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At least 73 records · Page 4

Thickness dependent itinerant ferromagnetism in ultrathin Ba-doped SrRu O 3 films

The electronic and magnetic properties in AB⁢O 3 perovskite oxides are extremely sensitive to lattice structure, but also to dimensionality, such as the thickness in thin film-form. Here, we report the thickness-dependent electromagnetic properties of ultrathin epitaxially stabilized Sr 1-x ⁢Ba x ⁢Ru⁢O 3 (x = 0.08, 0.2) thin films on a SrTi⁢O 3 (001) substrate. The results reveal that the barium doping (0.08 ≤ x ≤ 0.20) reduces Ru⁢O 6 orthorhombic distortions existing in SrRu⁢O 3 and induces a tetragonal distortion, as evidenced by out-of-plane lattice expansion. A metal-to-insulator transition, accompanied by a ferromagnetic to nonmagnetic transition occurs with reducing film thickness from 10 to 3 unit cells for both x = 0.08 and 0.2, regardless of the doping level. The results suggest that the effects of compositional vacancies and surface/interface contributions introduced via dimensional confinement are more dominant than A-site chemical disorder or structural distortion for the loss of metallicity and ferromagnetism in ultra-thin epitaxial films.

36 MATERIALS SCIENCE↗

Magnetic and electron transport properties of Co 2 Si nanomagnets

In this study, magnetotransport and ferromagnetism in thin films of Co 2 Si nanoclusters are investigated experimentally and theoretically. The nanoclusters are fabricated by an inert-gas condensation-type cluster-deposition method and have an average size of 11.3 nm. Unlike the bulk Co 2 Si that exhibits a very weak net magnetic moment only below 10 K, the nanoclusters exhibit room-temperature ferromagnetism with a substantial saturation magnetization. Key features of the system are its closeness to the Stoner transition, magnetic moments induced by spin polarization starting from surface atoms, and nonuniaxial anisotropy associated with the orthorhombic crystal structure of Co 2 Si . A method is introduced to determine the effective anisotropy using the experimental magnetization data of this complex system and its relationship with the two lowest-order nonuniaxial anisotropy constants. On decreasing temperature from 300 K, the nanoclusters show electron-transport properties unusual for a ferromagnetic metal, including an increase of Hall resistivity and a nonmonotonic change of negative magnetoresistance with a peak at around 100 K. The underlying physics is explained on the basis of the large polarization of surface spins and variation in the degree of their misalignments due to temperature-dependent effective anisotropy.

36 MATERIALS SCIENCE↗

Controlling the Magneto-Optical Response in Ultrathin Films of EuO 1– x via Interface Engineering with Ferroelectric BaTi 2 O 5

Utilizing pulsed laser deposition, a film of EuO 1–x was deposited onto a Si(001) substrate with MgO buffer and compared to the same heterostructure with an additional BaTi 2 O 5 thin film on top of the EuO 1–x surface. X-ray diffraction (XRD) indicates the films crystallize into a preferred EuO(111) orientation; it also reveals the clear presence of EuSi 2 , which suggests Si or Eu diffuses across the MgO buffer layer. EuO 1–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 BaTi 2 O 5 films grown on the EuO 1–x films. Furthermore, the antiferromagnetic behavior is not seen in thicker EuO 1–x thin films when integrated with other ferroelectric (FE) phases of the BaO–TiO 2 system, suggesting an origin in the perturbed charge population at the BaTi 2 O 5 /EuO 1–x interface.

36 MATERIALS SCIENCE↗

Spin switchable optical phenomena in Rashba band structures through intersystem crossing in momentum space in solution-processing 2D-superlattice perovskite film

Spin-switchable phenomena are a critical element for the development of spintronic and chiroptic devices. Herein we combine a 2D-superlattice perovskite (4,4-DFPD2PbI4) film with a ferromagnetic cobalt (Co) layer to form a multiferroic perovskite/Co interface, and demonstrate spin-switchable circularly polarized luminescence (CPL) between right-handed σ+ and left-handed σ− polarizations. When the ferromagnetic spins of Co at the Co/perovskite interface are altered between positive and negative magnetic field directions, the CPL from the 2D-superlattice perovskite switches from σ+ to σ− polarization. The magnetic field effects present a unique method to confirm that CPL is generated by the circular-orbital momentum of light-emitting excitons within Rashba band structures, eliminating artifacts involving structural birefringence. Our polarized neutron reflectometry measurements confirm a super long-range spin-orbit interaction occurring in the 2D-superlattice perovskite films. The temperature dependence of spin-switchable phenomenon indicates an extraordinarily long orbital polarization lifetime, reaching microseconds at room temperature and milliseconds at 5 K.

36 MATERIALS SCIENCE↗

Optically Induced Static Magnetization in Metal Halide Perovskite for Spin‐Related Optoelectronics

Abstract Understanding the feasibility to couple semiconducting and magnetic properties in metal halide perovskites through interface design opens new opportunities for creating the next generation spin‐related optoelectronics. In this work, a fundamentally new phenomenon of optically induced magnetization achieved by coupling photoexcited orbital magnetic dipoles with magnetic spins at perovskite/ferromagnetic interface is discovered. The depth‐sensitive polarized neutron reflectometry combined with in situ photoexcitation setup, constitutes key evidence of this novel effect. It is demonstrated that a circularly polarized photoexcitation induces a stable magnetization signal within the depth up to 7.5 nm into the surface of high‐quality perovskite (MAPbBr 3 ) film underneath a ferromagnetic cobalt layer at room temperature. In contrast, a linearly polarized light does not induce any detectable magnetization in the MAPbBr 3 . The observation reveals that photoexcited orbital magnetic dipoles at the surface of perovskite are coupled with the spins of the ferromagnetic atoms at the interface, leading to an optically induced magnetization within the perovskite’s surface. The finding demonstrates that perovskite semiconductor can be bridged with magnetism through optically controllable method at room temperature in this heterojunction design. This provides the new concept of utilizing spin and orbital degrees of freedom in new‐generation spin‐related optoelectronic devices.

36 MATERIALS SCIENCE↗

Vertical Strain-Driven Antiferromagnetic to Ferromagnetic Phase Transition in EuTiO 3 Nanocomposite Thin Films

Three-dimensional (3D) strain induced in self-assembled vertically aligned nanocomposite (VAN) epitaxial films provides an unrivaled method to induce very large strains in thin films. Here, by growing VAN films of EuTiO 3 (ETO)–Eu 2 O 3 (EO) with different EO fractions, the vertical strain was systematically increased in ETO, up to 3.15%, and the Eu–Ti–Eu bond angle along $\langle$111$\rangle$ decreased by up to 1°, leading to a weakening of the antiferromagnetic interactions and switching from antiferromagnetic to ferromagnetic behavior. Our work has shown for the first time that Eu–Ti–Eu superexchange interactions play a key role in determining the magnetic ground state of ETO. Broadly, our work serves as an exemplar to show that multifunctionalities in strong spin–lattice coupling perovskite oxides can be uniquely tuned at the atomic scale using simple VAN structures.

36 MATERIALS SCIENCE↗

Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO 3 thin films

Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be effectively engineered by strain, defects, and microstructure. An excellent example can be found in ferroelastic LaCoO 3 with paramagnetism in bulk. In contrast, unexpected ferromagnetism is observed in tensile-strained LaCoO 3 films, however, its origin remains controversial. Here we simultaneously reveal the formation of ordered oxygen vacancies and previously unreported long-range suppression of CoO 6 octahedral rotations throughout LaCoO 3 films. Supported by density functional theory calculations, we find that the strong modification of Co 3d-O 2p hybridization associated with the increase of both Co-O-Co bond angle and Co-O bond length weakens the crystal-field splitting and facilitates an ordered high-spin state of Co ions, inducing an emergent ferromagnetic-insulating state. Our work provides unique insights into underlying mechanisms driving the ferromagnetic-insulating state in tensile-strained ferroelastic LaCoO 3 films while suggesting potential applications toward low-power spintronic devices.

36 MATERIALS SCIENCE↗

Emergent Magnetic States and Tunable Exchange Bias at 3d Nitride Heterointerfaces

Abstract Interfacial magnetism stimulates the discovery of giant magnetoresistance (MR) and spin–orbital coupling across the heterointerfaces, facilitating the intimate correlation between spin transport and complex magnetic structures. Over decades, functional heterointerfaces composed of nitrides have seldom been explored due to the difficulty in synthesizing high‐quality nitride films with correct compositions. Here, the fabrication of single‐crystalline ferromagnetic Fe 3 N thin films with precisely controlled thicknesses is reported. As film thickness decreases, the magnetization dramatically deteriorates, and the electronic state changes from metallic to insulating. Strikingly, the high‐temperature ferromagnetism is maintained in a Fe 3 N layer with a thickness down to 2 u.c. (≈8 Å). The MR exhibits a strong in‐plane anisotropy; meanwhile, the anomalous Hall resistivity reverses its sign when the Fe 3 N layer thickness exceeds 5 u.c. Furthermore, a sizable exchange bias is observed at the interfaces between a ferromagnetic Fe 3 N and an antiferromagnetic CrN. The exchange bias field and saturation moment strongly depend on the controllable bending curvature using the cylinder diameter engineering technique, implying the tunable magnetic states under lattice deformation. This work provides a guideline for exploring functional nitride films and applying their interfacial phenomena for innovative perspectives toward practical applications.

Jin, Qiao↗

Effects of Sn substitution in SrRuO 3 epitaxial films

Epitaxial SrRu 1–x Sn x O 3 (0 ≤ x ≤ 1) thin films were deposited on SrTiO 3 (001) substrates by sequential two-target synthesis using pulsed laser deposition to achieve stable phases in this family of quaternary perovskites. The SrRu 1–x Sn x O 3 films exhibit a good crystalline quality, a sharp interface between film and substrate, and an atomically smooth surface. A gradual expansion of the c-axis lattice parameter was observed with Sn doping serving as a means to tune chemical pressure and magnetism. With an increase in Sn doping, the resistivity of the film increased, and the ferromagnetism decreased. These results illustrate use of lattice engineering, e.g., tuning of c-axis lattice parameter with chemical doping, to control electronic and magnetic properties of epitaxial thin films for applications in oxide electronics.

36 MATERIALS SCIENCE↗

Ultra-thin lithium aluminate spinel ferrite films with perpendicular magnetic anisotropy and low damping

Ultra-thin films of low damping ferromagnetic insulators with perpendicular magnetic anisotropy have been identified as critical to advancing spin-based electronics by significantly reducing the threshold for current-induced magnetization switching while enabling new types of hybrid structures or devices. Here, we have developed a new class of ultra-thin spinel structure Li 0.5 Al 1.0 Fe 1.5 O 4 (LAFO) films on MgGa 2 O 4 (MGO) substrates with: 1) perpendicular magnetic anisotropy; 2) low magnetic damping and 3) the absence of degraded or magnetic dead layers. These films have been integrated with epitaxial Pt spin source layers to demonstrate record low magnetization switching currents and high spin-orbit torque efficiencies. These LAFO films on MGO thus combine all of the desirable properties of ferromagnetic insulators with perpendicular magnetic anisotropy, opening new possibilities for spin based electronics.

36 MATERIALS SCIENCE↗

Spin and Charge Interconversion in Dirac-Semimetal Thin Films

We use spin torque ferromagnetic resonance and ferromagnetic-resonance-driven spin pumping to detect spin-charge interconversion at room temperature in heterostructure devices that interface an archetypal Dirac semimetal, Cd 3 As 2 , with a metallic ferromagnet, Ni 0.80 Fe 0.20 (permalloy). Angle-resolved photoemission directly reveals the Dirac-semimetal nature of the samples prior to device fabrication and high-resolution transmission electron microscopy is used to characterize the crystalline structure and the relevant heterointerfaces. We find that the spin-charge interconversion efficiency in Cd 3 As 2 /permalloy heterostructures is comparable to that in heavy metals and that it is enhanced by the presence of an interfacial oxide. Spin torque ferromagnetic resonance measurements reveal an in-plane spin polarization regardless of an oxidized or pristine interface. We discuss the underlying mechanisms for spin-charge interconversion by comparing our results with first principles calculations and conclude that extrinsic mechanisms dominate the observed phenomena. Our results indicate a need for caution in interpretations of spin-transport and spin-charge conversion experiments in Cd 3 As 2 devices that seek to invoke the role of topological Dirac and Fermi arc states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Escalated Phase Separation Driven Enhanced Magnetoresistance in Manganite/Iridate Epitaxial Heterostructures

Phase separation in manganites leads to unique magnetic and electronic properties. 50% Ca-doped LaMnO 3 (LCMO), at the boundary of ferromagnetic (FM) and antiferromagnetic (AFM) states in La 1-x Ca x MnO 3 (0 ≤ x ≤ 1), is an ideal system to study phase separation behavior. The investigation reveals the effect of a 5d-metal perovskite SrIrO 3 (SIO) on the phase separation, magnetic, and magnetoresistance (MR) properties of LCMO. Single-layer and bilayer LCMO films, both appear purely ferromagnetic along the in-plane (IP) magnetic field direction, but show the tendency of temperature-dependent ferromagnetic and antiferromagnetic or charge-ordered (CO) phase separation with the out-of-plane (OOP) applied field. The MR, and colossal magnetoresistance (CMR), observed in LCMO/SIO bilayers are two orders and an order of magnitude (in %) larger, respectively than that in the single-layer film. The coexistence of FM and AFM/CO phases is responsible for the CMR and MR enhancement in the LCMO/SIO bilayer, pointing toward the importance of the phase separation and competition of both the individual materials in enhancing their magnetic and electronic properties.

36 MATERIALS SCIENCE↗

Scanning SQUID study of ferromagnetism and superconductivity in infinite-layer nickelates

Infinite-layer nickelates R 1-x Sr x NiO 2 (R = La, Pr, Nd) are a class of superconductors with structural similarities to cuprates. Although long-range antiferromagnetic order has not been observed for these materials, magnetic effects such as antiferromagnetic spin fluctuations and spin-glass behavior have been reported. Different experiments have drawn different conclusions about whether the pairing symmetry is s or d wave. In this paper, we applied a scanning superconducting quantum interference device (SQUID) to probe the magnetic behavior of film samples of three infinite-layer nickelates (La 0.85 Sr 0.15 NiO 2 , Pr 0.8 Sr 0.2 NiO 2 , and Nd 0.775 Sr 0.225 NiO 2 ) grown on SrTiO 3 (STO), each with a nominal thickness of 20 unit cells. In all three films, we observed a ferromagnetic background. We also measured the magnetic susceptibility above the superconducting critical temperature in Pr 0.8 Sr 0.2 NiO 2 and La 0.85 Sr 0.15 NiO 2 and identified a non-Curie-Weiss dynamic susceptibility. Both magnetic features are likely due to NiO x nanoparticles. We investigated superconductivity in Pr 0.8 Sr 0.2 NiO 2 and Nd 0.775 Sr 0.225 NiO 2 , which exhibited inhomogeneous diamagnetic screening. The superfluid density inferred from the diamagnetic susceptibility in relatively homogeneous regions shows T-linear behavior in both samples. Finally, we observed superconducting vortices in Nd 0.775 Sr 0.225 NiO 2 . We determined a Pearl length of 330 µm for Nd 0.775 Sr 0.225 NiO 2 at 300 mK, both from the strength of the diamagnetism and from the size and shape of the vortices. These results highlight the importance of considering NiO x particles when interpreting experimental results for these films.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Axion insulator state in ferromagnetically ordered CrI 3 /Bi 2 Se 3 /MnBi 2 Se 4 heterostructures

Ferromagnetic (FM) axion insulators may greatly simplify experimental explorations of the topological magnetoelectric effect, as the FM ordering can be stable in a broad range of magnetic field. Through density functional theory calculations and four-band model studies, we find that two-dimensional van der Waals FM CrI 3 and MnBi 2 Se 4 overlayers induce opposite-sign exchange fields in the topological surface states of Bi 2 Se 3 film when they are ferromagnetically ordered. As a consequence, the CrI 3 /Bi 2 Se 3 /MnBi 2 Se 4 heterostructure is a robust FM axion insulator, according to surface-resolved Berry curvature calculations. Our work opens up opportunities for the design of materials with the topological magnetoelectric effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Thickness and temperature dependence of the atomic-scale structure of SrRuO 3 thin films

The temperature-dependent layer-resolved structure of 3 to 44 unit cell thick SrRuO 3 (SRO) films grown on Nb-doped SrTiO 3 substrates is investigated using a combination of high-resolution synchrotron x-ray diffraction and high-resolution electron microscopy to understand the role that structural distortions play in suppressing ferromagnetism in ultra-thin SRO films. The oxygen octahedral tilts and rotations and Sr displacements characteristic of the bulk orthorhombic phase are found to be strongly dependent on temperature, the film thickness, and the distance away from the film–substrate interface. For thicknesses, t, above the critical thickness for ferromagnetism (t > 3 uc), the orthorhombic distortions decrease with increasing temperature above T C . Below T C , the structure of the films remains constant due to the magneto-structural coupling observed in bulk SRO. The orthorhombic distortions are found to be suppressed in the 2–3 interfacial layers due to structural coupling with the SrTiO 3 substrate and correlate with the critical thickness for ferromagnetism in uncapped SRO films.

36 MATERIALS SCIENCE↗

Coexistence of unconventional spin Hall effect and antisymmetric planar Hall effect in IrO 2

Crystal symmetry plays an important role in the Hall effects. Unconventional spin Hall effect (USHE), characterized by Dresselhaus and out-of-plane spins, has been observed in materials with low crystal symmetry. Recently, antisymmetric planar Hall effect (APHE) was discovered in rutile RuO 2 and IrO 2 (101) thin films, which also exhibit low crystal symmetry. In this study, we report the observation of both USHE and APHE in IrO 2 (111) films, using spin-torque ferromagnetic resonance and harmonic Hall measurements, respectively. Notably, the unconventional spin-torque efficiency from Dresselhaus spin was more than double that of a previous report. Additionally, the temperature dependence of APHE suggests that it arises from the Lorentz force, constrained by crystal symmetry. Here, symmetry analysis supports the coexistence of USHE and APHE and demonstrates that both originate from the crystal symmetry of IrO 2 (111), paving the way for a deeper understanding of Hall effects and related physical phenomena.

Crystal structure↗

Ferroelectric Self-Polarization Controlled Magnetic Stratification and Magnetic Coupling in Ultrathin La 0.67 Sr 0.33 MnO 3 Films

Multiferroic oxide heterostructures consisting of ferromagnetic and ferroelectric components hold the promise for nonvolatile magnetic control via ferroelectric polarization, advantageous for the low-dissipation spintronics. Modern understanding of the magnetoelectric coupling in these systems involves structural, orbital, and magnetic reconstructions at interfaces. Previous works have long proposed polarization-dependent interfacial magnetic structures; however, direct evidence is still missing, which requires advanced characterization tools with near-atomic-scale spatial resolutions. Here, extensive polarized neutron reflectometry (PNR) studies have determined the magnetic depth profiles of PbZr 0.2 Ti 0.8 O 3 /La 0.67 Sr 0.33 MnO 3 (PZT/LSMO) bilayers with opposite self-polarizations. When the LSMO is 2–3 nm thick, the bilayers show two magnetic transitions on cooling. However, temperature-dependent magnetization is different below the lower-temperature transition for opposite polarizations. PNR finds that the LSMO splits into two magnetic sublayers, but the inter-sublayer magnetic couplings are of opposite signs for the two polarizations. Near-edge X-ray absorption spectroscopy further shows contrasts in both the Mn valences and the Mn–O bond anisotropy between the two polarizations. Finally, this work completes the puzzle for the magnetoelectric coupling model at the PZT/LSMO interface, showing a synergic interplay among multiple degrees of freedom toward emergent functionalities at complex oxide interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electric‐Field‐Driven Reversal of Ferromagnetism in (110)‐Oriented, Single Phase, Multiferroic Co‐Substituted BiFeO 3 Thin Films

Abstract While multiferroic materials are attractive systems for the promise of ultra‐low‐power‐consumption computational technologies, electric‐field‐induced magnetization reversal is a key challenge for realizing devices at scale. Though significant research efforts have been working toward the realization of a material which couples ferroelectricity and ferromagnetism, there are few, even composite, systems which are practical for device scale applications at room temperature. Co‐substituted multiferroic BiFe 0.9 Co 0.1 O 3 is a promising candidate system, due to coupled ferroelectricity and weak ferromagnetism at room temperature. Here, it is theoretically indicated that the ferroic orders in this material are statically coupled, where an in‐plane 109° ferroelectric switching event can result in the reversal of this out‐of‐plane component of magnetization, and the electric field‐induced magnetization reversal is experimentally observed. Such an in‐plane poling configuration is particularly desirable for device applications.

Chemistry↗