Optimized Route for the Fabrication of MnAlC Permanent Magnets by Arc Melting.

The rare-earth-free MnAlC alloy is currently considered a very promising candidate for permanent magnet applications due to its high anisotropy field and relatively high saturation magnetization and Curie temperature, besides being a low-cost material. In this work, we presented a simple fabrication route that allows for obtaining a magnetically enhanced bulk τ-MnAlC magnet. In the fabrication process, an electric arc-melting method was carried out to melt ingots of MnAlC alloys. A two-step solution treatment at 1200 °C and 1100 °C allowed us to synthesize a pure room-temperature ε-MnAlC ingot that completely transformed into τ-MnAlC alloy, free of secondary phases, after an annealing treatment at 550 °C for 30 min. The Rietveld refinements and magnetization measurements demonstrated that the quenched process produces a phase-segregated ε-MnAlC alloy that is formed by two types of ε-phases due to local fluctuation of the Mn. Room-temperature hysteresis loops showed that our improved τ-MnAlC alloy exhibited a remanent magnetization of 42 Am2/kg, a coercive field of 0.2 T and a maximum energy product, (BH)max, of 6.07 kJ/m3, which is higher than those reported in previous works using a similar preparation route. Experimental evidence demonstrated that the synthesis of a pure room-temperature ε-MnAlC played an important role in the suppression of undesirable phases that deteriorate the permanent magnet properties of the τ-MnAlC. Finally, magnetic images recorded by Lorentz microscopy allowed us to observe the microstructure and magnetic domain walls of the optimized τ-MnAlC. The presence of magnetic contrasts in all the observed grains allowed us to confirm the high-quality ferromagnetic behavior of the system.

Defect-induced monopole injection and manipulation in artificial spin ice.

Lithographically defined arrays of nanomagnets are well placed for application in areas such as probabilistic computing or reconfigurable magnonics due to their emergent collective dynamics and writable magnetic order. Among them are artificial spin ice (ASI), which are arrays of binary in-plane macrospins exhibiting geometric frustration at the vertex interfaces. Macrospin flips in the arrays create topologically protected magnetic charges, or emergent monopoles, which are bound to an antimonopole to conserve charge. In the absence of controllable pinning, it is difficult to manipulate individual monopoles in the array without also influencing other monopole excitations or the counter-monopole charge. Here, we tailor the local magnetic order of a classic ASI lattice by introducing a ferromagnetic defect with shape anisotropy into the array. This creates monopole injection sites at nucleation fields below the critical lattice switching field. Once formed, the high energy monopoles are fixed to the defect site and may controllably propagate through the lattice under stimulation. Defect programing of bound monopoles within the array allows fine control of the pathways of inverted macrospins. Such control is a necessary prerequisite for the realization of functional devices, e. g. reconfigurable waveguide in nanomagnonic applications.

Key Signatures of Magnetofossils Elucidated by Mutant Magnetotactic Bacteria and Micromagnetic Calculations.

Magnetotactic bacteria (MTB) produce single-stranded or multi-stranded chains of magnetic nanoparticles that contribute to the magnetization of sediments and rocks. Their magnetic fingerprint can be detected in ancient geological samples and serve as a unique biosignature of microbial life. However, some fossilized assemblages bear contradictory signatures pointing to magnetic components that have distinct origin(s). Here, using micromagnetic simulations and mutant MTB producing looped magnetosome chains, we demonstrate that the observed magnetofossil fingerprints are produced by a mixture of single-stranded and multi-stranded chains, and that diagenetically induced chain collapse, if occurring, must preserve the strong uniaxial anisotropy of native chains. This anisotropy is the key factor for distinguishing magnetofossils from other populations of natural magnetite particles, including those with similar individual crystal characteristics. Furthermore, the detailed properties of magnetofossil signatures depend on the proportion of equant and elongated magnetosomes, as well as on the relative abundances of single-stranded and multi-stranded chains. This work has important paleoclimatic, paleontological, and phylogenetic implications, as it provides reference data to differentiate distinct MTB lineages according to their chain and magnetosome morphologies, which will enable the tracking of the evolution of some of the most ancient biomineralizing organisms in a time-resolved manner. It also enables a more accurate discrimination of different sources of magnetite particles, which is pivotal for gaining better environmental and relative paleointensity reconstructions from sedimentary records.

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.

Customized MFM probes based on magnetic nanorods.

Focused Electron Beam Induced Deposition (FEBID) for magnetic tip fabrication is presented in this work as an alternative to conventional sputtering-based Magnetic Force Microscopy (MFM) tips. FEBID enables the growth of a high-aspect-ratio magnetic nanorod with customized geometry and composition to overcome the key technical limitations of MFM probes currently on the market. The biggest advantage of these tips, in comparison with CoCr coated pyramidal probes, lies in the capability of creating sharp ends, nearly 10 nm in diameter, which provides remarkable (topographic and magnetic) lateral resolution in samples with magnetic features close to the resolution limits of the MFM technique itself. The shape of the nanorods produces a very confined magnetic stray field, whose interaction with the sample is extremely localized and perpendicular to the surface, with negligible in-plane components. This effect can lead to a better analytical and numerical modelling of the MFM probes and to an increase in the sensitivity without perturbing the magnetic configuration of soft samples. Besides, the high-aspect ratio achievable in FEBID nanorod tips makes them magnetically harder than the commercial ones, reaching coercive fields higher than 900 Oe. According to the results shown, tips based on magnetic nanorods grown by FEBID can be eventually used for quantitative analysis in MFM measurements. Moreover, the customized growth of Co- or Fe-based tips onto levers with different mechanical properties allows MFM studies that demand different measuring conditions. To showcase the versatility of this type of probe, as a last step, MFM is performed in a liquid environment, which still remains a challenge for the MFM community largely due to the lack of appropriate probes on the market. This opens up new possibilities in the investigation of magnetic biological samples.

Exotic Transverse-Vortex Magnetic Configurations in CoNi Nanowires.

The magnetic configurations of cylindrical Co-rich CoNi nanowires have been quantitatively analyzed at the nanoscale by electron holography and correlated to local structural and chemical properties. The nanowires display grains of both face-centered cubic (fcc) and hexagonal close packed (hcp) crystal structures, with grain boundaries parallel to the nanowire axis direction. Electron holography evidences the existence of a complex exotic magnetic configuration characterized by two distinctly different types of magnetic configurations within a single nanowire: an array of periodical vortices separating small transverse domains in hcp-rich regions with perpendicular easy axis orientation and a mostly axial configuration parallel to the nanowire axis in regions with fcc grains. These vastly different domains are found to be caused by local variations in the chemical composition modifying the crystalline orientation and/or structure, which give rise to change in magnetic anisotropies. Micromagnetic simulations, including the structural properties that have been experimentally determined, allow for a deeper understanding of the complex magnetic states observed by electron holography.

Magnetic imaging using geometrically constrained nano-domain walls.

Magnetic nanostructures, as part of hybrid CMOS technology, have the potential to overcome silicon's scaling limit. However, a major problem is how to characterize their magnetization without disturbing it. Magnetic force microscopy (MFM) offers a convenient way of studying magnetization, but spatial resolution and sensitivity are usually boosted at the cost of increasing probe-sample interaction. By using a single magnetic domain wall (DW), confined in a V-shape nanostructure fabricated at the probe apex, it is demonstrated here that the spatial resolution and the magnetic sensitivity can be decoupled and both enhanced. Indeed, owing to the nanostructure's strong shape anisotropy, DW-probes have 2 high and 2 low magnetic moment states with opposite polarities, characterised by a geometrically constrained pinned DW, and curled magnetization, respectively. Electron holography studies, supported by numerical simulations, and in situ MFM show that the DW-probe state can be controlled, and thus used as a switchable tool with a low/high stray field intensity.

Calibration of multi-layered probes with low/high magnetic moments.

We present a comprehensive method for visualisation and quantification of the magnetic stray field of magnetic force microscopy (MFM) probes, applied to the particular case of custom-made multi-layered probes with controllable high/low magnetic moment states. The probes consist of two decoupled magnetic layers separated by a non-magnetic interlayer, which results in four stable magnetic states: ±ferromagnetic (FM) and ±antiferromagnetic (A-FM). Direct visualisation of the stray field surrounding the probe apex using electron holography convincingly demonstrates a striking difference in the spatial distribution and strength of the magnetic flux in FM and A-FM states. In situ MFM studies of reference samples are used to determine the probe switching fields and spatial resolution. Furthermore, quantitative values of the probe magnetic moments are obtained by determining their real space tip transfer function (RSTTF). We also map the local Hall voltage in graphene Hall nanosensors induced by the probes in different states. The measured transport properties of nanosensors and RSTTF outcomes are introduced as an input in a numerical model of Hall devices to verify the probe magnetic moments. The modelling results fully match the experimental measurements, outlining an all-inclusive method for the calibration of complex magnetic probes with a controllable low/high magnetic moment.

Quantitative Nanoscale Magnetic Study of Isolated Diameter-Modulated FeCoCu Nanowires.

The comprehension of the magnetic configuration in FeCoCu nanowires with a diameter-modulated cylindrical geometry will allow controlling the domain wall motion in this low-dimensional system under the application of magnetic fields and/or the injection of current pulses. Here we perform a quantitative magnetic characterization of isolated diameter-modulated FeCoCu nanowires by combining nanoscale magnetic characterization techniques such as electron holography, magnetic force microscopy, and micromagnetic simulations. Local reconstructions of the magnetic distribution show the diameter-modulated geometry of the wires induces the formation of vortex-like structures and magnetic charges in the regions where the diameter is varied. Vortex-like structures modify the axial alignment of the magnetization in large-diameter segments. Moreover, the magnetic charges control the demagnetizing field distribution, promoting a flux-closure stray field configuration around large-diameter segments and keeping the demagnetizing field parallel to the NW's magnetization around small diameter segments. The detailed description of the remanent state in diameter-modulated cylindrical FeCoCu nanowires allows us to provide a clear explanation of the origin of bright and dark contrast observed in magnetic force microscopy images, which have the same feature of magnetic domain walls. This work establishes the primary knowledge required for future magnetization reversal studies with the aim of searching efficient modulated geometries that allow an optimum and controlled domain wall propagation.

Realization of a tilted reference wave for electron holography by means of a condenser biprism.

As proposed recently, a tilted reference wave in off-axis electron holography is expected to be useful for aberration measurement and correction. Furthermore, in dark-field electron holography, it is considered to replace the reference wave, which is conventionally diffracted in an unstrained object area, by a well-defined object-independent reference wave. Here, we first realize a tilted reference wave by employing a biprism placed in the condenser system above three condenser lenses producing a relative tilt magnitude up to 20/nm at the object plane (300kV). Paraxial ray-tracing predicts condenser settings for a parallel illumination at the object plane, where only one half of the round illumination disc is tilted relative to the optical axis without displacement. Holographic measurements verify the kink-like phase modulation of the incident beam and return the interference fringe contrast as a function of the relative tilt between both parts of the illumination. Contrast transfer theory including condenser aberrations and biprism instabilities was applied to explain the fringe contrast measurement. A first dark-field hologram with a tilted - object-free - reference wave was acquired and reconstructed. A new application for bright/dark-field imaging is presented.

Size-Specific Spin Configurations in Single Iron Nanomagnet: From Flower to Exotic Vortices.

The different spin configurations in the vicinity of the single-domain/vortex transition are reported in isolated magnetic nanoparticles. By combining chemical synthesis, electron holography in a dedicated transmission electron microscope and micromagnetic simulations, we establish the "magnetic configurations vs size" phase diagram of Fe single-crystalline nanocubes. Room temperature high resolution magnetic maps reveal the transition between single-domain and vortex states for Fe nanocubes from 25 to 27 nm, respectively. An intermediate spin configuration consisting of an ⟨111⟩ vortex is for the first time evidenced.

Development of splitting convergent beam electron diffraction (SCBED).

Using a combination of condenser electrostatic biprism with dedicated electron optic conditions for sample illumination, we were able to split a convergent beam electron probe focused on the sample in two half focused probes without introducing any tilt between them. As a consequence, a combined convergent beam electron diffraction pattern is obtained in the back focal plane of the objective lens arising from two different sample areas, which could be analyzed in a single pattern. This splitting convergent beam electron diffraction (SCBED) pattern has been tested first on a well-characterized test sample of Si/SiGe multilayers epitaxially grown on a Si substrate. The SCBED pattern contains information from the strained area, which exhibits HOLZ lines broadening induced by surface relaxation, with fine HOLZ lines observed in the unstrained reference part of the sample. These patterns have been analyzed quantitatively using both parts of the SCBED transmitted disk. The fine HOLZ line positions are used to determine the precise acceleration voltage of the microscope while the perturbed HOLZ rocking curves in the stained area are compared to dynamical simulated ones. The combination of these two information leads to a precise evaluation of the sample strain state. Finally, several SCBED setups are proposed to tackle fundamental physics questions as well as applied materials science ones and demonstrate how SCBED has the potential to greatly expand the range of applications of electron diffraction and electron holography.

Oriented Metallic Nano-Objects on Crystalline Surfaces by Solution Epitaxial Growth.

Chemical methods offer the possibility to synthesize a large panel of nanostructures of various materials with promising properties. One of the main limitations to a mass market development of nanostructure based devices is the integration at a moderate cost of nano-objects into smart architectures. Here we develop a general approach by adapting the seed-mediated solution phase synthesis of nanocrystals in order to directly grow them on crystalline thin films. Using a Co precursor, single-crystalline Co nanowires are directly grown on metallic films and present different spatial orientations depending on the crystalline symmetry of the film used as a 2D seed for Co nucleation. Using films exposing 6-fold symmetry surfaces such as Pt(111), Au(111), and Co(0001), the Co heterogeneous nucleation and epitaxial growth leads to vertical nanowires self-organized in dense and large scale arrays. On the other hand, using films presenting 4-fold symmetry surfaces such as Pt(001) and Cu(001), the Co growth leads to slanted wires in discrete directions. The generality of the concept is demonstrated with the use of a Fe precursor which results in Fe nanostructures on metallic films with different growth orientations which depend on the 6-fold/4-fold symmetry of the film. This approach of solution epitaxial growth combines the advantages of chemistry in solution in producing shape-controlled and monodisperse metallic nanocrystals, and of seeded growth on an ad hoc metallic film that efficiently controls orientation through epitaxy. It opens attractive opportunities for the integration of nanocrystals in planar devices.

Influence of the shape and surface oxidation in the magnetization reversal of thin iron nanowires grown by focused electron beam induced deposition.

Iron nanostructures grown by focused electron beam induced deposition (FEBID) are promising for applications in magnetic sensing, storage and logic. Such applications require a precise design and determination of the coercive field (H C), which depends on the shape of the nanostructure. In the present work, we have used the Fe2(CO)9 precursor to grow iron nanowires by FEBID in the thickness range from 10 to 45 nm and width range from 50 to 500 nm. These nanowires exhibit an Fe content between 80 and 85%, thus giving a high ferromagnetic signal. Magneto-optical Kerr characterization indicates that H C decreases for increasing thickness and width, providing a route to control the magnetization reversal field through the modification of the nanowire dimensions. Transmission electron microscopy experiments indicate that these wires have a bell-type shape with a surface oxide layer of about 5 nm. Such features are decisive in the actual value of H C as micromagnetic simulations demonstrate. These results will help to make appropriate designs of magnetic nanowires grown by FEBID.

Crystal growth of bullet-shaped magnetite in magnetotactic bacteria of the Nitrospirae phylum.

Magnetotactic bacteria (MTB) are known to produce single-domain magnetite or greigite crystals within intracellular membrane organelles and to navigate along the Earth's magnetic field lines. MTB have been suggested as being one of the most ancient biomineralizing metabolisms on the Earth and they represent a fundamental model of intracellular biomineralization. Moreover, the determination of their specific crystallographic signature (e.g. structure and morphology) is essential for palaeoenvironmental and ancient-life studies. Yet, the mechanisms of MTB biomineralization remain poorly understood, although this process has been extensively studied in several cultured MTB strains in the Proteobacteria phylum. Here, we show a comprehensive transmission electron microscopy (TEM) study of magnetic and structural properties down to atomic scales on bullet-shaped magnetites produced by the uncultured strain MYR-1 belonging to the Nitrospirae phylum, a deeply branching phylogenetic MTB group. We observed a multiple-step crystal growth of MYR-1 magnetite: initial isotropic growth forming cubo-octahedral particles (less than approx. 40 nm), subsequent anisotropic growth and a systematic final elongation along [001] direction. During the crystal growth, one major {111} face is well developed and preserved at the larger basal end of the crystal. The basal {111} face appears to be terminated by a tetrahedral-octahedral-mixed iron surface, suggesting dimensional advantages for binding protein(s), which may template the crystallization of magnetite. This study offers new insights for understanding magnetite biomineralization within the Nitrospirae phylum.

3D Magnetic Induction Maps of Nanoscale Materials Revealed by Electron Holographic Tomography.

The investigation of three-dimensional (3D) ferromagnetic nanoscale materials constitutes one of the key research areas of the current magnetism roadmap and carries great potential to impact areas such as data storage, sensing, and biomagnetism. The properties of such nanostructures are closely connected with their 3D magnetic nanostructure, making their determination highly valuable. Up to now, quantitative 3D maps providing both the internal magnetic and electric configuration of the same specimen with high spatial resolution are missing. Here, we demonstrate the quantitative 3D reconstruction of the dominant axial component of the magnetic induction and electrostatic potential within a cobalt nanowire (NW) of 100 nm in diameter with spatial resolution below 10 nm by applying electron holographic tomography. The tomogram was obtained using a dedicated TEM sample holder for acquisition, in combination with advanced alignment and tomographic reconstruction routines. The powerful approach presented here is widely applicable to a broad range of 3D magnetic nanostructures and may trigger the progress of novel spintronic nonplanar nanodevices.

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.

Solution epitaxial growth of cobalt nanowires on crystalline substrates for data storage densities beyond 1 Tbit/in2.

The implementation of nano-objects in numerous emerging applications often demands their integration in macroscopic devices. Here we present the bottom-up epitaxial solution growth of high-density arrays of vertical 5 nm diameter single-crystalline metallic cobalt nanowires on wafer-scale crystalline metal surfaces. The nanowires form regular hexagonal arrays on unpatterned metallic films. These hybrid heterostructures present an important perpendicular magnetic anisotropy and pave the way to a high density magnetic recording device, with capacities above 10 Terabits/in(2). This method bypasses the need of assembling and orientating free colloidal nanocrystals on surfaces. Its generalization to other materials opens new perspectives toward many applications.

Imaging the fine structure of a magnetic domain wall in a Ni nanocylinder.

We present the first experimental imaging of the internal DW structure in 55 and 85 nm diameter Ni nanocylinders, using electron holography combined with micromagnetic calculations. We demonstrate the magnetic transition from a hybrid magnetic state with both vortex and transverse DW in 85 nm diameter Ni nanocylinders to a pure transverse wall in thinner nanowires. This is particularly important as DWs in nanocylinders are model systems to go beyond the classical Walker limit.