Spin Glass State in Strained La2/3Ca1/3MnO3 Thin Films.

Epitaxial strain modifies the physical properties of thin films deposited on single-crystal substrates. In a previous work, we demonstrated that in the case of La2/3Ca1/3MnO3 thin films the strain induced by the substrate can produce the segregation of a non-ferromagnetic layer (NFL) at the top surface of ferromagnetic epitaxial La2/3Ca1/3MnO3 for a critical value of the tetragonality τ, defined as τ = |c - a|a, of τC ≈ 0.024. Although preliminary analysis suggested its antiferromagnetic nature, to date a complete characterization of the magnetic state of such an NFL has not been performed. Here, we present a comprehensive magnetic characterization of the strain-induced segregated NFL. The field-cooled magnetic hysteresis loops exhibit an exchange bias mechanism below T ≈ 80 K, which is well below the Curie temperature of the ferromagnetic La2/3Ca1/3MnO3 layer. The exchange bias and coercive fields decay exponentially with temperature, which is commonly accepted to describe spin-glass (SG) behavior. The signatures of slow dynamics were confirmed by slow spin relaxation over a wide temperature regime. Low-energy muon spectroscopy experiments directly evidence the slowing down of the magnetic moments below ~100 K in the NFL. The experimental results indicate the SG nature of the NFL. This SG state can be understood within the context of the competing ferromagnetic and antiferromagnetic interactions of similar energies.

Tuning Coherent-Phonon Heat Transport in LaCoO3/SrTiO3 Superlattices.

Accessing the regime of coherent phonon propagation in nanostructures opens enormous possibilities to control the thermal conductivity in energy harvesting devices, phononic circuits, etc. In this paper we show that coherent phonons contribute substantially to the thermal conductivity of LaCoO3/SrTiO3 oxide superlattices, up to room temperature. We show that their contribution can be tuned through small variations of the superlattice periodicity, without changing the total superlattice thickness. Using this strategy, we tuned the thermal conductivity by 20% at room temperature. We also discuss the role of interface mixing and epitaxial relaxation as an extrinsic, material dependent key parameter for understanding the thermal conductivity of oxide superlattices.

Strong Crystallographic Influence on Spin Hall Mechanism in PLD-Grown IrO2 Thin Films.

Spin-to-charge conversion is a central process in the emerging field of spintronics. One of its main applications is the electrical detection of spin currents, and for this, the inverse spin Hall effect (ISHE) has become one of the preferred methods. We studied the thickness dependence of the ISHE in iridium oxide (IrO2) thin films, producing spin currents by means of the spin Seebeck effect in γ-Fe2O3/IrO2 bilayers prepared by pulsed laser deposition (PLD). The observed ISHE charge current density, which features a maximum as a consequence of the spin diffusion length scale, follows the typical behaviour of spin-Hall-related phenomena. By fitting to the theory developed by Castel et al., we find that the spin Hall angle θSH scales proportionally to the thin film resistivity, θSH∝ρc, and obtains a value for the spin diffusion length λIrO2 of λIrO2=3.3(7) nm. In addition, we observe a negative θSH for every studied thickness and temperature, unlike previously reported works, which brings the possibility of tuning the desired functionality of high-resistance spin-Hall-based devices. We attribute this behaviour to the textured growth of the sample in the context of a highly anisotropic value of the spin Hall conductivity in this material.

Observation of unexpected uniaxial magnetic anisotropy in La2/3Sr1/3MnO3 films by a BaTiO3 overlayer in an artificial multiferroic bilayer.

We studied in detail the in-plane magnetic properties of heterostructures based on a ferroelectric BaTiO3 overlayer deposited on a ferromagnetic La2/3Sr1/3MnO3 film grown epitaxially on pseudocubic (001)-oriented SrTiO3, (LaAlO3)0.3(Sr2TaAlO6)0.7 and LaAlO3 substrates. In this configuration, the combination of both functional perovskites constitutes an artificial multiferroic system with potential applications in spintronic devices based on the magnetoelectric effect. La2/3Sr1/3MnO3 single layers and BaTiO3/La2/3Sr1/3MnO3 bilayers using the pulsed-laser deposition technique. We analyzed the films structurally through X-ray reciprocal space maps and high-angle annular dark field microscopy, and magnetically via thermal demagnetization curves and in-plane magnetization versus applied magnetic field loops at room temperature. Our results indicate that the BaTiO3 layer induces an additional strain in the La2/3Sr1/3MnO3 layers close to their common interface. The presence of BaTiO3 on the surface of tensile-strained La2/3Sr1/3MnO3 films transforms the in-plane biaxial magnetic anisotropy present in the single layer into an in-plane uniaxial magnetic anisotropy. Our experimental evidence suggests that this change in the magnetic anisotropy only occurs in tensile-strained La2/3Sr1/3MnO3 film and is favored by an additional strain on the La2/3Sr1/3MnO3 layer promoted by the BaTiO3 film. These findings reveal an additional mechanism that alters the magnetic behavior of the ferromagnetic layer, and consequently, deserves further in-depth research to determine how it can modify the magnetoelectric coupling of this hybrid multiferroic system.

Chemical Disorder in Topological Insulators: A Route to Magnetism Tolerant Topological Surface States.

We show that the chemical inhomogeneity in ternary three-dimensional topological insulators preserves the topological spin texture of their surface states against a net surface magnetization. The spin texture is that of a Dirac cone with helical spin structure in the reciprocal space, which gives rise to spin-polarized and dissipation-less charge currents. Thanks to the nontrivial topology of the bulk electronic structure, this spin texture is robust against most types of surface defects. However, magnetic perturbations break the time-reversal symmetry, enabling magnetic scattering and loss of spin coherence of the charge carriers. This intrinsic incompatibility precludes the design of magnetoelectronic devices based on the coupling between magnetic materials and topological surface states. We demonstrate that the magnetization coming from individual Co atoms deposited on the surface can disrupt the spin coherence of the carriers in the archetypal topological insulator Bi2Te3, while in Bi2Se2Te the spin texture remains unperturbed. This is concluded from the observation of elastic backscattering events in quasiparticle interference patterns obtained by scanning tunneling spectroscopy. The mechanism responsible for the protection is investigated by energy resolved spectroscopy and ab initio calculations, and it is ascribed to the distorted adsorption geometry of localized magnetic moments due to Se-Te disorder, which suppresses the Co hybridization with the surface states.

Independent Control of the Magnetization in Ferromagnetic La2/3Sr1/3MnO3/SrTiO3/LaCoO3 Heterostructures Achieved by Epitaxial Lattice Mismatch.

We report the effect of interface symmetry-mismatch on the magnetic properties of LaCoO3 (LCO) thin films. Growing epitaxial LCO under tensile strain on top of cubic SrTiO3 (STO) produces a contraction along the c axis and a characteristic ferromagnetic response. However, we report here that ferromagnetism in LCO is completely suppressed when grown on top of a buffer layer of rhombohedral La2/3Sr1/3MnO3 (LSMO), in spite of identical in-plane and out-of-plane lattice deformation. This confirms that it is the lattice symmetry mismatch and not just the total strain, which determines the magnetism of LCO. On the basis of this control over the magnetic properties of LCO, we designed a multilayered structure to achieve independent rotation of the magnetization in ferromagnetic insulating LCO and half-metallic ferromagnet LSMO. This is an important step forward for the design of spin-filtering tunnel barriers based on LCO.

Epitaxial Stabilization of the Perovskite Phase in (Sr(1-x)Ba(x))MnO3 Thin Films.

A novel mechanism of ferroelectricity driven by off-centering magnetic Mn(4+) ions was proposed in (Sr1-xBax)MnO3, in its ideal perovskite phase, which yields enormous expectations in the search for strong magnetoelectric materials. Still, the desired perovskite phase has never been stabilized in thin films due to its extremely metastable character. Here, we report on a thorough study of the perovskite phase stabilization of (Sr1-xBax)MnO3 thin films, 0.2 ≤ x ≤ 0.5, grown by pulsed laser deposition onto (001)-oriented perovskite substrates. X-ray diffraction measurements and scanning transmission electron microscopy reveal that, under appropriate deposition conditions, the perovskite phase is fully stabilized over the nonferroelectric hexagonal phase, despite the latter being increasingly favored on increasing Ba-content. Moreover, we have managed to grow epitaxial coherent cube-on-cube (Sr1-xBax)MnO3 films upon strains ranging from 0% to 4%. Our results become a milestone in further studying perovskite (Sr1-xBax)MnO3 thin films and pave the way for tailoring ferroic and magnetoelectric properties either by strain engineering or Ba-doping.

Observation of the strain induced magnetic phase segregation in manganite thin films.

Epitaxial strain alters the physical properties of thin films grown on single crystal substrates. Thin film oxides are particularly apt for strain engineering new functionalities in ferroic materials. In the case of La(2/3)Ca(1/3)MnO(3) (LCMO) thin films, here we show the first experimental images obtained by electron holography demonstrating that epitaxial strain induces the segregation of a flat and uniform nonferromagnetic layer with antiferromagnetic (AFM) character at the top surface of a ferromagnetic (FM) layer, the whole film being chemical and structurally homogeneous at room temperature. For different substrates and growth conditions the tetragonality of LCMO at room temperature, defined as τ = |c - a|/a, is the driving force for a phase coexistence above an approximate critical value of τC ≈ 0.024. Theoretical calculations prove that the increased tetragonality changes the energy balance of the FM and AFM ground states in strained LCMO, enabling the formation of magnetically inhomogeneous states. This work gives the key evidence that opens a new route to synthesize strain-induced exchanged-biased FM-AFM bilayers in single thin films, which could serve as building blocks of future spintronic devices.

Tunnel conduction in epitaxial bilayers of ferromagnetic LaCoO3/La2/3Sr1/3MnO3 deposited by a chemical solution method.

We report magnetic and electronic transport measurements across epitaxial bilayers of ferromagnetic insulator LaCoO3 and half-metallic ferromagnet La2/3Sr1/3MnO3 (LCO/LSMO: 3.5 nm/20 nm) fabricated by a chemical solution method. The I-V curves at room temperature and 4K measured with conducting atomic force microscopy (CAFM) on well-defined patterned areas exhibit the typical features of a tunneling process. The curves have been fitted to the Simmons model to determine the height (φ) and width (s) of the insulating LCO barrier. The results yield φ = 0.40 ± 0.05 eV (0.50 ± 0.01 eV) at room temperature (4K) and s = 3 nm, in good agreement with the structural analysis. Our results demonstrate that this chemical method is able to produce epitaxial heterostructures with the quality required for this type of fundamental studies and applications.

Enhanced magnetotransport in nanopatterned manganite nanowires.

We have combined optical and focused ion beam lithographies to produce large aspect-ratio (length-to-width >300) single-crystal nanowires of La2/3Ca1/3MnO3 that preserve their functional properties. Remarkably, an enhanced magnetoresistance value of 34% in an applied magnetic field of 0.1 T in the narrowest 150 nm nanowire is obtained. The strain release at the edges together with a destabilization of the insulating regions is proposed to account for this behavior. This opens new strategies to implement these structures in functional spintronic devices.

Conductance steps in electromigrated Bi nanoconstrictions.

Bismuth nanostructures of initial lateral size of about 150 nm were successfully electromigrated at room temperature under high vacuum conditions through the application of voltage ramps and accurate control of their conductance. The imaging of the nanogap formation was followed by scanning electron microscopy. An appropriate design of the initial Bi nanostructures has made the electromigration process of semimetallic Bi feasible. Beyond the intrinsic interest in the generation of Bi structures with size tailored at the nanoscale, remarkable features have been observed in the time-dependent conductance curves of the Bi nanoconstrictions. In particular, sub-quantum conductance plateaus can be detected before the rupture of the constriction. An alternative procedure to study the transport through Bi nanoconstrictions has been explored using a focused-Ga-ion etching process with simultaneous control of the conductance. This second approach confirms the transport behavior observed in electromigrated Bi nanoconstrictions.

Structural distortion, charge modulation and local anisotropies in magnetite below the Verwey transition using resonant X-ray scattering.

The pattern of charge modulations and local anisotropies below the Verwey transition has been determined and quantified in high-quality Fe(3)O(4) single crystals and thin films grown on MgO by using resonant X-ray scattering at the Fe K-edge. The energy, polarization and azimuthal angle dependencies of an extensive set of reflections with potential sensitivity to charge or local anisotropy orderings have been analyzed to explore their origins. A charge disproportion on octahedral B sites of 0.20 ± 0.05 e(-) with [0 0 1] and [1 1 0] cubic periodicities has been confirmed, while no significant charge disproportion has been obtained with [0 0 1/2] cubic periodicity. Additional charge modulations in the monoclinic a-b plane are also present. In addition, the occurrence of new forbidden (1, 1, 0) and (0, 0, 2n + 1/2) cubic reflections that arise from the anisotropy of the local structure around different tetrahedral and octahedral Fe atoms is shown. This complex pattern of weak charge modulations and local anisotropies is fully compatible with the low-temperature crystal structure refined in the non-polar C2/c space group and disproves any bimodal charge disproportion of the octahedral Fe atoms.