Formation of precipitates in off-stoichiometric Ni-Mn-Sn Heusler alloys probed through the induced Sn-moment.

The shell-ferromagnetic effect originates from the segregation process in off-stoichiometric Ni-Mn-based Heusler alloys. In this work, we investigate the precipitation process of L21-ordered Ni2MnSn and L10-ordered NiMn in off-stoichiometric Ni50Mn45Sn5 during temper annealing, by X-ray diffraction (XRD) and 119Sn Mössbauer spectroscopy. While XRD probes long-range ordering of the lattice structure, Mössbauer spectroscopy probes nearest-neighbour interactions, reflected in the induced Sn magnetic moment. As shown in this work, the induced magnetic Sn moment can be used as a detector for microscopic structural changes and is, therefore, a powerful tool for investigating the formation of nano-precipitates. Similar research can be performed in the future, for example, on different pinning type magnets like Sm-Co or Nd-Fe-B.

Element-specific visualization of dynamic magnetic coupling in a Co/Py bilayer microstructure.

We present the element-specific and time resolved visualization of uniform ferromagnetic resonance excitations of a Permalloy (Py) disk-Cobalt (Co) stripe bilayer microstructure. The transverse high frequency component of the resonantly excited magnetization is sampled in the ps regime by a combination of ferromagnetic resonance (FMR) and scanning transmission X-ray microscopy (STXM-FMR) recording snapshots of the local magnetization precession of Py and Co with nanometer spatial resolution. The approach allows us to individually image the resonant dynamic response of each element, and we find that angular momentum is transferred from the Py disk to the Co stripe and vice versa at their respective resonances. The integral (cavity) FMR spectrum of our sample shows an unexpected additional third resonance. This resonance is observed in the STXM-FMR experiments as well. Our microscopic findings suggest that it is governed by magnetic exchange between Py and Co, showing for the Co stripe a difference in relative phase of the magnetization due to stray field influence.

Effect of High-Pressure Torsion on the Microstructure and Magnetic Properties of Nanocrystalline CoCrFeNiGax (x = 0.5, 1.0) High Entropy Alloys.

In our search for an optimum soft magnet with excellent mechanical properties which can be used in applications centered around "electro mobility", nanocrystalline CoCrFeNiGax (x = 0.5, 1.0) bulk high entropy alloys (HEA) were successfully produced by spark plasma sintering (SPS) at 1073 K of HEA powders produced by high energy ball milling (HEBM). SPS of non-equiatomic CoCrFeNiGa0.5 particles results in the formation of a single-phase fcc bulk HEA, while for the equiatomic CoCrFeNiGa composition a mixture of bcc and fcc phases was found. For both compositions SEM/EDX analysis showed a predominant uniform distribution of the elements with only a small number of Cr-rich precipitates. High pressure torsion (HPT) of the bulk samples led to an increased homogeneity and a grain refinement: i.e., the crystallite size of the single fcc phase of CoCrFeNiGa0.5 decreased by a factor of 3; the crystallite size of the bcc and fcc phases of CoCrFeNiGa-by a factor of 4 and 10, respectively. The lattice strains substantially increased by nearly the same extent. After HPT the saturation magnetization (Ms) of the fcc phase of CoCrFeNiGa0.5 and its Curie temperature increased by 17% (up to 35 Am2/kg) and 31.5% (from 95 K to 125 K), respectively, whereas the coercivity decreased by a factor of 6. The overall Ms of the equiatomic CoCrFeNiGa decreased by 34% and 55% at 10 K and 300 K, respectively. At the same time the coercivity of CoCrFeNiGa increased by 50%. The HPT treatment of SPS-consolidated HEAs increased the Vickers hardness (Hv) by a factor of two (up to 5.632 ± 0.188) only for the non-equiatomic CoCrFeNiGa0.5, while for the equiatomic composition, the Hv remained unchanged (6.343-6.425 GPa).

Magnetic phase diagram of (Mo2/3RE1/3)2AlC, RE=Tb and Dy, studied by magnetization, specific heat, and neutron diffraction analysis.

We report the results of magnetization, heat capacity, and neutron diffraction measurements on (Mo2/3RE1/3)2AlC with RE = Dy and Tb. Temperature and field-dependent magnetization as well as heat capacity were measured on a powder sample and on a single crystal allowing the construction of the magnetic field-temperature phase diagram. To study the magnetic structure of each magnetic phase, we applied neutron diffraction in a magnetic field up to 6 T. For (Mo2/3Dy1/3)2AlC in zero field, a spin density wave is stabilized at 16 K, with antiferromagnetic ordering at 13 K. Furthermore, we identify the coexistence of ferromagnetic and antiferromagnetic phases induced by magnetic fields for both RE = Tb and Dy. The origin of the field induced phases is resulting from the competing ferromagnetic and antiferromagnetic interactions.

The effect of the composition and pressure on the phase stability and electronic, magnetic, and elastic properties of M2AX (M = Mn, Fe; A = Al, Ga, Si, Ge; X = C, N) phases.

The magnetic properties of M2AX (M = Mn, Fe; A = Al, Ga, Si, Ge; X = C, N) phases were studied within DFT-GGA. The magnetic electronic ground state is determined. The investigation of the phase stability of M2AX phases is performed by comparing the total energy of MAX phases to that of the set of competitive phases for calculation of the phase formation enthalpy. As the result of such an approach, we have found one stable compound (Mn2GaC), and seven metastable ones. It is shown that several metastable MAX phases (Mn2AlC, Fe2GaC, Mn2GeC, and Mn2GeN) become stable at a small applied pressure (1.5-7 GPa). The mechanical, electronic and elastic properties of metastable MAX phases are studied.

Magnetic Nanoprobes for Spatio-Mechanical Manipulation in Single Cells.

Magnetic nanoparticles (MNPs) are widely known as valuable agents for biomedical applications. Recently, MNPs were further suggested to be used for a remote and non-invasive manipulation, where their spatial redistribution or force response in a magnetic field provides a fine-tunable stimulus to a cell. Here, we investigated the properties of two different MNPs and assessed their suitability for spatio-mechanical manipulations: semisynthetic magnetoferritin nanoparticles and fully synthetic 'nanoflower'-shaped iron oxide nanoparticles. As well as confirming their monodispersity in terms of structure, surface potential, and magnetic response, we monitored the MNP performance in a living cell environment using fluorescence microscopy and asserted their biocompatibility. We then demonstrated facilitated spatial redistribution of magnetoferritin compared to 'nanoflower'-NPs after microinjection, and a higher magnetic force response of these NPs compared to magnetoferritin inside a cell. Our remote manipulation assays present these tailored magnetic materials as suitable agents for applications in magnetogenetics, biomedicine, or nanomaterial research.

Formation of Fe-Ni Nanoparticle Strands in Macroscopic Polymer Composites: Experiment and Simulation.

Magnetic-field-induced strand formation of ferromagnetic Fe-Ni nanoparticles in a PMMA-matrix is correlated with the intrinsic material parameters, such as magnetization, particle size, composition, and extrinsic parameters, including magnetic field strength and viscosity. Since various factors can influence strand formation, understanding the composite fabrication process that maintains the strand lengths of Fe-Ni in the generated structures is a fundamental step in predicting the resulting structures. Hence, the critical dimensions of the strands (length, width, spacing, and aspect ratio) are investigated in the experiments and simulated via different intrinsic and extrinsic parameters. Optimal parameters were found by optical microscopy measurements and finite-element simulations using COMSOL for strand formation of Fe50Ni50 nanoparticles. The anisotropic behavior of the aligned strands was successfully characterized through magnetometry measurements. Compared to the unaligned samples, the magnetically aligned strands exhibit enhanced conductivity, increasing the current by a factor of 1000.

Towards laser printing of magnetocaloric structures by inducing a magnetic phase transition in iron-rhodium nanoparticles.

The development of magnetocaloric materials represents an approach to enable efficient and environmentally friendly refrigeration. It is envisioned as a key technology to reduce CO2 emissions of air conditioning and cooling systems. Fe-Rh has been shown to be one of the best-suited materials in terms of heat exchange per material volume. However, the Fe-Rh magnetocaloric response depends on its composition. Hence, the adaptation of material processing routes that preserve the Fe-Rh magnetocaloric response in the generated structures is a fundamental step towards the industrial development of this cooling technology. To address this challenge, the temperature-dependent properties of laser synthesized Fe-Rh nanoparticles and the laser printing of Fe-Rh nanoparticle inks are studied to generate 2D magnetocaloric structures that are potentially interesting for applications such as waste heat management of compact electrical appliances or thermal diodes, switches, and printable magnetocaloric media. The magnetization and temperature dependence of the ink's γ-FeRh to B2-FeRh magnetic transition is analyzed throughout the complete process, finding a linear increase of the magnetization M (0.8 T, 300 K) up to 96 Am2/kg with ca. 90% of the γ-FeRh being transformed permanently into the B2-phase. In 2D structures, magnetization values of M (0.8 T, 300 K) ≈ 11 Am2/kg could be reached by laser sintering, yielding partial conversion to the B2-phase equivalent to long-time heating temperature of app. 600 K, via this treatment. Thus, the proposed procedure constitutes a robust route to achieve the generation of magnetocaloric structures.

Room temperature synthesized solid solution AuFe nanoparticles and their transformation into Au/Fe Janus nanocrystals.

Solid solution AuFe nanoparticles were synthesized for the first time under ambient conditions by an adapted method previously established for the Fe3O4-Au core-shell morphology. These AuFe particles preserved the fcc structure of Au incorporated with paramagnetic Fe atoms. The metastable AuFe can be segregated by transformation into Janus Au/Fe particles with bcc Fe and fcc Au upon annealing. The ferromagnetic Fe was epitaxially grown on low index fcc Au planes. This preparation route delivers new perspective materials for magnetoplasmonics and biomedical applications and suggests the reconsideration of existing protocols for magnetite-gold core-shell synthesis.

Dipolar-stabilized first and second-order antiskyrmions in ferrimagnetic multilayers.

Skyrmions and antiskyrmions are topologically protected spin structures with opposite vorticities. Particularly in coexisting phases, these two types of magnetic quasi-particles may show fascinating physics and potential for spintronic devices. While skyrmions are observed in a wide range of materials, until now antiskyrmions were exclusive to materials with D2d symmetry. In this work, we show first and second-order antiskyrmions stabilized by magnetic dipole-dipole interaction in Fe/Gd-based multilayers. We modify the magnetic properties of the multilayers by Ir insertion layers. Using Lorentz transmission electron microscopy imaging, we observe coexisting antiskyrmions, Bloch skyrmions, and type-2 bubbles and determine the range of material properties and magnetic fields where the different spin objects form and dissipate. We perform micromagnetic simulations to obtain more insight into the studied system and conclude that the reduction of saturation magnetization and uniaxial magnetic anisotropy leads to the existence of this zoo of different spin objects and that they are primarily stabilized by dipolar interaction.

Long-Range Ordering Effects in Magnetic Nanoparticles.

The challenge for synthesizing magnetic nanoparticle chains may be achieved under the application of fixation fields, which are the externally applied fields, enhancing collective magnetic features due to adequate control of dipolar interactions among magnetic nanoparticles. However, relatively little attention has been devoted to how size, concentration of magnetic nanoparticles, and intensity of an external magnetic field affect the evolution of chain structures and collective magnetic features. Here, iron oxide nanoparticles are developed by the coprecipitation method at diameters below (10 and 20 nm) and above (50 and 80 nm) their superparamagnetic limit (at about 25 nm) and then are subjected to a tunable fixation field (40-400 mT). Eventually, the fixation field dictates smaller particles to form chain structures in two steps, first forming clusters and then guiding chain formation via "cluster-cluster" interactions, whereas larger particles readily form chains via "particle-particle" interactions. In both cases, dipolar interactions between the neighboring nanoparticles augment, leading to a substantial increase in their collective magnetic features which in turn results in magnetic particle hyperthermia efficiency enhancement of up to one order of magnitude. This study provides new perspectives for magnetic nanoparticles by arranging them in chain formulations as enhanced performance magnetic actors in magnetically driven magnetic applications.

Magnetic Nanoparticles as a Tool for Remote DNA Manipulations at a Single-Molecule Level.

Remote control of cells and single molecules by magnetic nanoparticles in nonheating external magnetic fields is a perspective approach for many applications such as cancer treatment and enzyme activity regulation. However, the possibility and mechanisms of direct effects of small individual magnetic nanoparticles on such processes in magneto-mechanical experiments still remain unclear. In this work, we have shown remote-controlled mechanical dissociation of short DNA duplexes (18-60 bp) under the influence of nonheating low-frequency alternating magnetic fields using individual 11 nm magnetic nanoparticles. The developed technique allows (1) simultaneous manipulation of millions of individual DNA molecules and (2) evaluation of energies of intermolecular interactions in short DNA duplexes or in other molecules. Finally, we have shown that DNA duplexes dissociation is mediated by mechanical stress and produced by the movement of magnetic nanoparticles in magnetic fields, but not by local overheating. The presented technique opens a new avenue for high-precision manipulation of DNA and generation of biosensors for quantification of energies of intermolecular interaction.

Asymmetric Interfaces in Epitaxial Off-Stoichiometric Fe3+xSi1-x/Ge/Fe3+xSi1-x Hybrid Structures: Effect on Magnetic and Electric Transport Properties.

Three-layer iron-rich Fe3+xSi1-x/Ge/Fe3+xSi1-x (0.2 < x < 0.64) heterostructures on a Si(111) surface with Ge thicknesses of 4 nm and 7 nm were grown by molecular beam epitaxy. Systematic studies of the structural and morphological properties of the synthesized samples have shown that an increase in the Ge thickness causes a prolonged atomic diffusion through the interfaces, which significantly increases the lattice misfits in the Ge/Fe3+xSi1-x heterosystem due to the incorporation of Ge atoms into the Fe3+xSi1-x bottom layer. The resultant lowering of the total free energy caused by the development of the surface roughness results in a transition from an epitaxial to a polycrystalline growth of the upper Fe3+xSi1-x. The average lattice distortion and residual stress of the upper Fe3+xSi1-x were determined by electron diffraction and theoretical calculations to be equivalent to 0.2 GPa for the upper epitaxial layer with a volume misfit of -0.63% compared with a undistorted counterpart. The volume misfit follows the resultant interatomic misfit of |0.42|% with the bottom Ge layer, independently determined by atomic force microscopy. The variation in structural order and morphology significantly changes the magnetic properties of the upper Fe3+xSi1-x layer and leads to a subtle effect on the transport properties of the Ge layer. Both hysteresis loops and FMR spectra differ for the structures with 4 nm and 7 nm Ge layers. The FMR spectra exhibit two distinct absorption lines corresponding to two layers of ferromagnetic Fe3+xSi1-x films. At the same time, a third FMR line appears in the sample with the thicker Ge. The angular dependences of the resonance field of the FMR spectra measured in the plane of the film have a pronounced easy-axis type anisotropy, as well as an anisotropy corresponding to the cubic crystal symmetry of Fe3+xSi1-x, which implies the epitaxial orientation relationship of Fe3+xSi1-x (111)[0-11] || Ge(111)[1-10] || Fe3+xSi1-x (111)[0-11] || Si(111)[1-10]. Calculated from ferromagnetic resonance (FMR) data saturation magnetization exceeds 1000 kA/m. The temperature dependence of the electrical resistivity of a Ge layer with thicknesses of 4 nm and 7 nm is of semiconducting type, which is, however, determined by different transport mechanisms.

Controlling the Oxidation of Magnetic and Electrically Conductive Solid-Solution Iron-Rhodium Nanoparticles Synthesized by Laser Ablation in Liquids.

This study focuses on the synthesis of FeRh nanoparticles via pulsed laser ablation in liquid and on controlling the oxidation of the synthesized nanoparticles. Formation of monomodal γ-FeRh nanoparticles was confirmed by transmission electron microscopy (TEM) and their composition confirmed by atom probe tomography (APT). For these particles, three major contributors to oxidation were analysed: (1) dissolved oxygen in the organic solvents, (2) the bound oxygen in the solvent and (3) oxygen in the atmosphere above the solvent. The decrease of oxidation for optimized ablation conditions was confirmed through energy-dispersive X-ray (EDX) and Mössbauer spectroscopy. Furthermore, the time dependence of oxidation was monitored for dried FeRh nanoparticles powders using ferromagnetic resonance spectroscopy (FMR). By magnetophoretic separation, B2-FeRh nanoparticles could be extracted from the solution and characteristic differences of nanostrand formation between γ-FeRh and B2-FeRh nanoparticles were observed.

Dynamics of chiral state transitions and relaxations in an FeGe thin plate via in situ Lorentz microscopy.

Studying the magnetic transition between different topological spin textures in noncentrosymmetric magnets under external stimuli is an important topic in chiral magnetism. Here, using in situ Lorentz transmission electron microscopy (LTEM) we directly visualize the thermal-driven magnetic transitions and dynamic characteristics in FeGe thin plates. A novel protocol-dependent phase diagram of FeGe thin plates was obtained via pulsed laser excitation. Moreover, by setting the appropriate specimen temperature, the relaxation of chiral magnetic states in FeGe specimens was recorded and analyzed with an Arrhenius-type relaxation mechanism. We present the field-dependent activation energy barriers for chiral state transitions and the magnetic transition pathways of these spin textures for FeGe thin plates. Our results unveil the effects of thermal excitation on the topological spin texture transitions and provide useful information about magnetic dynamics of chiral magnetic state relaxation.

Unravelling the nucleation, growth, and faceting of magnetite-gold nanohybrids.

The chemical synthesis of nanoparticles with a preassigned size and shape is important for an optimized performance in any application. Therefore, systematic monitoring of the synthesis is required for the control and detailed understanding of the nucleation and growth of the nanoparticles. Here, we study Fe3O4-Au hybrid nanoparticles in detail using probes of the reaction mixture during synthesis and their thorough characterization. The proposed approach eliminates the problem of repeatability and reproducibility of the chemical synthesis and was carried out using laboratory equipment (standard transmission electron microscopy, X-ray diffraction, and magnetometry) for typically 10 µL samples instead of, for example, a dedicated synthesis and inspection at a synchrotron radiation facility. From the three independent experimental techniques we extract the nanoparticle size at 12 stages of the synthesis. These diameters show identical trends and good quantitative agreement. Two consecutive processes occur during the synthesis of Fe3O4-Au nanoparticles, the nucleation and the growth of spherical Fe3O4 nanoparticles on the surface of Au seeds during the heating stage and their faceting towards octahedral shape during reflux. The final nanoparticles with sizes of 15 nm Fe3O4 and 4 nm Au exhibit superparamagnetic behavior at ambient temperature. These are high-quality, close to stoichiometric Fe3O4 nanocrystals with nearly volumetric magnetic behavior as confirmed by the presence of the Verwey transition. Understanding the processes occurring during the synthesis allows the nanoparticle size and shape to be adjusted, improving their capabilities in biomedical applications.

Dynamic unidirectional anisotropy in cubic FeGe with antisymmetric spin-spin-coupling.

Strong unidirectional anisotropy in bulk polycrystalline B20 FeGe has been measured by ferromagnetic resonance spectroscopy. Such anisotropy is not present in static magnetometry measurements. B20 FeGe exhibits inherent Dzyaloshinskii-Moriya interaction, resulting in a nonreciprocal spin-wave dispersion. Bulk and micron sized samples were produced and characterized. By X-band ferromagnetic resonance spectroscopy at 276 K ± 1 K, near the Curie temperature, a distribution of resonance modes was observed in accordance with the cubic anisotropy of FeGe. This distribution exhibits a unidirectional anisotropy, i.e. shift of the resonance field under field inversion, of KUD = 960 J/m3 ± 10 J/m3, previously unknown in bulk ferromagnets. Additionally, more than 25 small amplitude standing spin wave modes were observed inside a micron sized FeGe wedge, measured at 293 K ± 2 K. These modes also exhibit unidirectional anisotropy. This effect, only dynamically measurable and not detectable in static magnetometry measurements, may open new possibilities for directed spin transport in chiral magnetic systems.

Biologically encoded magnonics.

Spin wave logic circuits using quantum oscillations of spins (magnons) as carriers of information have been proposed for next generation computing with reduced energy demands and the benefit of easy parallelization. Current realizations of magnonic devices have micrometer sized patterns. Here we demonstrate the feasibility of biogenic nanoparticle chains as the first step to truly nanoscale magnonics at room temperature. Our measurements on magnetosome chains (ca 12 magnetite crystals with 35 nm particle size each), combined with micromagnetic simulations, show that the topology of the magnon bands, namely anisotropy, band deformation, and band gaps are determined by local arrangement and orientation of particles, which in turn depends on the genotype of the bacteria. Our biomagnonic approach offers the exciting prospect of genetically engineering magnonic quantum states in nanoconfined geometries. By connecting mutants of magnetotactic bacteria with different arrangements of magnetite crystals, novel architectures for magnonic computing may be (self-) assembled.

Extracting the Dynamic Magnetic Contrast in Time-Resolved X-ray Transmission Microscopy.

Using a time-resolved detection scheme in scanning transmission X-ray microscopy (STXM), we measured element resolved ferromagnetic resonance (FMR) at microwave frequencies up to 10 GHz and a spatial resolution down to 20 nm at two different synchrotrons. We present different methods to separate the contribution of the background from the dynamic magnetic contrast based on the X-ray magnetic circular dichroism (XMCD) effect. The relative phase between the GHz microwave excitation and the X-ray pulses generated by the synchrotron, as well as the opening angle of the precession at FMR can be quantified. A detailed analysis for homogeneous and inhomogeneous magnetic excitations demonstrates that the dynamic contrast indeed behaves as the usual XMCD effect. The dynamic magnetic contrast in time-resolved STXM has the potential be a powerful tool to study the linear and nonlinear, magnetic excitations in magnetic micro- and nano-structures with unique spatial-temporal resolution in combination with element selectivity.