Coherent Epitaxial Semiconductor-Ferromagnetic Insulator InAs/EuS Interfaces: Band Alignment and Magnetic Structure
Yu Liu, Alessandra Luchini, Sara Martí-Sánchez, Christian Koch, Sergej Schuwalow, Sabbir A. Khan, Tomaš Stankevič, Sonia Francoua, Jose R. L. Mardegan, Jonas A.… 展开作者
Yu Liu, Alessandra Luchini, Sara Martí-Sánchez, Christian Koch, Sergej Schuwalow, Sabbir A. Khan, Tomaš Stankevič, Sonia Francoua, Jose R. L. Mardegan, Jonas A. Krieger, Vladimir N. Strocov, Jochen Stahn, Carlos A. F. Vaz, Mahesh Ramakrishnan, Urs Staub, Kim Lefmann, Gabriel Aeppli, Jordi Arbiol, Peter Krogstrup
Hybrid semiconductor-ferromagnetic insulator heterostructures are interesting due to their tunable electronic transport, self-sustained stray field and local proximitized magnetic exchange. In this work, we present lattice matched hybrid epitaxy of semiconductor - ferromagnetic insulator InAs/EuS heterostructures and analyze the atomic-scale structure as well as their electronic and magnetic characteristics. The Fermi level at the InAs/EuS interface is found to be close to the InAs conduction band and in the bandgap of EuS, thus preserving the semiconducting properties. Both neutron and X-ray reflectivity measurements show that the ferromagnetic component is mainly localized in the EuS thin film with a suppression of the Eu moment in the EuS layer nearest the InAs. Induced moments in the adjacent InAs layers were not detected although our ab initio calculations indicate a small exchange field in the InAs layer. This work presents a step towards realizing high quality semiconductor - ferromagnetic insulator hybrids, which is a critical requirement for development of various quantum and spintronic applications without external magnetic fields.
Recently, the EuS/InAs interface has attracted attention for the possibility of inducing magnetic exchange correlations in a strong spin-orbit semiconductor, which could be useful for topological quantum devices. We use density functional theory (DFT) with a machine-learned Hubbard $U$ correction [npj Comput. Mater. 6, 180 (2020)] to elucidate the effect of the bonding configuration at the interface on the electronic structure. For all interface configurations considered here, we find that the EuS valence band maximum (VBM) lies below the InAs VBM. In addition, dispersed states emerge at the t…
We report different growth modes and corresponding magnetic properties of thin EuSe films grown by molecular beam epitaxy on BaF2, Pb1-xEuxSe, GaAs, and Bi2Se3 substrates. We show that EuSe growth predominantly in (001) orientation on GaAs(111) and Bi2Se3, but along (111) crystallographic direction on BaF2 (111) and Pb1-xEuxSe (111). High-resolution transmission electron microscopy measurements reveal an abrupt and highly crystalline interface for both (001) and (111) EuSe films. In agreement with previous studies, ordered magnetic phases include antiferromagnetic, ferrimagnetic, and ferromagn…
We created epitaxial magnetic tunnel junctions of FeCo/MgO/EuS on MgO buffered Si (100). Tunnel magnetoresistance reached up to 64% at 4.2 K. An unexpected fast drop of magnetoresistance was recorded for MgO thickness above 1 nm, which is attributed to the forced nonspecular conductance across the EuS conduction band minimum located at the X point, rather than the desired Delta_1 conductance centered around the Gamma point.
We report a method for making epitaxial superconducting contacts to semiconducting nanowires. The temperature and gate characteristics demonstrate barrier-free electrical contact, and the properties in the superconducting state are investigated at low temperature. Half-covering aluminum contacts are realized without the need of lithography and we demonstrate how to controllably insert high-band gap layers in the interface region. These developments are relevant to hybrid superconductor-nanowire devices that support Majorana zero energy states.
We combine electron beam lithography and masked anodization of epitaxial aluminium to define tunnel junctions via selective oxidation, alleviating the need for wet-etch processing or direct deposition of dielectric materials. Applying this technique to define Josephson junctions in proximity induced superconducting Al-InAs heterostructures, we observe multiple Andreev reflections in transport experiments, indicative of a high quality junction. We further compare the mobility and density of Hall-bars defined via wet etching and anodization. These results may find utility in uncovering new fabri…
We study the influence of epitaxial strain on the electronic properties of InAs/GaSb composite quantum wells (CQWs), host structures for quantum spin Hall insulators, by transport measurements and eight-band $\mathbf{k\cdot p}$ calculations. Using different substrates and buffer layer structures for crystal growth, we prepare two types of samples with vastly different strain conditions. CQWs with a nearly strain-free GaSb layer exhibit a resistance peak at the charge neutrality point that reflects the opening of a topological gap in the band-inverted regime. In contrast, for CQWs with 0.50\% b…
Hybrid semiconductor/superconductor nanowires constitute a pervasive platform for studying gate-tunable superconductivity and the emergence of topological behavior. Their low-dimensionality and crystal structure flexibility facilitate novel heterostructure growth and efficient material optimization; crucial prerequisites for accurately constructing complex multi-component quantum materials. Here, we present an extensive optimization of Sn growth on InSb, InAsSb and InAs nanowires. We demonstrate how the growth conditions and the crystal structure/symmetry of the semiconductor drive the formati…
The combination of ferromagnets with topological superconductors or insulators allows for new phases of matter that support excitations such as chiral edge modes and Majorana fermions. EuS, a wide-band-gap ferromagnetic insulator with a Curie temperature around 16 K, and SrTiO$_3$ (STO), an important substrate for engineering heterostructures, may support these phases. We present scanning superconducting quantum interference device (SQUID) measurements of EuS grown epitaxially on STO that reveal micron-scale variations in ferromagnetism and paramagnetism. These variations are oriented along th…
The structural and electronic properties in common anion (GaSb)_1/(InSb)_1 and common cation (InAs)_1/(InSb)_1 [111] ordered superlattices have been determined using the local density total energy full potential linearized augmented plane wave method. The influence of the ordering direction, strain conditions and atomic substitution on the electronic properties of technological and experimental interest (such as energy band-gaps and charge carrier localization in the different sublattices) were determined. The results show an appreciable energy band-gap narrowing compared to the band-gap avera…
Epitaxial InAs/GaAs Quantum Dots (QDs) are widely used as highly efficient and pure sources of single photons and entangled photon-pairs, however reliable wafer-scale growth techniques have proved elusive. Growth of two-dimensional Quantum Well (QW) thin-films can be achieved with atomic precision down to below the de Broglie wavelength of electrons in the material, exposing the quantum particle-in-a-box energy vs. thickness-squared relationship. However, difficulties in controlling the exact moment of nanostructure nucleation obscure this behaviour in epitaxial QD material, preventing a clear…
We use density functional theory calculations to study the electronic structure of epitaxial (111) interfaces of the topological crystalline insulators SnSe and SnTe with the magnetic insulator EuS and the non-magnetic insulator CaTe, respectively. We consider both interface slab models with a vacuum region and periodic heterostructures without vacuum. We find that gaps of 21 meV at the $Γ$ point and 9 meV at the M point arise in the topological state at the SnSe/EuS interface, due to the magnetic proximity effect, which breaks the time reversal symmetry. The surface state at $Γ$ is shifted be…
Continuum simulations of self-organized lateral compositional modulation growth in InAs/AlAs short-period superlattices on InP substrate are presented. Results of the simulations correspond quantitatively to the results of synchrotron x-ray diffraction experiments. The time evolution of the compositional modulation during epitaxial growth can be explained only including a nonlinear dependence of the elastic energy of the growing epitaxial layer on its thickness. From the fit of the experimental data to the growth simulations we have determined the parameters of this nonlinear dependence. It wa…
The large Landé g-factor, high spin-orbit coupling, and low effective mass of the two-dimensional electron gas in InSb quantum wells combined with proximal superconductivity may realize a scalable platform for topological quantum computation. Aluminum thin films directly deposited on top of InSb planar structures result in the formation of a reactive AlInSb layer at the interface. This interlayer progressively consumes the whole Al film, resulting in a disordered AlInSb layer after few months at room temperature. We report on a heterostructure design that results in a significant increase of t…
We report on the magnetic and structural properties of Ar and Mn implanted InAs epitaxial films grown on GaAs (100) by Molecular Beam Epitaxy (MBE) and the effect of Rapid Thermal Annealing (RTA) for 30 seconds at 750C. Channeling Particle Induced X- ray Emission (PIXE) experiments reveal that after Mn implantation almost all Mn atoms are subsbtitutional in the In-site of the InAs lattice, like in a diluted magnetic semiconductor (DMS). All of these samples show diamagnetic behavior. But, after RTA treatment the Mn-InAs films exhibit room-temperature magnetism. According to PIXE measurements t…
The spin-dependence of the interface resistance between ferromagnetic Fe and InAs is calculated from first-principles for specular and disordered (001) interfaces. Because of the symmetry mismatch in the minority-spin channel, the specular interface acts as an efficient spin filter with a transmitted current polarisation between 98 an 89%. The resistance of a specular interface in the diffusive regime is comparable to the resistance of a few microns of bulk InAs. Symmetry-breaking arising from interface disorder reduces the spin asymmetry substantially and we conclude that efficient spin injec…
The GaAs-based material system is well-known for the implementation of InAs quantum dots (QDs) with outstanding optical properties. However, these dots typically emit at a wavelength of around 900nm. The insertion of a metamorphic buffer (MMB) can shift the emission to the technologically attractive telecom C-band range centered at 1550nm. However, the thickness of common MMB designs limits their compatibility with most photonic resonator types. Here we report on the MOVPE growth of a novel InGaAs MMB with a non-linear indium content grading profile designed to maximize plastic relaxation with…
A virtual substrate for high quality InAs epitaxial layer has been attained via metalorganic vapor-phase epitaxy growth of Sb-assisted InxGa1-xAs metamorphic buffers, following a convex compositional continuous gradient of the In content from x = 53 % to 100 %. The use of trimethylantimony (or its decomposition products) as a surfactant has been found to crucially enable the control over the defect formation during the relaxation process. Moreover, an investigation of the wafer offcut-dependence of the defect formation and surface morphology has enabled the achievement of a reliably uniform gr…
We report on the spin-polarized electron injection through an Fe(100)/InAs(100) junction. The circularly polarized electroluminescence of injected electrons from epitaxially grown Fe thin film into InAs(100) in an external magnetic field is measured to investigate the spin injection efficiency. The obtained polarization of the electroluminescence is seen to increase up to about -12 % at the temperature of 6.5 K and the external magnetic field of 10 T. This result suggests that the efficient spin injection is possible through the ferromagnetic metal/semiconductor (FM/SC) interface without a tun…
Single Crystalline Fe3-deltaO4 (0<=delta<=0.33) films have been epitaxially grown on InAs (001) substrates by molecular beam epitaxy using O2 as source of active oxygen. Under optimum growth conditions in-situ real time reflection high-energy electron diffraction patterns along with ex-situ atomic force microscopy indicated the (001) Fe3-deltaO4 to be grown under step-flow-growth mode with a characteristic surface reconstruction. X-ray photoelectron spectroscopy demonstrate the possibility to obtain iron oxides with compositions ranging from Fe3O4 to gamma-Fe2O3. Superconducting quantum interf…
Near surface indium arsenide quantum wells have recently attracted a great deal of interest since they can be interfaced epitaxially with superconducting films and have proven to be a robust platform for exploring mesoscopic and topological superconductivity. In this work, we present magnetotransport properties of two-dimensional electron gases confined to an indium arsenide quantum well near the surface. The electron mass extracted from the envelope of the Shubnikov-de Haas oscillations shows an average effective mass $m^{*}$ = 0.04 at low magnetic field. Complementary to our magnetotransport…
Many present and future applications of superconductivity would benefit from electrostatic control of carrier density and tunneling rates, the hallmark of semiconductor devices. One particularly exciting application is the realization of topological superconductivity as a basis for quantum information processing. Proposals in this direction based on proximity effect in semiconductor nanowires are appealing because the key ingredients are currently in hand. However, previous instances of proximitized semiconductors show significant tunneling conductance below the superconducting gap, suggesting…
Hybrid semiconductor-superconductor InAs-Al nanowires with uniform and defect-free crystal interfaces are one of the most promising candidates used in the quest for Majorana zero modes (MZMs). However, InAs nanowires often exhibit a high density of randomly distributed twin defects and stacking faults, which result in an uncontrolled and non-uniform InAs-Al interface. Furthermore, this type of disorder can create potential inhomogeneity in the wire, destroy the topological gap, and form trivial sub-gap states mimicking MZM in transport experiments. Further study shows that reducing the InAs na…
Here, we demonstrate an approach that provides a precise control of the dimension of InAs from one-dimensional nanowires to wafer-scale free-standing two-dimensional nanosheets, which have a high degree of crystallinity and outstanding electrical and optical properties, using molecular-beam epitaxy by controlling catalyst alloy segregation. In our approach, two-dimensional InAs nanosheets can be obtained directly from one-dimensional InAs nanowires by silver-indium alloy segregation, which is much easier than all previously reported method, such as traditional buffering technique and select ar…
We demonstrate a new fabrication process for hybrid semiconductor-superconductor heterostructures based on anodic oxidation (AO), allowing controlled thinning of epitaxial Al films. Structural and transport studies of oxidized epitaxial Al films grown on insulating GaAs substrates reveal spatial non-uniformity and enhanced critical temperature and magnetic fields. Oxidation of epitaxial Al on hybrid InAs heterostructures with a conducting quantum well show similarly enhanced superconducting properties transferred to the two-dimensional electron gas (2DEG) by proximity effect, with critical per…
We demonstrate how first-principles calculations using density-functional theory (DFT) can be applied to gain insight into the molecular processes that rule the physics of materials processing. Specifically, we study the molecular beam epitaxy (MBE) of arsenic compound semiconductors. For homoepitaxy of GaAs on GaAs(001), a growth model is presented that builds on results of DFT calculations for molecular processes on the beta2-reconstructed GaAs(001) surface, including adsorption, desorption, surface diffusion and nucleation. Kinetic Monte Carlo simulations on the basis of the calculated ener…
Ultrathin InAs nanowires (NW) with one-dimensional (1D) sub-band structure are promising materials for advanced quantum-electronic devices, where dimensions in the sub-30 nm diameter limit together with post-CMOS integration scenarios on Si are much desired. Here, we demonstrate two site-selective synthesis methods that achieve epitaxial, high aspect ratio InAs NWs on Si with ultrathin diameters below 20 nm. The first approach exploits direct vapor-solid growth to tune the NW diameter by interwire spacing, mask opening size and growth time. The second scheme explores a unique reverse-reaction …
First-principles full potential linearized augmented plane wave (FLAPW) calculations have been performed for lattice-mismatched common-atom III-V interfaces. In particular, we have examined the effects of epitaxial strain and ordering direction on the valence band offset in [001] and [111] GaSb/InSb and InAs/InSb superlattices, and found that the valence band maximum is always higher at the InSb side of the heterojunction, except for the common-anion system grown on an InSb substrate. The comparison between equivalent structures having the same substrate lattice constant, but different growth …
We present a first-principles study of the electronic and magnetic properties of epitaxial interfaces between the Heusler compounds Ti$_2$MnIn and Ni$_2$MnIn and the III-V semiconductors, InSb and InAs, respectively. We use density functional theory (DFT) with a machine-learned Hubbard $U$ correction determined by Bayesian optimization. We evaluate these interfaces for prospective applications in Majorana-based quantum computing and spintronics. In both interfaces, states from the Heusler penetrate into the gap of the semiconductor, decaying within a few atomic layers. The magnetic interaction…
Controlling the properties of semiconductor/metal interfaces is a powerful method for designing functionality and improving the performance of electrical devices. Recently semiconductor/superconductor hybrids have appeared as an important example where the atomic scale uniformity of the interface plays a key role for the quality of the induced superconducting gap. Here we present epitaxial growth of semiconductor-metal core-shell nanowires by molecular beam epitaxy, a method that provides a conceptually new route to controlled electrical contacting of nanostructures and for designing devices f…
The classical Heisenberg model is applied in a Monte Carlo study to investigate the distance dependence of the indirect nearest neighbor (NN) exchange and next-nearest neighbor (NNN) superexchange interaction in EuO, EuS, EuSe and EuTe. For this purpose, first, the dependence of the magnetic ordering temperature, i.e., Curie, respectively, Néel temperature for ferromagnetic and antiferromagnetic ordering on the exchange constants was determined. This was then employed for the analysis of experimental data of hydrostatic pressure experiments. It is shown that all experimental findings, i.e., th…
We present a new version of the Ogre open source Python package with the capability to perform structure prediction of epitaxial inorganic interfaces by lattice and surface matching. In the lattice matching step a scan over combinations of substrate and film Miller indices is performed to identify the domain-matched interfaces with the lowest mismatch. Subsequently, surface matching is conducted by Bayesian optimization to find the optimal interfacial distance and in-plane registry between the substrate and film. For the objective function, a geometric score function is proposed, based on the …
Over the past several years, the inherent scaling limitations of electron devices have fueled the exploration of high carrier mobility semiconductors as a Si replacement to further enhance the device performance. In particular, compound semiconductors heterogeneously integrated on Si substrates have been actively studied, combining the high mobility of III-V semiconductors and the well-established, low cost processing of Si technology. This integration, however, presents significant challenges. Conventionally, heteroepitaxial growth of complex multilayers on Si has been explored. Besides compl…
