Tunneling magnetoresistance in trilayer structures composed of group-IV ferromagnetic semiconductor Ge1-xFex, MgO, and Fe

Group-IV-based ferromagnetic semiconductor Ge1-xFex (GeFe) is one of the most promising materials for efficient spin injectors and detectors for Si and Ge. Recent first principles calculations (Sakamoto et al., Ref. 9) suggested that the Fermi level is located in two overlapping largely spin-polarized bands formed in the bandgap of GeFe; spin-down d(e) band and spin-up p-d(t2) band. Thus, it is important to clarify how these bands contribute to spin injection and detection. In this study, we show the first successful observation of the tunneling magnetoresistance (TMR) in magnetic tunnel junctions (MTJs) containing a group-IV ferromagnetic semiconductor, that is, in MTJs composed of epitaxially grown Fe/MgO/Ge0.935Fe0.065. We find that the p-d(t2) band in GeFe is mainly responsible for the tunneling transport. Although the obtained TMR ratio is small (0.3%), the TMR ratio is expected to be enhanced by suppressing leak current through amorphous-like crystal domains observed in MgO

Impurity band conduction in group-IV ferromagnetic semiconductor Ge1-xFex with nanoscale fluctuations in Fe concentration

We study the carrier transport and magnetic properties of group-IV-based ferromagnetic semiconductor Ge1-xFex thin films (Fe concentration x = 2.3 - 14 %) with and without boron (B) doping, by measuring their transport characteristics; the temperature dependence of resistivity, hole concentration, mobility, and the relation between the anomalous Hall conductivity versus conductivity. At relatively low x (= 2.3 %), the transport in the undoped Ge1-xFex film is dominated by hole hopping between Fe-rich hopping sites in the Fe impurity band, whereas that in the B-doped Ge1-xFex film is dominated by the holes in the valence band in the degenerated Fe-poor regions. As x increases (x = 2.3 - 14 %), the transport in the both undoped and B-doped Ge1-xFex films is dominated by hole hopping between the Fe-rich hopping sites of the impurity band. The magnetic properties of the Ge1-xFex films are studied by various methods including magnetic circular dichroism, magnetization and anomalous Hall resistance, and are not influenced by B-doping. We show band profile models of both undoped and B-doped Ge1-xFex films, which can explain the transport and the magnetic properties of the Ge1-xFex films.Comment: 32 pages, 14 figure

Electronic Structure of the Ferromagnetic Semiconductor Fe-doped Ge Revealed by Soft X-ray Angle-Resolved Photoemission Spectroscopy

Ge$_{1-x}$Fe$_{x}$ (Ge:Fe) shows ferromagnetic behavior up to a relatively high temperature of 210 K, and hence is a promising material for spintronic applications compatible with Si technology. We have studied its electronic structure by soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) measurements in order to elucidate the mechanism of the ferromagnetism. We observed finite Fe 3$d$ components in the states at the Fermi level ($E_{F}$) in a wide region in momentum space and $E_{F}$ was located above the valence-band maximum (VBM). First-principles supercell calculation also suggested that the $E_{F}$ is located above the VBM, within the narrow spin-down $d$($e$) band and within the spin-up impurity band of the deep acceptor-level origin derived from the strong $p$-$d$($t_{2}$) hybridization. We conclude that the narrow $d$($e$) band is responsible for the ferromagnetic coupling between Fe atoms while the acceptor-level-originated band is responsible for the transport properties of Ge:Fe

Machine-learning-assisted thin-film growth: Bayesian optimization in molecular beam epitaxy of SrRuO3 thin films

Materials informatics exploiting machine learning techniques, e.g., Bayesian optimization (BO), has the potential to offer high-throughput optimization of thin-film growth conditions through incremental updates of machine learning models in accordance with newly measured data. Here, we demonstrated BO-based molecular beam epitaxy (MBE) of SrRuO3, one of the most-intensively studied materials in the research field of oxide electronics, mainly owing to its unique nature as a ferromagnetic metal. To simplify the intricate search space of entangled growth conditions, we ran the BO for a single condition while keeping the other conditions fixed. As a result, high-crystalline-quality SrRuO3 film exhibiting a high residual resistivity ratio (RRR) of over 50 as well as strong perpendicular magnetic anisotropy was developed in only 24 MBE growth runs in which the Ru flux rate, growth temperature, and O3-nozzle-to-substrate distance were optimized. Our BO-based search method provides an efficient experimental design that is not as dependent on the experience and skills of individual researchers, and it reduces experimental time and cost, which will accelerate materials research

Origin of the large positive magnetoresistance in Ge1-xMnx granular thin films

GeMn granular thin films are a unique and promising material for spintronics applications due to large positive magnetoresistance (MR). Previous studies on GeMn have suggested that the large MR is related to nanospinodal decomposition of GeMn into Mn-rich ferromagnetic nanoparticles and Mn-poor paramagnetic matrix. However, its microscopic origin of the MR has not been clarified yet. Here, using X-ray magnetic circular dichroism (XMCD), which is extremely sensitive to the local magnetic state of each atom, we investigate the magnetic properties of the nanoparticles and the matrix in GeMn separately. We find that the MR ratio is proportional to the product of the magnetizations originating from the nanoparticles and the matrix. This result indicates that spin-polarized holes in the nanoparticles penetrate into the matrix and that these holes undergo spin-disorder magnetic scattering by the paramagnetic Mn atoms in the matrix, which induces the large MR

Ferromagnetism above 1000 K in highly cation-ordered double-perovskite insulator Sr3OsO6

Magnetic insulators have been intensively studied for over 100 years, and they, in particular ferrites, are considered to be the cradle of magnetic exchange interactions in solids. Their wide range of applications include microwave devices and permanent magnets . They are also suitable for spintronic devices owing to their high resistivity, low magnetic damping, and spin-dependent tunneling probabilities. The Curie temperature is the crucial factor determining the temperature range in which any ferri/ferromagnetic system remains stable. However, the record Curie temperature has stood for over eight decades in insulators and oxides (943 K for spinel ferrite LiFe5O8). Here we show that a highly B-site ordered double-perovskite, Sr2(SrOs)O6 (Sr3OsO6), surpasses this long standing Curie temperature record by more than 100 K. We revealed this B-site ordering by atomic-resolution scanning transmission electron microscopy. The density functional theory (DFT) calculations suggest that the large spin-orbit coupling (SOC) of Os6+ 5d2 orbitals drives the system toward a Jeff = 3/2 ferromagnetic (FM) insulating state. Moreover, the Sr3OsO6 is the first epitaxially grown osmate, which means it is highly compatible with device fabrication processes and thus promising for spintronic applications

Electronic structure and magnetic properties of magnetically dead layers in epitaxial CoFe2O4/Al2O3/Si(111) films studied by X-ray magnetic circular dichroism

Epitaxial CoFe2O4/Al2O3 bilayers are expected to be highly efficient spin injectors into Si owing to the spin filter effect of CoFe2O4. To exploit the full potential of this system, understanding the microscopic origin of magnetically dead layers at the CoFe2O4/Al2O3 interface is necessary. In this paper, we study the crystallographic and electronic structures and the magnetic properties of CoFe2O4(111) layers with various thicknesses (thickness d = 1.4, 2.3, 4, and 11 nm) in the epitaxial CoFe2O4(111)/Al2O3(111)/Si(111) structures using soft X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) combined with cluster-model calculation. The magnetization of CoFe2O4 measured by XMCD gradually decreases with decreasing thickness d and finally a magnetically dead layer is clearly detected at d = 1.4 nm. The magnetically dead layer has frustration of magnetic interactions which is revealed from comparison between the magnetizations at 300 and 6 K. From analysis using configuration-interaction cluster-model calculation, the decrease of d leads to a decrease in the inverse-to-normal spinel structure ratio and also a decrease in the average valence of Fe at the octahedral sites. These results strongly indicate that the magnetically dead layer at the CoFe2O4/Al2O3 interface originates from various complex networks of superexchange interactions through the change in the crystallographic and electronic structures. Furthermore, from comparison of the magnetic properties between d = 1.4 and 2.3 nm, it is found that ferrimagnetic order of the magnetically dead layer at d = 1.4 nm is restored by the additional growth of the 0.9-nm-thick CoFe2O4 layer on it

Local Magnetic States of the Weakly Ferromagnetic Iron-Based Superconductor Sr2_2VFeAsO3−δ_{3-\delta} Studied by X-ray Magnetic Circular Dichroism

We have performed x-ray magnetic circular dichroism (XMCD) measurements on the iron-based superconductor Sr$_2$VFeAsO$_{3-\delta}$ to study the origin of weak ferromagnetism (WFM) reported for this compound. While Fe 3$d$ electrons show a magnetic response similar to the other iron pnictides, signals from V 3$d$ electrons remain finite at zero magnetic field and may be responsible for the WFM

Thickness-dependent quantum transport of Weyl fermions in ultra-high-quality SrRuO3 films

The recent observation of Weyl fermions in the itinerant 4d ferromagnetic perovskite SrRuO3 points to this material being a good platform for exploring novel physics related to a pair of Weyl nodes in epitaxial heterostructures. In this letter, we report the thickness-dependent magnetotransport properties of ultra-high-quality epitaxial SrRuO3 films grown under optimized conditions on SrTiO3 substrates. Signatures of Weyl fermion transport, i.e., unsaturated linear positive magnetoresistance accompanied by a quantum oscillation having a {\pi} Berry phase, were observed in films with thicknesses as small as 10 nm. Residual resistivity increased with decreasing film thickness, indicating disorder near the interface between SrRuO3 and the SrTiO3 substrate. Since this disorder affects the magnetic and electrical properties of the films, the Curie temperature decreases and the coercive field increases with decreasing thickness. Thickness-dependent magnetotransport measurements revealed that the threshold residual resistivity ratio (RRR) to observe Weyl fermion transport is 21. These results provide guidelines for realizing quantum transport of Weyl fermions in SrRuO3 near heterointerfaces

Structural and transport properties of highly Ru-deficient SrRu0.7O3 thin films prepared by molecular beam epitaxy: comparison with stoichiometric SrRuO3

We investigate structural and transport properties of highly Ru-deficient SrRu0.7O3 thin films prepared by molecular beam epitaxy on (001) SrTiO3 substrates. To distinguish the influence of the two types of disorders in the films, Ru vacancies within lattices and disorders near the interface, SrRu0.7O3 thin films with various thicknesses (t = 1-60 nm) were prepared. It was found that the influence of the former dominates the electrical and magnetic properties when t > 5-10 nm, while that of the latter does when t < 5-10 nm. Structural characterizations revealed that the crystallinity, in terms of the Sr and O sublattices, of SrRu0.7O3 thin films, is as high as that of the ultrahigh-quality SrRuO3 ones. The Curie temperature (TC) analysis elucidated that SrRu0.7O3 (TC = 140 K) is a material distinct from SrRuO3 (TC = 150 K). Despite the large Ru deficiency (30%), the SrRu0.7O3 films showed metallic conduction when t > 5 nm. In high-field magnetoresistance measurements, the fascinating phenomenon of Weyl fermion transport was not observed for the SrRu0.7O3 thin films irrespective of thickness, which is in contrast to the stoichiometric SrRuO3 films. The (magneto)transport properties suggest that a picture of carrier scattering due to the Ru vacancies is appropriate for SrRu0.7O3, and also that proper stoichiometry control is a prerequisite to utilizing the full potential of SrRuO3 as a magnetic Weyl semimetal and two-dimensional spin-polarized system. Nevertheless, the large tolerance in Ru composition (30 %) to metallic conduction is advantageous for some practical applications where SrRu1-xO3 is exploited as an epitaxial conducting layer