silicon and Selenium implanted structures. Individual contacts to the back-gate …
We present a systematic study of the morphology of homoepitaxial InP films grown by metalorganic vapor-phase epitaxy which are imaged with ex situ atomic force microscopy. These films show a dramatic range of different surface morphologies as a function of the growth conditions and substrate (growth temperature, V/III ratio, and miscut angle < 0.6deg and orientation toward A or B sites), ranging from stable step flow to previously unreported strong step bunching, over 10 nm in height. These observations suggest a window of growth parameters for optimal quality epitaxial layers. We also present…
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…
Motivated by recent breakthrough in molecular beam epitaxy of GaAs/AlGaAs quantum wells [Y. J. Chung \textit{et al.}, Nature Materials \textbf{20}, 632 (2021)], we examine contributions to mobility and quantum mobility from various scattering mechanisms and their dependencies on the electron density. We find that at lower electron densities, $n_e \lesssim 1 \times 10^{11}$ cm$^{-2}$, both transport and quantum mobility are limited by unintentional background impurities and follow a power law dependence, $\propto n_e^α$, with $α\approx 0.85$. Our predictions for quantum mobility are in reasonab…
Several semiconductor quantum dot techniques have been investigated for the generation of entangled photon pairs. Among the other techniques, droplet epitaxy enables the control of the shape, size, density, and emission wavelength of the quantum emitters. However, the fraction of the entanglement-ready quantum dots that can be fabricated with this method is still limited to around 5%, and matching the energy of the entangled photons to atomic transitions (a promising route towards quantum networking) remains an outstanding challenge. Here, we overcome these obstacles by introducing a modified …
