EuO Films Research Articles

Ferromagnetic semiconductor EuO thin films characterized by vacuum electrochemical process with ionic liquid

In this study, the electrochemical impedance analysis was demonstrated for thin film EuO, a ferromagnetic semiconductor, by taking the advantage of our original instrument, which enables to perform the entire process from thin film deposition to electrochemical measurement with ionic liquid in a vacuum. Effects of whether surface protecting layers were insulative or metallic, as well as their thickness on the electrochemical measurement of EuO thin films were examined by comparing the choices of amorphous alumina and Ag metal as the protecting layer. As a result, the relative permittivity of EuO films, even with a thickness of 2 nm, was successfully estimated and the averaged value was 6.6 within an error of 10 %. Furthermore, the donor density accordingly estimated was found well correlated with the Curie temperature TC of the EuO films.

Magnetic polarons reach a hundred thousand Bohr magnetons.

The ability of light to manipulate fundamental interactions in a medium is central to research in optomagnetism and applications in electronics. A prospective approach is to create composite quasiparticles, magnetic polarons, highly susceptible to external stimuli. To control magnetic and transport properties by weak magnetic and electric fields, it is important to find materials that support photoinduced magnetic polarons with colossal net magnetic moments. Here, we demonstrate that magnetic polarons with a record-high magnetic moment, reaching and exceeding a hundred thousand Bohr magnetons, can be optically generated in EuO, an archetypal ferromagnetic semiconductor. The phenomenon is established employing the photoinduced Faraday effect studied in EuO films by a two-color pump-probe technique. The giant magnetic polarons are generated just above the Curie temperature once EuO is exposed to photons of an energy exceeding the bandgap. Picosecond temporal dynamics of magnetic polarons follows relaxation processes in the spin-split 5d conduction band occupied by the photoexcited electron. The study is expected to provide a platform for implementation of an efficient optical control over the magnetic state in solids.

Controlling the Magneto-Optical Response in Ultrathin Films of EuO1-x via Interface Engineering with Ferroelectric BaTi2O5.

Utilizing pulsed laser deposition, a film of EuO1-x was deposited onto a Si(001) substrate with MgO buffer and compared to the same heterostructure with an additional BaTi2O5 thin film on top of the EuO1-x surface. X-ray diffraction (XRD) indicates the films crystallize into a preferred EuO(111) orientation; it also reveals the clear presence of EuSi2, which suggests Si or Eu diffuses across the MgO buffer layer. EuO1-x films exhibit a ferromagnetic (FM) signature and temperature-dependent exchange bias, indicated by MOKE measurements, suggesting the presence of a magnetic order well above the EuO Curie temperature with possible origins in charge carrier density near the interface. In comparison, an antiferromagnetic character persists well above the EuO Curie temperature of 69 K and the enhanced Curie temperature of 150 K for BaTi2O5 films grown on the EuO1-x films. The antiferromagnetic behavior is not seen in thicker EuO1-x thin films when integrated with other ferroelectric (FE) phases of the BaO-TiO2 system, suggesting an origin in the perturbed charge population at the BaTi2O5/EuO1-x interface.

Observation of Thickness-Dependent Exchange Interaction in EuO Ultrathin Films

The electronic structure of single-crystalline EuO (100) ultrathin films, together with their exchange splitting energy (ΔEEX) and ferromagnetic phase transition temperature (TC), was investigated by temperature- and thickness-dependent angle-resolved photoemission spectroscopy. Both ΔEEX and TC decreased monotonically with decreasing film thickness. The band shift showed an opposite thickness dependence at the Γ and X points, reflecting the balance of the hybridization between the Eu 4f and O 2p states (super-exchange interaction) and between the Eu 4f, O 2p, and Eu 5d states (indirect-exchange interaction). The observed transition from an indirect energy gap in the bulk to a direct gap in the ultrathin films of the ferromagnetic semiconductor EuO could be potential in future spintronic devices.

Damping of dipole-exchange spin waves in ferromagnetic thin films at elevated temperatures

A non-bosonic technique, based on the drone-fermion perturbation method and a high-density expansion, is employed to study the spin-wave (SW) scattering processes in a ferromagnetic thin film with exchange and dipole–dipole interactions. Specifically, the diagrammatic contributions to the spin–spin Green’s functions are evaluated within a 1/z perturbation expansion, where z is the number of spins interacting with any given spin. The results are used to calculate the SW damping at temperatures below the Curie temperature T C. It is found that, apart from the usual contributions due to three-magnon and four-magnon processes in the film, which are dominant at relatively low temperatures (consistent with boson expansion methods), there is an additional mechanism that becomes important for temperatures above about This is spin disorder damping, previously studied in bulk magnetic materials; it occurs when a spin wave is scattered by the instantaneous disorder produced when a longitudinal spin component undergoes a large thermal fluctuation. Numerical estimates are presented for thin films of Permalloy and EuO.

Growth and Characterisation Studies of Eu3O4 Thin Films Grown on Si/SiO2 and Graphene.

We report the growth, structural and magnetic properties of the less studied Eu-oxide phase, EuO, thin films grown on a Si/SiO substrate and Si/SiO/graphene using molecular beam epitaxy. The X-ray diffraction scans show that highly textured crystalline EuO(001) films are grown on both substrates, whereas the film deposited on graphene has a better crystallinity than that grown on the Si/SiO substrate. The SQUID measurements show that both films have a Curie temperature of ∼ K, with a magnetic moment of ∼ emu/cm at 2 K. The mixed valence of the Eu cations has been confirmed by the qualitative analysis of the depth-profile X-ray photoelectron spectroscopy measurements with the : ratio of . However, surprisingly, our films show no metamagnetic behaviour as reported for the bulk and powder form. Furthermore, the microscopic optical images and Raman measurements show that the graphene underlayer remains largely intact after the growth of the EuO thin films.

Exploring the intrinsic limit of the charge-carrier-induced increase of the Curie temperature of Lu- and La-doped EuO thin films

Raising the Curie temperature ${T}_{\mathrm{C}}$ of the highly spin-polarized semiconductor EuO by doping it with rare-earth elements is a strategy to make EuO more technologically relevant to spintronics. The increase of ${T}_{\mathrm{C}}$ with free carrier density $n$ and the surprisingly low dopant activation $p$, found in Gd-doped EuO thin films [Mairoser et al., Phys. Rev. Lett. 105, 257206 (2010)], raised the important question of whether ${T}_{\mathrm{C}}$ could be considerably enhanced by increasing $p$. Using a low-temperature growth method for depositing high-quality Lu-doped EuO films we attain high dopant activation ($p$) values of up to 67%, effectively more than doubling $p$ as compared to adsorption-controlled growth of Lu- and Gd-doped EuO. Relating $n, p$, and lattice compression of La- and Lu-doped EuO films grown at different temperatures to the ${T}_{\mathrm{C}}$ of these samples allows us to identify several different mechanisms influencing ${T}_{\mathrm{C}}$ and causing an experimental maximum in ${T}_{\mathrm{C}}$. In addition, scanning transmission electron microscopy in combination with electron energy loss spectroscopy measurements on La-doped EuO indicate that extensive dopant clustering is one, but not the sole reason for dopant deactivation in rare-earth doped EuO films.

Pulsed Laser Deposition of Rocksalt Magnetic Binary Oxides

Magnetic binary oxides with the rocksalt structure constitute an important class of materials for potential applications as electronic or electrochemical devices. Moreover, they often become a theoretical playground, due to the simple electronic and crystal structures, in the quest for novel phenomena. For these possibilities to be realized, a necessary prerequisite would be to grow atomically ordered and controllably-strained binary oxides on proper substrates. Here we systematically explore the use of pulsed laser deposition technique (PLD) to grow three basic oxides that have rocksalt structure but different chemical stability in the ambient atmosphere: NiO (stable), MnO (metastable) and EuO (unstable). By tuning laser fluence FL, an epitaxial single-phase NiO thin-film growth can be achieved in a wide range of growth temperatures 10 ≤ TG ≤750 °C. At the lowest TG, the out-of-plane strain raises to 1.5%, which is five times higher than in NiO film grown at 750 °C. MnO thin films that had long-range order were successfully deposited on the MgO substrates after appropriate tuning of deposition parameters. The growth of MnO phase was strongly influenced by FL and the TG. EuO films with satisfactory quality were deposited by PLD after oxygen availability had been minimized. Synthesis of EuO thin films at rather low TG = 350 °C prevented thermally-driven lattice relaxation and allowed growth of strained films. Overall, PLD was a quick and reliable method to grow binary oxides with rocksalt structure in high quality that can satisfy requirements for applications and for basic research.

Redox-controlled epitaxy and magnetism of oxide heterointerfaces: EuO/SrTiO3

We demonstrate a route to prepare thin films of the ferromagnetic insulator europium monoxide. Key is a redox-controlled interface reaction between metallic Eu and the substrate ${\mathrm{SrTiO}}_{3}$ as the supplier of oxygen. The process allows tuning the electronic, magnetic, and structural properties of the EuO films. Furthermore, we apply this technique to various oxidic substrates and demonstrate the universality and limits of a redox-controlled EuO film synthesis.

Phonon confinement and spin-phonon coupling in tensile-strained ultrathin EuO films.

Reducing the material sizes to the nanometer length scale leads to drastic modifications of the propagating lattice excitations (phonons) and their interactions with electrons and magnons. In EuO, a promising material for spintronic applications in which a giant spin-phonon interaction is present, this might imply a reduction of the degree of spin polarization in thin films. Therefore, a comprehensive investigation of the lattice dynamics and spin-phonon interaction in EuO films is necessary for practical applications. We report a systematic lattice dynamics study of ultrathin EuO(001) films using nuclear inelastic scattering on the Mössbauer-active isotope 151Eu and first-principles theory. The films were epitaxially grown on YAlO3(110), which induces a tensile strain of ca. 2%. By reducing the EuO layer thickness from 8 nm to a sub-monolayer coverage, the Eu-partial phonon density of states (PDOS) reveals a gradual enhancement of the number of low-energy phonon states and simultaneous broadening and suppression of the peaks. These deviations from bulk features lead to significant anomalies in the vibrational thermodynamic and elastic properties calculated from the PDOS. The experimental results, supported by first-principles theory, unveil a reduction of the strength of the spin-phonon interaction in the tensile-strained EuO by a factor of four compared to a strain-free lattice.

Spin splitting in EuO(111)/Si(111) spin-filter tunnel junctions with atomically sharp interface

We demonstrate the tunneling in spin-split barriers made of ferromagnetic EuO grown on Si(111) substrates by molecular beam epitaxy. For 6 nm thick EuO films with high crystal quality and atomically sharp interfaces, we find a barrier height lowering driven by the spin splitting below the Curie temperature of 35 K. We determined the splitting energy to be 0.56 ± 0.03 eV at 20 K which results in a spin polarization above 90%.

Europium monoxide nanocrystalline thin films with high near-infrared transparency

Nanocrystalline textured EuO thin films are prepared by an oxygen loss process from a pure Eu2O3 bulk ceramic target through pulsed laser deposition in vacuum at room temperature. X-ray diffraction spectra evidence a well-defined diffraction peak corresponding to the EuO phase textured along the (1 1 0) direction. Analysis of the XRD peak profile indicates that the films are nanocrystalline (average crystallite size of 11 nm) with a compressive residual strain. The formation of stoichiometric EuO is further confirmed by a strong signal from Eu2+ in the X-ray photoelectron spectra. The complex refractive index in the near infrared has been determined by spectroscopic ellipsometry and shows that the EuO films have a high transparency (k < 10−3) and a refractive index of 2.1. A band-gap shift of 0.25 eV is found with respect to the EuO bulk. These films, deposited by an accessible and efficient method, open a new route to produce EuO films with optical quality, suitable for NIR optoelectronic components.

High-Temperature Magnetism in Graphene Induced by Proximity to EuO.

Addition of magnetism to spectacular properties of graphene may lead to novel topological states and design of spin logic devices enjoying low power consumption. A significant progress is made in defect-induced magnetism in graphene-selective elimination of p z orbitals (by vacancies or adatoms) at triangular sublattices tailors graphene magnetism. Proximity to a magnetic insulator is a less invasive way, which is being actively explored now. Integration of graphene with the ferromagnetic semiconductor EuO has much to offer, especially in terms of proximity-induced spin-orbit interactions. Here, we synthesize films of EuO on graphene using reactive molecular beam epitaxy. Their quality is attested by electron and X-ray diffraction, cross-sectional electron microscopy, and Raman and magnetization measurements. Studies of electron transport reveal a magnetic transition at TC* ≈ 220 K, well above the Curie temperature 69 K of EuO. Up to TC*, the dependence R xy( B) is strongly nonlinear, suggesting the presence of the anomalous Hall effect. The role of synthesis conditions is highlighted by studies of an overdoped structure. The results justify the use of the EuO/graphene system in spintronics.

Role of La doping for topological Hall effect in epitaxial EuO films

We report the critical role of La doping in the topological Hall effect observed in $\mathrm{L}{\mathrm{a}}_{x}\mathrm{E}{\mathrm{u}}_{1\ensuremath{-}x}\mathrm{O}$ thin films $(\ensuremath{\sim}50\phantom{\rule{0.16em}{0ex}}\mathrm{nm})$ grown by molecular beam epitaxy. When the La doping exceeds 0.036, topological Hall effect emerges, which we attribute to the formation of magnetic skyrmions. Besides, the La doping is found to play a critical role in determining the phases, densities, and sizes of the skyrmions in the $\mathrm{L}{\mathrm{a}}_{x}\mathrm{E}{\mathrm{u}}_{1\ensuremath{-}x}\mathrm{O}$ thin films. The maximum region of the skyrmion phase diagram is observed on the $\mathrm{L}{\mathrm{a}}_{0.1}\mathrm{E}{\mathrm{u}}_{0.9}\mathrm{O}$ thin film. As the La doping increases, the skyrmion density increases while the skyrmion size decreases. Our findings demonstrate the important role of La doping for the skyrmions in EuO films, which could be important for future studies of magnetic skyrmions in Heisenberg ferromagnets.

Anomalous Hall effect in the prospective spintronic material Eu1−xGdxO integrated with Si

Remarkable properties of EuO make it a versatile spintronic material. Despite numerous experimental and theoretical studies of EuO, little is known about the anomalous Hall effect in this ferromagnet. So far, the effect has not been observed in bulk EuO, though has been detected in EuO films with uncontrolled distribution of defects. In the present work doping is taken under control: epitaxial films of Gd-doped EuO are synthesized integrated with Si using molecular beam epitaxy and characterized with x-ray diffraction and magnetization measurements. Nanoscale transport studies reveal the anomalous Hall effect in the ferromagnetic region for samples with different Gd concentration. The saturated anomalous Hall effect conductivity value of 5.0 S·cm−1 in Gd-doped EuO is more than an order of magnitude larger than those reported so far for Eu chalcogenides doped with anion vacancies.

Elevated Curie temperature and half-metallicity in the ferromagnetic semiconductorLaxEu1−xO

Here we study the effect of La doping in EuO thin films using SQUID magnetometry, muon spin rotation ($\mu$SR), polarized neutron reflectivity (PNR), and density functional theory (DFT). The $\mu$SR data shows that the La$_{0.15}$Eu$_{0.85}$O is homogeneously magnetically ordered up to its elevated $T_{\rm C}$. It is concluded that bound magnetic polaron behavior does not explain the increase in $T_{\rm C}$ and an RKKY-like interaction is consistent with the $\mu$SR data. The estimation of the magnetic moment by DFT simulations concurs with the results obtained by PNR, showing a reduction of the magnetic moment per La$_{x}$Eu$_{1-x}$O for increasing lanthanum doping. This reduction of the magnetic moment is explained by the reduction of the number of Eu-4$f$ electrons present in all the magnetic interactions in EuO films. Finally, we show that an upwards shift of the Fermi energy with La or Gd doping gives rise to half-metallicity for doping levels as high as 3.2 %.

Topological Hall effect in thin films of the Heisenberg ferromagnet EuO

We report on the topological Hall effect (THE) in centrosymmetric EuO thin films. This THE signal persists down to the lowest temperature in the metallic region below 50 K for the films thinner than 200 nm. The signal rapidly disappears by tilting the applied magnetic field from surface normal, suggestive of noncoplanar spin configuration such as two-dimensional skyrmions. This observation possibly substantiates the theoretical proposal of magnetic skyrmions in 2D Heisenberg ferromagnets in marked contrast to better established $B20\text{\ensuremath{-}}\mathrm{type}$ chiral helimagnets.

Direct epitaxial integration of the ferromagnetic semiconductor EuO with silicon for spintronic applications.

Following a remarkable success of metallic spintronics, tremendous efforts have been invested into the less developed semiconductor spintronics, in particular, with the aim to produce three-terminal spintronic devices, e.g., spin transistors. One of the most important prerequisites for such a technology is an effective injection of spin-polarized carriers into a nonmagnetic semiconductor, preferably one of those currently used for industrial applications such as Si-a workhorse of modern electronics. Ferromagnetic semiconductor EuO is long believed to be the best candidate for integration with Si. Although EuO proved to offer optimal conditions for effective spin injection into silicon and in spite of considerable efforts, the direct epitaxial stabilization of stoichiometric EuO thin films on Si without any buffer layer has not been demonstrated to date. Here we report a new technique for control of EuO/Si interface on submonolayer level. Using this technique we solve a long-standing problem of direct epitaxial growth on silicon of thin EuO films which exhibit structural and magnetic properties of EuO bulk material. This result opens up new possibilities in developing all-semiconductor spintronic devices.

Epitaxial growth of magnetic semiconductor EuO on silicon by molecular beam epitaxy

Functional oxides demonstrate a wide range of magnetic, optical and transport properties. Their integration with silicon promises significant advances in electronics. An important key in enabling brand-new oxide technologies is the utilization of silicon/oxide epitaxy, thus making quality of the interface a critical issue. The progress depends on our ability to avoid formation of impurity phases at the interface and to tackle structural mismatch of the oxide and Si. We design a novel chemical protection of Si (001) surface on the submonolayer scale based on the surface metal silicide with the (1×5) reconstruction. This new technique is applied to the long-standing problem of integration of a ferromagnetic semiconductor with Si. Direct epitaxial growth of EuO on Si without any buffer layer, so far inaccessible, is achieved by molecular beam epitaxy. The nucleation step, comprising first 10 monolayers of EuO, is followed by a distillation-controlled growth. An alternative to standard capping procedures for EuO, based on controlled formation of an amorphous Eu2O3 layer, is devised. Crystal perfection of the films is established ex situ by x-ray diffraction and Rutherford backscattering. Magnetic properties of the EuO films match those of the bulk.

Epitaxial growth of magnetic semiconductor EuO on silicon by molecular beam epitaxy

Functional oxides demonstrate a wide range of magnetic, optical and transport properties. Their integration with silicon promises significant advances in electronics. An important key in enabling brand‐new oxide technologies is the utilization of silicon/oxide epitaxy, thus making quality of the interface a critical issue. The progress depends on our ability to avoid formation of impurity phases at the interface and to tackle structural mismatch of the oxide and Si. We design a novel chemical protection of Si (001) surface on the submonolayer scale based on the surface metal silicide with the (1×5) reconstruction. This new technique is applied to the long‐standing problem of integration of a ferromagnetic semiconductor with Si. Direct epitaxial growth of EuO on Si without any buffer layer, so far inaccessible, is achieved by molecular beam epitaxy. The nucleation step, comprising first 10 monolayers of EuO, is followed by a distillation‐controlled growth. An alternative to standard capping procedures for EuO, based on controlled formation of an amorphous Eu2O3 layer, is devised. Crystal perfection of the films is established ex situ by x‐ray diffraction and Rutherford backscattering. Magnetic properties of the EuO films match those of the bulk.